Effects of acid deposition on 150 forest stands in the Netherlands Input output budgets for sulphur, nitrogen, base cations and aluminium W. de Vries P.C. Jansen Report 69.3 DLO Winand Staring Centre, Wageningen (The Netherlands), 1994 ABSTRACT De Vries, W. and P.C. Jansen, 1994.Effects of acid deposition on 150forest stands in the Netherlands; 3. Input output budgets for sulphur, nitrogen, base cations and aluminium. Wageningen (The Netherlands), DLO Winand Staring Centre. Report 69.3 60 pp.; 12Figs; 21 Tables; 38 Refs; 1 Annex. Input fluxes of sulphur, nitrogen, base cations and aluminium to 148 Dutch forest stands were derived from results of an atmospheric deposition model (sulphur and nitrogen) and by interpolating available data at several weather stations (aluminium and base cations). Output fluxes from the rootzone and the unsaturated zone were obtained by multiplying an estimated precipitation excess for each stand with measured element concentrations in soil solution at 60-100 cm depth (all 148 stands) and in upper groundwater (only 71 stands),respectively. A comparison of input and output fluxes showed that on average sulphur behaved as a tracer whereas nitrogen was strongly retained in the soil. The net acid input was mainly buffered by aluminium mobilization. However, base cations dominated in the soil solution and in groundwater due to large inputs from the atmosphere. Keywords: sulphur, nitrogen, aluminium, budget, soil acidification, eutrophication, weathering ISSN 0927-4537 ©1994 DLO Winand Staring Centre for Integrated Land, Soil and Water Research (SC-DLO), P.O. Box 125, NL-6700 AC Wageningen (The Netherlands). Phone: 31 837074200;fax: 31 837024812. The DLO Winand Staring Centre is continuing the research of: Institute for Land and Water Management Research (ICW), Institute for Pesticide Research, Environment Division (IOB), Dorschkamp Research Institute for Forestry and Landscape Planning, Division of Landscape Planning (LB), and Soil Survey Institute (STIBOKA). No part of this publication may be reproduced or published in any form or by any means, or stored in a data base or retrieval system, without the written permission of the DLO Winand Staring Centre. Project 7241 [Rep69.3.HM/05.94] Contents page Preface 9 Summary 11 1 Introduction 1.1 Input-output budgets for Dutch forests 1.2 Aim of the present research 1.3 Contents of the report 2 Methods 2.1 Choice and characterization of the locations 2.2 Sampling and chemical analysis of soil and groundwater 15 3 Atmospheric deposition 3.1 Sulphur and nitrogen 3.2 Base cations, chloride and aluminium 15 16 17 19 19 22 23 23 25 4 Chemical composition of soil solution and groundwater 4.1 Chloride and sodium 4.2 Sulphur and nitrogen 4.3 Base cations 4.4 Aluminium and pH 27 5 Hydrological conditions 5.1 Precipitation, évapotranspiration and precipitation excess 5.2 Residence time of the percolation water 5.3 Relation between precipitation excess and budgets for chloride and sodium 33 33 34 6 Input-Output budgets 6.1 Budgets of sulphur and nitrogen 6.1.1 The rootzone 6.1.2 The unsaturated zone 6.2 Budgets of base cations and aluminium 6.2.1 The rootzone 43 43 43 45 47 47 27 28 29 30 38 6.2.2 The unsaturated zone 49 7 Discussion and conclusions 53 References Annex On interception and évapotranspiration of the forest stands 55 59 Tables 1 Number of forest stands per tree species where the chemical composition of soil solution and groundwater was measured 20 2 Distribution of the 150 forest stands over soil type 20 3 Distribution of the 150 forest stands over groundwaterlevel class 21 4 Filtering factors for the deposition of S0 4 , N0 3 and NH4 on different types of forests 25 5 Effect of tree species on the median concentration of CI and Na in the soil solution (148 stands) and in upper groundwater (71 stands) 27 6 Effect of tree species on the median Na/Cl ratio in the soil solution (148 stands) and in upper groundwater (71 stands) 28 7 Effect of tree species on the median concentration of S0 4 , N0 3 and NH4 in the soil solution (148 stands) and in upper groundwater (71 stands) 29 8 Effect of tree species on the median concentration of Ca, Mg and Kin the soil solution (148 stands) and in upper groundwater (71 stands) 30 9 Effect of tree species on the median Al concentration and the median pH in the soilsolution (148 stands) and in upper groundwater (71 stands) 31 10 Estimated average spring level for the groundwaterlevel classes occurring at the 148 'soil solution' stands 35 11 Waterretention characteristics of three major soil types in the 148 soil solution stands 35 12 Estimated watercontent in the rootzone (0-80 cm below the soil surface) and the unsaturated zone (75 cm below the spring groundwaterlevel) of three major soil types in the 148 soil solution stands 36 13 Estimated residence times of percolation water in the rootzone and unsaturated zone as a function of tree species, soil type and groundwaterlevel class 36 14 Wet deposition of major ions in De Bilt (RIVM/KNMI, 1988) 37 15 Actual évapotranspiration and precipitation excess of the tree species occurring at the 148 'soil solution' stands and the 71 'groundwater' stands 40 16 Median annual deposition (in), leaching (out) and their difference (in-out) of CI and Na for the rootzone and the unsaturated zone for different tree species1* 41 17 Median annual deposition (in), leaching from the rootzone (out) and their difference (in-out) of S0 4 , N, N0 3 and NH4 for the tree species occurring at the 148 'soil solution' stands 45 18 Median annual deposition (in), leaching from the unsaturated zone (out) and their difference (in-out) of S04, N, N0 3 and NH4 for the tree species occuring at hte 71 'groundwater' stands 47 19 Median annual deposition (in), leaching from the rootzone (out) and their difference (in-out) of Al, K, Ca and Mg for the tree species occurring at the 148 'soil solution' stands 49 20 Median annual deposition (in), leaching from the unsaturated zone (out) and their difference (in-out) of AI, K, Ca and Mg for the tree species occurring at the 71 'groundwater' stands 51 21 Summary of the net budgets (input-output) of major ions for the rootzone and unsaturated zone 54 Figures 1 Distribution of sampling locations over the Netherlands 21 2 Inverse cumulative frequency distributions of the total deposition of S0 4 (A), N (B), NH4 (C) and N0 3 (D) on the forest stands where the chemical composition of soil solution (148) and groundwater (71) was measured 24 3 Inverse cumulative frequency distributions of the bulk deposition of CI (A), Na (B), Ca (C) and Mg (D) on the forest stands where the chemical soil (148) and groundwater composition (71) was measured 26 4 Inverse cumulative frequency distributions of the calculated precipitation excess of the tree species occurring at the 148 'soil solution' stands 34 5 Wet CI deposition in Eelde in 1989 and 1990 37 6 Wet S0 4 deposition in Eelde in 1989 and 1990 38 7 Inverse cumulative frequency distributions of the deposition and leaching of CI (A) and Na (B) from the rootzone at the 148 'soil solution' stands 39 8 Inverse cumulative frequency distributions of the deposition and leaching of CI (A) and Na (B) from the unsaturated zone at the 71 'groundwater' stands 39 9 Inverse cumulative frequency distributions of the deposition and leaching of S0 4 (A), N (B), N0 3 (C) and NH4 (D) from the rootzone at the 148 'soil solution' stands 44 10 Inverse cumulative frequency distributions of deposition and leaching of S0 4 (A), N (B), N0 3 (C) and NH4 (D) from the unsaturated zone at the 71 'groundwater' stands 46 11 Inverse cumulative frequency distributions of the deposition and leaching of Al (A), K (B), Ca (C) and Mg (D) from the rootzone at the 148 'soil solution' stands 48 12 Inverse cumulative frequency distributions of the deposition and leaching of Al (A), K (B), Ca (C) and Mg (D) from the unsaturated zone at the 71 'groundwater' stands 50 Preface To examine the impact of atmospheric deposition on non-calcareous soils of Dutch forests, a survey of the chemical soil and soil solution composition below 150 forest stands, including seven major tree species, was carried out by the DLO Winand Staring Centre. This research was financially supported by the Ministry of Agriculture, Nature Management and Fisheries and the Ministry of Housing, Physical Planning and Environment of the Netherlands. The results of the research are presented in four reports with the common title: Effects of acid deposition on 150forest stands in the Netherlands, with the following subtitles: 1 Chemical composition of the humus layer, mineral soil and soil solution; 2 Relationships between forest vitality characteristics and the chemical composition of foliage, humus layer, mineral soil and soil solution; 3 Input output budgets for sulphur, nitrogen, base cations and aluminium; 4 Predictions of the chemical composition of foliage, mineral soil, soil solution and groundwater on a national scale. In this report, number 3,results are given of element budgets for both the rootzone and the unsaturated zone. In this context, use was made of research results on the quality oftheupper groundwater at 71 of these sites assessed bythe National Institute of Public Health and Environmental Protection. We thankfully acknowledge all colleagues who assited in site characterisation and soil sampling i.e. A.H. Booy, D. Eilander, H. van het Loo, P. Mekkink and R. Zwijnen, in analyzing the various soil samples, i.e. M.M.T. Meulenbrugge, A. Louwerse and W. Balkema, and in dataprocessing, i.e. J.C. Voogd. Furthermore, we thank Ir.L.J.M. Boumans and Dr. J.W. Erisman of the National Institute of Public Health and Environmental Protection who supplied us the data on chemical groundwater composition and atmospheric deposition of sulphur and nitrogen, respectively. Summary The aim of this report is to give a rough estimate of input-output budgets for S, N, (NH4, N0 3 ), Ca, Mg, K, Na and Al, of Dutch forest soils based on a nation-wide assessment of deposition and leaching data. Nearly all former research activities on input-output budgets have been limited to a number of intensively monitored forest sites. To gain insight in element leaching a national assessment has been made of the chemical composition of the soil solution and phreatic groundwater of forest ecosystems. The chemical composition of the phreatic groundwater was determined by the National Institute of Public Health and Environmental Protection. The study concerned the quality of the upper groundwater at 156 sites with forests or a heather vegetation on sandy soils. The samples were taken per grid of 0.5 x 0.5 km. In each grid 10 watersamples were taken every 50 meters along a transect. Samples were withdrawn from a tube, placed till one meter below the groundwater table, of which the last 0.5 m was perforated The sampling took