Š‹‡•‡‘—”ƒŽ‘ˆƒ–ƒŽ›•‹•͵͹ȋʹͲͳ͸Ȍͳ͹ʹͻȂͳ͹͵͹
ۢौᆜᣛʹͲͳ͸ᒪㅢ͵͹ভㅢͳͲᵕȁ™™™Ǥ…Œ…ƒ–ƒŽǤ‘”‰
availableatwww.sciencedirect.com
journalhomepage:www.elsevier.com/locate/chnjc
Article(SpecialIssueonGoldCatalysis)
Goldstabilizedonvariousoxidesupportscatalyzingformaldehyde
oxidationatroomtemperature
‹‰„‹‰Š‡ƒǡ‹ƒ‘„‹‰Š—„ǡ‹†‹ƒ‰ƒǡ‹‡‹—ƒǡŠ—ƒŠ‹ƒǡȗ
StateKeyLaboratoryofFineChemicals,SchoolofChemistry,DalianUniversityofTechnology,Dalian116024,Liaoning,China
LaboratoryofPlasmaPhysicalChemistry,DalianUniversityofTechnology,Dalian116024,Liaoning,China
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Articlehistory:
‡…‡‹˜‡†ͳͷ’”‹ŽʹͲͳ͸
……‡’–‡†ʹͳƒ›ʹͲͳ͸
—„Ž‹•Š‡†ͷ…–‘„‡”ʹͲͳ͸
Keywords:
‘Ž†…ƒ–ƒŽ›•–
š‹†‡•—’’‘”–
‘”ƒŽ†‡Š›†‡‘š‹†ƒ–‹‘
‡†—…‹„‹Ž‹–›
ƒ–ƒŽ›–‹…•–ƒ„‹Ž‹–›
‘Ž† •–ƒ„‹Ž‹œ‡† ‘ ”‡†—…‹„Ž‡ ‘š‹†‡ ȋ‡ʹ ƒ† ‡xȌ ƒ† ‹””‡†—…‹„Ž‡ ‘š‹†‡ ȋɀǦŽʹ͵ǡ ‹ʹǡ ƒ†
ǦͷȌ ™‡”‡ ’”‡’ƒ”‡† „› †‡’‘•‹–‹‘ ’”‡…‹’‹–ƒ–‹‘ ‡–Š‘† ƒ† –‡•–‡† ˆ‘” …ƒ–ƒŽ›–‹… ‘š‹†ƒ–‹‘ ‘ˆ
ˆ‘”ƒŽ†‡Š›†‡ȋȌƒ–”‘‘–‡’‡”ƒ–—”‡—†‡”Š‹‰Š
‘ˆ͸ͲͲͲͲͲŽȀȋ‰ȉ•ȌǤ—ȀɀǦŽʹ͵…ƒ–ƒǦ
Ž›•–•Š‘™‡††‹•–‹…–‹˜‡…ƒ–ƒŽ›–‹…’‡”ˆ‘”ƒ…‡ǡ’”‡•‡–‹‰–Š‡Š‹‰Š‡•–‹‹–‹ƒŽ…‘˜‡”•‹‘ƒ†
•–ƒ„‹Ž‹–›Ǥ‘””‡Žƒ–‹‰–Š‡”‡ƒ…–‹‘”ƒ–‡™‹–Š—’ƒ”–‹…Ž‡•‹œ‡ǡ–Š‡”‡‹•ƒŽ‹‡ƒ””‡Žƒ–‹‘•Š‹’ǡ•—‰‰‡•–‹‰
–Šƒ––Š‡•ƒŽŽ‡”—’ƒ”–‹…Ž‡•‹œ‡™‹–ŠŠ‹‰Š‡”†‹•’‡”•‹‘’‘••‡••‡•Š‹‰Š”‡ƒ…–‹˜‹–›ˆ‘”‘š‹†ƒǦ
–‹‘ǤŽŽ–Š‡…ƒ–ƒŽ›•–•†‡ƒ…–‹˜ƒ–‡†ƒ–Š‹‰Š
ȋ͸ͲͲͲͲͲŽȀȋ‰ȉ•ȌȌǡ„—–‹ƒ“—‹–‡†‹ˆˆ‡”‡–”ƒ–‡Ǥ‡Ǧ
†—…‹„Ž‡‘š‹†‡ȋ‡ʹƒ†‡xȌ…‘—Ž†•–ƒ„‹Ž‹œ‡‰‘Ž†–Š”‘—‰ŠŽ‹ƒ‰‡ƒ†–Š‡”‡ˆ‘”‡‡šŠ‹„‹–•ƒ„‡––‡”
•–ƒ„‹Ž‹–› ˆ‘” ‘š‹†ƒ–‹‘ ”‡ƒ…–‹‘Ǥ ‘™‡˜‡”ǡ –Š‡ ƒ‰‰”‡‰ƒ–‹‘ ‘ˆ ‰‘Ž† ’ƒ”–‹…Ž‡• ‘……—””‡† ‘˜‡”
—Ȁ‹ʹƒ†—ȀǦͷ…ƒ–ƒŽ›•–•ǡ™Š‹…Š”‡•—Ž–‹–Š‡ˆƒ•–†‡ƒ…–‹˜ƒ–‹‘ǤŠ‡”‡ˆ‘”‡ǡ‘—””‡•—Ž–••—‰Ǧ
‰‡•––Šƒ––Š‡”‡†—…‹„‹Ž‹–›‘ˆ–Š‡•—’’‘”–•ˆ‘”—…ƒ–ƒŽ›•‹•Šƒ•‘†‹”‡…–‹ˆŽ—‡…‡‘–Š‡ƒ…–‹˜‹–›ǡ„—–
ƒˆˆ‡…–•–Š‡…ƒ–ƒŽ›–‹…•–ƒ„‹Ž‹–›Ǥ
̹ʹͲͳ͸ǡƒŽ‹ƒ•–‹–—–‡‘ˆŠ‡‹…ƒŽŠ›•‹…•ǡŠ‹‡•‡…ƒ†‡›‘ˆ…‹‡…‡•Ǥ
—„Ž‹•Š‡†„›Ž•‡˜‹‡”ǤǤŽŽ”‹‰Š–•”‡•‡”˜‡†Ǥ
1. Introduction
‹˜‡–Šƒ–ˆ‘”ƒŽ†‡Š›†‡‹•ƒƒŒ‘”‹†‘‘”ƒ‹”’‘ŽŽ—–ƒ–ǡ•‹‰Ǧ
‹ˆ‹…ƒ–‡ˆˆ‘”–•Šƒ˜‡„‡‡†‹”‡…–‡†ƒ–‹†‘‘””‡‘˜ƒŽ–‘
‡‡– ‡˜‹”‘‡–ƒŽ ”‡‰—Žƒ–‹‘• ƒ† Š—ƒ Š‡ƒŽ–Š ‡‡†•
ȏͳȂͶȐǤƒ–ƒŽ›–‹… ‘š‹†ƒ–‹‘‹•”‡…‘‰‹œ‡†ƒ•–Š‡ ‘•–’”‘‹•‹‰
”‡‘˜ƒŽ –‡…Š‘Ž‘‰›Ǥ ƒ–ƒŽ›•–• ƒ’’Ž‹‡† ˆ‘” ‘š‹†ƒǦ
–‹‘‹…Ž—†‡„‘–Š•—’’‘”–‡†„ƒ•‡‡–ƒŽ•ƒ†‘„Ž‡‡–ƒŽ•ȏͷǡ͸ȐǤ
‘™‡˜‡”ǡ„ƒ•‡‡–ƒŽ•”‡“—‹”‡–Š‡—•‡‘ˆ‡Ž‡˜ƒ–‡†–‡’‡”ƒ–—”‡•
ˆ‘” ‘š‹†ƒ–‹‘Ǥ ‘” ‡šƒ’Ž‡ǡ –Š‡ ‘’‡”ƒ–‹‰ –‡’‡”ƒ–—”‡•
‘ˆ ‘͵Ǧʹǡ xǦ‡ʹ ƒ† ‰Ȁ‡ʹ …ƒ–ƒŽ›•–• ƒ”‡ ‹ –Š‡
”ƒ‰‡ ‘ˆ ͳͲͲǦ͵ͲͲ ι ȏ͹ȂͻȐǤ  …‘–”ƒ•–ǡ ‘„Ž‡ ‡–ƒŽ …ƒ–ƒŽ›•–•
•—…Šƒ•—ǡ†ƒ†–…ƒ‡ˆˆ‡…–‹˜‡Ž›”‡‘˜‡ƒ–Ž‘™–‡Ǧ
’‡”ƒ–—”‡ ȏͳͲȂͳʹȐǤ ‘‰ –Š‡ǡ •—’’‘”–‡† – …ƒ–ƒŽ›•–• Šƒ˜‡
„‡‡’”‘˜‡–‘„‡–Š‡‘•–ƒ…–‹˜‡ȏͳͲǡͳ͵ȂͳͷȐǤ
˜ƒ”‹‡–› ‘ˆ ‘š‹†‡Ǧ•—’’‘”–‡† — …ƒ–ƒŽ›•–•ǡ •—…Š ƒ•
—Ȁ‘͵ͶǦ‡ʹǡ —Ȁ”ʹǡ ƒ† —Ȁ‡ʹǡ Šƒ˜‡ „‡‡ –‡•–‡† ˆ‘”
…ƒ–ƒŽ›–‹…‘š‹†ƒ–‹‘ȏͳ͸ȂʹʹȐǤŠƒ‰‡–ƒŽǤȏʹͲȐ•—……‡••ˆ—ŽŽ›
•›–Š‡•‹œ‡† –Š”‡‡Ǧ†‹‡•‹‘ƒŽŽ› ‘”†‡”‡† ƒ…”‘’‘”‘—• ͵
—Ȁ‡ʹ…ƒ–ƒŽ›•–ǡ™Š‹…Š™ƒ•ˆ‘—†–‘‡šŠ‹„‹–•—’‡”‹‘”…ƒ–ƒŽ›–‹…
ƒ…–‹˜‹–›ƒ•‡š‡’Ž‹ˆ‹‡†„›ͳͲͲΨ…‘˜‡”•‹‘ƒ–͹ͷιǤŠ‡
—‹“—‡•–”—…–—”‡‘ˆ͵‡ʹˆƒ˜‘”‡†Š‹‰Š‰‘Ž††‹•’‡”•‹‘•ǡ
™Š‹…Š ™ƒ• „‡Ž‹‡˜‡† –‘ „‡ ƒ ‡› ˆƒ…–‘” ‹ –Š‡ ‡Šƒ…‡‡– ‘ˆ
…ƒ–ƒŽ›–‹…‡ˆˆ‹…‹‡…›ˆ‘”‘š‹†ƒ–‹‘Ǥ‡…‡–Ž›ǡƒ‡–ƒŽǤȏͳ͹Ȑ
”‡’‘”–‡† –Šƒ– ͷͲΨ …‘˜‡”•‹‘ ™ƒ• ƒ…Š‹‡˜‡† ‘˜‡” ƒ
‡•‘’‘”‘—• —Ȁ‘͵Ͷ …ƒ–ƒŽ›•– ƒ– ”‘‘ –‡’‡”ƒ–—”‡Ǥ – ™ƒ•
