Š‹‡•‡‘—”ƒŽ‘ˆƒ–ƒŽ›•‹•͵͹ȋʹͲͳ͸Ȍͳ͹Ͷ͹Ȃͳ͹ͷͷ
ۢौᆜᣛʹͲͳ͸ᒪㅢ͵͹ভㅢͳͲᵕȁ™™™Ǥ…Œ…ƒ–ƒŽǤ‘”‰
availableatwww.sciencedirect.com
journalhomepage:www.elsevier.com/locate/chnjc
Article(SpecialIssueonGoldCatalysis)
CatalyticcrackingoflightdieseloverAu/ZSMǦ5catalystfor increasingpropyleneproduction
ƒ‹š‹ƒ‹ȗǡ—š‹ƒƒ‰ǡ‹ƒ‘–ƒ‘‹‰ǡ—‹Œ—ƒ—
ShandongAppliedResearchCenterofGoldNanotechnology(AuǦSDARC),SchoolofChemistryandChemicalEngineering,YantaiUniversity,Yantai
264005,Shandong,China
Articlehistory:
‡…‡‹˜‡†ͳ͹ƒ›ʹͲͳ͸
……‡’–‡†ʹͺ—‡ʹͲͳ͸
—„Ž‹•Š‡†ͷ…–‘„‡”ʹͲͳ͸
Keywords:
Ž—‹†…ƒ–ƒŽ›–‹……”ƒ…‹‰
Ǧͷ
‘Ž†‘†‹ˆ‹…ƒ–‹‘
”‘’›Ž‡‡•‡Ž‡…–‹˜‹–›
‹…”‘Ǧƒ…–‹˜‹–›–‡•–
Š‡…ƒ–ƒŽ›–‹……”ƒ…‹‰‘ˆŽ‹‰Š–†‹‡•‡Ž‘‹Žȋʹ͵ͷȂ͵͵͹ιȌ‘˜‡”‰‘Ž†Ǧ‘†‹ˆ‹‡†Ǧͷ™ƒ•‹˜‡•–‹‰ƒ–‡†‹
ƒ•ƒŽŽ…‘ˆ‹‡†ˆŽ—‹†‹œ‡†„‡†ƒ–Ͷ͸Ͳ郐†ƒ„‹‡–’”‡••—”‡Ǥ‹ˆˆ‡”‡–—ȀǦͷ…ƒ–ƒŽ›•–•™‡”‡
’”‡’ƒ”‡† „› ƒ ‘†‹ˆ‹‡† †‡’‘•‹–‹‘Ǧ’”‡…‹’‹–ƒ–‹‘ ‡–Š‘† „› …Šƒ‰‹‰ –Š‡ ’”‡’ƒ”ƒ–‹‘ ’”‘…‡†—”‡
ƒ† –Š‡ ƒ‘—– ‘ˆ ‰‘Ž† Ž‘ƒ†‹‰ ƒ† ™‡”‡ …Šƒ”ƒ…–‡”‹œ‡† „› Ǧ”ƒ› †‹ˆˆ”ƒ…–‹‘ǡ ʹ ƒ†•‘”’Ǧ
–‹‘Ǧ†‡•‘”’–‹‘ǡ –‡’‡”ƒ–—”‡Ǧ’”‘‰”ƒ‡† †‡•‘”’–‹‘ ‘ˆ ͵ǡ –”ƒ•‹••‹‘ ‡Ž‡…–”‘ ‹…”‘•…‘’›
ƒ†‹†—…–‹˜‡Ž›…‘—’Ž‡†’Žƒ•ƒ•’‡…–”‘‡–‡”Ǥ–™ƒ•ˆ‘—†–Šƒ–ƒ•ƒŽŽƒ‘—–‘ˆ‰‘Ž†Šƒ†ƒ’‘•‹Ǧ
–‹˜‡‡ˆˆ‡…–‘–Š‡…ƒ–ƒŽ›–‹……”ƒ…‹‰‘ˆŽ‹‰Š–†‹‡•‡Ž‘‹Žƒ†‹…”‡ƒ•‡†’”‘’›Ž‡‡’”‘†—…–‹‘ƒ–ƒ”‡ŽƒǦ
–‹˜‡Ž›Ž‘™–‡’‡”ƒ–—”‡ǤŠ‡ƒ‹–‡ƒ…‡‘ˆ–Š‡Ǧͷ•–”—…–—”‡ǡ’‘”‡•‹œ‡†‹•–”‹„—–‹‘ƒ†–Š‡
†‡•‹–›‘ˆ™‡ƒƒ†•–”‘‰ƒ…‹†•‹–‡•‘ˆ–Š‡—ȀǦͷ…ƒ–ƒŽ›•–•†‡’‡†‡†‘–Š‡’”‡’ƒ”ƒ–‹‘’ƒǦ