place in the period 1 October 1989 15 april 1990. The RIVM locations were used for the selection of 150 sites for soil moisture sampling by the DLO Winand Staring Centre. Sites were restricted to major tree species (Scots pine, black pine, douglas fir, Norway spruce, Japanese larch, oak and beech) on non-calcareous soils. Soil samples, from which the soil moisture was withdrawn, were taken of the mineral (top)soil layer (0-30 cm) and the (sub)soil layer (60-100 cm). Per location the sample of each mineral layer consisted of a composite sample of 20 subsamples. The soil was sampled in 1990 in the period February 15 to May 16. This period is supposed to be representative for the annual flux weighted solute concentration. Only 71 of the sites coincided with sites where groundwater was sampled as well. The budgets of the elements were derived by subtracting input (deposition) and output (leaching). S 0 4 and N (NH 4 , N0 3 ) deposition values were obtained from the results of a model for 5 km x 5 km grids for 1989, multiplied by filtering factors since the deposition of these ions on forests is higher due to filtering activity. Bulk deposition data of 22 weatherstations for the period 1978 -1986 were used to estimate the bulk deposition of Ca, Mg, Na, K and Cl. Based on the ratio between Na in throughfall and bulk deposition the total deposition of base cations and CI on the forest stands was calculated. Leaching of elements from the rootzone and unsaturated zone respectively, was calculated by multiplying element concentrations in the layer 60-100 cm and in groundwater with the precipitation excess. Compared to the layer 60-100 cm, concentrations in the upper groundwater were generally lower for NH 4 , N 0 3 CI, Ca, K, Na, Al and H (increased pH), whereas it was nearly comparable for S 0 4 and Mg. The precipitation excess was calculated by subtracting the interception and the actual évapotranspiration of each type of forest from the precipitation of the gridcell in which the site is situated. For the precipitation the average of the 30 years period 1950-1980 was used. Interception was calculated as a percentage of the precipitation. 11 To investigate whether the measured concentration of the soil solution represents an average annual concentration, the expected residence time of soil water was calculated for the various tree species as a function of soil type, by dividing an estimated moisture content in the rootzone, by the estimated precipitation excess. Since the estimated residence times for water in the rootzone were mostly less than one year, especially for the deciduous trees, we investigated how the precipitation excess should be adjusted such that the median CI deposition coincided with the median CI leaching for each of the seven tree species. This caused a remarkable decrease in the average precipitation excess of Japanese larch, beech and oak, i.e. the tree species where concentrations are likely to deviate from annual average values due to short residence times. In order to obtain reliable leaching fluxes adjusted precipitation excesses were thus used for the rootzone whereas original values were used for the unsaturated zone. For all stands the S0 4 budget was -29 molc ha"1yr"1in the rootzone and -186 molc ha* yr* in the unsaturated zone. Overall S0 4 thus seems tobehave like atracer. The estimated large leaching under oak is likely to be unreliable due to lateral seepage. The median leaching of N from the rootzone (834 molc ha* yr"1) was reduced by 80% compared to the median N deposition (4159 molc ha"1yr"1). The contribution of N0 3 to the deposition of Nwas relative small (971 molcha"1yr"1).However, the median leaching of N0 3 (700 molc ha"1 yr"1) almost equalled the median N0 3 deposition. NH4 contributes most to the deposition of N (3188 molc ha"1 yr"1), but a lot of it disappeared due to (preferential) uptake and nitrification. The median net retention was 3054 molc ha_1yr"1.The output fluxes of N from the unsaturated zone were generally smaller than from the rootzone. NH4 almost disappeared and the leaching of N0 3 was also less than at the depth of the rootzone (490 molc ha"1yr"1). Together 90% disappeared as compared to the deposition. Thedeposition of Al is neglectable.Therefore the entire leaching of this ion is caused by Al mobilization. Al leaching from the rootzone was relatively small (less than 1000molc ha"1yr_1)below deciduous trees, including Japanese larch and relatively large for coniferous trees, especially douglas fir (more than 2000 molc ha! yr"1).For all stands the median mobilization was 976 molc ha"1 yr_1. Al leaching from the unsaturated zone was nearly similar, i.e. a median mobilization of 1054 molc ha"1 yr"1.Leaching of K, Ca and Mg was mostly larger than the deposition of these ions, because of weathering and ion-exchange. Median values for the net mobilization of K, Ca and Mg in the rootzone and the unsaturated zone were 221 and 253 molc ha"1yr"1,which is close to the average weathering rate of non-calcareous sandy soils in the Netherlands. Striking was the large mobilization of Ca and Mg under oaks, butthis is likely tobe influenced by seepage since most oak stands occurred on wet sites. From this study we concluded that in Dutch forest soils (i) S0 4 generally behaves like a tracer, (ii) N is still largely retained and complete N saturation hardly occurs yet, (iii) Al mobilization is the major buffermechanism in the soil, whereas base cation input from the atmosphere largely neutralizes S0 4 and N0 3 input and (iv) the acidification (Al mobilization) is much larger below coniferous trees, especially 12 douglas fir and Norway spruce, than below deciduous trees (including the Japanese larch). 13 1 Introduction Impacts of elevated deposition levels of SOx, NOx and NHX on the chemical composition of forest soils, and its effect on forest vitality, has received much attention in the Netherlands during the last decade (Heij and Schneider, 1991). Impacts of atmospheric deposition on the soil have been derived by the determination of input-output budgets of major ions, i.e. sulphate (S04), nitrate (N03), ammonium (NH4), aluminium (Al), base cations (Ca, Mg, K, Na) and protons (H). This was done to gain insight in (1) the fate of S and N in the ecosystem and (2) the buffermechanism in the soil to neutralize the acid input associated with it. However \ nearly all research activities havebeen carried out on a limited number of intensively Imonitored forest sites.These sites are not representative for Dutch forest regarding jj deposition level, stand characteristics such as tree species and site characteristics Isuch as soil type. The aim of this report is to give rough estimates of input-output "budgets for S, N,Ca, Mg, K, Na and Al of major tree species based on a nation-wide assessment of deposition and leaching data. 1.1 Input-output budgets for Dutch forests f «A .1* Research on soil acidification and N accumulation at various forest sites in the Netherlands has mainly been carried out within the Dutch Priority Program on Acidification that started in 1985.An overview of the results of seventeen budget studies thus carried out has been given in Van Breemen and Verstraten (1991). Research results include nine intensively and eight extensively monitored sites. In the intensively monitored sites input fluxes were derived from fortnightly or monthly measurements of the chemical composition of throughfall water, multiplied by the throughfall flux. Output fluxes were derived by multiplying monthly measurements of the soil solution composition at various depths with simulated unsaturated soil water fluxes (Van Grinsven et al., 1987). In the eight extensively monitored sites (all douglas stands) input fluxes were also derived from monthly measurements of throughfall (Kleijn et al., 1989).However, the soil solution composition was only measured four times i.e. inJune, september and december 1986 and in april 1987. Unlike the intensively monitored sites, where the soil solution was extracted with porous cups permanently installed in the field, soil solution was extracted by centrifugation from a previously sampled soil.This was done to enable measurements in mid-summer and to put more emphasis on spatial variability inthe field. Results on the soil and soil solution composition have been given in Kleijn and De Vries (1987) and Kleijn et al. (1989).Output fluxes were derived by multiplying the annual average precipitation excess for these stands (Reurslag et al., 1990) by the soil solution composition measured in april. This was done since analyses of the data of several intensively measured sites indicated that the concentration in early spring (march, april) is generally most representative for the annual flux weighted solute concentration. i M, 15 Results showed that the average S0 4 input equalled the average S0 4 output, suggesting that the forests are sulfur-saturated. N saturation occurred at five sites. On average about 1.5kmol (± 20 kg) N ha"1yr"1was removed from the soil, either by uptake or denitrification, or retained in organic matter by immobilization. Furthermore, on average 70% of the amount of S0 4 and N0 3 leaching from the system was accompanied by Al, indicating that Al mobilization is a major buffermechanism in non-calcareous sandy forest soils in the Netherlands (Van Breemen and Verstraten, 1991; Heij et al., 1991). The dominating role of Ali *, mobilization in the investigated forest sites was due to the low base saturation of rJ' ! the adsorption complex (nearly always less than 20%).Laboratory experiments with ?l ,J*- V -!s o ^ s a m p l e s from these sites showed that the Al-pool responsible for buffering was "9V V ^ ' i V- ff" * m a m l y limited to organically bound Al and amorphous Al-hydroxides (Mulder et «j/* s j, | al., 1989).This implies that major physio-chemical soil changes are presently taken -® * place by the depletion of this limited pool. J "if I ,¥* 1.2 Aim of the present research Soil acidification research conducted sofar has greatly increased ourknowledge about the present impact of atmospheric deposition on non-calcareous sandy forest soils. However the sites that were studied are not representative for the Dutch forests. First of all, most sites were located in areas with intensive animal husbandry with a bias towards high N loads. Secondly, the tree species studied was mainly douglas fir, since the Dutch Priority Program on Acidification was particularly focused on this tree. However douglas fir isnot representative for needleforest asfar as hydrological characteristics are concerned. The high needle amount (and canopy coverage) causes a large rate of interception evaporation thus increasing soil solution concentrations due to low water fluxes (De Vries and Kros, 1989).It also causes a relatively large input of elements by dry deposition. Finally, both soil type and groundwater level of most intensively studied sites are not representative for sandy forest soils in the Netherlands. They are either too loamy or too wet. In order to overcome the various limitations of the research carried out so far a national assessment has been made of the chemical composition of the soil solution and phreatic groundwater of forest ecosystems. The soil solution composition was measured in 150stands for seven major tree species (Scots pine, black pine, douglas fir, Norway spruce, Japanese larch, oak and beech) on non-calcareous sandy soils. The limitation to these soil types is because they are most sensitive to N accumulation and most Dutch forests (about 85%) are located on these soiltypes (De Vries et al., 1989). Forest vitality characteristics were known for the stands as they are part of the forest vitality study by the State Forestry Service (e.g. IKC-NBLF, 1992). ^ <^- j The chemical composition of the phreatic groundwater was determined by the 1 National Institute of Public Health and Environmental Protection. The study »Kxj concerned the quality of the upper groundwater at.156 sites with forests or aheather V y** vegetation on sandy soils. 