ˆ‘—† –Šƒ– …‘—Ž† „‡ ‘š‹†‹œ‡† ‹–‘ ˆ‘”ƒ–‡ „› ‘͵Ϊǡ ƒ†
…‘—Ž† „‡ ˆ—”–Š‡” –”ƒ•ˆ‘”‡† ‹–‘ „‹…ƒ”„‘ƒ–‡ ‘” …ƒ”„‘ƒ–‡
ȗ‘””‡•’‘†‹‰ƒ—–Š‘”Ǥ‡ŽǣΪͺ͸ǦͶͳͳǦͺͶͻͺ͸Ͳͺ͵ǢǦƒ‹Žǣ…Š—ƒ•Š‹̷†Ž—–Ǥ‡†—Ǥ… Š‹• ™‘” ™ƒ• •—’’‘”–‡† „› –Š‡ ƒ–‹‘ƒŽ ƒ–—”ƒŽ …‹‡…‡ ‘—†ƒ–‹‘ ‘ˆ Š‹ƒ ȋʹͳ͵͹͵Ͳ͵͹ǡ ʹͳͷ͹͹Ͳͳ͵Ȍǡ Š‹ƒ ‘•–†‘…–‘”ƒŽ …‹‡…‡ ‘—†ƒ–‹‘
ȋʹͲͳͶͷ͸ͲʹͲͳȌǡƒ†–Š‡—†ƒ‡–ƒŽ‡•‡ƒ”…Š—†•ˆ‘”–Š‡‡–”ƒŽ‹˜‡”•‹–‹‡•ȋͳͷͶͻǡͳ͸ʹʹͶȌǤ ǣͳͲǤͳͲͳ͸Ȁͳͺ͹ʹǦʹͲ͸͹ȋͳ͸Ȍ͸ʹͶ͹ͲǦͳȁŠ––’ǣȀȀ™™™Ǥ•…‹‡…‡†‹”‡…–Ǥ…‘Ȁ•…‹‡…‡ȀŒ‘—”ƒŽȀͳͺ͹ʹʹͲ͸͹ȁŠ‹ǤǤƒ–ƒŽǤǡ‘ŽǤ͵͹ǡ‘ǤͳͲǡ…–‘„‡”ʹͲͳ͸ ͳ͹͵Ͳ
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
•’‡…‹‡•ǡ™Š‹…Š–Š‡†‡…‘’‘•‡†‹–‘ʹƒ†ʹǤ
 ‘—” ’”‡˜‹‘—• •–—†›ǡ ”‡†—…‹„Ž‡ ‡ʹ ƒ† ‡x •—’’‘”–‡†
ƒ‘Ǧ‰‘Ž† …ƒ–ƒŽ›•–• ™‡”‡ ‹˜‡•–‹‰ƒ–‡† ˆ‘” …ƒ–ƒŽ›–‹… ‘š‹Ǧ
†ƒ–‹‘ǡ —Ȁ‡ʹ …ƒ–ƒŽ›•– ’”‡’ƒ”‡† „› †‡’‘•‹–‹‘Ǧ’”‡…‹’‹–ƒ–‹‘
ȋȌ ‡–Š‘† —•‹‰ —”‡ƒ ƒ• ’”‡…‹’‹–ƒ–• ƒ† —Ȁ‡x …ƒ–ƒŽ›•–
’”‡’ƒ”‡†„›…‘Ǧ’”‡…‹’‹–ƒ–‹‘ƒ†…ƒŽ…‹‡†ƒ–ʹͲͲι•Š‘™‡†–Š‡
„‡•–…ƒ–ƒŽ›–‹…ƒ…–‹˜‹–›ǡ…‘’Ž‡–‡‘š‹†ƒ–‹‘‘ˆ‹–‘ʹƒ†
ʹ „‡‹‰ ƒ…Š‹‡˜‡† ƒ– ”‘‘ –‡’‡”ƒ–—”‡ ƒ† ‹ Š—‹† ƒ‹”
ȏʹ͵ǡʹͶȐǤ —…Š ”‡†—…‹„Ž‡ ‘š‹†‡• •Š‘™ •–”‘‰ ‹–‡”ƒ…–‹‘ ™‹–Š
•—’’‘”–‡† ƒ‘Ǧ‰‘Ž† ’ƒ”–‹…Ž‡•ǡ Ž‡ƒ†‹‰ –‘ ™‡ƒ‡ ‡Ȃ ƒ†
‡Ȃ „ƒ†ǡ ƒ† ‹…”‡ƒ•‡ –Š‡ ”‡†—…‹„‹Ž‹–› ”‡ƒ…–‹˜‹–› ‘ˆ –Š‡•‡
•—”ˆƒ…‡ ƒ…–‹˜‡ ‘š›‰‡ •’‡…‹‡• –‘™ƒ”†• ‘š‹†ƒ–‹‘
ȏʹͷȂʹ͹ȐǤ
ƒ”‡…‡–•–—†›ǡ™‡”‡’‘”–‡†ˆ‘”–Š‡ˆ‹”•––‹‡–Šƒ–ɀǦŽʹ͵
•—’’‘”–‡†—™ƒ•ƒ˜‡”›ƒ…–‹˜‡…ƒ–ƒŽ›•–ˆ‘”‘š‹†ƒ–‹‘ƒ–
”‘‘–‡’‡”ƒ–—”‡‡˜‡‹–Š‡’”‡•‡…‡‘ˆ‘‹•–—”‡ȏʹͺȐǤ–‹•
ˆ‘—† –Šƒ– ƒŽ–Š‘—‰Š –Š‡”‡ ‹• ‘ ƒ…–‹˜‡ •—”ˆƒ…‡ ‘š›‰‡ ‘
ɀǦŽʹ͵ǡ •—”ˆƒ…‡ Š›†”‘š›Ž• Šƒ˜‡ –Š‡ ƒ„‹Ž‹–› –‘ ’ƒ”–‹ƒŽŽ› ‘š‹†‹œ‡
‹–‘ ˆ‘”ƒ–‡ ‹–‡”‡†‹ƒ–‡•ǡ ™Š‹…Š …ƒ „‡ ˆ—”–Š‡” ‘š‹Ǧ
†‹œ‡†‹–‘ʹƒ†ʹ„›ƒ‘Ǧ—ȏʹͺȐǤŠ‹••–—†›…ŠƒŽŽ‡‰‡•
–Š‡ –”ƒ†‹–‹‘ƒŽ ‹†‡ƒ ‘ˆ •—’’‘”–‹‰ ‘„Ž‡ ‡–ƒŽ• ‘ ”‡†—…‹„Ž‡
‘š‹†‡•ˆ‘”‘š‹†ƒ–‹‘ƒ–”‘‘–‡’‡”ƒ–—”‡ȏʹͺȐǤ
‡”‡‹ǡ —†‡” •‹‹Žƒ” …‘†‹–‹‘•ǡ ™‡ …‘’ƒ”‡ –Š‡ …ƒ–ƒŽ›–‹…
’”‘’‡”–‹‡• ‘ˆ —Ȁ‡ʹǡ —Ȁ‡xǡ —ȀɀǦŽʹ͵ǡ —ȀǦͷ ƒ†
—Ȁ‹ʹ …ƒ–ƒŽ›•–• ˆ‘” ‘š‹†ƒ–‹‘ ƒ– ”‘‘ –‡’‡”ƒ–—”‡Ǥ
Š‡‰‘ƒŽ‘ˆ–Š‡’”‡•‡–•–—†›‹•–‘’”‘˜‹†‡ƒ…Ž‡ƒ”‹ƒ‰‡‘–Š‡
‡ˆˆ‡…–‘ˆ”‡†—…‹„‹Ž‹–›‘ˆ–Š‡•—’’‘”–•ˆ‘”‰‘Ž†…ƒ–ƒŽ›•‹•ƒ†–Š‡
ˆƒ…–‘”• –Šƒ– ‹ˆŽ—‡…‡ –Š‡ ‰‘Ž† …ƒ–ƒŽ›•–•ǯ ƒ…–‹˜‹–› ƒ† •–ƒ„‹Ž‹–›
ˆ‘”‘š‹†ƒ–‹‘Ǥ
2. Experimental
2.1. Catalystspreparation —ȀɀǦŽʹ͵ǡ —Ȁ‡ʹ ƒ† —Ȁ‡x •ƒ’Ž‡• ™‹–Š ‘‹ƒŽ
‰‘Ž†…‘–‡–•‘ˆͳ™–Ψ™‡”‡’”‡’ƒ”‡†„›‡–Š‘†™‹–Š—”‡ƒ
ƒ•–Š‡’”‡…‹’‹–ƒ–Ǥ›’‹…ƒŽŽ›ǡʹǤͳ‘ˆ—ŽͶ•‘Ž—–‹‘ȋͲǤͲʹͶ
‘ŽȀȌǡ ͲǤ͵ͺ ‰ ‘ˆ —”‡ƒ ȋ—”‡ƒȀ— α ͳʹͷǡ ‘Žƒ” ”ƒ–‹‘Ȍǡ ͳǤͲ ‰
ɀǦŽʹ͵ǡ ‡ʹ ‘” ‡x ȋɀǦŽʹ͵ ’”‘˜‹†‡† „› ƒœŠ‘— ‡–”‘Ǧ
…Š‡‹…ƒŽ ‘’ƒ› ‡–”‘Ž‡—ǡ ‡ʹ ’”‘˜‹†‡† „› ‹ƒŒ‹ ƒ›ŽǦ
‹‡™ƒ–‡”‹ƒŽ•‘Ǥǡ–†Ǥƒ†‡x™ƒ•’”‡’ƒ”‡†ƒ……‘”†‹‰–‘
ƒ…‘Ǧ’”‡…‹’‹–ƒ–‹‘‡–Š‘†ȏʹͻȐȌ’‘™†‡”•ȋ‡•Š•‹œ‡εͳͲͲȌƒ†
ͳͷͲ  ‘ˆ †‡‹‘‹œ‡† ™ƒ–‡” ™‡”‡ …‘Ǧƒ††‡† ‹–‘ ƒ –Š”‡‡Ǧ‡…
ˆŽƒ•‹š‡†ƒ†‡“—ƒ–‡Ž›‹–Š‡™ƒ–‡”„ƒ–Š–Š‡”‘•–ƒ–‡†ƒ–ͺͲιǡ
ƒ†–Š‡ˆŽƒ•™ƒ•…‘˜‡”‡†™‹–Šƒ‘’ƒ“—‡’ƒ…ƒ‰‡–‘‡‡’‘ˆˆ
–Š‡ ”‘‘ Ž‹‰Š–Ǥ Š‡ •—•’‡•‹‘• ™‡”‡ –Š‡ •–‹””‡† ˜‹‰‘”‘—•Ž›
ˆ‘” ͺ Š ȋˆ‹ƒŽ ’ γ ͹ǤͲȌǡ ˆ‘ŽŽ‘™‡† „› ‘˜‡”‹‰Š– ƒ‰‹‰ ƒ– ”‘‘
–‡’‡”ƒ–—”‡Ǥ Š‡ •‘Ž‹† ™ƒ• ˆ‹Ž–‡”‡† ƒ† ™ƒ•Š‡† ‡š–‡•‹˜‡Ž›
™‹–Š †‡‹‘‹œ‡† ™ƒ–‡” —–‹Ž ‹– ™ƒ• ˆ”‡‡ ‘ˆ …ŠŽ‘”‹†‡ ‹‘•ǡ –Š‡
†”‹‡†ƒ–ͺͲιˆ‘”ͺŠƒ†…ƒŽ…‹‡†ƒ–͵ͲͲ鋐ƒ‹”ˆ‘”ͶŠǤ
Š‡ —ȀǦͷ ȋ‹ʹȀŽʹ͵ α ͷͲͲȌ ƒ† —Ȁ‹ʹ …ƒ–ƒŽ›•–•
™‹–Š ‘‹ƒŽ — …‘–‡–• ‘ˆ ͳ ™–Ψ ™‡”‡ ’”‡’ƒ”‡† „› ƒ ‡–Š‘†™‹–Š͵ȉʹƒ•–Š‡’”‡…‹’‹–ƒ–Ǥ›’‹…ƒŽŽ›ǡƒƒ“—‡‘—•
•‘Ž—–‹‘‘ˆ—ŽͶȋͲǤͲʹͶ‘ŽȀȌǡǦͷ‘”‹ʹ•—’’‘”–ȋͳǤͲ