”ƒ‡–‡”•ƒ†–Š‡—Ž‘ƒ†‹‰Ǥ‹—Ž–ƒ‡‘—•‡Šƒ…‡‡–‘ˆ–Š‡‹…”‘Ǧƒ…–‹˜‹–›ƒ†’”‘’›Ž‡‡’”‘Ǧ
†—…–‹‘”‡Ž‹‡•‘ƒ•›‡”‰›„‡–™‡‡–Š‡’‘”‡•‹œ‡†‹•–”‹„—–‹‘ƒ†–Š‡”‡Žƒ–‹˜‡‹–‡•‹–›‘ˆ–Š‡™‡ƒ
ƒ†•–”‘‰ƒ…‹†•‹–‡•Ǥ•‹‰‹ˆ‹…ƒ–‹’”‘˜‡‡–‹–Š‡‹…”‘Ǧƒ…–‹˜‹–›‹†‡š™‹–Šƒ‹…”‡ƒ•‡‘ˆͶǤͷ
—‹–• ƒ† ‹ –Š‡ ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ™‹–Š ƒ ‹…”‡ƒ•‡ ‘ˆ ʹ͵Ǥʹ —‹–• ™ƒ• ‘„–ƒ‹‡† ‘˜‡” –Š‡
—ȀǦͷ…ƒ–ƒŽ›•–™‹–Šƒƒ…–—ƒŽ—Ž‘ƒ†‹‰‘ˆͲǤͳ͹™–ΨǤ
̹ʹͲͳ͸ǡƒŽ‹ƒ•–‹–—–‡‘ˆŠ‡‹…ƒŽŠ›•‹…•ǡŠ‹‡•‡…ƒ†‡›‘ˆ…‹‡…‡•Ǥ
—„Ž‹•Š‡†„›Ž•‡˜‹‡”ǤǤŽŽ”‹‰Š–•”‡•‡”˜‡†Ǥ
1. Introduction
 ”‡…‡– †‡…ƒ†‡•ǡ ƒ† ‡•’‡…‹ƒŽŽ› ‹ –Š‡ Žƒ•– ͳͲ ›‡ƒ”•ǡ ‰‘Ž†
…ƒ–ƒŽ›•–• Šƒ˜‡ „‡…‘‡ ƒ ˜‹–ƒŽ ‡™ ˆ‘”…‡ ‹ –Š‡ ˆ‹‡Ž† ‘ˆ ‰”‡‡
…Š‡‹•–”› ȏͳȐ ‘™‹‰ –‘ –Š‡ ‡š’Ž‘•‹˜‡ ‰”‘™–Š ‘ˆ ”‡•‡ƒ”…Š ƒ†
†‡˜‡Ž‘’‡– ‹ –Š‡ ˆ‹‡Ž†• ‘ˆ ’‘ŽŽ—–‹‘ …‘–”‘Žǡ ˆ‹‡ …Š‡‹…ƒŽ
•›–Š‡•‹•ƒ†‡‡”‰›Ǥ”‘•‹’Ž‡”‡ƒ…–‹‘•ǡ•—…Šƒ•‘š‹†ƒǦ
–‹‘ ƒ† ‡’‘š‹†ƒ–‹‘ ‘ˆ ’”‘’›Ž‡‡ ȏʹǡ͵Ȑǡ –Š‡ •–—†‹‡† ”‡ƒ…–‹‘
•›•–‡• Šƒ˜‡ „‡‡ ‡š–‡†‡† –‘ Š›†”‘‰‡ƒ–‹‘ǡ …ƒ”„‘›Žƒ–‹‘ǡ
…‘†‡•ƒ–‹‘ƒ†‘–Š‡”‹†•‘ˆ”‡ƒ…–‹‘•‹‘”‰ƒ‹…•›–Š‡•‹•
ȏͶȂ͸ȐǤ Š‡ ”‡•‡ƒ”…Š …ƒ–‡‰‘”› Šƒ• ‡š’ƒ†‡† ˆ”‘ Š‡–‡”‘‰‡‡Ǧ
‘—•…ƒ–ƒŽ›•‹•ȏ͹Ȑ–‘Š‘‘‰‡‡‘—•…ƒ–ƒŽ›•‹•ȏͺȐƒ†’Š‘–‘…ƒ–ƒŽ›Ǧ
•‹•ȏͻȐǤ–—†‹‡•‘ˆƒ›†‹ˆˆ‡”‡–”‡ƒ…–‹‘•›•–‡•‘˜‡”—…ƒ–Ǧ
ƒŽ›•–• Šƒ˜‡ •Š‘™ –Šƒ– …‘’ƒ”‡† ™‹–Š ‘–Š‡” ’”‡…‹‘—• ‡–ƒŽ•ǡ
— …ƒ–ƒŽ›•–• ™‡”‡ …Šƒ”ƒ…–‡”‹œ‡† „› •‘‡ ’ƒ”–‹…—Žƒ” ˆ‡ƒ–—”‡•ǡ
•—…Š ƒ• ƒ ”‡Žƒ–‹˜‡Ž› Š‹‰Š …ƒ–ƒŽ›–‹… ƒ…–‹˜‹–› ƒ– Ž‘™ –‡’‡”ƒ–—”‡
ȏʹǡͶȐǡŠ‹‰Š •‡Ž‡…–‹˜‹–›‘ˆ–Š‡–ƒ”‰‡– ’”‘†—…–ȏ͵Ȃ͸Ȑƒ† ƒ •‹’Ž‡