71 of these sites coincided with sites where soil moisture was sampled. 16 I J i JMajor aims of the research are the determination of the regional variability in soil Iand soil solution composition in relation to deposition level, stana^cTîaracteristics |and site characteristics. Results thus obtained are given in De Vries and Leeter§ _;* WlJA (1993). Another important aim was the assessment of a relationship between soil and soil solution composition and forest vitality characteristics for major tree species ^ as reported in Hendriks et al. (1993). Here we report the results of input-output budgets for sulphur, N, Al and base cations of the 150 forest stands and apart also of the 71 stands where moisture and groundwater was analyzed. This was done to gain insight in the influence of deposition level and tree species on element budgets. Element budgets for the rootzone and the unsaturated zone were calculated by subtracting the output (leaching) fluxes at the bottom of these zones from the input (deposition) fluxes via the surface. Output fluxes were obtained by multiplying the concentration of the elements in the soil moisture and upper groundwater with the precipitation excess. 1.3 Contents of the report A description of the methods that were used to gain insight in the soil and groundwater quality below forest stands is given in chapter 2. This includes the selection of the locations, and the sampling procedure and chemical analyses of soil moisture and upper groundwater. The input (deposition) fluxes of the different ions are given in chapter 3. The chemical composition of the soil solution and groundwater and the precipitation excess, which form the basic information to derive the output fluxes, are given in chapters 4 and 5, respectively. In chapter 5 the relation of the precipitation excess with the budgets of CI and Na is also discussed because it is assumed that the waterbalance and the balances of the inert ions CI and Na matches. In chapter 6 the final results are given, i.e. the input- output budgets, of S, N, base cations and Al for the rootzone and the unsaturated zone. Finally conclusions and a discussion are given in chapter 7. 17 f • — » i' ,ï Hj 2 Methods 2.1 Choice and characterization of the locations Choice In infiltration areasthe chemical composition of soil moisture and groundwater under forests is largely determined by the quantity and quality of the precipitation that infiltrates via the surface and the interaction with the soil and the vegetation. Stand characteristics such as tree species, canopy coverage, structure of the stand, height of the trees and position and distance to the edge are of major importance for the 1 the total deposition on forest and precipitation excess of forests. In choosing the locations, allowance for these factors was made in order to isolate their influences. \t f$ To select locations for groundwater sampling, RIVM used adatabase of 0.5 km x 0.5 km grids, containing information about soil use and the total N deposition. The atmospheric Ndeposition was calculated by using the TREND model (Van Jaarsveldf and Onderdelinden, 1993).It"was"sïïppösedTthat the soil use causes differences in the emission and deposition of N. Taking into account that grids had to be representative for the Netherlands and that they had to show as much as possible differences inN deposition levels, 168locations were selected. Preferentially, sites were chosen where throughfall was monitored orwhere the vitality of thetrees was established in 1988 and/or 1989.More information on the selection procedure has been given by Boumans and Beltman (1991). The RIVM locations formed the starting-point for the selection of 150sites for soil moisture sampling by the DLOWinand Staring Centre. However, some additional requirements that were made,i.e. restriction to major tree species (Scots pine, black pine, douglas fir, Norway spruce, Japanese larch, oak and beech) and ensuring a large range in soil type and groundwater level caused that only 89 of the 150 locations that were selected coincided withRTVMlocations.More information onthe selection procedure has been given by de Vries and Leeters (1993). Of the 89 locations that are in common 18 were dropped when processing the data, mostly because other tree^srjecies dominated at the transect alonjgjwhkhj^yj^sampled the groundwater. Furthermore, tKë*chemical corlposition of the soil solution of two locations was doubtful. V^. ^ r € K JÙfa^4ÊfhÂ^ * * * * c6 ***'*» 6 Table 1gives an overview of the distribution of the tree species over the locations and Figure 1 gives the distribution of the locations over the Netherlands. "«*i e? Characterization Site characteristics, such as soil type and groundwaterlevel, and stand characteristics, such as canopy coverage, tree height, distance to -and soil use at the edge of the forest and the presence of forest roads were listed. Results on the distribution of the tree species over soil type and groundwaterclass are given in Table 2and 3. The complete dataset and acomprehensive description of the sampling procedure has been given by De Vries and Leeters (1993). 19 Table 1 Number offorest stands per tree species where the chemical composition of soil solution and groundwater was measured Tree species Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech Number of stands Soil solution Groundsrater1' original dropped final original 442) dropped final 15 15 30 15 0 0 0 1 0 1 0 44 15 16 14 15 29 15 23 10 10 11 11 22 2 5 1 1 1 2 7 1 18 9 9 10 9 15 1 150 2 148 89 18 71 15 162> " At these sites the chemical soil solution composition was measured as well. 2) At one stand the major tree species appeared to be Douglas fir instead of Scots pine (as expected). Table 2 Soil type Distribution of the 150forest stands over soil type Number of stands Scots pine Haplic Arenosol1) 14 Gleyic Podzol2) 21 Cambic Podzol 9 Fimic Anthrosol 1 0 Umbric Gleysol3' 0 fDystric Gleysol Black pine Douglas Norway Japanese Oak fir spruce larch Beech 6 9 0 0 0 0 1 7 3 3 1 0 0 7 2 2 3 1 0 11 0 0 3 0 0 13 1 1 0 0 3 10 2 3 7 4 i „ l^ u " Including Gleyic Arenosols 2) *,;',}-• Including Carbic Podzols e 3) I ' Including organic rich soils Most tree species occurred on Gleyic and Carbic Podzols, especially Norway spruce and Japanese larch and to a lesser extent on Arenosols. Scots pine and black pine occurred almost exclusively onthese 'nutrient-poor' soiltypes.Douglas fir has greater needs for nutrients (and moisture) and occurred more often on 'nutrient-rich' soil types such as the Cambic Podzol and Fimic Anthrosol. Oak and beech occurred on nearly all soil types (cf Table 2). Table 3 showsthatthe coniferous trees mainly occurred on well-drained soils whereas the deciduous trees also occurred relatively often on poorly-drained soils. In these soils removal of N by denitrification may play an important role. 20 A Ç=^ soil solution stands A [ soil solution and groundwater stands Fig. 1 Distribution of sampling locations over the Netherlands Table 3 Distribution of the 150forest stands over groundwaterlevel class Groundwaterlevel Number of stands ciass II+III V IV+VI VII Scots pine Black pine Douglas Norway Japanese Oak fir spruce larch 2 5 3 35 0 2 2 11 1 0 3 11 1 1 6 6 1 0 3 11 4 5 11 9 Beech 2 2 2 9 21 2.2 Sampling and chemical analysis of soil and groundwater p t)A ^ç Sampling The soil was sampled in the period 15february 1990 - 16 may 1990. This period is based on results of the intensive soil solution in Hackfort (van Breemen et al., 1988). Results indicated that the concentration in early spring (march, april) is generally most representative for the average annual flux weighted solute concentration. Soil samples were taken of the humus layer and three mineral soil layers, i.e. 0-30 cm, 30-60 cm and 60-100 cm. Samples of each mineral layer consisted of one composite sample of 20 subsamples. The sample points were chosen along a steady pattern in a square of 20x 20meters inthe middle of the forest stand. Soil moisture, was withdrawn from the samples of twomineral layers ,i.e. 0-30 cm and 60-100 cm. Phreatic groundwater was sampled by the RIVM per grid of 0.5 km x 0.5 km. In each grid 10 samples were taken every 50 meters along a transect in the biggest united area of forest and other nature grounds (heather). When the transect turned to be shorter than 450 meters, the remaining samples were taken along the middle leadline of the transect. At least 3 groundwater samples were taken in a forest stand where the vitality was observed and where the DLO Winand Staring Centre also collected soil samples. Sampling took place in the period 1October 1989 - 15 april 1990.At each sampling site a hole was bored till one meter below the water table in which a tube was placed of which the last 0.5 mwas perforated. The water-sample was withdrawn from the tube.Detailed information has been given by Boumans and Beltman (1991). Chemical analysis Soil moisture was released from the soilsamples by using acentrifugation method. Next the water waspressed through afilter with aporesize of 0.45um and the acidity (pH) and electric conductivity was measured. In diluted samples the concentrations of Si,Al,Fe,Ca,Mg, K, Na,NH4, N03, Cl, S0 4 , H2P04 and dissolved organic carbon (DOC) were measured (cf. de Vries and Leeters, 1993). The groundwater samples were sucked by vacuum through a filter with a poresize of 0.2 mm within 24 hours after sampling. Next the water was analyzed for AI, Ca, Mg, K, Na, NH4, N0 3 , S0 4 , Cl, DOC, electric conductivity and acidity (cf. Boumans and Beltman, 1991). 