‰ȌȋǦͷ‹ʹȀŽʹ͵αͷͲͲǡƒƒ‹‹˜‡”•‹–›ǡŠ‹ƒƒ†‹ʹ
‹•’”‘˜‹†‡†„›‹‰†ƒ‘ƒ‹›ƒ‰Š‡‹…ƒŽ‘Ǥǡ–†Ȍƒ††‹•–‹ŽŽ‡†
™ƒ–‡” ȋͷͲ Ȍ ™‡”‡ …‘Ǧƒ††‡† –‘ ƒ –Š”‡‡Ǧ‡…‡† ˆŽƒ• ƒ†
‹š‡† ƒ†‡“—ƒ–‡Ž›ǤŠ‡ •Ž—””› ™ƒ••–‹””‡† ƒ– ͸Ͳιˆ‘”͵Ͳ‹ǡ
–Š‡ ƒ“—‡‘—• ͵ȉʹ •‘Ž—–‹‘ ȋͳ ‘ŽȀȌ ™ƒ• ƒ††‡† —†‡”
•–‹””‹‰–‘ƒ†Œ—•––Š‡’‘ˆ–Š‡•›•–‡–‘ƒ„‘—–ͻǡˆ‘ŽŽ‘™‡†„›
•–‹””‹‰ƒ–͸Ͳιˆ‘”ͺŠǤˆ–‡”–Šƒ–ǡ–Š‡”‡•—Ž–‹‰’”‡…‹’‹–ƒ–‡™ƒ•
ˆ‹Ž–‡”‡†ƒ†™ƒ•Š‡†™‹–ŠŠ‘–†‹•–‹ŽŽ‡†™ƒ–‡”ǡ–Š‡†”‹‡†ƒ–͸Ͳι
ˆ‘” ͸ Š ƒ† •–‘”‡† ‹ †ƒ”‡••Ǥ Š‡ •‘Ž‹† ™ƒ• –Š‡ –”‡ƒ–‡† ƒ–
͵ͲͲ ι ‹ ”‡†—…‹„Ž‡ ƒ–‘•’Š‡”‡• ȋͳͲΨ ʹ ‹ ʹǡ ͺͲ Ȁ‹Ȍ
ˆ‘”ͶŠ–‘‘„–ƒ‹–Š‡ˆ‹ƒŽ…ƒ–ƒŽ›•–•Ǥ
2.2. Catalystcharacterization Š‡ ƒ…–—ƒŽ — …‘–‡– ‹ ‡ƒ…Š •ƒ’Ž‡ ™ƒ• †‡–‡”‹‡† „›
‹†—…–‹˜‡Ž› …‘—’Ž‡† ’Žƒ•ƒǦƒ–‘‹… ‡‹••‹‘ •’‡…–”‘•…‘’›
ȋǦǡ’–‹ƒʹͲͲͲǡȌǤ•—”ˆƒ…‡ƒ”‡ƒ†‡–‡”‹ƒǦ
–‹‘• ™‡”‡ ’‡”ˆ‘”‡† —•‹‰ ƒ ‹–”‘‰‡ ƒ†•‘”’–‹‘ ƒ’’ƒ”ƒ–—•
ȋ‹…”‘‡”‹–‹…•ǡ ”‹•–ƒ” ͵ͲͲͲȌǤ ‹‰ŠǦ”‡•‘Ž—–‹‘ –”ƒ•‹••‹‘
‡Ž‡…–”‘ ‹…”‘•…‘’› ȋȌ ‹…”‘‰”ƒ’Š• ™‡”‡ ‘„–ƒ‹‡†
™‹–Šƒ ‡…ƒ‹
ʹʹͲ Ǧ‹…”‘•…‘’‡ ƒ†‘’‡”ƒ–‡† ƒ–ʹͲͲ
Ǥ
”ƒ•‹••‹‘‡Ž‡…–”‘‹…”‘•…‘’›ȋȌ‹ƒ‰‡•‘ˆ–Š‡…ƒ–Ǧ
ƒŽ›•–•™‡”‡‘„–ƒ‹‡†‘ƒǦʹͲͲͲ‹…”‘•…‘’‡‘’‡”Ǧ
ƒ–‡†ƒ–ʹͲͲǤ‡ˆ‘”‡‘„•‡”˜ƒ–‹‘ǡ–Š‡•ƒ’Ž‡•™‡”‡—Ž–”ƒ•‘Ǧ
‹…ƒŽŽ›†‹•’‡”•‡†‹‡–Šƒ‘Žƒ†–Š‡ƒ†”‘’‘ˆ–Š‡•‘Ž—–‹‘™ƒ•
’—–‘–‘‹…”‘‰”‹†…ƒ”„‘’‘Ž›‡”•—’’‘”–‡†‘…‘’’‡”‰”‹†Ǥ
– Ž‡ƒ•– ͳͲͲ — ƒ‘’ƒ”–‹…Ž‡• ™‡”‡ ‡ƒ•—”‡† –‘ ƒƒŽ›œ‡ –Š‡
’ƒ”–‹…Ž‡•‹œ‡†‹•–”‹„—–‹‘Ǥ
‡’‡”ƒ–—”‡ ’”‘‰”ƒ‡† ‘š‹†ƒ–‹‘ ȋȌ ‡š’‡”‹‡–•
™‡”‡—•‡†–‘•–—†›–Š‡†‡’‘•‹–•‘–Š‡ƒŽŽ–Š‡•’‡–—ȀɀǦŽʹ͵ǡ
—Ȁ‹ʹǡ—ȀǦͷǡ—Ȁ‡ʹƒ†—Ȁ‡x…ƒ–ƒŽ›•–•ǡƒˆ–‡”͵͸Ͳ
‹‘ˆ”‡ƒ…–‹‘ǤŠ‡…ƒ–ƒŽ›•–•™‡”‡’—”‰‡†™‹–Šƒ†”›•‹—Žƒ–Ǧ
‡† ƒ‹” •–”‡ƒ ȋͳͲͲ Ȁ‹Ȍ ƒ– ”‘‘ –‡’‡”ƒ–—”‡ ˆ‘” ͵Ͳ ‹
’”‹‘” –‘ –Š‡ ‡š’‡”‹‡–Ǥ Š‡ –‡’‡”ƒ–—”‡ ™ƒ• Š‡ƒ–‡† ˆ”‘
”‘‘ –‡’‡”ƒ–—”‡ –‘ ͶͲͲ ι ƒ– ƒ ”ƒ–‡ ‘ˆ ͳͲ ιȀ‹ ‹ ƒ ƒ‹”
ˆŽ‘™ ƒ† –Š‡ ‰ƒ• ’”‘†—…–• ™‡”‡ ƒƒŽ›œ‡† „› –Š‡ ‘ǦŽ‹‡ x
ƒƒŽ›œ‡” ƒ† ƒ•• •’‡…–”‘‡–‡” ȋȌǤ ‘ ‘–Š‡” …ƒ”Ǧ
„‘Ǧ…‘–ƒ‹‹‰ …‘’‘—†• ‡š…‡’– ʹ ‹ –Š‡ ’”‘†—…–• ™‡”‡
†‡–‡…–‡†ˆ‘”ƒŽŽ–Š‡–‡•–‡†…ƒ–ƒŽ›•–•Ǥ
2.3. Measurementofcatalyticactivity Š‡ƒ…–‹˜‹–›‘ˆ…ƒ–ƒŽ›•–•‹‘š‹†ƒ–‹‘™ƒ•…ƒ””‹‡†‘—–
‹ ƒ ˆ‹š‡†Ǧ„‡† “—ƒ”–œ ”‡ƒ…–‘” ȋ‹Ǥ†Ǥ α Ͷ ȌǤ ͳͲ ‰ …ƒ–ƒŽ›•–
’‘™†‡”†‹Ž—–‡†™‹–ŠͷͲ‰‹ʹ™ƒ•Ž‘ƒ†‡†‹–Š‡“—ƒ”–œ”‡ƒ…Ǧ
–‘”Ǥˆ‡‡†‰ƒ•ȋͺͲ’’ǡʹͳ˜‘ŽΨʹǡͳǤ͸˜‘ŽΨʹȋα
ͷͲΨǡ ʹͷ ιȌǡ ƒ† „ƒŽƒ…‡† ™‹–Š ʹȌ ™ƒ• ƒŽŽ‘™‡† –‘ ’ƒ••
–Š”‘—‰Š–Š‡…ƒ–ƒŽ›•–„‡†ƒ–ƒˆŽ‘™”ƒ–‡‘ˆͳͲͲŽȀ‹ǡ”‡•—Ž–‹‰
‹ƒ•’ƒ…‡˜‡Ž‘…‹–›ȋȌ‘ˆ͸ͲͲͲͲͲŽȀȋ‰ȉŠȌǤŽŽ–Š‡ˆ‡‡†‰ƒ•‡•
—•‡†‹–Š‹•™‘”™‡”‡‘ˆŠ‹‰ŠǦ’—”‹–›‰”ƒ†‡ȋͻͻǤͻͻͻΨȌǤŠ‡‰ƒ•
ˆŽ‘™ ”ƒ–‡• ™‡”‡ …‘–”‘ŽŽ‡† „› ƒ•• ˆŽ‘™ …‘–”‘ŽŽ‡”•Ǥ ƒ•‡‘—•
™ƒ• ‰‡‡”ƒ–‡† „› ˆŽ‘™‹‰ ʹ ‘˜‡” ’ƒ”ƒˆ‘”ƒŽ†‡Š›†‡
ȋͻͻΨǡŽ†”‹…ŠȌ‹ƒ–Š‡”‘•–ƒ–‡†„ƒ–Šƒ†–Š‡…‘…‡–”ƒ–‹‘‘ˆ
™ƒ•…‘–”‘ŽŽ‡†„›ƒ†Œ—•–‹‰–Š‡ˆŽ‘™”ƒ–‡‘ˆʹƒ†–Š‡
–‡’‡”ƒ–—”‡ ‘ˆ –Š‡ –Š‡”‘•–ƒ–‡† „ƒ–ŠǤ ƒ•‡‘—• ʹ ™ƒ• …ƒ”Ǧ
”‹‡†‹–‘–Š‡ ‰ƒ• •–”‡ƒ „›’ƒ••‹‰ ʹ–Š”‘—‰Šƒ„—„„Ž‡”‹ ƒ
™ƒ–‡” „ƒ–Š ƒ– ”‘‘ –‡’‡”ƒ–—”‡Ǥ Š‡ ƒ‘—– ‘ˆ ™ƒ–‡” ™ƒ•
…‘–”‘ŽŽ‡† „› ƒ†Œ—•–‹‰ –Š‡ ˆŽ‘™ ”ƒ–‡ ‘ˆ ʹǡ ™Š‹Ž‡ ‡‡’‹‰ –Š‡
–‘–ƒŽ ˆŽ‘™ …‘•–ƒ–Ǥ Š‡ Ȁʹ ƒ† ʹȀʹ •–”‡ƒ• ™‡”‡
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
–Š‡ ‹š‡† ™‹–Š –Š‡ ƒ‹ ‰ƒ• •–”‡ƒ ‘ˆ ʹȀʹǡ Ž‡ƒ†‹‰ –‘ ƒ
–›’‹…ƒŽˆ‡‡†‰ƒ•Ǥ ‘…‡–”ƒ–‹‘• ‘ˆ ƒ† ʹ ™‡”‡ ‡ƒ•—”‡† —•‹‰ ƒ
‘Ž‹‡ ‘Ǧ†‹•’‡”•‹˜‡ ‹ˆ”ƒ”‡† ƒƒŽ›œ‡” ȋǦǦ͹ͳͲǡ
‡”ƒ›ȌǤ  –Š‹• ™‘”ǡ ‹– ™ƒ• ‘– ’‘••‹„Ž‡ –‘ ‘‹–‘” –Š‡
…‘…‡–”ƒ–‹‘ †‹”‡…–Ž› „› ‘—”‹‡” –”ƒ•ˆ‘”Ǧ‹ˆ”ƒ”‡†
•’‡…–”‘•…‘’› ȋǦȌ †—‡ –‘ –Š‡ ‹–‡”ˆ‡”‹‰ ‡ˆˆ‡…–• ‘ˆ ™ƒ–‡”Ǥ