”‘—–‡ ˆ‘” –Š‡ ‰”‡‡ •›–Š‡•‹• ‘ˆ …Š‡‹…ƒŽ• ȏͶȂ͸ȐǤ ‘™‡˜‡”ǡ
‘•–‘ˆ–Š‡•–—†‹‡†”‡ƒ…–‹‘•Šƒ˜‡„‡‡’‡”ˆ‘”‡†—†‡”‹Ž†
”‡ƒ…–‹‘ …‘†‹–‹‘•Ǣ –Š‡ ‹˜‡•–‹‰ƒ–‹‘ ‘ˆ ‰‘Ž† …ƒ–ƒŽ›•–• ‹ ”‡ŽƒǦ
–‹˜‡Ž›Šƒ”•Š…ƒ–ƒŽ›–‹…”‡ƒ…–‹‘•›•–‡•ǡ•—…Šƒ•…ƒ–ƒŽ›–‹……”ƒ…Ǧ
‹‰ ‘ˆ Š‡ƒ˜› ‘‹Ž ƒ– –‡’‡”ƒ–—”‡• Š‹‰Š‡” –Šƒ ͶͲͲ ι ™‹–Š —Ǧ
‡”‘—•”‡ƒ…–ƒ–•ǡŠƒ•”ƒ”‡Ž›„‡‡”‡’‘”–‡†Ǥ
”‘’›Ž‡‡ǡƒ•ƒ‹’‘”–ƒ–‘”‰ƒ‹…•›–Š‡–‹…”ƒ™ƒ–‡”‹ƒŽǡ
ȗ‘””‡•’‘†‹‰ƒ—–Š‘”Ǥ‡ŽȀƒšǣΪͺ͸Ǧͷ͵ͷǦ͸ͻͳͳ͹͵ʹǢǦƒ‹Žǣ“‹…š̷›–—Ǥ‡†—Ǥ… Š‹•™‘”™ƒ••—’’‘”–‡†„›–Š‡Šƒ†‘‰ƒ‹•Šƒ…Š‘Žƒ”•Š‹’ǡ–Š‡ƒ–ƒ‹†‘—„Ž‡ǦŠ—†”‡†•–ƒŽ‡–•’Žƒǡƒ†–Š‡Šƒ†‘‰ƒ–—”ƒŽ…‹‡…‡‘—†ƒǦ
–‹‘ȋʹͲͳͷͲͲ͸ȌǤ
ǣͳͲǤͳͲͳ͸Ȁͳͺ͹ʹǦʹͲ͸͹ȋͳ͸Ȍ͸ʹͶͻͻǦ͵ȁŠ––’ǣȀȀ™™™Ǥ•…‹‡…‡†‹”‡…–Ǥ…‘Ȁ•…‹‡…‡ȀŒ‘—”ƒŽȀͳͺ͹ʹʹͲ͸͹ȁŠ‹ǤǤƒ–ƒŽǤǡ‘ŽǤ͵͹ǡ‘ǤͳͲǡ…–‘„‡”ʹͲͳ͸ ͳ͹Ͷͺ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
…ƒ„‡—•‡†–‘’”‘†—…‡’‘Ž›’”‘’›Ž‡‡ǡƒ…”›Ž‘‹–”‹Ž‡ǡ’”‘’›Ž‡‡
‘š‹†‡ǡ‹•‘’”‘’›Ž„‡œ‡‡ǡ‹•‘’”‘’›ŽƒŽ…‘Š‘Žƒ†‘–Š‡”‹†—•–”‹Ǧ
ƒŽ”ƒ™ƒ–‡”‹ƒŽ•ǤŠ‡…‘•—’–‹‘‘ˆ’”‘’›Ž‡‡™‘”Ž†™‹†‡Šƒ•
‹…”‡ƒ•‡† †”ƒƒ–‹…ƒŽŽ› ‘™‹‰ –‘ ƒ”‡– †‡ƒ†• ˆ‘” –Š‡
†‘™•–”‡ƒ †‡”‹˜ƒ–‹˜‡• ȋƒ‹Ž› ’‘Ž›’”‘’›Ž‡‡ȌǤ Š‡ ”ƒ–‡ ƒ–
™Š‹…Š–Š‡…‘•—’–‹‘‘ˆ’”‘’›Ž‡‡Šƒ•‰”‘™‹”‡…‡–›‡ƒ”•
‹•ˆƒ•–‡”–Šƒ–Šƒ–‘ˆ‡–Š›Ž‡‡Ǥ”‘’›Ž‡‡‹•‘•–Ž›’”‘†—…‡†„›
•–‡ƒ…”ƒ…‹‰ƒ†ˆŽ—‹†‹œ‡†…ƒ–ƒŽ›–‹……”ƒ…‹‰ȋȌƒ•™‡ŽŽƒ•
†‡Š›†”‘‰‡ƒ–‹‘ ‘ˆ ’”‘’ƒ‡Ǥ ‡…ƒ—•‡ ‘ˆ Ž‘™‡” ’‘™‡” …‘Ǧ
•—’–‹‘ǡ …Š‡ƒ’‡” ƒ–‡”‹ƒŽ• ƒ† ƒ†ƒ’–ƒ„Ž‡ †‡˜‹…‡•ǡ –Š‡ ’”‘…‡•• Šƒ• ’Žƒ›‡† ƒ ‹…”‡ƒ•‹‰Ž› ‹’‘”–ƒ– ”‘Ž‡ ‹ –Š‡ ’”‘Ǧ
†—…–‹‘ ‘ˆ ’”‘’›Ž‡‡ǡ ™Š‡”‡ƒ• –Š‡ ”ƒ–‹‘ ‘ˆ ’”‘’›Ž‡‡ ƒ†‡