22 3 Atmospheric deposition Human activities cause an increase of the deposition of particular sulphur and N, while other ions, like Cl,Na and Mg are strongly influenced by the distance to the sea. Next to this,considerable changes in deposition can occur at short time intervals, mainly due to the variability of the precipitation and the direction and velocity of the wind. W1 fc; J'. W** iJ 3.1 Sulphur and nitrogen " ' ddM^ The concentration of NHX,NOx and SOx that was measured at several weather stations and stations of the National Air Quality Monitoring/Network formed the inception for an empirical model (Erisman, 1991) through vWiichthe wet and dry deposition of these elements for 5km x 5km grids was calculated. Results for 1989,the year preceding the sampling of the soil moisture and groundwater (Erisman, 1991) were recalculated to averages for 10km x 10km grids since data for thebase cations were available on this gridsize (cf Section 3.2). Cumulative frequency diagrams of the total deposition of sulphur (S04) and nitrogen (NH4and N0 3 ) on the 148 stands where soil moisture and the 71 stands where also the upper groundwater was sampled, are given in Figure 2. The frequency distribution of the 71 stands agreed quite well with that of the 148 stands, which means that the distribution of both groups over the Netherlands isfairly similar (cf Figure 1).Only the number of stands with a high deposition level of N0 3 is under-represented in the group with 71 stands. High deposition levels of N0 3 are mostly found near industrial zones.The cumulative frequency distribution of S0 4 deposition shows that at 50% of the locations the deposition lies between 1000 and 1200 molc ha_1yr"1. Those locations are situated in the northeastern part of the Netherlands. At the other locations the deposition is greater, up to 2000 molc ha"1 yr"1. The NHX deposition varied from 1500up to 5000 molc ha"1yr"1, with the highest amounts in areas with intensive animal husbandry. The range in the NOx deposition at more than 90 %of both groups of locations is small and lies between 1050 and 1250 molc ha"1yr"1. The deposition given in Figure 2 equals the total average deposition on the gridcells where the forest stands are situated. However, the deposition of most ions on forests is higher due to filtering activity. To account for this effect, total deposition values weremultiplied byfiltering factors (Table 4).Thesefactors were taken from DeVries (1991) who derived these data by comparing throughfall data in42 forested stands with deposition estimates derived by the TREND model. 23 Cumulative frequency Cumulative frequency (*) 71stands 1000 1250 1500 1750 2000 2000 2500 3000 3500 4000 4500 5000 Ndeposition (mol.ha1.yr1 ) S0 4 deposition (mol.ha' .yr' ) Cumulative frequency Cumulative frequency (%) D 148stands 71stands 1000 2000 3000 4000 5000 NH< deposition (moLha' .yr' ) 1000 1100 1200 1300 1400 1500 N0 5 déposition (mol.ha' .yr'1 ) Fig. 2 Inverse cumulative frequency distributions of the total deposition of S04 (A), N (B), NH4 (C) and N03 (D) on theforest stands where the chemical composition of soil solution (148) and groundwater (71) was measured 24 Table 4 Filtering factors for the deposition of SO^ N03 and NH4 on different types of forests Forest type Scots pine, Black pine Douglas fir, Norway spruce Japanese larch, Oak, Beech Filtering factor (-) so 4 N03 NH4 1.40 1.60 1.15 0.85 1.00 0.70 1.30 1.50 1.10 3.2 Base cations, chloride and aluminium At several places in the Netherlands the quality of theprecipitation is measured. From these data the average concentration of several elements, including base cations and CIwas calculated for theperiod 1978-1986 (KNMI/RIVM, 1988).These data were used to estimate the bulk deposition of calcium (Ca),magnesium (Mg), sodium (Na), potassium (K) and chloride (CI) for grids of 10 km x 10 km, using interpolation techniques (De Leeuw, RIVM,pers.comm.).The bulk deposition includes the wet deposition and the soluble fraction of the dry deposition ontheprecipitation collector. Cumulative frequency diagrams of the bulk deposition of CI,Na, Ca and Mg on the 148 stands where soil moisture was sampled and the 71 stands where also the upper groundwater was sampled, are given in Figure 3.The deposition of Alis negligible and of K very small (in most stands 30 molc ha"1yr"1) and therefore not given. As with N and Sthe frequency distribution of the 71 stands agreed quite well with that of the 148 stands.The bulk deposition of CIis high; in 10%of the stands even 1000-2000 molc ha"1yr"1.These are all situated in the northern province Friesland. Thedeposition decreases in south eastern direction. These differences are connected with the distance to the sea. The same sea spray effect explains the differences in Na and Mg deposition. The Na deposition differs from 300 to 1300 molc ha"1yr"1 with a median of 650 and the Mg deposition from 80 to 350 molc ha"1yr"1 with a median of 140.The highest deposition-rates of Ca are not only found near the coast, but also in the extreme south of the Netherlands due to occurence of limestone quarries. In the middle and in the northeastern part, where about 50 %of the stands are situated, the Ca deposition is less than 200 molc ha_1 yr"1. The deposition of K is small, in most stands 30 molc ha_1yr"1. The total deposition of base cations on forests is mostly much higher than the bulk deposition, especially near forest edges (Draaijers et al., 1992).It also depends on the tree species, density and height of the forest (Stuijfzand, 1984;Verstraten et.al., 1984). Insight in the effect of dry deposition can be derived from the ratio between Na in throughfall and bulk deposition assuming that canopy interactions for Na are negligible, i.e. throughfall equals total depostion (Bredemeier, 1988).Using data on Na in throughfall and bulk deposition in 42 forests, de Vries (1991) derived a ratio of 2.0 for Japanese larch, oak andbeech; 2.5 for black pine and Scots pine and 2.75 for Norway spruce and douglas fir. Total deposition of base cations and CIon each forest stand was thus calculated by multiplying the bulk deposition with these factors. 25 Cumulative frequency Cumulative frequency (ft) (ft) B 7Islands 500 1000 500 1500 1000 1500 J Nadeposition (mol.ha' .yr ) Cldeposition (mol.ha' .yr' ) Cumulative frequency Cumulative frequency (%) (ft) D 71 stands 200 250 300 Cadeposition (molc.ha"'.yr ' ) 71stands 50 100 150 200 250 300 Mgdeposition (moLha' .yr'' ) Fig. 3 Inverse cumulative frequency distributions of the bulk deposition of CI (A), Na (B), Ca (C) and Mg (D) on theforest stands where the chemical soil (148) and groundwater composition (71) was measured 26 4 Chemical composition of soil solution and groundwater Leaching of elements from therootzone andunsaturated zone, respectively,was calculated bymultiplying the element concentration inboth compartments withthe precipitation excess. Regarding theelement concentration, data were availablefor the soil solution inthelayers 0-30cmand60-100 cmin spring 1990 andfor the groundwater intheupper 50-100 cmbelow thephreatic surface in autumn1989. Soil solution data forthe layer 60-100 cm were used tocalculate leaching fromthe rootzone, whereas thegroundwater data were used todothe same for thewhole unsaturated zone. It wasassumed that theelement concentrations in the various periods equalled theflux weighed average annual concentration (cf. section2.2). For groundwater this islikely tobeabetter assumption than forthesoil solution which varies considerable over the year dueto seasonal differences in litterfall, deposition, hydrology, etc. This aspect isfurther elaborated inChapter5. 4.1 Chloride and sodium Table 5gives themedian CIandNa,concentrations fortheentire data setand for singletree species.The concentration insoil moisture was much higherthaninupper groundwater. For CIthe concentration difference between soil moisture at60-100 cm and upper groundwater varied from afactor 1.1(beech) upto3.1 (Norway spruce) and forNafrom 1.0 (beech) to2.3(black pine). These differences imply thatthe CIand Na concentrations donot represent the annual average concentration either in soil moisture below therootzone orinthe groundwater orinboth compartments. This problem isdiscussed further inchapter 5.2, where water- and CIbalancesare compared. Table 5 Effect of tree species on the median concentration of CIand Na in the soil solution (148 stands) and in upper groundwater (71 stands) Tree species CI concentration (molc m • 3 Na concentration (molcm :3) ) 0-30cm 60-100 cm groundwater 0-30 cm 60-100cm groundwater Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech 1.10 (0.95)1' 1.15 (0.86) 2.32 (1.89) 1.89 (1.80) 1.63 (1.35) 1.03 (0.93) 1.06 -2> 0.88 (0.87) 0.84 (0.84) 1.58 (1.58) 1.99 (1.74) 1.25 (1.22) 1.07 (0.93) 1.07 -2) 0.38 0.35 0.62 0.64 0.59 0.72 0.99 0.70 (0.64) 0.73 (0.61) 1.26 (1.25) 1.15 (1.02) 0.97 (0.74) 0.70 (0.55) 0.69 -2) 0.69 (0.69) 0.69 (0.69) 1.17 (1.18) 1.13 (0.94) 0.87 (0.84) 0.72 (0.59) 0.83 -2) 0.35 0.30 0.60 0.53 0.56 0.61 0.80 Total 1.29 (1.15) 1.06 (1.06) 0.58 0.77 (0.74) 0.78 (0.72) 0.51 Values between brackets are median concentrations at the 71locations where the groundwater composition was measured aswell Not enough data 27 The difference in concentration between the various tree species was considerable. The CIand Na concentration was high in soil moisture under douglas fir and Norway spruce, which is explainable by the small precipitation excess and therelatively high deposition. The opposite is expected for deciduous trees and the needle-loosing Japanese larch. However, the CI and Na concentration under the pine forests was much smaller. In the groundwater even much lower concentrations were found. CIis an almost inert element apart from a small uptake by the vegetation. Na is also relatively inert, although it can take part in weathering and cation exchange. Consequently, the (soil solution) concentration of both ions is expected to be related to the precipitation excess and the deposition. The ratio between Na and CI in sea water is about 0.86. TheNa/Cl ratio's were lower in soil moisture and groundwater especially in the upper layer whereas a similar ratio (median of 0.88) was found for groundwater (Table 6). Apparently CI recycles via uptake and litterfall and/or Na plays a role in the ion exchange, in particular in the upper layer. However, these two processes cannot really explain the relatively low ratios in the subsoil. Table 6 Effect of tree species on the median Na/Cl ratio in the soil solution (148 stands) and in upper groundwater (71 stands) Tree species Na/Cl ratio (-) 0-30 cm 1 60-100 cm groundwater Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech 0.64 (0.67) ' 0.63 (0.71) 0.54 (0.66) 0.61 (0.57) 0.60 (0.55) 0.68 (0.59) 2) 0.65 0.78 (0.79) 0.82 (0.82) 0.74 (0.75) 0.57 (0.54) 0.70 (0.69) 0.67 (0.63) 2) 0.78 0.92 0.86 0.97 0.83 0.95 0.85 0.81 Total 0.60 (0.64) 0.74 (0.68) 