Š‡”‡ˆ‘”‡ǡ ™ƒ• ‡ƒ•—”‡† „› …‘˜‡”–‹‰ ‹– –‘ ʹ ‹ ƒ
Š‘‡ƒ†‡ Ǧ–‘Ǧʹ …‘˜‡”–‡” ȋ—ǦʹȀɀǦŽʹ͵ …ƒ–ƒǦ
Ž›•–Ȍ ƒ– ͵ͲͲ ι ƒ† †‡–‡”‹‹‰ –Š‡ ƒ‘—– ‘ˆ ʹ ˆ‘”‡†Ǥ
‡˜‡”ƒŽ’”‡˜‹‘—•”‡’‘”–•Šƒ†’‘‹–‡†‘—––Šƒ–ˆ‘”–Š‡ƒ……—”ƒ–‡
†‡–‡”‹ƒ–‹‘ ‘ˆ ǡ –Š‡ •Š‘—Ž† ˆ‹”•– „‡ ‘š‹†‹œ‡† –‘
ʹ ȏ͵ͲȂ͵ʹȐǤ  –›’‹…ƒŽ ”—•ǡ –Š‡ ”‡ƒ…–‹‘ †ƒ–ƒ ™‡”‡ ‘„–ƒ‹‡†
ƒˆ–‡” ‘š‹†ƒ–‹‘ ™ƒ• ’‡”ˆ‘”‡† ˆ‘” ͶͲ ‹ ‹ ‘”†‡” –‘
ƒ…Š‹‡˜‡ –Š‡ •–‡ƒ†› •–ƒ–‡Ǥ ‘ ‘–Š‡” …ƒ”„‘Ǧ…‘–ƒ‹‹‰ …‘Ǧ
’‘—†• ‡š…‡’– ʹ ‹ –Š‡ ’”‘†—…–• ™‡”‡ †‡–‡…–‡† ˆ‘” ƒŽŽ –Š‡
–‡•–‡†…ƒ–ƒŽ›•–•Ǥ
Š‡…‘˜‡”•‹‘‘ˆ™ƒ•…ƒŽ…—Žƒ–‡†ƒ•ˆ‘ŽŽ‘™•ǣ
…‘˜‡”•‹‘ȋΨȌαȏʹȐ‘—–ȀȏȐ‹uͳͲͲΨǡ
™Š‡”‡ ȏʹȐ‘—– ‹• –Š‡ ʹ …‘…‡–”ƒ–‹‘ ‹ –Š‡ ’”‘†—…– ‰ƒ•
•–”‡ƒȋ˜‘ŽΨȌƒ†ȏȐ‹‹•–Š‡…‘…‡–”ƒ–‹‘‹–Š‡
ˆ‡‡†‰ƒ•ȋ˜‘ŽΨȌǤ
‹‡–‹… ‡ƒ•—”‡‡–• ™‡”‡ …‘†—…–‡† ‹ ƒ ˆ‹š‡†Ǧ„‡† ˆŽ‘™
‹…”‘Ǧ”‡ƒ…–‘”ǡ ‡‡’‹‰ –Š‡ …‘˜‡”•‹‘ „‡Ž‘™ ʹͲΨǤ Š‡
•ƒ’Ž‡•™‡”‡Š‡ƒ–‡†‹ʹˆ”‘͵Ͳ–‘͹Ͳιǡ–Š‡–Š‡‰ƒ•™ƒ•
•™‹–…Š‡†–‘–Š‡ˆ‡‡†‰ƒ•ȋͺͲ’’ǡʹͳ˜‘ŽΨʹǡͳǤ͸˜‘ŽΨ
ʹ ƒ† „ƒŽƒ…‡† ™‹–Š ʹǡ ˆŽ‘™ ”ƒ–‡ ͳͲͲ Ȁ‹ǡ ͷǦͳͲ ‰
•ƒ’Ž‡™ƒ•—•‡†–‘…Šƒ‰‡–Š‡…‘–ƒ…––‹‡•—…Š–Šƒ––Š‡…‘Ǧ
˜‡”•‹‘”‡ƒ‹‡†δʹͲΨȌǤŠ‡‰ƒ•’”‘†—…–•™‡”‡ƒƒŽ›œ‡†„›
–Š‡‘ǦŽ‹‡xƒƒŽ›œ‡”Ǥ
3. Resultsanddiscussion
‡ʹǡ‡xǡɀǦŽʹ͵ǡ‹ʹǡƒ†Ǧͷ•—’’‘”–‡†ͳ™–Ψ—
…ƒ–ƒŽ›•–• ƒ”‡ ‡˜ƒŽ—ƒ–‡† ˆ‘” ‘š‹†ƒ–‹‘ ƒ– ”‘‘ –‡’‡”ƒǦ
–—”‡ —†‡” Š—‹† ƒ‹” ƒ† Š‹‰Š ‘ˆ ͸ͲͲͲͲͲ ŽȀȋ‰ȉ•Ȍǡ ƒ†
–Š‡”‡•—Ž–•ƒ”‡•Š‘™‹‹‰ǤͳȋƒȌǤ—ȀɀǦŽʹ͵…ƒ–ƒŽ›•–‡šŠ‹„‹–•
–Š‡Š‹‰Š‡•–…‘˜‡”•‹‘‘ˆ…ƒǤͺͺΨƒ––Š‡„‡‰‹‹‰‘ˆ–Š‡
lnr (Pmol/(gcat˜s)
HCHO conversion to CO2 (%)
Fig.2. ʹǦ’”‘ˆ‹Ž‡•‘ˆ˜ƒ”‹‘—•‘š‹†‡•—’’‘”–‡†—…ƒ–ƒŽ›•–•Ǥ
Au/J-Al2O3
Ea = 9 r 1 kJ/mol
-1.5
Au/SiO2
Ea = 10 r1 kJ/mol
Au/CeO2
-2.0
Ea = 13 r 1 kJ/mol
Au/HZ
Ea = 13 r1 kJ/mol
-2.5
20
120 150 180 210 240 270 300
Temperature (oC)
100
80
40
90
(b)
-1.0
60
60
”‡ƒ…–‹‘ǡƒ†”‡ƒ‹•–Š‡…‘˜‡”•‹‘Š‹‰Š‡”–Šƒ ͹ͺΨ™‹–Š‹
ʹͷͲ ‹Ǥ Š‡ …‘˜‡”•‹‘ †‡…”‡ƒ•‡• –‘ ͹͵Ψ —’‘ ͵͸Ͳ ‹ ‘ˆ
”‡ƒ…–‹‘ǡ™Š‹…Š‹••–‹ŽŽ–Š‡‘•–ƒ…–‹˜‡…ƒ–ƒŽ›•–ǤŠ‘—‰Š—Ȁ‹ʹ
…ƒ–ƒŽ›•–•Š‘™•ƒŠ‹‰Š‡”…‘˜‡”•‹‘‘ˆ͹ͻΨƒ–‹–•‹‹–‹ƒŽǡ‹–
†‡ƒ…–‹˜ƒ–‡•ˆƒ•–™‹–Š‹–Š‡ˆ‹”•–ͳͲͲ‹ǡƒ†–Š‡†‡…”‡ƒ•‡•ƒ–
ƒ•Ž‘™‡””ƒ–‡Ǥ —ȀǦͷ …ƒ–ƒŽ›•–‡šŠ‹„‹–•ƒ •‹‹Žƒ” †‡ƒ…–‹˜ƒǦ
–‹‘ –”‡† ƒ• —Ȁ‹ʹ …ƒ–ƒŽ›•–ǡ „—– –Š‡ ‹‹–‹ƒŽ ƒ…–‹˜‹–› ‹• Ž‘™‡”ǡ
–Š‡‹‹–‹ƒŽ…‘˜‡”•‹‘‹•‘Ž›…ƒǤͶͶΨǤ•–‘–Š‡‡ʹƒ†‡x
•—’’‘”–‡†—…ƒ–ƒŽ›•–•ǡ–Š‡‹‹–‹ƒŽƒ…–‹˜‹–‹‡•—†‡”•—…ŠŠ‹‰Š‡”
ƒ”‡ “—‹–‡ Ž‘™‡”ǡ ƒ† –Š‡› ‡šŠ‹„‹– ƒ ‰”ƒ†—ƒŽ †‡…”‡ƒ•‡†
ƒ…–‹˜‹–›™‹–Š–‹‡‘•–”‡ƒǤ Ž•‘ǡ –Š‡ ‹‡–‹… –‡•–• ƒ”‡ …‘†—…–‡† –‘ ˆ—”–Š‡” …Š‡… –Š‡
•—’’‘”–•ǯ‡ˆˆ‡…–‘…‘˜‡”•‹‘Ǥ‹‰Ǥͳȋ„Ȍ•Š‘™•””Š‡‹Ǧ
—•’Ž‘–•ˆ‘”–Š‡”ƒ–‡‘ˆ‘š‹†ƒ–‹‘ƒ––Š‡…‘˜‡”•‹‘δʹͲΨ
ȋ–Š‡†ƒ–ƒƒ”‡…‘ŽŽ‡…–‡†ƒ––Š‡”‡Žƒ–‹˜‡Ž›•–ƒ„Ž‡•–ƒ‰‡‘ˆͶͲ‹ǯ•
”‡ƒ…–‹‘ƒ–™Š‹…Š–Š‡”‡ƒ…–‹‘–‡’‡”ƒ–—”‡”ƒ‰‡™ƒ•ˆ”‘͵Ͳ
–‘͹ͲιȌǤ–‹•…Ž‡ƒ”–Šƒ––Š‡ƒ’’ƒ”‡–‡‡”‰›†‹ˆˆ‡”•ˆ”‘ͻ–‘
ͳͶ Ȁ‘Žǡ ƒ† ˆ‘ŽŽ‘™• –Š‡ ‘”†‡” ‘ˆ —ȀɀǦŽʹ͵ δ —Ȁ‹ʹ δ
—ȀǦͷ γ —Ȁ‡ʹ δ —Ȁ‡xǤ Š‡ “—‹–‡ Ž‘™‡” ƒ’’ƒ”‡–
‡‡”‰›‹†‹…ƒ–‡•–Š‡Š‹‰Šƒ…–‹˜‹–‹‡•‘ˆ–Š‡•‡•—’’‘”–‡†—…ƒ–ƒǦ
Ž›•–• ˆ‘” ‘š‹†ƒ–‹‘ƒ–”‘‘–‡’‡”ƒ–—”‡Ǥ †–Š‡‘”†‡”
ˆ—”–Š‡”ƒ……‘—–•ˆ‘”–Š‡‹†‹”‡…–‡ˆˆ‡…–‘ˆ–Š‡”‡†—…‹„‹Ž‹–›‘ˆ–Š‡
•—’’‘”–• ˆ‘” ‰‘Ž† …ƒ–ƒŽ›•‹• ‹ ‘š‹†ƒ–‹‘ ”‡ƒ…–‹‘Ǥ ȋŠ‡
ʹǦ ’”‘ˆ‹Ž‡• ‘ˆ ˜ƒ”‹‘—• ‘š‹†‡• •—’’‘”–‡† — …ƒ–ƒŽ›•–• ™ƒ•
•Š‘™‹‹‰ǤʹȌǤ
(a)
Au/J-Al2O3
Au/SiO2
Au/HZ
Au/CeO2
Au/FeOx
ͳ͹͵ͳ
Au/FeOx
Au/CeO2
Au/HZSM-5
Au/SiO2
Au/J-Al2O3
Au/FeOx
HCHO conversion to CO2 (%)
100
20
18
16
14
12
10
8
6
4
2
0
30
Intensity (a.u.)