ˆ”‘ •–‡ƒ …”ƒ…‹‰ Šƒ• ‰”ƒ†—ƒŽŽ› †‡…”‡ƒ•‡† ȏͳͲȂͳʹȐǤ Š‡
’”‘’›Ž‡‡ ›‹‡Ž† ‘„–ƒ‹‡† ™‹–Š –Š‡ ’”‘…‡•• …ƒ „‡ ‹Ǧ
…”‡ƒ•‡†•‹‰‹ˆ‹…ƒ–Ž›„›—•‹‰Š‹‰Š“—ƒŽ‹–›”ƒ™ƒ–‡”‹ƒŽ•ǡ‘˜‡Ž
•‡Ž‡…–‹˜‡ …ƒ–ƒŽ›•–•Ȁƒ††‹–‹˜‡• ƒ† „› ‘’–‹‹œ‹‰ –Š‡ ’”‘…‡••
ȏͳ͵ȐǤ
Ǧͷƒ”‡–Š‡‘•–™‹†‡Ž›—•‡†ƒ…–‹˜‡…‘’‘‡–•‹…ƒ–ƒǦ
Ž›–‹… …”ƒ…‹‰ …ƒ–ƒŽ›•–• –‘ ‹…”‡ƒ•‡ –Š‡ ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–›
‘™‹‰ –‘ –Š‡‹” •’‡…‹ƒŽ ’‘”‡ •–”—…–—”‡ ™‹–Š •Šƒ’‡ •‡Ž‡…–‹˜‹–›ǡ
•–”‘‰ ƒ…‹†‹–›ǡ Ž‘™ Š›†”‘‰‡ –”ƒ•ˆ‡” ƒ…–‹˜‹–› ƒ† Š›†”‘–Š‡”Ǧ
ƒŽ•–ƒ„‹Ž‹–›ȏͳͲǡͳͳǡͳͶȐǤŠ‡‘†‹ˆ‹…ƒ–‹‘‘ˆǦͷ‹•‘‡‘ˆ–Š‡
ƒ‹ ‡–Š‘†• —•‡† –‘ †‡˜‡Ž‘’ ‘”‡ ƒ…–‹˜‡ …ƒ–ƒŽ›•–• ƒ† ‹Ǧ
…”‡ƒ•‡–Š‡’”‘’›Ž‡‡›‹‡Ž†Ǥ‘ˆ—”–Š‡”‹…”‡ƒ•‡–Š‡ƒ……‡••‹„‹Ž‹–›
‘ˆ –Š‡ ƒ…–‹˜‡ •‹–‡• ‘ˆ Ǧͷǡ –Š‡ •–—†› ‘ ƒ‘‡–‡” Ǧͷ
ȏͳͷǡͳ͸Ȑǡ •‹‰Ž‡ ȏͳ͹Ȑ ‘” ‡•‘Ǧ ƒ† ‹…”‘’‘”‘—• …‘’‘•‹–‡
Ǧͷ ȏͳͺȐǡ ƒ† ‡•‘’‘”‘—• Ǧͷ ȏͳͻȐ Šƒ• ƒ––”ƒ…–‡† ƒ––‡Ǧ
–‹‘Ǥ‘™‡˜‡”ǡ –Š‡ƒŒ‘”‡–Š‘†ˆ‘”‘†‹ˆ‹…ƒ–‹‘‘ˆǦͷ‹•
–Š”‘—‰Š –Š‡ ƒ††‹–‹‘ ‘ˆ †‹ˆˆ‡”‡– ‡Ž‡‡–• ‹…Ž—†‹‰ ‡Ž‡…–”‘Ǧ
‡‰ƒ–‹˜‡ ‡Ž‡‡–• •—…Š ƒ• ƒ† ǡ ƒŽƒŽ‹ ƒ† ƒŽƒŽ‹‡ ‡ƒ”–Š
‡Ž‡‡–• •—…Š ƒ• ‰ǡ ƒǡ ƒǡ ƒ† ƒǡ ‘–Š‡” ”ƒ”‡ ‡ƒ”–Š ‡Ž‡Ǧ
‡–••—…Šƒ•ƒƒ†‡ǡƒ†–”ƒ•‹–‹‘‡–ƒŽ‡Ž‡‡–••—…Šƒ•
—ǡǡ–ǡ‡ƒ†‹ȏͳ͹ǡʹͲȐǤ
Š‡‘†‹ˆ‹‡†Ǧͷ–Šƒ–‹•…—””‡–Ž›ƒ˜ƒ‹Žƒ„Ž‡Šƒ•„‡‡‡ˆǦ
ˆ‡…–‹˜‡ˆ‘”–Š‡’”‘†—…–‹‘‘ˆ’”‘’›Ž‡‡„›…ƒ–ƒŽ›–‹……”ƒ…‹‰‘ˆ
ͶŠ›†”‘…ƒ”„‘•ƒ†’›”‘Ž›•‹•‘ˆƒ’Š–Šƒƒ†ƒ•ƒƒ††‹–‹˜‡‹
–Š‡’”‘…‡••Ǥ‘™‡˜‡”ǡ–Š‡™‘”‹‰–‡’‡”ƒ–—”‡•ƒ”‡”‡ŽƒǦ
–‹˜‡Ž›Š‹‰ŠȋεͷͳͲιȌƒ†–Š‡…ƒ’ƒ„‹Ž‹–›–‘’”‘†—…‡’”‘’›Ž‡‡