0.88 11 2) Values between brackets are median ratios at the 71 locations where the groundwater composition was measured as well Not enough data 4.2 Sulphur and nitrogen In Table 7 the median concentration of S0 4 , N0 3 and NH4in the soil solution and upper groundwater are given. The S0 4 concentration at different depths was rather stable for most tree species. Only douglas fir andNorway spruce showed a decreasing concentration. Furthermore, it is striking that the median S0 4 concentration in the layer 60-100 cm was exceptional high at the oak-locations where the groundwater composition was measured as well. 28 Table 7 Effect of tree species on the median concentration of SO^ N03 and NH4 in the soil solution (148 stands) and in upper groundwater (71 stands) Tree species S 0 4 concentration (molc m"3) 0-30 cm 60-100 cm Scots pine 0.97 (1.04)1* Black pine 0.81 (0.77) Douglas fir 2.45 (1.53) Norway spruce 1.99 (1.92) Japanese larch 1.01 (0.76) Oak 0.81 (0.75) Beech 0.63 - 2) 1.00 (1.12) 0.90 (0.88) 1.81 (1.11) 1.78 (1.78) 0.94 (0.87) 1.22 (2.18) 0.94 - 2) Total 1.10 (1.08) 0.97 (0.97) N 0 3 concentration (molc m"3) ground- 0-30 cm 60-100 cm groundwater water 0.93 0.48 (0.42) 0.53 (0.59) 0.49 0.70 0.30 (0.25) 0.34 (0.25) 0.14 0.95 0.93 (0.88) 1.28 (1.20) 0.79 1.20 0.48 (0.44) 0.47 (0.41) 0.16 0.92 0.65 (0.59) 0.49 (0.47) 0.21 1.04 0.57 (0.64) 0.26 (0.25) 0.12 1.14 0.20 - 2) 0.17 - 2) 0.00 1.04 0.53 (0.54) 0.48 (0.53) 0.24 NH4 concentration (mol m'3) Scots pine 0.21 (0.22) Black pine 0.19 (0.19) Douglas fir 0.61 (0.47) Norway spruce 0.47 (0.45) Japanese larch 0.22 (0.22) Oak 0.12 (0.12) Beech 0.14 -2) 0.10 (0.09) 0.10 (0.11) 0.10 (0.09) 0.08 (0.09) 0.09 (0.10) 0.07 (0.07) 0.09 -2) 0.00 0.00 0.00 0.00 0.00 0.00 0.00 Total 0.09 (0.09) 0.00 11 2) 0.18 (0.20) Values between brackets are median concentrations at the 71 locations where the groundwater composition was measured as well Not enough data The NH4 concentration decreased with depth, most likely due to uptake and nitrification. In the upper groundwater NH4 completely disappeared. The N0 3 concentration increased between the layers 0-30 and 60-100 cm under stands of pine and (Douglas) fir, but decreased,just like the other stands,on its way to groundwater. This might be due to denitrification. 4.3 Base cations The median Ca, Mg and Kconcentrations are given in Table 8. Except for oak, the Ca concentration decreased with depth. Apparently, deeper in the soil profile Ca is absorbed and probably exchanged by Al. The increase in Ca concentration under oak stands, which is sometimes 3-5 times greater in upper groundwater than in the upper soil solution, may be due to seepage, since oak occurs relatively often on wet soils (cf Table 3).The Mg concentration under the different species remained rather stable, also under oak. The concentration was lowest under black pines,but in general the differences between the tree species were modest. The Kconcentration was small, differed not much between the tree species and decreased in all cases with depth. 29 Table 8 Effect of tree species on the median concentration of Ca, Mg and K in the soil solution (148 stands) and in upper groundwater (71 stands) Tree species Ca concentration (molc m'3) Mg concentration (molc m •3) 60-100 cm ground'• 0-30 cm water 60-100 cm groundwater 0.39 (0.41)1' Scots pine Black pine 0.37 (0.34) 0.92 (0.72) Douglas fir Norway spruce 0.58 (0.59) Japanese larch 0.45 (0.44) Oak 0.51 (0.58) Beech 0.27 - 2) 0.29 (0.42) 0.40 (0.30) 0.37 (0.33) 0.47 (0.47) 0.38 (0.38) 0.70 (1.16) 0.19 - 2) 0.27 0.22 0.19 0.33 0.32 1.03 0.09 0.20 (0.19) 0.18 (0.18) 0.53 (0.46) 0.39 (0.34) 0.29 (0.22) 0.27 (0.23) 0.19 - 2) 0.20 (0.20) 0.15 (0.15) 0.33 (0.30) 0.39 (0.39) 0.24 (0.23) 0.41 (0.45) 0.23 - 2) 0.34 0.11 0.22 0.42 0.35 0.47 0.25 Total 0.39 (0.41) 0.26 0.25 (0.25) 0.23 (0.21) 0.31 0-30 cm 0.44 (0.45) K concentration (molc m 3 ) 0.19 (0.18) Scots pine Black pine 0.17 (0.17) 0.21 (0.17) Douglas fir Norway spruce 0.18 (0.17) Japanese larch 0.14 (0.14) Oak 0.24 (0.22) Beech 0.19 -2) 0.11 (0.09) 0.08 (0.08) 0.13 (0.10) 0.09 (0.07) 0.09 (0.09) 0.11 (0.10) 0.07 -2) 0.05 0.04 0.05 0.05 0.05 0.06 0.05 0.19 (0.18) 0.10 (0.09) 0.05 Total 11 21 Values between brackets are median concentrations at the 71 locations where the groundwater composition was measured as well Not enough data Due to a recycling effect the concentration of Ca, Mg and K will be influenced in the upper layer by litterfall whileuptake also takes place deeper in the soil profile. This effect clearly occured for Ca and K. 4.4 Aluminium and pH Table 9 shows the median pH and Al concentration. The pH increased in all cases with depth. The Al concentration did not show a comparable decrease. Between the layer 0-30 cm and 60-100 cm the concentration increased. This is due to the fact that the soil solution in the topsoil was undersaturated with respect to all minerals containing Al (e.g. gibbsite). The Al concentration thus increased with depth because of the mobilization of Al(OH)3, causing apH increase. The lowest Al concentrations were found under oaks and the highest Al concentrations under firs and spruces. Deeper in the soil profile the Al concentration was generally in equilibrium with Al hydroxide and here the opposite occurred: the pH increased and the Al concentration decreased due to base cation weathering. Only for black pine, there was an increase in Al concentration between the layer 60-100 cm and the upper groundwater. 30 Table 9 Effect of tree species on the median Al concentration and the median pH in the soil solution (148 stands) and in upper groundwater (71 stands) Tree species Al concentration (molc m f3) 0-30cm PH ground'- 0-30cm water 60-100cm groundwater Scots pine 0.71 (0.75)1» 0.68 (0.80) Black pine 0.50 (0.53) 0.60 (0.63) Douglas fir 1.43 (1.43) 1.77 (1.60) Norway sprue« : 1.05 (1.05) 1.43 (1.43) Japanese larch 0.70 (0.69) 0.85 (0.85) Oak 0.40 (0.40) 0.35 (0.35) Beech 0.44 - 2) 0.27 - 2) 0.53 0.78 1.14 1.10 0.31 0.14 1.45 3.61 (3.62) 3.70 (3.76) 3.41 (3.53) 3.43 (3.43) 3.58 (3.61) 3.70 (3.62) 3.77 - 2) 3.89 (3.86) 3.95 (3.95) 3.79 (3.81) 3.80 (3.79) 3.89 (3.89) 4.02 (4.01) 3.98 - 2) 4.45 4.37 4.27 4.32 4.48 4.43 4.24 Total 0.54 3.61 (3.59) 3.90 (3.88) 4.37 1] 2> 0.63 (0.69) 60-100cm 0.58 (0.67) Values between brackets are median concentrations at the 71 locations the groundwater composition was measured as well Not enough data where 31 5 Hydrological conditions As stated before (chapter 4), element leaching was calculated by multiplying the measured element concentration in spring in the soil solution and in the upper groundwater with the precipitation excess. This was based on the assumption that the concentrations that are measured represent flux weighed annual average concentrations. The precipitation excess was calculated from the annual precipitation minus the annual interception and actual annual évapotranspiration.First an estimate was made of annual precipitation excesses for the seven tree species included in this study on the basis of literature data on average precipitation, interception and transpiration (Section 5.1). Next a calculation was made about the residence time of soil water to investigate whether it is likely that the data on element concentrations reflect the effect of the deposition of 1989, the year preceding the sampling and represent annual average values (Section 5.2). Information thus obtained was used to adjust several precipitation excesses by using CI concentration data and assuming that CI behaves as a tracer (Section 5.3). 5.1 Precipitation, évapotranspiration and precipitation excess To calculate element budgets, information is required about the precipitation of the year that preceded the sampling. However, during the period October 1989 -March 1990 an amount of 350 -400 mmrain has fallen, a quantity that equals the average value for the period 1950 - 1980.Since adata set for this period was available for gridcells of 10 km x 10 km (interpolated from data of 280 weather stations; Hootsmans and Van Uffelen, 1991),it was used to calculate the average precipitation on the forest stands. In order to obtain the precipitation excess,the interception and the actual evaporation and transpiration have to be known. Literature data about interception, evaporation and transpiration of different types of forests are often not comparable (Nonhebel, 1987; Mulder, 1985; Gash, 1979; De Visser en De Vries, 1989; Hendriks et al., 1990). Based on the review in the Annex the following, interception percentages of the precipitation were selected: 25%for beech, oak and Japanese larch; 30% for black pine and Scots pine; 40% for douglas fir and 45%for Norway spruce. Data used for the sum of average actual transpiration and evaporation were 325 mm for beech, black pine, Scots pine and Japanese larch and 350mmfor douglas fir, Norway spruce and oak (cf Annex). The precipitation excess was calculated by subtracting the interception and the actual evaporation and transpiration of each tree species from the precipitation of the grid square in which the site is situated. Cumulative frequency distributions of the precipitation excesses thus calculated for the tree species occurring at the 148 'soil solution' stands (Fig.4) show that theranges for the different tree species were small. 33 Cumulative Frequency Norway spruce (%) 100 \ 'x 80 \ \ Y\ 60 'Ai '1 \\ \\\ fir Black pine l\ \ ' 40 Douglas l\ y 1 'i Scots pine Oak \\ft *i 20 V \ 0 50 100 150 200 250 300 Beech 350 ~ ~ ' JapanCSe Larch Precipitation Excess (mm.yr ' ) Fig. 4 Inverse cumulative frequency distributions of the calculated precipitation excess of the tree species occurring at the 148 'soil solution' stands This isbecause only regional differences in precipitation caused adifference in the precipitation excess of a tree species. Consequently, the frequencies of the tree species at the 71 'groundwater' stands were quite similar. Actually, the range will be greater because of differences in évapotranspiration induced by differences in canopy coverage, tree height, vitality, soil cover, available moisture, etc. However, it is supposed that the median that will be used to calculate the leaching is fairly reliable. Further Fig. 4 shows that the calculated precipitation excesses were smallest below Norway spruce, and Douglas fir, greatest below beech and Japanese larch and intermediate below Scots pine and black pine and oak. The precipitation excesses given above were used for a first approximation of the element leaching from the rootzone and unsaturated zone, respectively. 