(c)
3%
80
Initial activity
120 min activity
60
33%
40
15%
4%
20
4%
Ea = 14 r 1 kJ/mol
0
0
-3.0
50 100 150 200 250 300 350
Time (min)
3.00
3.25
1000/T (K1)
3.50
0
3
Al2O Au/SiO2 HZSM-5Au/CeO2 FeOx
J
/
u
A Au/
Au/
Catalyst
Fig.1.ȋƒȌ‘’ƒ”‹•‘‘ˆ…‘˜‡”•‹‘•˜ƒ”‹ƒ–‹‘™‹–Š–‹‡‘˜‡”˜ƒ”‹‘—•‘š‹†‡•—’’‘”–‡†—…ƒ–ƒŽ›•–•Ǥ‡ƒ…–‹‘…‘†‹–‹‘•ǣͺͲ’’ǡʹͳ
˜‘ŽΨʹǡͳǤ͸˜‘ŽΨʹǡʹ„ƒŽƒ…‡ǡ
α͸ͲͲͲͲͲŽȀȋ‰ȉ•ȌǡʹͷιǢȋ„Ȍ””Š‡‹—•Ǧ–›’‡’Ž‘–‘ˆ‘š‹†ƒ–‹‘”‡ƒ…–‹‘”ƒ–‡•‘˜‡”–Š‡•—’’‘”–‡†—
…ƒ–ƒŽ›•–•Ǥ‡ƒ…–‹‘…‘†‹–‹‘•ǣͺͲ’’ǡʹͳ˜‘ŽΨʹǡͳǤ͸˜‘ŽΨʹǡʹ„ƒŽƒ…‡ǡʹͷιǢȋ…Ȍ‘’ƒ”‹•‘‘ˆ–Š‡‹‹–‹ƒŽ…‘˜‡”•‹‘•™‹–Š–Š‘•‡
ƒˆ–‡”ͳʹͲ‹‘ˆ”‡ƒ…–‹‘‘˜‡”•—’’‘”–‡†—…ƒ–ƒŽ›•–•Ǥ
ͳ͹͵ʹ
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
Table1
Š›•‹…‘…Š‡‹…ƒŽ’”‘’‡”–›‘ˆ–Š‡•—’’‘”–‡†—…ƒ–ƒŽ›•–•Ǥ
—”ˆƒ…‡ƒ”‡ƒ
—…‘–‡–
˜‡”ƒ‰‡—•‹œ‡Ǧˆ”‡•Šƒ
‹•’‡”•‹‘„ —ƒ˜‡”ƒ‰‡’ƒ”–‹…Ž‡
…
ȋʹȀ‰Ȍ
ȋȌ
ȋΨȌ
•‹œ‡Ǧ•’‡–ȋȌ
ȋɊ‘ŽȀ‰Ȍ
ȋΨȌ
—ȀɀǦŽʹ͵
ͳͺͻ
ͲǤͺʹ
ͳǤͺ
͸͸Ǥͷ
ʹǤʹ
͵Ͳͻ
—Ȁ‹ʹ
͵͵Ͳ
ͲǤͻʹ
ͳǤ͸
͹ʹǤ͵
͵Ǥͳ
ͳͺͻ
—ȀǦͷ
ʹͳʹ
ͲǤͻͲ
͵ǤͲ
͵ͺǤ͵
ͶǤʹ
ʹͷʹ
—Ȁ‡ʹ
͹ͺ
ͲǤͺ͵
ʹǤ͹
Ͷ͵Ǥͳ
ͶǤͳ
ͷͺ͸
—Ȁ‡x
ͳͺ͹
ͲǤͺͲ
ͶǤͻ
ʹ͵Ǥ͹
ͷǤ͵
Ͷͷʹ
ƒƒŽ…—Žƒ–‡†ˆ”‘–Š‡‹ƒ‰‡ƒ……‘”†‹‰–‘ƒ–Ž‡ƒ•–ͳͲͲ—ƒ‘’ƒ”–‹…Ž‡•‡ƒ•—”‡†–‘ƒƒŽ›œ‡–Š‡’ƒ”–‹…Ž‡•‹œ‡†‹•–”‹„—–‹‘Ǥ
„ƒŽ…—Žƒ–‡†ƒ……‘”†‹‰–‘–Š‡…‘””‡•’‘†‹‰ƒ˜‡”ƒ‰‡—’ƒ”–‹…Ž‡•ˆ”‘†ƒ–ƒȏͶͶȐǤ‘”‡šƒ’Ž‡ǣ–Š‡—„‡”‘ˆ‰‘Ž†’ƒ”–‹…Ž‡•ǣNͳαͳʹm—ȀɎd—͵ɏ—Ǣ
–Š‡‰‘Ž†’ƒ”–‹…Ž‡†‹ƒ‡–‡”ȋd—Ȍ‘ˆ—ȀɀǦŽʹ͵…ƒ–ƒŽ›•–‹•ͳǤͺǡɏ—αͳͻǤ͵uͳͲ͵‰Ȁ͵ǡ–Š‡‘˜‡”ƒŽŽ•—”ˆƒ…‡ƒ”‡ƒ‘ˆ‰‘Ž†’ƒ”–‹…Ž‡•SαͳȀʹɎd—ʹNͳǡ‹•Ǧ
’‡”•‹‘αN•ȀN–αSkȀn—NǡNα–‘–ƒŽ—„‡”‘ˆ•—”ˆƒ…‡‰‘Ž†ƒ–‘•ǡNα–‘–ƒŽ—„‡”‘ˆ‰‘Ž†ƒ–‘•ǡ–Š‡‰‘Ž†ƒ–‘†‡•‹–›ȋkȌ‹•ͳǤͳͷuͳͲͳͻȂʹǡNAα
͸ǤͲʹuͳͲʹ͵‘ŽȂͳǡn—αm—ȀM—
…Š‡ƒ‘—–‘ˆ–Š‡•—”ˆƒ…‡•’‡…‹‡•ƒ……——Žƒ–‡††—”‹‰–Š‡”‡ƒ…–‹‘™ƒ•…ƒŽ…—Žƒ–‡†„›‹–‡‰”ƒ–‹‰–Š‡ƒ”‡ƒ‘ˆ–Š‡’‡ƒˆ‘”‡†‹–Š‡’”‘…‡••Ǥ
ƒ–ƒŽ›•–
‡…‘’ƒ”‡–Š‡‹‹–‹ƒŽ…‘˜‡”•‹‘•ȋ–Š‡†ƒ–ƒ™ƒ•…‘ŽŽ‡…–‡†
ƒ––Š‡…ƒǤͳͲ‹Ȍ™‹–Š–Š‘•‡ƒˆ–‡”ͳʹͲ‹‘ˆ”‡ƒ…–‹‘ˆ‘”‡ƒ…Š
•—’’‘”–‡†—…ƒ–ƒŽ›•–ǡ–Š‡”‡•—Ž–•„‡‹‰•Š‘™‹‹‰Ǥͳȋ…ȌǤ–ǯ•
‘„˜‹‘—•–Šƒ–ˆƒ•–†‡ƒ…–‹˜ƒ–‹‘™‡”‡‘„•‡”˜‡†‘˜‡”—Ȁ‹ʹƒ†
—ȀǦͷ…ƒ–ƒŽ›•–•ǤŠ‹Ž‡—ȀɀǦŽʹ͵ǡ—Ȁ‡ʹƒ†—Ȁ‡x
…ƒ–ƒŽ›•–• †‡ƒ…–‹˜ƒ–‡ ƒ– —…Š •Ž‘™‡” ”ƒ–‡•Ǥ ”‘ ‹‰Ǥ ͳǡ ‹– •—‰Ǧ
‰‡•–• –Šƒ– †‹ˆˆ‡”‡– •—’’‘”–• Ž‘ƒ†‡† — …ƒ–ƒŽ›•–• ’‘••‡•• †‹ˆǦ
ˆ‡”‡– …ƒ–ƒŽ›–‹… ’”‘’‡”–‹‡• ˆ‘” ‘š‹†ƒ–‹‘Ǥ † –Š‡”‡ ƒ”‡
–™‘ –›’‡• ‘ˆ †‡ƒ…–‹˜ƒ–‹‘ ‘„•‡”˜‡†ǡ ˆƒ•– †‡ƒ…–‹˜ƒ–‹‘ ˆ‘”
—Ȁ‹ʹ ƒ† —ȀǦͷ …ƒ–ƒŽ›•–• ƒ† •Ž‘™ †‡ƒ…–‹˜ƒ–‹‘ ˆ‘”
—ȀɀǦŽʹ͵ǡ—Ȁ‡ʹƒ†—Ȁ‡x…ƒ–ƒŽ›•–•Ǥ–‹•™‘”–Š”ƒ‹•‹‰
–Šƒ– —ȀɀǦŽʹ͵ …ƒ–ƒŽ›•– ‡šŠ‹„‹–• –Š‡ Š‹‰Š‡•– ‹‹–‹ƒŽ ƒ…–‹˜‹–› ƒ•
™‡ŽŽƒ•ƒ‘”‡•–ƒ„Ž‡ƒ…–‹˜‹–›ˆ‘”‘š‹†ƒ–‹‘Ǥ Š‡ǡ™Šƒ–‹•–Š‡ ˆƒ…–‘” †‡–‡”‹‰–Š‡‹‹–‹ƒŽƒ…–‹˜‹–›ǫ †
Š‘™ ‹• –Š‡ •–ƒ„‹Ž‹–› „‡‹‰ ƒˆˆ‡…–‡†ǫ ƒ„Ž‡ ͳ •—ƒ”‹œ‡• –Š‡
’Š›•‹…ƒŽ ƒ† …Š‡‹…ƒŽ ’”‘’‡”–‹‡• ‘ˆ –Š‡ ‰‘Ž† Ž‘ƒ†‡† •ƒ’Ž‡•Ǥ
(b)
(c)
40
Frequency (%)
Frequency (%)
50 Au/J-Al2O3
30
20
10
0
0.5 1.0 1.5 2.0 2.5
Particle size (nm)
(d)
60
80
Au/SiO2
70
60
50
40
30
20
10
0
2.3
0.8 1.5
Particle size (nm)
Au/HZSM5
50
Frequency (%)
(a)
40
30
20
10
0
1 2 3 4
Particle size (nm)
Au/CeO2
50
Frequency (%)
Frequency (%)
(e)
40
30
20
10
0
0
2 4 6 8
Particle size (nm)
40
35
30
25
20
15
10
5
0
Au/FeOx
0123456789
Particle size (nm)
Fig.3.‹ƒ‰‡•‘ˆ–Š‡ˆ”‡•Š—ȀɀǦŽʹ͵ȋƒȌǡ—Ȁ‹ʹȋ…Ȍǡ—ȀǦͷȋ„Ȍǡ—Ȁ‡ʹȋ†Ȍǡƒ†—Ȁ‡xȋ‡Ȍ•ƒ’Ž‡•Ǥ
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
—Ȁ‹ʹ…ƒ–ƒŽ›•–•Š‘™•–Š‡Š‹‰Š‡•–•—”ˆƒ…‡ƒ”‡ƒǡ–Š‡ˆ‘ŽǦ
Ž‘™• „› —ȀǦͷ ƒ† —ȀɀǦŽʹ͵ …ƒ–ƒŽ›•–•Ǥ ‡ʹ ƒ† ‡x
•—’’‘”–‡†—…ƒ–ƒŽ›•–•Šƒ˜‡Ž‘™‡”•—”ˆƒ…‡ƒ”‡ƒǡƒ†–Š‡Ž‘™‡•–
‘‡ ‹• —Ȁ‡ʹ …ƒ–ƒŽ›•– ™‹–Š •—”ˆƒ…‡ ƒ”‡ƒ ‘ˆ ͹ͺ ʹȀ‰Ǥ ”‡Ǧ
•—Ž–• ‹†‹…ƒ–‡ –Šƒ– –Š‡ ‰‘Ž† …‘–‡– ‹• …Ž‘•‡ –‘ –Š‡ –Š‡‘”‡–‹…ƒŽ
˜ƒŽ—‡„—–‘–…‘’Ž‡–‡Ž›–Š‡•ƒ‡Ǥ—…Šƒ†‡˜‹ƒ–‹‘‹•ƒ……‡’–ƒǦ
„Ž‡‹˜‹‡™‘ˆ–Š‡’‘–‡–‹ƒŽ‡š’‡”‹‡–ƒŽ‡””‘”Ǥ ‹‰Ǥ͵’”‡•‡–••‡˜‡”ƒŽ–›’‹…ƒŽ‹ƒ‰‡•‘ˆ–Š‡•—’’‘”–‡†
— …ƒ–ƒŽ›•–•Ǥ – …ƒ „‡ •‡‡ –Šƒ– — ƒ‘’ƒ”–‹…Ž‡• ƒ”‡ Š‹‰ŠŽ›