‹• ‰”‡ƒ–Ž› ”‡†—…‡† ‹ˆ –Š‡ ”‡ƒ…–‹‘ –‡’‡”ƒ–—”‡ ‹• ”‡†—…‡†
ȏͳͲǡͳͶǡͳ͹ǡͳͻǡʹͳǡʹʹȐǤ ƒ‘’ƒ”–‹…Ž‡•ǡ …Ž—•–‡”• ƒ† …‘’Ž‡š‡• ‘ˆ
‰‘Ž†Šƒ˜‡™‹†‡Ž›„‡‡—•‡†–‘…ƒ–ƒŽ›œ‡†‹ˆˆ‡”‡––›’‡•‘ˆ”‡ƒ…Ǧ
–‹‘•ƒ†Šƒ˜‡•‹‰‹ˆ‹…ƒ–…ƒ–ƒŽ›–‹…ƒ…–‹˜‹–›—†‡”‹Ž†”‡ƒ…–‹‘
…‘†‹–‹‘•ȏʹȂͻȐǤƒ‰‘Ž†„‡—•‡†–‘”‡†—…‡–Š‡”‡ƒ…–‹‘–‡Ǧ
’‡”ƒ–—”‡‘ˆƒ†ƒ‹–ƒ‹–Š‡’”‘’›Ž‡‡›‹‡Ž†ǫ
…‹’‹‡–™‡–‡••‹’”‡‰ƒ–‹‘ȏʹ͵Ȑǡ‹‘‡š…Šƒ‰‡ȏʹͶǡʹͷȐǡ
…Š‡‹…ƒŽ ˜ƒ’‘” †‡’‘•‹–‹‘ ȏʹ͸Ȑ ƒ† †‡’‘•‹–‹‘ ’”‡…‹’‹–ƒ–‹‘
ȋȌ ȏʹ͹Ȑ Šƒ˜‡ „‡‡ —•‡† –‘ †‡’‘•‹– ‰‘Ž† ‹–‘ ǦͷǤ ‘‘†
–Š‡”ƒŽ•–ƒ„‹Ž‹–›‘ˆ—ȀǦͷ…ƒ–ƒŽ›•–ƒ––‡’‡”ƒ–—”‡•ƒ•Š‹‰Š
ƒ• ͺͲͲ ι Šƒ• ƒŽ•‘ „‡‡ ”‡’‘”–‡† ȏʹͺȐǡ ‹†‹…ƒ–‹‰ –Š‡ ’‘••‹„Ž‡
ƒ’’Ž‹…ƒ–‹‘ ‘ˆ —ȀǦͷ ‹ –Š‡ ’”‘…‡••Ǥ  –Š‡ ’”‡•‡–
•–—†›ǡ—ȀǦͷ…ƒ–ƒŽ›•–•ƒ’Ž‡•™‡”‡’”‡’ƒ”‡†—•‹‰ƒ‘†‹Ǧ
ˆ‹‡†‡–Š‘††‡•…”‹„‡†’”‡˜‹‘—•Ž›ȏʹͻǡ͵ͲȐǤ‡‹˜‡•–‹‰ƒ–‡†
–Š‡‹” •‡Ž‡…–‹˜‹–› ˆ‘” –Š‡ •›–Š‡•‹• ‘ˆ ’”‘’›Ž‡‡ ƒ† –Š‡ ‹Ǧ
…”‘Ǧƒ…–‹˜‹–› ‹†‡š ‹ –Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰ ‘ˆ Ž‹‰Š– †‹‡•‡Ž ‘‹Ž
ȋʹ͵ͷȂ͵͵͹ ιȌ ƒ– ƒ ”‡Žƒ–‹˜‡Ž› Ž‘™ –‡’‡”ƒ–—”‡ ‘ˆ Ͷ͸Ͳ ιǤ Š‡
‘†‹ˆ‹…ƒ–‹‘‘ˆǦͷ„›ƒ•ƒŽŽƒ‘—–‘ˆ‰‘Ž†Šƒ†ƒ’‘•‹–‹˜‡
‡ˆˆ‡…–‘–Š‡’”‘†—…–‹‘‘ˆ’”‘’›Ž‡‡ƒ†ƒ‹–ƒ‹‡†‘”‡˜‡
‡Šƒ…‡†–Š‡‹…”‘Ǧƒ…–‹˜‹–›Ǥ 2. Experimental
2.1. Catalystpreparation
Š‡ ”‡…‡‹˜‡† Ǧͷ œ‡‘Ž‹–‡ ȋ‹ȀŽ α ͵ͷǡ •—”ˆƒ…‡ ƒ”‡ƒ ʹͺͳǤͻ
ʹȀ‰Ȍ™ƒ•…ƒŽ…‹‡†ƒ–ͷͶͲ鋐ƒ‹”ˆ‘”ʹŠ’”‹‘”–‘ˆ—”–Š‡”ƒ’Ǧ
’Ž‹…ƒ–‹‘Ǥ ‹”•–ǡ –‘ ‹˜‡•–‹‰ƒ–‡ –Š‡ ‹’ƒ…– ‘ˆ –Š‡ ’”‡’ƒ”ƒ–‹‘ ’ƒ”ƒ‡Ǧ
–‡”•ǡ ˆ‘—” —ȀǦͷ …ƒ–ƒŽ›•–•ǡ †‡‘–‡† ƒ• —ȀǦͷǦƒǡ
—ȀǦͷǦ„ǡ —ȀǦͷǦ… ƒ† —ȀǦͷǦ†ǡ ™‡”‡ ’”‡’ƒ”‡† „›