5.2 Residence time of the percolation water To answer the question whether the measured concentrations, in the soil solution and in the upper groundwater represent an average annual concentration, and if so for which year, the expected residence time of soil water was calculated for the various tree species on major soil types. The residence time (yr) was estimated by dividing an estimated moisture content (mm) in the rootzone and in the whole unsaturated zone respectively (mm), by the estimated precipitation excess (mmyr"1). For the rootzone a soil layer of 80cm was used and for the unsaturated zone alayer with a thickness from the surface till 75 cm below the phreatic groundwaterlevel (middle of the sampled layers). Calculations were made for three major soil types, i.e. fine loamy sand, fine sand poor in loam and coarse sand. To estimate the water content it was assumed that (i) the top soil is 40 cm thick, (ii) the groundwaterlevel during sampling equalled 34 the average spring level and (iii) fieldcapacity occurs up to 100 cm above the groundwaterlevel (above that level a soil water profile was supposed). Average spring levels were related to groundwaterlevel classes as given in Table 10 (Van der Sluis, 1982). The distribution of groundwaterlevel classes is given inTable 3. Relatively many deciduous stands were located on fine, loamy sand and onwet soils, whereas most coniferous stands were located on coarse sand and on dry soils (groundwaterclass VII), especially the pine stands (cf Table 3). Table 10 Estimated average spring level for the groundwaterlevel classes occurring at the 148 'soil solution ' stands Groundwaterlevel Groundwaterlevel (cm) class average highest II III V VI VII <40 <40 <40 40-80 >80 average lowest spri 50-80 80-120 >120 >120 >160 35 45 55 100 150 The watercontent was derived from the waterretention curves that belong to the standard soils (Table 11).Results are given in Table 12.Comparison of these data with the (original) precipitation excesses (cf Table 14) gives an indication of the residence time of the water as given in Table 13. Table 11 Waterretention characteristics of three major soil types in the 148 'soil solution' stands Soil type Occurrence in Water retention characteristics1' 148 stands (%) fine sand, loamy fine sand, poor in coarse sand 11 18 loam 63 12 topsoil subsoil b3 bl 1 ' bl o3 ol o5 For the actual water retention characteristics related to these codes we refer to Wösten et al., 1987 35 Table 12 Estimated watercontent in the rootzone (0-80 cm below the soil surface) and the unsaturated zone (75 cm below the spring groundwaterlevel) of three major soil types in the 148 'soil solution stands' Soil type Estimated watercontent (mm) Gt V1' Gt VI root zone Fine sand, loamy 300 Fine sand, poor in loam 267 Coarse sand 260 11 unsaturated zone 485 455 437 Gt VII root unsaturated root unsaturated zone zone zone zone 255 579 213 680 195 524 129 593 151 461 112 497 Gt is groundwaterlevel class Table 13 Estimated residence times ofpercolation water in the rootzone and unsaturated zone as afunction of tree species, soil type and groundwaterlevel class Soil type Gt Traveltime (yr) Pine/Oak Fine sand, loamy Fine sand, poor in loam Course sand V VI VII V VI VII V VI VII 1 Douglas ßr Norway spruce Larch/Beech RZ * uz * RZ UZ RZ UZ RZ UZ 1.3 1.1 1.0 1.2 0.9 0.6 1.2 0.7 0.5 2.2 2.7 3.1 2.1 2.4 2.7 2.0 2.1 2.3 2.5 2.1 1.7 2.2 1.6 1.1 2.1 1.2 0.9 3.7 4.4 5.2 3.5 4.0 4.5 3.3 3.5 3.8 3.2 2.7 2.3 2.9 2.1 1.4 2.8 1.6 1.2 5.2 6.2 7.3 4.9 5.6 6.4 4.7 5.0 5.3 1.1 1.0 0.9 0.9 0.7 0.6 0.8 0.5 0.4 1.7 2.1 2.4 1.6 1.9 2.1 1.6 1.7 1.8 1 " RZ is rootzone and UZ is unsaturated zone Residence times in the unsaturated zone were nearly almost always more than two years (Table 13). Consequently, the influence of deposition fluctuation on groundwater quality will be small. Besides the sample formed a mix of 50 cm of the saturated zone that, assuming a poresize of 0.36, contains 180 mm water. For some tree species this is more than the annual precipitation excess. Consequently, it is likely that the concentration in groundwater represents an annual average value. Unlike the unsaturated zone,the calculated residence time in the rootzone was nearly always less than one year for all tree species on moderately to well drained soils (Gt VI and VII) except for douglas fir and Norway spruce (Table 13).Below the latter tree species, the watercontent in the rootzone will be descended from at least the winter before. However, the sampled soil moisture below stands of pine, Japanese larch, oak and beech on soils with groundwaterlevel classes VI and VU, will generally be infiltrated during the preceding months, i.e. the autumn and winter of 1989/1990. This implies that the measured concentrations will certainly not represent annual average values below these tree species. This is specifically true for CI and Na. It is known that sea-spray effects occur particularly during the autumn/winter period. This is illustrated by the deposition of CIin Eelde, aplace situated in the northeastern part of the Netherlands (Fig. 5). It shows that the deposition in the winter of 36 1989/1990 was 2.5 times the average of nearly 5 mmolc m"2 month"1. Na and to a lesser extent Mg show comparable variations in deposition as shown in Table 14. Table 14 Wet deposition of major ions in De Bilt (RIVM/KNMI, 1988) Wet deposition (molc ha"1yr"1) Period Winters 1978-1986 Summers 1978-1986 Na K Mg Ca NH4 N03 so 4 CI 510 230 17 16 57 32 49 63 460 380 190 220 270 240 600 260 It is likely that the concentrations of S0 4 , N0 3 and NH4will also deviate from annual average values, although the deposition of Sand N varies much less in time (cf Table 14).For Sthis is also illustrated in Fig. 6 (cf Fig. 5).However, use of the original precipitation excess from the rootzone calculated for the various tree species might not give reliable leaching estimates of S, N,BC and Al, with thepossible exception of douglas fir and Norway spruce. Consequently, we investigated how the precipitation excess changed while assuming that seasonal changes in S0 4 , N0 3 , BC and Al are equal tothose of CI.This is notunlikely since hydrological changes have a larger influence ondifferences in concentrations throughout the year than deposition changes, especially at greater depth. The tracer behaviour of CI was thus used to estimate the precipitation excess. CI Cldeposition (mol.ha' ) 2001 100" 1 ...•mA Ife —-T- i .i 1 i ..•. .... J F M A M J J A S O N D J 1989 I F M A M J J A S O N D 1990 Fig. 5 Wet Cl deposition in Eelde in 1989 and 1990 37 SOt deposition (molt.ha' ) ïoo80 60 * i 40" 20 0 "- il i I ill „u». JF M A M J J A S O N D J F M A M J 1989 "11 I J A S O N D 1990 Fig. 6 Wet S04 deposition in Eelde in 1989 and 1990 5.3 Relation between precipitation excess and budgets for chloride and sodium In Figure 7 the cumulative frequency distributions of CI deposition and CI leaching of the 148 'moisture' sites are given and in Figure 8 the same is given for the 71 'groundwater' sites. Total deposition was calculated from the wet deposition, according the method discussed in chapter 3.2 and leaching of CI and Na was calculated by multiplying the precipitation excess with the concentration in the soil moisture at 60 - 100 cm and the upper groundwater. In these figures the cumulative frequency distribution for CIleaching is also given after adjusting the precipitation excess in such away, that the median deposition coincides with the median leaching for each of the seven tree species. Figure 7 shows that leaching of CI and Na from the rootzone, calculated with the original precipitation excess, exceeds CI and Na deposition. Inversely, calculated CIand Na leaching from the unsaturated zone is less than CI and Na deposition (Fig. 8). Fitting the medians of the deposition and the leaching of CI and Na from the rootzone by changing the average precipitation excess hardly influenced the precipitation excesses of the coniferous tree species, but it caused a large decrease in the precipitation excesses of the deciduous trees, including the needle shedding Japanese larch (Table 15). This corresponds with the high concentrations of CI 38 Cumulative frequency Cumulative frequency deposition deposition leaching (original) leaching (adjusted) X 0 1000 2000 3000 4000 0 5000 1000 2000 3000 4000 5000 1 Nafluxes (moKha .yr') Cl fluxes (moLha' .yr') Fig. 7 Inverse cumulative frequency distributions of the deposition and leaching of Cl (A) and Na (B)from the rootzone at the 148 'soil solution ' stands Cumulative frequency Cumulative frequency (%) deposition deposition leaching (original) leaching (adjusted) 1000 2000 3000 4000 5000 Clfluxes (moLha' .yr"1) 0 1000 2000 3000 4000 5000 Nafluxes (moLna' .yr'1) Fig. 8 Inverse cumulative frequency distributions of the deposition and leaching of Cl (A) and Na (B)from the unsaturated zone at the 71 'groundwater' stands and Na in the soil solution under these tree species (Section 4.1) induced by the influence of sea-spray in autumn-winter as explained in Section 5.2. 39 It is not clear whether the dry summer of 1989,with 100 mm less rainfall than the annual average amount, also attributed to this fact. Apparently it didn't increase the concentration of CI and Na in the soil solution under the other tree species. Since ion concentrations below deciduous tree species will not represent annual average values, the adjusted precipitation excesses most likely produces more reliable results for the leaching of S, N, BC and Al from the rootzone. Table 15 Actual évapotranspiration and precipitation excess of the tree species occurring at the 148 'soil solution' stands and the 71 'groundwater' stands Tree species Soil Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech Precipitation excess (mm yr"1) Actual évapotranspiration (mm yr 1 ) 2) Groundwater Soil Groundwater O" A O A O A O A 325 325 350 350 325 350 325 319 365 341 337 480 450 440 325 335 350 350 325 350 325 50 68 148 117 368 390 216 225 122 93 276 230 271 222 185 131 106 121 130 156 216 214 131 93 280 219 - 491 471 333 326 237 179 3 > 3) _3) 11 0 = Original values A = Adjusted values based on a fitted CI budget 31 Not enough data 2) The precipitation excesses that were adjusted with the concentration in the groundwater, approached the original values for oak and larch (beech has not enough locations) but the values for Douglas fir, Norway spruce and especially the pine became unexplainably high. It is unlikely that the CI deposition values used are related to the concentration in groundwater and therefore the original precipitation excesses are likely tobe morereliable. Consequently, adjusted precipitation excesses wereused for the rootzone whereas the original values wereused for the unsaturated zone.Net budgets for CIand Na (Table 16),however, giveunreliable results for the unsaturated zone when precipitation excesses are not adjusted. 