†‹•’‡”•‡† ‘ –Š‡ •—’’‘”–•Ǥ •–‹ƒ–‡† ƒ……‘”†‹‰ –‘ –Š‡ ‹ƒ‰‡•ȋεͳͲͲ’ƒ”–‹…Ž‡•‡ƒ•—”‡†Ȍǡ–Š‡ƒ˜‡”ƒ‰‡’ƒ”–‹…Ž‡•‹œ‡‘ˆ
‰‘Ž†ƒ†–Š‡†‹•’‡”•‹‘ƒ”‡ƒŽ•‘Ž‹•–‡†‹ƒ„Ž‡ͳǤ—Ȁ‹ʹƒ†
—ȀɀǦŽʹ͵ …ƒ–ƒŽ›•–• •Š‘™ Š‹‰Š‡” ‰‘Ž† †‹•’‡”•‹‘•ǡ ™‹–Š ƒ
ƒ˜‡”ƒ‰‡’ƒ”–‹…Ž‡•‹œ‡‘ˆͳǤ͸ƒ†ͳǤͺǡ”‡•’‡…–‹˜‡Ž›Ǥƒ”‰‡•‹œ‡
†‹•–”‹„—–‹‘• ƒ”‡ ‘„•‡”˜‡† ‘˜‡” —Ȁ‡ʹǡ —ȀǦͷ ƒ†
—Ȁ‡x …ƒ–ƒŽ›•–•Ǥ ‘‰ –Š‡ǡ –Š‡ ’‘‘”‡•– — †‹•’‡”•‹‘
ƒ’’‡ƒ”•‘˜‡”—Ȁ‡x•ƒ’Ž‡Ǥ•’‹–‡‘ˆ‹–••—”ˆƒ…‡ƒ”‡ƒ‘ˆͳͺ͹
ʹȀ‰ǡ –Š‡ ƒ˜‡”ƒ‰‡ — ’ƒ”–‹…Ž‡ ‹• –Š‡ Žƒ”‰‡•– ȋͶǤͻ Ȍǡ ™Š‹…Š
•—‰‰‡•–• –Šƒ– –Š‡ — †‹•’‡”•‹‘ ‹• ‘– ‘Ž› ‹ˆŽ—‡…‡† „› –Š‡
•—”ˆƒ…‡ ƒ”‡ƒ ‘ˆ –Š‡ •—’’‘”–ǡ „—– ƒŽ•‘ –Š‡ ’”‡’ƒ”ƒ–‹‘ ‡–Š‘†
ƒ†–Š‡•—”ˆƒ…‡‹–‡”ƒ…–‹‘„‡–™‡‡‰‘Ž†ƒ†‘š‹†‡ȏ͵͵ǡ͵ͶȐǤ
‘•–—†›–Š‡‡ˆˆ‡…–‘ˆ—’ƒ”–‹…Ž‡•‹œ‡‘…ƒ–ƒŽ›–‹…ƒ…–‹˜‹–‹‡•ǡ
100
Rate (Pmol/(gAu˜s)
80
60
Au/J-Al2O3
Au/SiO2
40
Au/HZSM-5
20
0
Au/CeO2
1.6
4.9
Fig. 4. ‘””‡Žƒ–‹‘ –Š‡ ”ƒ–‡ ‘ˆ ‘š‹†ƒ–‹‘ ™‹–Š –Š‡ ƒ˜‡”ƒ‰‡ ‰‘Ž†
’ƒ”–‹…Ž‡•‹œ‡‘˜‡”–Š‡˜ƒ”‹‘—••—’’‘”–‡†—…ƒ–ƒŽ›•–•Ǥ
–Š‡”‡ƒ…–‹‘”ƒ–‡‹•…‘””‡Žƒ–‡†™‹–Š–Š‡ƒ˜‡”ƒ‰‡—’ƒ”–‹…Ž‡•‹œ‡ǡ
•Š‘™‹‹‰ǤͶǤŠ‡”‡‹•ƒŽ‹‡ƒ””‡Žƒ–‹‘„‡–™‡‡–Š‡ǡ‰‹˜‡
•–”‘‰‡˜‹†‡…‡‘ˆ —’ƒ”–‹…Ž‡ •‹œ‡ †‡–‡”‹‡ –Š‡…ƒ–ƒŽ›–‹…ƒ…Ǧ
–‹˜‹–›Ǥ —ȀɀǦŽʹ͵ ƒ† —Ȁ‹ʹ …ƒ–ƒŽ›•–• ™‹–Š –Š‡ Š‹‰Š‡” —
†‹•’‡”•‹‘ƒ†•ƒŽŽ‡”‰‘Ž†’ƒ”–‹…Ž‡•‹œ‡”‡†‡”–Š‡„‡•–…ƒ–ƒǦ
(c)
50
70
AuSiO2
60
Frequency (%)
40
Frequency (%)
Frequency (%)
80
70 Au/J-Al2O3
60
50
40
30
20
10
0
1.0 1.5 2.0 2.5 3.0 3.5
Particle size (nm)
Au/FeOx
2.7 3.0
Au particle size (nm)
1.8
(b)spent
(b)
(a)
ͳ͹͵͵
30
20
10
0
2.0
Au/HZSM-5
50
40
30
20
10
0
2.5 3.0 3.5
Particle size (nm)
3 4 5 6
Particle size (nm)
(e)
50
50
Au/CeO2
Au/FeOx
40
40
Frequency (%)
Frequency (%)
(d)
30
20
10
0
30
20
10
0
0
2 4 6 8
Particle size (nm)
4 5 6 7
Particle size (nm)
Fig.5.‹ƒ‰‡•‘ˆ–Š‡•’‡–—ȀɀǦŽʹ͵ȋƒȌǡ—Ȁ‹ʹȋ„Ȍǡ—ȀǦͷȋ…Ȍǡ—Ȁ‡ʹȋ†Ȍǡƒ†—Ȁ‡xȋ‡Ȍ•ƒ’Ž‡•Ǥ
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
6
Au/J-Al2O3
Au/HZSM-5
Au/FeOx
3
2
Au/SiO2
Au/CeO2
1
3600
3400
1
Wavenumber (cm )
3200
3000
300
350 C
40
200
20
100
0
100
400
(b)
80
o
60
300
350 C
40
200
20
100
(c)
80
300
o
385 C
60
400
o
0
100
40
200
20
100
0
100
o
400
115 C
80
(d)
o
256 C
300
60
40
200
20
100
0
100
o
400
288 C
(e)
80
60
300
40
200
20
100
0
0
10
20
30
40
50
60
70
Time (min)
Fig. 6.”‡•—Ž–•‘ˆ–Š‡—ȀɀǦŽʹ͵ȋƒȌǡ—Ȁ‹ʹȋ„Ȍǡ—ȀǦͷȋ…Ȍǡ
—Ȁ‡ʹȋ†Ȍƒ†—Ȁ‡xȋ‡Ȍƒˆ–‡””‡ƒ…–‹‘ˆ‘”͵͸Ͳ‹Ǥ
•—”ˆƒ…‡Š›†”‘š›Ž•’‡…‹‡•‘ˆɀǦŽʹ͵ǡƒ†–Š‡”‡•—Ž–•ƒ”‡•Š‘™
‹‹‰Ǥ͹Ǥ‘™‡˜‡”ǡ†—‡–‘–Š‡Žƒ…‘ˆ•—”ˆƒ…‡Ȃƒ†Ȃǡ–Š‡
„‹†‹‰ „‡–™‡‡ ƒ‘Ǧ‰‘Ž† ƒ† ‹ʹȀǦͷ ‹• Ž‘•‡”ǡ ™Š‹…Š
”‡•—Ž–‡†‹–Š‡‡ƒ•‹‡”ƒ‰‰”‡‰ƒ–‹‘‘ˆ‰‘Ž†’ƒ”–‹…Ž‡•Ǥ
‘•–—†›–Š‡ •—”ˆƒ…‡ •’‡…‹‡•–Šƒ–†‡’‘•‹–‡†‘–Š‡…ƒ–ƒŽ›•–
(b)
3500
3000
2500
2000
1500
1000
500
0
3800
o
60
Integrate area of OH species
KM
4
400
(a)
80
(a)
5
0
4000
100
Temperature ( C)
Ž›–‹…‘š‹†ƒ–‹‘ƒ…–‹˜‹–‹‡•Ǥ‘”‡‘˜‡”ǡ–Š‡‡ˆˆ‡…–‘ˆŠ›†”‘š›Ž
‰”‘—’•‘–Š‡ɀǦŽʹ͵ƒ†‹ʹ•Š‘—Ž†ƒŽ•‘„‡…‘…‡”‡†ǡ™Š‹…Š
…‘—Ž†ƒ••‹•––Š‡†‡…‘’‘•‹–‹‘‘ˆ‘””‡ƒ…–‹‘‹–‡”‡†‹Ǧ
ƒ–‡•Ǥ Š‡•‡ ”‡•—Ž–• •—‰‰‡•–‡† –Šƒ– –Š‡ •›‡”‰‹•–‹… ‡ˆˆ‡…– ‘ˆ –Š‡
•ƒŽŽ — ’ƒ”–‹…Ž‡ •‹œ‡ ƒ† –Š‡ Š›†”‘š›Ž ‰”‘—’• ™‘—Ž† Ž‡ƒ† –‘
–Š‡ Š‹‰Š‡” ‹‹–‹ƒŽ ƒ…–‹˜‹–‹‡• ‘ˆ –Š‡ —Ȁ‹ʹ ƒ† —ȀɀǦŽʹ͵Ǥ
‘™‡˜‡”ǡ —Ȁ‡x …ƒ–ƒŽ›•– ™‹–Š –Š‡ Žƒ”‰‡” — ’ƒ”–‹…Ž‡ •‹œ‡
•Š‘™•–Š‡’‘‘”‡•–ƒ…–‹˜‹–›Ǥ
‘ •–—†› –Š‡ ˆƒ…–‘”• –Šƒ– ƒˆˆ‡…– –Š‡ …ƒ–ƒŽ›•–•ǯ •–ƒ„‹Ž‹–›ǡ –Š‡
•’‡–…ƒ–ƒŽ›•–•—’‘͵͸Ͳ‹‘ˆ”‡ƒ…–‹‘ƒ”‡…Šƒ”ƒ…–‡”‹œ‡†„›
ƒ†ǡƒ••Š‘™‹‹‰•Ǥͷƒ†͸ǡ”‡•’‡…–‹˜‡Ž›Ǥ‘”–Š‡
•’‡– —ȀɀǦŽʹ͵ …ƒ–ƒŽ›•– ȋ‹‰Ǥ ͷȋƒȌȌǡ ƒ‘Ǧ‰‘Ž† ’ƒ”–‹…Ž‡• ƒ”‡
•–‹ŽŽ Š‹‰ŠŽ› †‹•’‡”•‡† ‘ –Š‡ •—’’‘”–ǡ ™‹–Š ƒ ƒ˜‡”ƒ‰‡ ’ƒ”–‹…Ž‡
•‹œ‡‘ˆ…ƒǤʹǤʹǡ™Š‹…Š‹•ƒŽ‹––Ž‡Žƒ”‰‡”–Šƒ–Šƒ–‘ˆ–Š‡ˆ”‡•Š
•ƒ’Ž‡Ǥ Š‡ •‹‹Žƒ” –”‡†• ƒ”‡ ‘„•‡”˜‡† ‘˜‡” –Š‡ •’‡–
—Ȁ‡ʹ ƒ† —Ȁ‡x …ƒ–ƒŽ›•–•ǡ ƒ‘Ǧ‰‘Ž† ’ƒ”–‹…Ž‡• ƒ”‡ •–‹ŽŽ
Š‹‰ŠŽ›†‹•’‡”•‡†‘–Š‡•—’’‘”–ǡ™‹–Šƒ•ƒŽŽ‹…”‡ƒ•‡‹‰‘Ž†