—•‹‰ ‘—” ‘†‹ˆ‹‡† ‡–Š‘† †‡•…”‹„‡† ’”‡˜‹‘—•Ž› ȏʹͻǡ͵ͲȐǤ
”‹‡ˆŽ›ǡǦͷ ™ƒ• ˆ‹”•–‹’”‡‰ƒ–‡†—•‹‰ƒ ‰‹˜‡ …‘…‡–”ƒǦ
–‹‘‘ˆ—ŽͶ•‘Ž—–‹‘ƒ–’αͻǡ™Š‹…Š™ƒ•ƒ†Œ—•–‡†—•‹‰ƒ
•‘Ž—–‹‘Ǥ Š‡ ‘‹ƒŽ — Ž‘ƒ†‹‰ ™ƒ• ͳǤͲ ™–ΨǤ
—ȀǦͷǦƒ ™ƒ• ‘„–ƒ‹‡† „› ”‡†—…‹‰ –Š‡ ‹’”‡‰ƒ–‡† ’”‡Ǧ
…—”•‘” ‹Ǧ•‹–— —•‹‰ ƒͶǤ —ȀǦͷǦ„ ™ƒ• ‘„–ƒ‹‡† „›
•‘ƒ‹‰–Š‡‹’”‡‰ƒ–‡†’”‡…—”•‘”‹ƒƒ‘‹ƒ•‘Ž—–‹‘ƒ–
’αͳͲˆ‘”ʹͶŠǡ™ƒ•Š‹‰–Š”‡‡–‹‡•ˆ‘ŽŽ‘™‡†„›”‡†—…–‹‘‹
•‹–——•‹‰ƒͶǤ—ȀǦͷǦ…™ƒ•‘„–ƒ‹‡†„›‘Ž›†”›‹‰–Š‡
‹’”‡‰ƒ–‡†’”‡…—”•‘”ƒ–ͳͳͲιˆ‘”ʹŠǤ—ȀǦͷǦ†™ƒ•‘„Ǧ
–ƒ‹‡† „› •‘ƒ‹‰ –Š‡ ‹’”‡‰ƒ–‡† ’”‡…—”•‘” ‹ ƒ ƒ‘‹ƒ
•‘Ž—–‹‘ƒ–’αͳͲˆ‘”ʹͶŠˆ‘ŽŽ‘™‡†„›ˆ‹Ž–”ƒ–‹‘ƒ†™ƒ•Š‹‰
–Š”‡‡–‹‡•™‹–Š™ƒ–‡”ǡƒ•”‡’‘”–‡†’”‡˜‹‘—•Ž›ȏʹͻǡ͵ͲȐǤŽŽˆ‘—”
…ƒ–ƒŽ›•–•’”‡…—”•‘”•™‡”‡…ƒŽ…‹‡†ƒ–͵ͲͲιˆ‘”ʹŠǤ
‡…‘†Ž›ǡ –‘ ‹˜‡•–‹‰ƒ–‡ –Š‡ ‹’ƒ…– ‘ˆ — Ž‘ƒ†‹‰ǡ –Š‡
—ȀǦͷǦ† …ƒ–ƒŽ›•–• ™‹–Š –Š‡‘”‡–‹…ƒŽ — …‘–‡–• ‘ˆ ͲǤͷǡ ͲǤͺǡ
ͳǤʹ ƒ† ͳǤͷ ™–Ψ ‡š…‡’– ˆ‘” ͳǤͲ ™–Ψ ™‡”‡ ƒŽ•‘ ’”‡’ƒ”‡† „›
ƒ„‘˜‡ †‡•…”‹„‡† ’”‘…‡†—”‡Ǥ Š‡ ‘„–ƒ‹‡† …ƒ–ƒŽ›•–• ™‡”‡ †‡•Ǧ
‹‰ƒ–‡†ƒ•xΨ—ȀǦͷǦ†ǡ‹™Š‹…ŠxΨ‹•–Š‡‘‹ƒŽ“—ƒǦ
–‹–›’‡”…‡–ƒ‰‡‘ˆ—Ǥ ‡…ƒ—•‡–Š‡‹…”‘Ǧƒ…–‹˜‹–›‘ˆˆ”‡•Š…ƒ–ƒŽ›•–•‹•Š‹‰Šƒ†
—•–ƒ„Ž‡ǡ™Š‹…Š™‘—Ž†‘–”‡ˆŽ‡…––Š‡”‡ƒŽ•‹–—ƒ–‹‘‹ƒ’”ƒ…–‹Ǧ
…ƒŽ ƒ’’Ž‹…ƒ–‹‘ǡ Š›†”‘–Š‡”ƒŽ –”‡ƒ–‡– ‹• —•—ƒŽŽ› ƒ†‘’–‡†
’”‹‘” –‘ ‹…”‘Ǧƒ…–‹˜‹–› –‡•–‹‰ –‘ †‡ƒ…–‹˜ƒ–‡ –Š‡ ˆ”‡•Š …ƒ–ƒŽ›•–Ǥ
Š‡”‡ˆ‘”‡ǡ ƒŽŽ –Š‡ •ƒ’Ž‡• ‹…Ž—†‹‰ –Š‡ ’ƒ”‡– Ǧͷ ™‡”‡
ƒ‰‡†ƒ–ͺͲͲ鋐ˆŽ‘™‹‰™ƒ–‡”•–‡ƒˆ‘”ͶŠƒ†–Š‡…ƒŽ…‹‡†
ƒ–͵ͲͲιˆ‘”ͳŠǤ
2.2. Characterization