40 Table 16 Median annual deposition (in), leaching (out) and their difference (in-out) of CIand Nafor the rootzone and the unsaturated zone for different tree species^ CI budget (molc ha ' yr"1) Na budget (molc ha"1yr"1) in out in out in-out Rootzone: Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech 1855 1655 2035 2035 1480 1480 1480 1803 2013 1906 1772 3421 2580 2738 1538 1350 1752 1756 1280 1697 1280 1523 1615 1428 1040 2365 1697 2112 (1558) 15 (-20) (1319) -265 (31) (1533) 324 (219) (1187) 716 (569) (1005) -1085 (275) (981) -417 (299) (1117) -832 (163) total 1605 2144(1669) -539 (0) Tree species Unsaturated zone Scotspine Blackpine Douglasfir Norwayspruce Japaneselarch Oak Beech2' total in-out (1855) 52 (1655) -358 (2035) 129 (2035) 263 (1480) -1941 (1480) -1100 (1480) -1258 1855 891 (1855) 964 1827 850 (1827) 977 2035 816 (2035) 1219 2035 591 (2035) 1444 1480 1746 (1480) -266 1480 1768 (1480) -288 1660 - - 941 (1846) - (0) (0) (0) (0) (0) (0) (0) 13201634(1204) -314 (116) (0) (0) (0) (0) (0) (0) - 719 (186) " Valuesbetweenbracketsareadjustedvaluesaccordingto foreachtree species 2) Notenoughdata 1538 644 (1469) 894 (69) 1499 838 (1772) 661(-273) 1760 733 (1946) 1027(-186) 1756 502 (1725) 1254 (31) 1280 1560 (1302) -280 (-22) 1280 1314 (1098) -34(182) 1444 - - 803 (1511) 641 (-67) afittedCIbalance 41 6 Input-Output budgets Element input is defined here as the deposition of an element that enters the soil and element output as the amount that percolates with the precipitation excess to lower soil layers. Positive differences between input and output fluxes indicate removal from the soil (e.g. uptake by the vegetation, denitrification) or storage in the soil profile (immobilization, adsorption). Negative differences indicate mobilization from the soil profile (e.g. weathering, mineralization, desorption). Equal input and output budgets normally occur with inert elements and elements with which the soil is saturated. 6.1 Budgets of sulphur and nitrogen 6.1.1 The rootzone The cumulative frequency distributions of the input- and output fluxes of S and N of 148forest stands (Figure 9), show that the variation in deposition of S0 4 and N0 3 was small and of NH4 wide whereas the opposite was true for leaching. Leaching data in Figure 9 were only based on precipitation excesses that were adjusted on the basis of a fitted CIbalance (cf Table 15).The medians of the input and output fluxes and the net budgets of the separate tree species (Table 17) show that use of the original precipitation excesses lead to a large removal of S0 4 from the soil for the deciduous trees (including Japanese larch) which is very unlikely. Using precipitation excesses that were calculated according to a fitted CI balance (5.3) the difference between median input and output fluxes was small for each tree species. S0 4 thus seems to behave like a tracer. The median leaching of N was reduced by 80%compared to its median deposition, using the adjusted values for the precipitation excess.The decrease was smallest for Douglas fir (63%) and greatest for Norway spruce (90%).The contribution of N0 3 to the deposition of N was relatively small but the average leaching of N0 3 almost equalled its deposition. Most likely, the occurrence of nitrification compensates denitrification anduptake. The differences between the tree species, however, were considerable. NH4contributed most to N deposition, but hardly toNleaching. Nearly all NH4 was removed by immobilization, nitrification and (preferential) NH4uptake. 43 Cumulative frequency Cumulative frequency (%) deposition leaching 0 1000 2000 3000 4000 5000 1 0 1000 2000 3000 4000 5000 Nfluxes (mcJ.ha'' .yr'1 ) 1 SO^ fluxes (moLha .yr" ) Cumulative frequency Cumulative frequency (*) D deposition deposition leaching leaching v. 0 1000 2000 3000 4000 5000 NO, fluxes (moI_.ha' .yr ' ) 0 1000 2000 3000 4000 5000 NHt fluxes (mol.ba' .yr'1) Fig. 9 Inverse cumulative frequency distributions of the deposition and leaching of S04 (A), N (B), N03 (C) and NH4 (D)from the rootzone at the 148 'soil solution' stands 44 Table 17 Median annual deposition (in), leaching from the rootzone (out) and their difference (in-out) of SO^ N, N03 and NH4for the tree species occurring at the 148 'soil solution ' stands^ Tree species S 0 4 budget (molc ha * yr' N budget (m( )lc ha J yr 1 ) ) in out in-out Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech 2013 1926 2646 1798 1286 1283 1403 2001 1924 2493 1822 1024 1771 1415 12 (1935) (78) (2371) 2 (-445) (2339) 153 (307) (1592) -24 (206) (2509) 244 (-1223) (2972) -488 (-1689) (2569) -12 (-1166) Total 1744 1773 (2355) -29 N 0 3 budget (molc ha"1yr" Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech Total 11 999 665 (649) 334 999 981 (1185) 18 1227 1756 (1648) -529 1113 363 (303) 750 769 540 (1277) 229 769 368 (621) 401 852 227 (489) 625 971 700 (999) 271 in (-611) l out in-out 4092 892 (871) 4954 1157 (1405) 5034 1885 (1768) 4510 453 (382) 3206 651 (1540) 3428 462 (788) 3473 347 (706) 3200(3221) 3797 (3549) 3149 (3266) 4057 (4128) 2555(1666) 2966 (2640) 3126 (2767) 834 (1187) 3325(2972) 4159 NH4 budget (molc ha'1 yr 1 ) ) (350) (-186) (-421) (810) (-508) (148) (363) 3093 3955 3807 3397 2437 2659 2621 227 176 129 90 111 94 120 (222) (220) (120) (79) (263) (167) (217) 2866 (2871) 3779 (3735) 3678 (3687) 3307 (3318) 2326(2174) 2565 (2492) 2501 (2404) (-28) 3188 134 (188) 3054 (3000) Values between brackets are calculated with the orginal precipitation excess (not adjusted) according to a fitted CI balance. 6.1.2 The unsaturated zone Budgets for S and N in the unsaturated zone are given in Figure 10and Table 18. Compared to the roötzone, the output fluxes of S0 4 from the unsaturated zone were somewhat smaller below the coniferous trees, whereas the leaching under Japanese larch and oak was much larger (when the adjusted precipitation excesses were used for the rootzone; cf Table 17 and 18). However, it is likely that for the latter tree species S0 4 in groundwater not only originates from leaching from the rootzone but also from lateral seepage (wet sites). The output fluxes of N from the unsaturated zone were mostly smaller than from the rootzone. NH4 almost disappeared due to nitrification and also the leaching of N0 3 was less than at the depth of the rootzone. The greatest leaching took place under Norway spruces and the smallest under black pines. 45 Cumulative frequency Cumulative frequency (%) 0 1000 2000 3000 4000 deposition deposition leaching leaching 0 5000 1000 2000 3000 4000 5000 Nfluxes (moKha'.yr'1) S0 4 fluxes (mol.ba'.yr ' ) Cumulative frequency Cumulative frequency (%) (%) deposition deposition leaching leaching 40 ' \ 0 1000 2000 3000 4000 5000 1 NO, fluxes (moLha' .yr' ) Fig. 10 46 0 \ 1000 2000 3000 4000 5000 NH4 fluxes (molo.ha' .yr'1 ) Inverse cumulative frequency distributions of deposition and leaching of S04 (A), N (B), N03 (C) and NH4 (D)from the unsaturated zone at the 71 'groundwater' stands Table 18 Median annual deposition (in), leaching from the unsaturated zone (out) and their difference (in-out) of SO^, N, N03 and NH4for the tree species occurring at the 71 'groundwater' stands Tree species1' S 0 4 budget (molc ha 1 yr J ) N budget (molc] ha'1 yr'1) in out in-out in out in-out Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak 2198 2093 1789 1817 1267 1283 1802 1828 1228 1098 2723 2628 396 265 561 719 -1456 -1400 4092 4988 4691 4624 3027 3514 303 986 890 147 587 292 3789 4002 3801 4477 2440 3222 Total 1763 1949 -186 4328 490 3838 Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Total N 0 3 budget (molc ha 1 yr l ) NH 4 budget (molc ha x yr_1) 999 1001 1122 1113 774 769 303 986 890 144 587 292 696 15 232 969 187 477 3093 3987 3569 3511 2253 2745 0 0 0 3 0 0 3093 3987 3569 3508 2253 2745 999 490 509 3329 0 3329 11 For beech no budgets are given because only one value was available 6.2 Budgets of base cations and aluminium 6.2.1 The rootzone The input and output fluxes and the net budgets of Al and the base cations, K, Ca and Mg for each tree species are given in Table 19. In Figure 11 the cumulative frequency distributions of the 148 stands are given. Al deposition is neglectable. Therefor the entire leaching of this ion is caused by the mobilization of Al (hydroxide). This occurs when other buffering mechanisms are exhausted and the acidity increases. Figure IIA shows that the range in Al leaching was large. Al leaching was small under beech and oak, and large under douglas fir and Norway spruce (Table 19). Ca leaching and on less account also that of K and Mg is likely to be greater than the deposition of these ions in acid soils because of weathering and ion-exchange. In most cases this appeared to be the case. Striking is the great difference between the output and input of Ca, and to a lesser extent of Mg at the oak stands. Some locations with oaks have high water tables with probable influences of deep groundwater (seepage).Another explanation is the possibly larger Ca (and Mg) input on oak stands which generally border agricultural land. 47 Cumulative frequency Cumulative frequency (%) A B deposition leaching. leaching. V O 1000 2000 3000 4000 5000 1 250 500 1 750 1000 1 Alleaching (moLba .yr" ) Kfluxes (moLha .yr' ) Cumulative frequency Cumulative frequency (%) (%) D deposition deposition leaching. leaching. \ 0 1000 2000 3000 4000 5000 Cafluxes (moLha' .yr' ) Fig. 11 48 0 1000 2000 3000 4000 5000 1 Mgfluxes (molJu .yr' ) Inverse cumulative frequency distributions ofthe deposition and leaching of Al (A), K (B), Ca (C) and Mg (D)from therootzone atthe 148 'soil solution' stands Table 19 Median annual deposition (in), leaching from the rootzone (out) and their difference (in-out) of Al, K, Ca and Mgfor the tree species occurring at the 148 'soil solution 'stands'* Tree species Al budget (molc ha'1 1 yr 1 ) K budget (molcha"1 yr 1 ) in in-out in in-ou t out Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech 0 0 0 0 0 0 0 Total 0 1042 1273 2284 1533 897 422 523 (1018) (1528) (2140) (1337) (2220) (778) (830) -1042 -1273 -2284 -1533 -897 -422 -523 976 (1210) Ca budget (molc ha" Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Beech 563 475 536 454 320 430 380 863 (837) 556 (668) 512 (480) 496 (435) 470 (1073) 943 (1650) 303 (524) Total 457 530 (770) 1 out (-1018) H528) (-2140) (-1337) (-2220) (-778) (-830) 80 75 83 83 60 60 64 179 194 138 98 109 130 119 (174) (243) (128) (86) (234) (260) (203) -976 (-1210) 75 151 (203) -99 -119 -55 -15 -49 -70 -55 -76 (-128) yr 1 ) Mg budget (molc ha i-1 yr1: ) -300 (-274) -81 (-193) 24 (56) -42 (19) -150 (-753) -513 (-1220) -77 (-144) 363 313 385 385 280 280 280 320 (310) 334 (412) 430 (400) 369 (306) 257 (629) 525 (909) 382 (641) 308 380 -73 (-313) (479) (-94) (-168) (-45) (-3) (-174) (-200) (-139) 43 (53) -21 (-99) -45 (-15) 16 (79) 23 (-349) -245 (-629) -102 (-361) -72 (-171) " Values between brackets are calculated with the original precipitation excess (not adjusted according to a fitted CI balance). 