IAQVEC 2016, 9th International Conference on Indoor Air Quality Ventilation & Energy Conservation In Buildings Evaluation of a new thermal-regenerative air purifier for indoor formaldehyde removal Ru XIAO1,2, Jinhan MO1,2,*, Lin LIN1, Yuchen SHI1, Jiaqi SUN1 1 2 Department of Building Science, Tsinghua University, Beijing, China Beijing Key Laboratory of Indoor Air Quality Evaluation and Control, Beijing, China * Corresponding email: [email protected] ABSTRACT Formaldehyde is a common indoor pollutant which has been named as carcinogenic to humans by International Agency for Research on Cancer. This work aims to develop a new thermalregenerated air purifier to remove indoor formaldehyde for long-term applications. There are four working modes in the air purifier: cleaning mode, thermal-regeneration mode, exhaust mode and fresh air in-take mode. A small scale prototype purifier with commercial activated carbon as adsorbent was developed and the modes were controlled by switching five valves through a programmable logic controller (PLC). Experimental results indicate that the formaldehyde removal efficiency of the prototype remained stable after 3 cycles of adsorption and desorption. Compared with traditional purifiers without thermal regeneration, the proposed purifier has longer lifespan for indoor formaldehyde removal. Moreover, the energy consumption for thermal regeneration is small and acceptable. KEYWORDS Indoor air quality; Formaldehyde; Air cleaning; Adsorption; Desorption INTRODUCTION More than 65% of formaldehyde produced is used to synthesize resins used in wood-based construction materials (Tang et al., 2009), which is therefore a main source of indoor formaldehyde pollution (Bohm et al., 2012). In past decades, China has been experiencing rapid urbanization and modernization. The urban residential building area grew from 4 to 21 billion m2 from 1990 to 2010 (National Bureau of Statistics of China, 2010) and the production of synthetic wood-based decorating materials was more than 150000 km2 in 2010 (Zhang et al., 2013) , which leads to severe formaldehyde pollution in Chinese homes, especially in newly built homes. Yao et al. (2005) had measured the formaldehyde concentrations in newly-built homes in six Chinese cities in summer and winter. The average formaldehyde concentrations in the six cities were between 200 to 500 μg/m3, which were 3 to 6 times greater than China indoor formaldehyde standard level, 80 μg/m3 (GB/T 18801, 2002). Furthermore, formaldehyde has adverse health impact on people and has been named as carcinogenic to humans by International Agency for Research on Cancer (IARC, 2016). Du et al. reported that formaldehyde was the top one cancer risk contributors among various indoor volatile organic compounds inhaled for both males and females in urban China(Du et al., 2014). Therefore, effective technologies for formaldehyde removal are in great need in urban China homes. Common technologies for indoor air purification are adsorption, catalytic oxidation, photocatalytic oxidation (PCO), and non-thermal-plasma (NTP). Catalytic oxidation, PCO and NTP have problems of material poisoning and may produce potentially harmful intermediates and by-products (Zhang et al., 2011). Besides, little is known about the practical PCO and NTP air cleaning performance in real situations (Gallego et al., 2013). In contrast, adsorption technology using activated carbon (AC) is cheap, stable and won’t produce secondary pollutions, which is the most widely used to remove gas-phase contaminants in buildings (VanOsdell et al., 1996). Some researchers had measured the adsorption performance of activated carbon for formaldehyde (Chen et al., 2005a; Jing et al., 2008; Rengga et al., 2013; Lee et al., 2013). However, most of the studies were finished in laboratory and using much higher formaldehyde concentrations than those in real dwellings. Moreover, due to the low adsorption capacity, the life span of activated carbon for formaldehyde is short, which limits the application of activated carbon in indoor formaldehyde removal. In this study, a new thermal-regenerated air purifier was developed to remove indoor formaldehyde for long-term applications. The performance of the new air purifier was evaluated for sub-ppm formaldehyde removal. METHODS Principal of the new thermal-regenerative air purifier (a) Cleaning mode (b) Regeneration mode (c) Exhaust mode (d) Fresh air in-take mode Figure 1. Schematic