Š‹ƒ†œ—Ǧ͸ͳͲͲ†‹ˆˆ”ƒ…–‘‡–‡”—•‹‰—KȽ”ƒ†‹ƒ–‹‘
ȋͶͲǡ͵ͲȌ™ƒ•‡’Ž‘›‡†–‘‘„–ƒ‹Ǧ”ƒ›†‹ˆˆ”ƒ…–‹‘ȋȌ
’ƒ––‡”• ‘ˆ ƒŽŽ •–—†‹‡† •ƒ’Ž‡• ™‹–Š ƒ •…ƒ‹‰ ”ƒ‰‡ ‘ˆ ʹɅ
ˆ”‘ ͳͲ –‘ ͺͲι ƒ– ƒ •…ƒ‹‰ ”ƒ–‡ ‘ˆ ͸ιȀ‹Ǥ Ǧ͵ͲͲͲ
ȋ—ƒ–ƒ…Š”‘‡ ‘”’ǤȌ ™ƒ• —•‡† –‘ ‘„–ƒ‹ ʹ ƒ†•‘”’Ǧ
–‹‘Ǧ†‡•‘”’–‹‘ ‹•‘–Š‡”• ƒ– Ϋͳͻ͸ ιǤ ”‹‘” –‘ ƒƒŽ›•‹•ǡ ‡ƒ…Š
•ƒ’Ž‡™ƒ•‡˜ƒ…—ƒ–‡†ƒ–ͳʹͲιˆ‘”ͶŠǤ ’ǦͷͲͺͲ —Ž–‹Ǧˆ—…–‹‘ƒŽ ƒ—–‘ƒ–‹… ƒ†•‘”’–‹‘ ‹•–”—Ǧ
‡– ȋ‹ƒŒ‹ ‹ƒ“—ƒ †—•–”› ƒ† ”ƒ†‡ ‡˜‡Ž‘’‡– ‘Ǥǡ
ǡ ‹ƒŒ‹ǡ Š‹ƒȌ ™ƒ• —•‡† –‘ –ƒ‡ –‡’‡”ƒ–—”‡Ǧ’”‘Ǧ
‰”ƒ‡† †‡•‘”’–‹‘ ‘ˆ ͵ ȋ͵ǦȌ …—”˜‡• ˆ‘” ƒŽŽ •–—†‹‡†
…ƒ–ƒŽ›•–•Ǥ Š‡ •ƒ’Ž‡ ™ƒ• Ž‘ƒ†‡† ‹–‘ ƒ •–ƒ‹Ž‡•• Ǧ•Šƒ’‡†
‹…”‘”‡ƒ…–‘”ƒ†’”‡–”‡ƒ–‡†ƒ–͸ͲͲ鋐ˆŽ‘™‹‰‡•–”‡ƒȋʹͲ
Ȁ‹Ȍˆ‘”ͲǤͷŠ„‡ˆ‘”‡‹–™ƒ••ƒ–—”ƒ–‡†™‹–Š͵‰ƒ•ƒ–Ž‘™
–‡’‡”ƒ–—”‡Ǥ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
–”ƒ•‹••‹‘ ‡Ž‡…–”‘‹…”‘•…‘’‡ ȋǡǦʹͳͲͲǡ
‘’ƒ›ǡ ‘›‘ǡ ƒ’ƒȌ ‡“—‹’’‡† ™‹–Š ƒ šˆ‘”† •’‡…–”‘‡–‡” ˆ‘” Ǧ”ƒ› ‡‡”‰› †‹•’‡”•‹˜‡ ȋȌ •’‡…–”‘•…‘’›
ƒƒŽ›•‹•™ƒ•—•‡†ƒ–ʹͲͲƒ……‡Ž‡”ƒ–‹‰˜‘Ž–ƒ‰‡–‘‡˜ƒŽ—ƒ–‡–Š‡
†‹•’‡”•‹‘ ’”‘’‡”–‹‡• ‘ˆ –™‘ ”‡’”‡•‡–ƒ–‹˜‡ —ȀǦͷ •ƒǦ
’Ž‡•Ǥ
 ‹†—…–‹˜‡Ž› …‘—’Ž‡† ’Žƒ•ƒ •’‡…–”‘‡–‡”
ȋǦǡ Š‡”‘ Ž‡…–”‘ ‘”’‘”ƒ–‹‘ǡ Ȍ ™ƒ• —•‡† –‘
‡ƒ•—”‡–Š‡“—ƒ–‹–›‘ˆ‰‘Ž†‹–Š‡•ƒ’Ž‡•ƒ–™‘”‹‰…‘†‹Ǧ
–‹‘•‘ˆʹ͹œƒ†ͳͳʹǤŠ›†”‘ˆŽ—‘”‹…ƒ…‹†•‘Ž—–‹‘ƒ†
ƒ“—ƒ”‡‰‹ƒ™‡”‡—•‡†–‘†‹••‘Ž˜‡–Š‡•ƒ’Ž‡•Ǥ
Diesel
Gasoline
Feedstock oil
0
2.2. MicroǦactivitytest
ͳ͹Ͷͻ
21.18
U (mV)
10
20
30
40
Retention time (min)
50
60
Fig.2.—–Ǧ‘ˆˆ’‘‹–‘ˆ–Š‡‰ƒ•‘Ž‹‡ƒ††‹‡•‡Ž‹–Š‡ˆ‡‡†‘‹ŽǤ