’ƒ”–‹…Ž‡ •‹œ‡Ǥ ‘™‡˜‡”ǡ –Š‡ ‹ƒ‰‡• …Šƒ‰‡ ‘„˜‹‘—•Ž› ˆ‘” –Š‡
—•‡† —Ȁ‹ʹ …ƒ–ƒŽ›•–Ǥ  •‘‡ ƒ”‡ƒ•ǡ •Š‘™ ‹ ‹‰Ǥ ͷȋ„Ȍǡ –Š‡
’ƒ”–‹…Ž‡• „‡…‘‡ …”‘™†‡† –‘‰‡–Š‡”ǡ ‹†‹…ƒ–‹‰ –Šƒ– –Š‡ ‰‘Ž†
’ƒ”–‹…Ž‡•ƒ‰‰”‡‰ƒ–‡†‘„˜‹‘—•Ž›‘˜‡”–Š‡‹ʹ•—’’‘”–ǡ‡˜‡—’Ǧ
‘–Š‡”‘‘–‡’‡”ƒ–—”‡”‡ƒ…–‹‘Ǥ‘‡ƒ‰‰”‡‰ƒ–‡†‰‘Ž†’ƒ”Ǧ
–‹…Ž‡•…‘—Ž†ƒŽ•‘„‡‘„•‡”˜‡†‘˜‡”–Š‡•’‡–—ȀǦͷ•ƒǦ
’Ž‡Ǥ
Š‡ǡ ™Š› …‘—Ž† ɀǦŽʹ͵ǡ ‡ʹ ƒ† ‡x •—’’‘”–• •–ƒ„‹Ž‹œ‡
ƒ‘Ǧ‰‘Ž†’ƒ”–‹…Ž‡•‹ƒ„‡––‡”™ƒ›–Šƒ‹ʹƒ†Ǧͷ•—„Ǧ
•–”ƒ–‡•ǫ ‘” –Š‡ ”‡†—…‹„Ž‡ ‘š‹†‡• •—…Š ƒ• ‡ʹ ƒ† ‡xǡ ‹– ‹•
‰‡‡”ƒŽŽ› ”‡‰ƒ”†‡† –Šƒ– –Š‡”‡ ƒ”‡ •–”‘‰ •—”ˆƒ…‡ ‹–‡”ƒ…–‹‘
„‡–™‡‡–Š‡‰‘Ž†ƒ†–Š‡‘š‹†‡•ȏʹͷǡ͵ͷȐǤ
‘Ž†Ǧ‡–ƒŽ‘š‹†‡’‡Ǧ
”‹‡–‡” ‹–‡”ˆƒ…‡ ƒ…–• ƒ• •‹–‡• ˆ‘” ƒ…–‹˜ƒ–‹‰ –Š‡ ”‡ƒ…–ƒ–•
ȏ͵͸ǡ͵͹ȐǤŠ‡…ƒ’ƒ…‹–›‘ˆŠ‹‰ŠŽ›†‹•’‡”•‡†•ƒŽŽ‰‘Ž†’ƒ”–‹…Ž‡•–‘
™‡ƒ‡ –Š‡ ‡Ǧ ƒ† ‡Ǧ „ƒ†ǡ –Š—• ‹…”‡ƒ•‹‰ –Š‡ ”‡†‘š
’”‘’‡”–‹‡• ‘ˆ –Š‡ —Ȁ‡ʹ ƒ† —Ȁ‡x …ƒ–ƒŽ›•–• Šƒ• „‡‡
•–—†‹‡† ‹ ƒ› Ž‹–‡”ƒ–‡• ƒ• ™‡ŽŽ ƒ• ‘—” ’”‡˜‹‘—• ™‘”•
ȏʹ͵ȂʹͷȐǤ‡ƒ™Š‹Ž‡ǡ–Š‡ƒ‘Ǧ‰‘Ž†…‘—Ž†„‡ƒ…Š‘”‡†™‹–Š–Š‡
‘š‹†‡ –Š”‘—‰ŠǦ Ž‹ƒ‰‡•Ǥ Šƒ– ’”‘˜‹†‡• –Š‡ ’‘••‹„Ž‡ ™ƒ› ˆ‘”
•–ƒ„‹Ž‹œƒ–‹‘‘ˆƒ‘Ǧ‰‘Ž†’ƒ”–‹…Ž‡•ȏ͵ͺȐǤ•–‘–Š‡Š‹‰Š‡”•–ƒ„‹ŽǦ
‹–›‘ˆƒ‘Ǧ‰‘Ž†‘˜‡”ɀǦŽʹ͵•—„•–”ƒ–‡ǡ‹–‹••—’’‘•‡†–Šƒ––Š‡
‡”‹…Š‡–‘ˆ•—”ˆƒ…‡Š›†”‘š›Ž‰”‘—’•ƒ…–ƒ•DzŽ‹‰ƒ†•dz„‹†‹‰
–Š‡ ‰‘Ž† •’‡…‹‡• ȏ͵ͻȂͶͳȐǤ ‘ „‡ ”‡Žƒ–‡† –‘ –Š‡ ƒ„—†ƒ…‡ ‘ˆ
The concentration of CO2 (ppm)
ͳ͹͵Ͷ
Au/J-Al2O3 Au/SiO2 Au/HZSM-5 Au/CeO2 Au/FeOx
Catalyst
Fig.7.InǦsitu•’‡…–”ƒ‘ˆ•—”ˆƒ…‡•’‡…‹‡•ȋƒȌƒ†–Š‡‹–‡‰”ƒ–‡ƒ”‡ƒ•ȋ͵ͺͲͲ̱͵ʹͲͲ… Ȍ‘ˆ–Š‡•’‡…‹‡•ȋ„Ȍ‘˜‡”–Š‡•—’’‘”–‡†—…ƒ–ƒŽ›•–•
–”‡ƒ–‡†ƒ–ͶͲͲιǤ
Ȃͳ
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
•—”ˆƒ…‡†—”‹‰–Š‡”‡ƒ…–‹‘™Š‹…Š‹‰Š–”‡•—Ž–‹–Š‡…‘˜‡”ƒ‰‡
‘ˆ –Š‡ ƒ…–‹˜‡ •‹–‡• ƒ† †‡ƒ…–‹˜ƒ–‹‘ ‘ˆ –Š‡ …ƒ–ƒŽ›•–ǡ –Š‡ •’‡–
•ƒ’Ž‡•ƒ”‡–‡’‡”ƒ–—”‡Ǧ’”‘‰”ƒ‡†‘š‹†‹œ‡†‹ʹͳΨʹȀʹ
‰ƒ•‡•ǡ ƒ† –Š‡ ”‡•—Ž–• ƒ”‡ •Š‘™ ‹ ‹‰Ǥ ͸Ǥ Š‡”‡ ‹• ‘ ȋ‰Ȍ
†‡–‡…–‡†ǡ‡š…‡’–ʹȋ‰Ȍ‹–Š‡’”‘†—…–•ˆ‘”ƒŽŽ–Š‡•ƒ’Ž‡•Ǥ‘”
–Š‡ •’‡– —Ȁ‹ʹ ƒ† —ȀǦͷ •ƒ’Ž‡•ǡ ™‹–Š ‹…”‡ƒ•‹‰
–‡’‡”ƒ–—”‡ǡ ƒ •Šƒ”’ ’‡ƒ ƒ’’‡ƒ”• ƒ– ƒ”‘—† ͷͲ ƒ† ͳͲͲ ιǡ
‘™‹‰–‘–Š‡”‡Ž‡ƒ•‡‘ˆ’Š›•‹…ƒŽƒ†•‘”’–‹‘ʹ‘–Š‡…ƒ–ƒŽ›•–
•—”ˆƒ…‡†—‡–‘–Š‡”‡ƒ…–‹‘Ǥ†ƒ–…ƒǤ͵ͷͲιǡ–Š‡”‡‹•ƒ‘„˜‹Ǧ
‘—• ʹ ’‡ƒ ‘„•‡”˜‡† ‘˜‡” —ȀɀǦŽʹ͵ǡ —Ȁ‹ʹ ƒ†
—ȀǦͷ …ƒ–ƒŽ›•–•ǡ ™Š‹Ž‡ –Š‡ –‡’‡”ƒ–—”‡ •Š‹ˆ–• –‘ Ž‘™‡”
”‡‰‹‘ȋδ͵ͲͲιȌ‘˜‡”–Š‡•’‡–‡ʹƒ†‡x•—’’‘”–‡†‰‘Ž†
…ƒ–ƒŽ›•–•ǡ™Š‹…Š•Š‘—Ž†…‘‡ˆ”‘–Š‡‘š‹†ƒ–‹‘‘ˆ–Š‡†‡’‘•Ǧ
‹–‡† •—”ˆƒ…‡ •’‡…‹‡• ‹–‘ ʹȋ‰Ȍ ƒ– ‡Ž‡˜ƒ–‡† –‡’‡”ƒ–—”‡•Ǥ
ƒ•‡†‘–Š‡Ž‹–‡”ƒ–—”‡•ƒ†‘—”’”‡˜‹‘—••–—†‹‡•ǡ–Š‡†‡’‘•‹–•
‹‰Š– „‡ –Š‡ †‹‘š›‡–Š›Ž‡‡ ȋȌ ƒ† ˆ‘”ƒ–‡ •’‡…‹‡•ǡ ƒ•
•Š‘™ ‹ –Š‡ ‹‰Ǥ ͺ ȏʹ͵ǡʹͶǡʹͺǡͶʹǡͶ͵ȐǤ ……‘”†‹‰Ž›ǡ ‘”‡ ʹ
‰‡‡”ƒ–‡†‡ƒ•‘”‡ †‡’‘•‹–•Ǥ› …ƒŽ…—Žƒ–‹‰–Š‡ƒ‘—–‘ˆ
ʹ‰‡‡”ƒ–‡†•Š‘™‹ƒ„Ž‡ͳǡ‹–‹•…Ž‡ƒ”–Šƒ––Š‡”‡ƒ”‡‘•–
†‡’‘•‹–•‘—Ȁ‡ʹ…ƒ–ƒŽ›•–ǡ–Š‡ˆ‘ŽŽ‘™•„›–Š‡—Ȁ‡xƒ†
—ȀɀǦŽʹ͵ …ƒ–ƒŽ›•–•ǡ ƒ† –Š‡ †‡’‘•‹–• ‘ —Ȁ‹ʹ …ƒ–ƒŽ›•– ‹•
–Š‡ Ž‡ƒ•–ǡ ™Š‹…Š …‘””‡Žƒ–‡† ™‡ŽŽ ™‹–Š inǦsitu • ”‡•—Ž–•
•Š‘™ ‹ ‹‰Ǥ ͺǤ ‘”‡ ˆ‘”ƒ–‡ •’‡…‹‡• ˆ‘”‡† ‘˜‡” —Ȁ‡ʹ
…ƒ–ƒŽ›•–•ǡ•‘–Š‡‘”‡†‡’‘•‹–•ƒ”‡ƒ……——Žƒ–‡†‘‹–Ǥ
—–™Š›†‘‡•–Š‡—Ȁ‹ʹƒ†—ȀǦͷ•ƒ’Ž‡•†‡ƒ…–‹Ǧ
˜ƒ–‡ ƒ– ƒ ˆƒ•–‡” ”ƒ–‡ǡ ‡•’‡…‹ƒŽŽ› ƒ– –Š‡ ‹‹–‹ƒŽ •–ƒ‰‡ ‘ˆ –Š‡ ”‡ƒ…Ǧ
–‹‘ǫ”‘–Š‡‹ƒ‰‡•‘ˆ–Š‡•’‡–…ƒ–ƒŽ›•–•ǡ‹–‹•…Ž‡ƒ”–Šƒ–
‰‘Ž†ƒ‰‰”‡‰ƒ–‡†–‘‰‡–Š‡”‘„˜‹‘—•Ž›ˆ‘”–Š‡—Ȁ‹ʹ…ƒ–ƒŽ›•–Ǥ
…‘–”ƒ•–ǡ ‰‘Ž† ’ƒ”–‹…Ž‡• ‡‡’ ™‡ŽŽ †‹•’‡”•‡† ˆ‘” –Š‡ •’‡–
—ȀɀǦŽʹ͵ǡ—Ȁ‡ʹƒ†—Ȁ‡x…ƒ–ƒŽ›•–•ǡ™Š‹…Š‘Ž›‡šŠ‹„Ǧ
‹–‡†ƒ‰”ƒ†—ƒŽ†‡ƒ…–‹˜ƒ–‹‘†—”‹‰‘š‹†ƒ–‹‘Ǥ—…Š”‡•—Ž–•
•—‰‰‡•––Šƒ––Š‡ƒ‰‰”‡‰ƒ–‹‘‘ˆ‰‘Ž†ƒ†–Š‡‰”‘™‹‰‰‘Ž†’ƒ”Ǧ
–‹…Ž‡•‹œ‡•ƒ”‡”‡•’‘•‹„Ž‡–‘–Š‡ˆƒ•–†‡ƒ…–‹˜ƒ–‹‘‘ˆ—Ȁ‹ʹƒ•
™‡ŽŽ ƒ• —ȀǦͷ •ƒ’Ž‡•Ǥ Š‹Ž‡ –Š‡ †‡’‘•‹–‹‘ ‘ˆ •—”ˆƒ…‡
‹–‡”‡†‹ƒ–‡•‘–Š‡…ƒ–ƒŽ›•–•—”ˆƒ…‡…ƒ—•‡•–Š‡‰”ƒ†—ƒŽ†‡ƒ…Ǧ
–‹˜ƒ–‹‘‘ˆ‰‘Ž†…ƒ–ƒŽ›•–Ǥ
3.0
1581
2.5
KM
2.0
1636
1320
1362
Au/FeOx
Au/CeO2
1442
1.5
Au/HZSM-5
1.0
Au/SiO2
0.5
Au/Al2O3
0.0
2000
1800
1600
1400
1
Wavenumber (cm )
1200