of the thermal-regenerative air purifier Figure 1 shows the configuration of the new thermal-regenerative air purifier, which is installed on the inner wall of homes and can achieve four modes by switching five valves, K1 - K5. The arrows with different colors in Figure 1 represent the air flow paths. (a) Cleaning mode, valves K1 and K2 are opened and valves K3, K4 and K5 are closed. Indoor polluted air is driven into the purifier and passes through the adsorption filter and fan, respectively. The adsorption filter with activated carbon removes the indoor formaldehyde; (b) Thermal-regeneration mode, valves K3 and K4 are opened and valves K1, K2 and K5 are closed. The inlet and outlet of the air purifier are closed and the air inside the thermal-insulated purifier will continuously cycle and is heated up to 80 °C by an electrical heater, which will results in the desorption of adsorbed formaldehyde from the adsorption filter; (c) Exhaust mode, valves K2, K3 and K5 are opened and valves K1 and K4 are closed. The air inside the purifier will be exhausted out after completely desorption; (d) Fresh air mode, valve K1, K4 and K5 are opened and valve K2 and K3 are closed. Outdoor fresh air is introduced indoor to dilute other indoor pollutants such as carbon dioxide, and improve indoor air quality. All the four working modes are controlled by a programmable logic controller (PLC). Prototype set-up A small-scale prototype purifier was produced with the basic parameters listed in Table 1. Table 1. Basic parameters of the prototype. Inner volume 0.036 m3 Inner size Sealing material 0.2 m × 0.3 m × 0.6 m Adsorbent material 1.5 kg activated carbon Airflow rate 20 m³/h Face velocity through filter 0.19 m/s Power of the heater 100 W Polystyrene Performance evaluation of the prototype The formaldehyde removal performance of the prototype purifier was measured in a 3m3 airtight glass chamber (1.28 m ×1.28m × 1.88 m). A fan was placed inside the chamber to mix the air inside the chamber. The temperature and relative humidity inside the chamber were controlled at 20 ºC and 20%, respectively. A micro-syringe-pump based generator using formalin solution with 37% formaldehyde by mass was located in the chamber to generate initial formaldehyde concentrations or constant emission rates. The concentration of formaldehyde in the chamber was real-time monitored by a gas analyzer (INNOVA 1312). INNOVA 1312 has been calibrated using MBTH (3-methyl-2-benzothiazolinonehydrazone hydrochloride) spectrophotometry method with UV spectrophotometer (Unico, WFJ7200). The performance evaluation experiment was carried out in four repeated cycles, each cycle is consisted of 4 stages. Firstly, the purifier was switched to “cleaning mode”. The initial CADR (Clean Air Delivery Rate) and single-pass efficiency at each cycle were measured by a “Pull-down” test procedure (Chen et al., 2005b). The micro-syringe-pump based generator rapidly evaporated formalin into the chamber with the rate of 2 µL/min for 2 min. After the concentration of formaldehyde in the chamber kept stable (roughly 0.5 mg/m3), the prototype purifier was turned on to purify the air in the chamber. The concentration of formaldehyde in the chamber was continuously measured for 60 min. Secondly, the formaldehyde removal performance of the purifier was aged by continuously absorbing formaldehyde. In this period, the purifier was kept at cleaning mode, while formalin was evaporated with a constant rate of 0.8 µL/min for 12 hours. Another “pull-down” test was performed to obtain the CADR and single-pass efficiency of the purifier after aging period. Thirdly, the purifier was switched to “thermal-regeneration mode”. The air inside the purifier was heated up to 80 ºC and then passed through activated carbon module, which resulted in the desorption of formaldehyde from activated carbon. The desorption period lasted for 8 hours with a total heating energy consumption of 0.4 kWh. Fourthly, the purifier was switched to “exhaust mode”. The hot and high-polluted air inside the purifier was exhausted out for 30 min. The regenerated activated carbon was cooled down during the exhaust period. These 4 stages took place in order during each cycle. After the exhaust period in the i# cycle, the initial “Pull-down” test in the i+1# cycle begin. Thus, the performance in the first stage of the i# cycle could represent the adsorption performance of the adsorbent after i-1 times of adsorption-desorption