6.2.2 The unsaturated zone The output fluxes of AI, K, Ca and Mg that were calculated for the unsaturated zone were quite comparable to those that were calculated for the rootzone (cf. Fig. 11and Fig. 12).Al leaching was nearly equal for black pine, Japanese larch and oak, larger for Scots pine and lower for Douglas fir and Norway spruce (Table 20).In the last case this might be due to precipitation of Al-hydroxide, induced by BC weathering, and by exchange of Al with adsorbed Ca and other base cations deeper in the soil profile. Compared totherootzone median Ca leaching of all stands was nearly equal, Mg leaching was larger and K leaching was less in the unsaturated zone. The calculated leaching of K, Ca and Mg from the unsaturated zone under Douglas fir and Norway spruce was even smaller than the deposition of theseions.Striking, again is the extremely large Ca leaching below oak stands which is definitely influenced by seepage at wet sites. 49 Cumulative frequency Cumulative frequency (%) B deposition leaching. leaching . X, \ 0 1000 2000 3000 4000 5000 250 500 Alleaching (moLha' .yr') 750 Kfh»es (moLha' .yr ') Cumulative frequency Cumulative frequency (%) 0 1000 2000 3000 4000 5000 Cafluxes (moLba' .yr' ) Fig. 12 50 1000 D deposition deposition leaching. leaching. 0 1000 2000 3000 4000 5000 Mgfluxes (moKha' .yr') Inverse cumulative frequency distributions ofthe deposition and leaching of Al (A), K(B), Ca (C) and Mg (D)from theunsaturated zone atthe71 'groundwater' stands Table 20 Median annual deposition (in), leaching front the unsaturated zone (out) and their difference (in-out) of Al, K, Ca and Mgfor the tree species occurring at the 71 'groundwater' stands Tree species1' Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak Al budget (molc ha* yr') K budget (molc ha J yr ] ) in in 0 0 0 0 0 0 Total out out in-out 1670 1283 1553 918 864 386 -1670 -1283 -1553 -918 -864 -386 75 75 83 83 60 60 86 133 63 47 135 139 -11 -58 20 36 -75 -79 1054 -1054 75 98 -23 Ca budget (molc ha"1yr'1) in-out Mg budget (molc ha'1 yr'1) Scots pine Black pine Douglas fir Norway spruce Japanese larch Oak 563 512 495 447 320 440 516 564 264 306 832 2119 47 -52 231 141 -512 -1679 363 350 385 385 280 280 269 796 269 341 1007 1143 94 -446 116 44 -727 -863 Total 454 520 -66 320 484 -164 " For beach no budgets are given because only one value was available 51 7 Discussion and conclusions Results of input-output budgets for seven major Dutch forests types are given in this report as medians to mimic the large uncertainty in deposition and leaching estimates of the elements. However, even these results may strongly be influenced by methodological errors, i.e.: 1. Concentrations inMarch and April are only an approximation of the flux-weighted annual average concentration. Especially for S0 4 , N0 3 and NH4, correlations between concentrations in these months and annual average concentrations appear to be rather weak (R2adjbetween 0.42 and 0.60). For Al and Ca, the correlation is better but here the regression coefficients indicate that Ca concentrations in March and April are likely to be higher than the annual average concentration whereas the opposite is true for Al (cf De Vries et al., 1994); 2. Centrifuge soil solutions deviate from lysimeter soil solutions.For example base\ J',. ff^ cation (Ca) concentrations in soil solution obtained by centrifugation (soil survey| A? sites) are generally higher than base cation (Ca) concentrations in soil solution | yy,fß obtained by suction cups, whereas the opposite is true for Al (Zabowski and f . v S Ugolini, 1990; Verhagen and Diederen, 1991). These two aspects may have j v'""*' "''" caused that the Al mobilization is underestimated whereas BC mobilization is ^.tf yt/f,<J) overestimated; 3. The use of a Cl-corrected precipitation excess, to correct for concentration deviations from annual average values, may cause errors in leaching estimates inforest-soil combinations with a short soil water residence time in therootzone. CIdeposition ishighly variable over the year and high CIconcentrations in the subsoil may there be caused by a considerable CI deposition in the beginning of 1990. Calculated residence times for the various tree species were mostly more than one year for the coniferous trees, whereas it was often less than one year for deciduous trees. The correction in precipitation excess for deciduous trees may thus be too large causing an underestimation in leaching estimates. However, combining the original precipitation excesses with measured S0 4 concentrations would result in a large removal of S0 4 from the soil for the deciduous trees (including Japanese larch), which is very unlikely; 4. The deposition is derived from grid squares for which yearly sums have been determined. For some ions seasonal variations are great. The filtering factors that are used to obtain the bulk deposition from the total or wet deposition are based upon scant research through which particularly the filtering factors for the base cations are roughly assessed; 5. The groundwater is withdrawn 50-100 cmbelow the groundwaterlevel and forms a mix of the precipitation excess of often more than a year. The point of time that it infiltrated via the soil surface was several years before. The sampled groundwater therefore seems a reliable indication of the average leaching. However, at greater depth the chance increases that the samples are influenced by the horizontal groundwaterflux and thus represent a greater area. Despite theuncertainties involved, the summary of thebudgets of all species (Table 21), warrants the general conclusions that: 1. S0 4 behaves as a tracer; 53 A. I / k i A\ê-^ v L 2. N is strongly retained (especially NH 4 ); 3. Al mobilization is the dominant buffer mechanism and 4. most interactions occurred in the rootzone. The increased N (NH 4 and N0 3 ) retention between rootzone and groundwater is conform the expectation (denitrification). For all cations, i.e. Al, K, Ca and Mg, an ^increased mobilization was expected between rootzone and groundwater due to weathering, but this was only the case for Al and Mg. This is, however, due to the reliability of data (see above). J rvj'i -f/ Table 21 Summary of the net budgets (input-output) of major ionsfor the rootzone and unsaturated zone »y- • ,-0 'j*d* Element so 4 •u*- N N03 NH4 Al K Ca Mg Net budgets (molc ha'1 yr 1 ) Rootzone1' Unsaturated zone2' Unsaturated - Rootzone zone -29 3325 271 3054 -976 -76 -73 -72 -186 3838 509 3329 -1054 -23 -66 -164 -157 513 238 275 -78 -53 7 -92 11 Values according to a fitted CI balance Values calculated with original precipitation excesses 21 The uncertainties involved affect reliable conclusions about input-output budgets for each tree species. 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VANUFFELEN, 1991.Assessment of input datafor a simple mass balance model derivation a map of critical loads for Dutch forest soils. Wageningen, DLO The Winand Staring Centre for Integrated Land, Soil and Water Research, Internal Report. 58 Annex On interception and évapotranspiration of the forest stands Interception Using models, Nonhebel (1987) determined the interception and transpiration of different types of forests at five places inthe Netherlands: De Kooy,Eelde, DeBilt, Vlissingen and Zuid Limburg. For the transpiration he distinguished sand and clay soils.The interception as percentage of theprecipitation over the yearremained rather stable for the different types of forest, although there were differences up to 18% between the two models he used (Mulder, 1985 and Gash, 1979).In Table 1.1the averages of both models for six forest types are given for places in the eastern parts of the Netherlands during the period 1974-1978. Table LI Calculated average interception lossfor different tree species during the period 1974-1978 as percentage of the annual precipitation at three places in the eastern part of the Netherlands (from Nonhebel, 1987) Tree species Scots pine Douglas fir Norway spruce Japanese larch Oak Beech Interception (%) De Bilt Eelde Zuid -Limburg Average 33 55 56 22 19 18 38 61 60 27 24 22 35 57 56 24 21 20 35 58 57 24 21 20 The interception percentages for spruce and douglas fir that are given in Table1.1 are very high. It implies that in a year with an average amount of precipitation (780 mm) there is only about 325 mm available for evaporation and transpiration which seems unlikely. A much lower average interception percentage for douglas fir was derived byDe Visser and de Vries (1989) who computed water balances for different tree species with the model SWATRE (Belmans et al., 1983). For Scots pine, douglas fir and deciduous forests they found an annual average interception loss of 39%, 33%and 23%of the precipitation, respectively. Based on their data and on a literature survey of Hiege (1985) we used the following interception percentages: 20%for oak, 25%for Japanese larch, 30%for beech, black and Scots pine, 40% for douglas fir and 45% for Norway spruce (cf De Vries, 1991). Evapotranspiration In Table 1.2 results are given of the sum of actual evaporation and transpiration of several tree species as computed by Nonhebel (1987).He found that differences in transpiration between forests on sand and clay were small (about 15 mm yr"1). Transpiration of forest stands on sandy soils was reduced at a moisture deficit of more than 70 mm. During the considered period 1974-1978 this only occurred in 1976.However, the differences between the succeeding years were small. This was confirmed by Hendriks et al. (1990) with measured data for American oaks. 59 Table 1.2 The average annual évapotranspiration for different tree species on sand during the period 1974-1978 (from Nonhebel, 1987) Tree species Scots pine Douglas fir Norway spruce Japanese larch Oak Beech Evapotranspiration (mm yr 1 ) De Bilt Eelde Zuid •Limburg Average 189 237 300 206 286 211 170 208 267 192 267 195 183 233 314 198 293 202 181 226 294 199 282 203 De Visser and de Vries (1989) computed much larger values for actual evaporation and transpiration. Furthermore, they found considerable differences in actual transpiration for different soil types and groundwaterlevel classes. For example, transpiration values for adry, coarse sand and a wet, fine sand varied between 225 and 375 mm for Scots pine, between 250 and 375 mm for Douglas fir and between 265 and 380 mm for a deciduous stand. The actual evaporation varied from 55 to 75 mm. Although Nonhebel did not give an explanation for the small transpiration amounts, thedifferences areprobably partly due to assumed hydrological conditions. The transpiration amounts of Visser and de Vries fit better with actual measured data (Hendriks et al., 1990).Based on their results weused the following data for the sum of the average actual transpiration and evaporation: 325 mmfor beech, black pine, Scots pine and Japanese larch and 350 mm for Douglas fir, Norway spruce and oak. 60
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