Fig.8.‘’ƒ”‹•‘‘ˆ•—”ˆƒ…‡‹–‡”‡†‹ƒ–‡•‘˜‡”˜ƒ”‹‘—••—’’‘”–‡†—
…ƒ–ƒŽ›•–•ƒˆ–‡”‡š’‘•—”‡–‘ͺͲ’’ʹͳ˜‘ŽΨʹȀͳǤ͸˜‘ŽΨʹȀʹ
‰ƒ•ˆ‘”͸Ͳ‹Ǥ
ͳ͹͵ͷ
Table2
InǦsitu•„ƒ†’‘•‹–‹‘‘ˆ•—”ˆƒ…‡•’‡…‹‡•‘˜‡”•—’’‘”–‡†—…ƒ–Ǧ
ƒŽ›•–•Ǥ
ƒ˜‡—„‡”ȋ…ȂͳȌ
ͳ͸͵͸
ͳͷͺͶ
ͳ͵͸ʹǡͳ͵ʹͲ
ͳͶͶʹ
’‡…‹‡•
ɁȋȂȂȌƒ†•‘”„‡†™ƒ–‡”
ɋƒ•ȋȌˆ‘”ƒ–‡
ɋ•ȋȌˆ‘”ƒ–‡
ɘȋʹȌ†‹‘š›‡–Š›Ž‡‡ȋȌ
‡ˆǤ
ȏͶǡʹͶȐ
ȏͶͷǡͶ͸Ȑ
ȏͶ͹Ȑ
4. Conclusions Š‡ …ƒ–ƒŽ›–‹… ’”‘’‡”–‹‡• ‘ˆ —ȀɀǦŽʹ͵ǡ —Ȁ‹ʹǡ
—ȀǦͷǡ —Ȁ‡ʹ ƒ† —Ȁ‡x …ƒ–ƒŽ›•–• ˆ‘” ‘š‹†ƒǦ
–‹‘ ™‡”‡ …‘’ƒ”‡† ƒ– ”‘‘ –‡’‡”ƒ–—”‡ —†‡” Š‹‰Š Ǥ
Š‡‰‘Ž†’ƒ”–‹…Ž‡•‹œ‡‹•…”—…‹ƒŽ‹†‡–‡”‹‹‰–Š‡‹‹–‹ƒŽƒ…–‹˜‹Ǧ
–›ǡ ƒ† —ȀɀǦŽʹ͵ ƒ† —Ȁ‹ʹ …ƒ–ƒŽ›•–• ™‹–Š –Š‡ Š‹‰Š‡” —
†‹•’‡”•‹‘ƒ†•ƒŽŽ‡”—’ƒ”–‹…Ž‡•‹œ‡”‡†‡”–Š‡„‡•–…ƒ–ƒŽ›–‹…
‘š‹†ƒ–‹‘ƒ…–‹˜‹–‹‡•ǡ•—‰‰‡•–‹‰–Šƒ––Š‡‹†‹”‡…–‡ˆˆ‡…–‘ˆ
–Š‡”‡†—…‹„‹Ž‹–›‘ˆ–Š‡•—’’‘”–•ˆ‘”‰‘Ž†…ƒ–ƒŽ›•‹•‹‘š‹Ǧ
†ƒ–‹‘”‡ƒ…–‹‘Ǥƒ†”‡•—Ž–••—‰‰‡•–‡†–Šƒ––Š‡™‡ƒ
‹–‡”ƒ…–‹‘ „‡–™‡‡—ƒ† ‹ʹȀǦͷ •—„•–”ƒ–‡Ž‡†–‘–Š‡
‰”‘™–Š ‘ˆ — ’ƒ”–‹…Ž‡•ǡ ƒ† ”‡•—Ž–‡† ‹ ˆƒ•–‡” †‡ƒ…–‹˜ƒ–‹‘Ǥ
‘”‡‘˜‡”ǡ–Š‡ƒ……——Žƒ–‹‘‘ˆ–Š‡•—”ˆƒ…‡ˆ‘”ƒ–‡‹–‡”‡†‹Ǧ
ƒ–‡• ƒ……‘—–• ˆ‘” –Š‡ ‰”ƒ†—ƒŽŽ› †‡ƒ…–‹˜ƒ–‹‘Ǥ Š‡ ’”‡•‡– ”‡Ǧ
•—Ž–••—‰‰‡•––Šƒ––Š‡”‡†—…‹„‹Ž‹–›‘ˆ–Š‡•—’’‘”–•‹•‘––Š‡‡›
ˆƒ…–‘”–Šƒ–‹ˆŽ—‡…‡•–Š‡‰‘Ž†…ƒ–ƒŽ›•–•ƒ…–‹˜‹–‹‡•ǡ„—–ƒˆˆ‡…–•–Š‡
•–ƒ„‹Ž‹–›‘ˆ–Š‡•—’’‘”–‡†—…ƒ–ƒŽ›•–ˆ‘”‘š‹†ƒ–‹‘Ǥ
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ͳ͹͵͸
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
GraphicalAbstract
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oxidationatroomtemperature
Activity
Auparticlesize
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Au
Š‡ ’‡”ˆ‘”ƒ…‡ ‘ˆ –Š‡ •—’’‘”–‡† ‰‘Ž† …ƒ–ƒŽ›•– ˆ‘” ‘š‹†ƒ–‹‘ †‡Ǧ
’‡†•‘‰‘Ž†’ƒ”–‹…Ž‡•‹œ‡†‹”‡…–Ž›ǤŠ‡”‡†—…‹„‹Ž‹–›‘ˆ–Š‡•—’’‘”–•Šƒ•‘
†‹”‡…–‹ˆŽ—‡…‡‘ƒ…–‹˜‹–›ǡ„—–ƒˆˆ‡…–•–Š‡…ƒ–ƒŽ›–‹…•–ƒ„‹Ž‹–›Ǥ
Au
Au
Au
Au
Variousoxides
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ȏͳ͹Ȑ ǤǤƒǡǤǤƒ‰ǡǤǤ—‡ǡǤǤ‘—ǡǤǤƒ‰ǡǤǤƒ‘ǡEnǦ
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ͳ͵͹ǡʹ͵ͻȂʹͶ͸Ǥ
ȏͶ͹Ȑ Ǥ—•…ƒǡǤƒ‘––‡ǡǤǤƒ˜ƒŽŽ‡›ǡǤ‘”‡œ‡ŽŽ‹ǡJ.Am.Chem.SocǤǡ
1987ǡͳͲͻǡͷͳͻ͹ȂͷʹͲʹǤ
уੂ䖳։どᇐⲺ㓩㊩䠇ۢौࡸᇚ⑟ۢौ≝ौ⭨䟑⹊ガ
⧣⢚⢚a, 䑍㼟⢙b, 㶖䄬⭰a, 䇻㏗㗘a, 㬐
⪉a,*
⫔㑍㏎⹅⫔䁈⿐䁈䁈䊛, ㈌㻙⿐⹅⺛コ䐹⮄㬖䂊㬳, 㑪㛟⫔㑍116024
b
⫔㑍㏎⹅⫔䁈⭩㏌䓴㳆㹐㏎⿐䁈㬖䂊㬳, 㑪㛟⫔㑍116024
a
᪎㾷: ⭢䟋ᱟа⿽ᑨ㿱Ⲵᇔ޵オ≄⊑ḃ⢙, ӪԜ䪸ሩަ⎸䲔ᐢ㓿‫ڊ‬Ҷབྷ䟿Ⲵ⹄ウᐕ֌. ۜॆ≗ॆ⌅ᱟ㝡䲔ᥕਁᙗᴹᵪ⢙Ⲵ
а⿽䟽㾱ᯩ⌅, 㜭൘䖳վ⑙ᓖл䙊䗷ۜॆࡲ֌⭘ሶ⭢䟋ᆼ‫ॆ≗ޘ‬Ѫᰐ∂ⲴCO2઼H2O. ᡰ⭘ۜॆࡲѫ㾱Ѫ䍏䖭ර䍥䠁኎ۜ
BingbingChenetal./ChineseJournalofCatalysis37(2016)1729–1737
ͳ͹͵͹
ॆࡲ઼䶎䍥䠁኎ۜॆࡲ, նਚᴹᣵ䖭䍥䠁኎PtᡆPdⲴۜॆࡲਟ൘ᇔ⑙лሶ⭢䟋ᆼ‫ॆ≗ޘ‬, 㘼䶎䍥䠁኎а㡜ࡉ䴰㾱䖳儈Ⲵ⑙
ᓖ.
Auۜॆࡲᱟ䘁ᒤᶕۜॆ亶ฏⲴањ⹄ウ✝⛩, նᱟ‫ޣ‬Ҿ㓣㊣Auۜॆࡲᇔ⑙⎸䲔⭢䟋Ⲵ⹄ウ䖳ቁ. ᵜ䈮仈㓴ࡽᵏ⹄ウ
ਁ⧠, ԕਟ䘈৏ᙗ≗ॆ⢙(CeO2, FeOx)Ѫ䖭փ䍏䖭ⲴAuۜॆࡲާᴹՈᔲⲴᇔ⑙≗ॆ⭢䟋⍫ᙗ; ᒦфケ⹤ԕਟ䘈৏ᙗ䖭փ䍏
䖭䠁ⲴՐ㔏ᙍ䐟, 俆⅑ਁ⧠“ᜠᙗ䖭փ”Ȗ-Al2O3, 䍏䖭Ⲵ䠁ۜॆࡲ൘ᇔ⑙ǃᴹ≤ᶑԦлާᴹՈᔲⲴ⭢䟋≗ॆ⍫ᙗ. ᵜ᮷ሩ∄
Ҷ䘈৏ᙗ≗ॆ⢙(CeO2, FeOx)઼䶎䘈৏ᙗ≗ॆ⢙(Al2O3, SiO2઼HSZM-5)䖭փ䍏䖭䠁ۜॆࡲ, ⹄ウҶ䖭փ≗ॆ䘈৏ᙗ䍘ሩ䍏
䖭䠁ۜॆࡲ൘儈オ䙏(600000 ml/(g·s))ᶑԦлᇔ⑙ۜॆ≗ॆ⭢䟋Ⲵ⍫ᙗ઼っᇊᙗᖡ૽. 㔃᷌㺘᰾, ൘ᇔ⑙ǃ儈オ䙏ф⴨ሩ⒯
ᓖѪ50%ⲴᶑԦл, Au/Al2O3ۜॆࡲⲴࡍ⍫ᙗᴰ儈, ф䖳Ѫっᇊ. Au/SiO2઼Au/HZSM-5ۜॆࡲⲴࡍ⍫ᙗ㲭❦䖳儈, նᖸᘛ
ཡ⍫. 㘼䘈৏ᙗ≗ॆ⢙䖭փ(CeO2, FeOx)䍏䖭Ⲵ䠁ۜॆࡲࡍ⍫ᙗ䖳վ, նᱟっᇊᙗ䖳ྭ.
䙊䗷⭥䮌ሩ䍏䖭䠁ۜॆࡲ㺘䶒Au㋂ᆀབྷሿⲴ㺘ᖱ, ᒦሶ㋂ᆀቪረо䍏䖭䠁ۜॆࡲᇔ⑙≗ॆ⭢䟋ࡍ⍫ᙗ⴨‫ޣ‬㚄, ᆳоۜ
ॆ≗ॆ⭢䟋৽ᓄ䙏⦷ᡀ㓯ᙗ‫ޣ‬㌫. Au㋂ᆀቪረ䖳ሿⲴۜॆࡲ(Au/Al2O3઼Au/SiO2), ൘儈オ䙏ᶑԦлާᴹᴤ儈Ⲵ≗ॆ⭢䟋
⍫ᙗ, 㘼Au㋂ᆀቪረ䖳བྷⲴAu/FeOxۜॆࡲ⍫ᙗ䖳ᐞ. 䖭փⲴ≗ॆ䘈৏ᙗ䍘㲭❦нⴤ᧕ᖡ૽Auۜॆࡲࡍ⍫ᙗ, նⴤ᧕ᖡ૽
ۜॆࡲっᇊᙗ. ⭡ҾAuоSiO2 ᡆHZSM-5䖭փⲴ⴨ӂ֌⭘䖳ᕡ, ሬ㠤৽ᓄ䗷〻ѝAu㋂ᆀ㚊䳶䮯བྷ, ֯ަཡ⍫䖳ᘛ; 㘼
Au/Al2O3ۜॆࡲ㺘䶒ࡉᇼਜ਼㗏ส⢙⿽, 㜭ཏоAuᖒᡀ䝽փᡆӗ⭏䭊ᇊ֌⭘, ഐ↔৽ᓄ䗷〻ѝ䠁㋂ᆀ⋑ᴹ᰾ᱮ䮯བྷ. 㘼㺘䶒
ѝ䰤⢙⿽Ⲵ⊹〟ᒦ㾶ⴆ⍫ᙗսᱟ䍏䖭䠁ۜॆࡲ㕃ធཡ⍫Ⲵѫ㾱৏ഐ.
ީ䭤䈃: 䠁ۜॆࡲ; ≗ॆ⢙䖭փ; ⭢䟋≗ॆ; 䘈৏ᙗ; ۜॆっᇊᙗ
㬶ⷆ㦶㠻: 2016-04-15. ㅴ㬽㦶㠻: 2016-05-21. ⨗⟇㦶㠻: 2016-10-05.
*㵉䁗㑋㻖㦬. ⮈⿑: (0411)84986083; ⮈䓴㾦㼅: [email protected]
〚㆑㎕䊕: ⺛コ䓵㦜㋧䁈〚㆑(21373037, 21577013); 䐱⺛⤊㬠⽔㋧䁈〚㆑(2014M560201); 䐱䂌ⷀ㾄〚⡟㋧䁱䄖㹒Ⳳ䓉㼏䓫㆑䓫
䑛(DUT15TD49, DUT16ZD224).
⡟㸥⭥䇃㸥⮈䓴⟇䇪Elsevier⨗⟇㪈䊻ScienceDirect㩰⨗⟇(http://www.sciencedirect.com/science/journal/18722067).