cycles. Mass conservation of formaldehyde in the chamber Assuming that the air is well mixed in the chamber and other formaldehyde removal mechanisms such as surface deposition and chamber leakage, can be characterized by a firstorder rate constant kn, the mass conservation of formaldehyde in each “pull-down” test can be written as follows: 𝑉 d𝐶 = −(𝑘𝑛 𝑉 + 𝐶𝐴𝐷𝑅)𝐶 = −(𝑘𝑛 𝑉 + 𝑄𝜂)𝐶 𝑑𝑡 (1) Where, V is the volume of the chamber [m3]; C is the average formaldehyde concentration in the test chamber [mg/m3]; kn is the formaldehyde concentration decay rate without air purifier operating [h-1], which was measured as 0.001 h-1 in this study; Q is the volumetric flow rate through the purifier [m3/h]; η is the single-pass efficiency of purifier [%]. Assuming that CADR does not change during the test period, an analytical solution can be obtained from Equation (1) as: 𝐶 = 𝐶0 exp [− (𝑘𝑛 + 𝑄𝜂 ) t] = 𝐶0 exp[−(𝑘𝑛 + 𝑘𝑒 )t] 𝑉 (2) Where, C0 is the initial formaldehyde concentration in the chamber [mg/m3]; ke is the total formaldehyde concentration decay rate with air purifier operating [h-1]. CADR can be determined by linear regression of ln(C/C0) vs. t from measured concentration decay curve, and the single pass efficiency can be calculated as: 𝜂= 𝑉(𝑘𝑒 − 𝑘𝑛 ) 𝑄 (3) RESULTS AND DISCUSSIONS Figure 2 shows the adsorption performance in different periods of the first cycle and the first stage of the second cycle. The initial removal efficiency for formaldehyde was 34.92%, and CADR was 6.99 m³/h, which was relatively low due to the low air flow rate in the prototype. After the aging period, the concentration of formaldehyde in the chamber continuously grew up, indicating that the activated carbon in the purifier had reached saturation and the adsorbed formaldehyde during aging period were released out in the “pull-down” test. However, after the desorption period, it is found that the decay curve of formaldehyde was almost the same with the initial test, which meant a full recovery of the adsorption capacity. The results prove that the desorption process can effectively and totally remove adsorbed formaldehyde from activated carbon. Figure 3 shows the adsorption performance of the “pull-down test” for 4 cycles in the experiment. It was found that the CADR and the removal efficiency remained stable after 3 adsorption and desorption cycles. From Figure 2 and Figure 3, we can conclude that the purifier can effectively achieve self-regeneration by the adsorption and desorption cycle. The thermal-regenerative process will greatly extend the life span of the purifier. Concentration( mg/m3) 1.00 0.80 cycle 1#, adsorption period 热再生前 0.60 cycle 1#, after aging period 已饱和 cycle 2#, adsorption period 脱附完全后 0.40 0.20 0.00 0 10 20 30 40 50 60 time (min) -0.20 Figure 2. “Pull-down test” performance in different periods of cycle 1# and cycle 2# 9 50 8 7 40 6 5 30 4 20 3 CADR (m³/h) removal efficiency (%) 10 60 2 10 1 0 0 cycle1 cycle2 CADR cycle3 cycle4 EFFICIENCY Figure 3. Comparison of the adsorption performance in the first stage of different cycles Considering the energy consumption in the desorption period, we calculated the extra electricity consumption compared with purifiers without the function of thermal-regeneration. Common commercial activated carbon module for formaldehyde removal is recommended to replace every three months. We assume that the desorption process of this thermal-regenerative purifier repeats once a month. Thus the extra electricity consumption for the desorption period will be 4.8 kWh per year. We can expect that the energy consumption is also small even for large scale air purifier (with high CADR value, more activated carbon). ACKNOWLEDGEMENT The research was supported by the Natural Science Foundation of China (Nos. 51478235 and 51521005) and Beijing Municipal Science & Technology Commission (No. Z151100001515007). CONCLUSIONS In this study, we develop a new thermal-regenerated air purifier with indoor formaldehyde cleaning and self-regeneration function. We choose activated carbon as the adsorbent for formaldehyde and the performance of the prototype is proved to be stable after 3 cycles of adsorption-desorption process. The preliminary results indicate that the new purifier has a good application prospect for indoor formaldehyde removal. Further evaluation for the real-scale prototype is ongoing. REFERENCES Bohm M., Salem M.Z.M. and Srba J. 2012. 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