‹…”‘Ǧƒ…–‹˜‹–› –‡•–• ‘ˆ –Š‡ …ƒ–ƒŽ›•–• ™‡”‡ ‘„–ƒ‹‡† —•‹‰
ƒ‰ƒ‰ Ž‹‰Š– †‹‡•‡Ž ȋʹ͵ͷȂ͵͵͹ ιȌ ƒ• –Š‡ ˆ‡‡†•–‘… ‹ ƒ •ƒŽŽ
…‘ˆ‹‡† ˆŽ—‹†‹œ‡† „‡† ƒ– Ͷ͸Ͳ ιǤ Š”‡‡ ‰”ƒ• ‘ˆ …ƒ–ƒŽ›•– ™ƒ•
’Žƒ…‡† ‹–‘ ƒ •‡ŽˆǦ…‘•–”—…–‡† ”‡ƒ…–‹‘ †‡˜‹…‡ ȋ‹‰Ǥ ͳȌ ƒ† –Š‡
‘‹Ž™ƒ•‹Œ‡…–‡†‹–‘–Š‡ˆ—”ƒ…‡„›ƒ•›”‹‰‡™Š‡–Š‡–‡’‡”Ǧ
ƒ–—”‡ ”‡ƒ…Š‡† ƒ ’”‡•‡– –‡’‡”ƒ–—”‡Ǥ Š‡ ™‡‹‰Š– ”ƒ–‹‘ ‘ˆ –Š‡
…ƒ–ƒŽ›•––‘‘‹Žƒ†–Š‡…‘–ƒ…––‹‡™‡”‡͵Ǥʹƒ†͹Ͳ•ǡ”‡•’‡…Ǧ
–‹˜‡Ž›ǤŠ‡’”‘†—…–•™‡”‡’—”‰‡†„›—•‹‰Š‹‰ŠǦ’—”‹–›‹–”‘‰‡
ƒˆ–‡” –Š‡ …‘’Ž‡–‹‘ ‘ˆ –Š‡ ˆ‡‡† ƒ† •‡’ƒ”ƒ–‡† –Š”‘—‰Š ƒ
‹…‡Ǧ™ƒ–‡”„ƒ–ŠǤ Š‡ ‰ƒ•‡‘—• ’”‘†—…–• ™‡”‡ †‡–‡”‹‡† „› ƒ ‘ǦŽ‹‡
ǦͻʹͲ ™‹–Š ƒ ˆŽƒ‡ ‹‘‹œƒ–‹‘ †‡–‡…–‘” ‡“—‹’’‡† ™‹–Š ƒ
ǦͳͲͳ…ƒ’‹ŽŽƒ”›…‘Ž—ǤŠ‡Ž‹“—‹†’”‘†—…–•™‡”‡ƒƒŽ›œ‡†„›
ƒ—ƒŽ •ƒ’Ž‹‰ ƒˆ–‡” …‘ŽŽ‡…–‹‘ ‹ ƒ ‰Žƒ•• …‘–ƒ‹‡”Ǥ Š‡
…‘’‘•‹–‹‘‘ˆ‰ƒ•‘Ž‹‡ƒ††‹‡•‡Ž‹–Š‡Ž‹“—‹†’Šƒ•‡™ƒ•†‡Ǧ
–‡”‹‡†ƒ––Š‡”‡–‡–‹‘–‹‡‘ˆnǦ†‘†‡…ƒ‡ȋ‹‰ǤʹȌǤ
Š‡ ƒ”‡ƒ ‘”ƒŽ‹œƒ–‹‘ ‡–Š‘† ™ƒ• ƒ’’Ž‹‡† –‘ …‘ŽŽ‡…– –Š‡
†ƒ–ƒǤ ”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ™ƒ• †‡ˆ‹‡† „› –Š‡ …‘–‡– ‘ˆ ’”‘Ǧ
’›Ž‡‡‹–Š‡‰ƒ•‡‘—•’”‘†—…–•ǤŠ‡‹…”‘Ǧƒ…–‹˜‹–›‹†‡šȋȌ
ƒ† …‘˜‡”•‹‘ ‘ˆ –Š‡ ‘‹Ž ™‡”‡ …ƒŽ…—Žƒ–‡† ƒ……‘”†‹‰ –‘ –Š‡
ͻʹǦͻͲ‡–Š‘†—•‹‰‡“—ƒ–‹‘•ȋͳȌƒ†ȋʹȌǣ
αͳͲͲȂͳͲͲέȋͳΫGΨȌέWͳȀW
ȋͳȌ
‘˜‡”•‹‘αȋWέDͲΨΫDΨέWͳȌȀWέDͲΨ ȋʹȌ
™Š‡”‡DͲΨ”‡ˆ‡”•–‘–Š‡’”‘’‘”–‹‘‘ˆ†‹‡•‡Ž…‘’‘‡–•‹–Š‡
Ž‹‰Š– †‹‡•‡Ž ‘‹Ž ˆ‡‡† ™‹–Š Š›†”‘…ƒ”„‘• Š‡ƒ˜‹‡” –Šƒ
nǦ†‘†‡…ƒ‡ǢWƒ†Wͳ”‡ˆ‡”–‘–Š‡“—ƒŽ‹–›‘ˆ–Š‡Ž‹“—‹†•„‡ˆ‘”‡
ƒ†ƒˆ–‡””‡ƒ…–‹‘ǢDΨƒ†GΨ”‡ˆ‡”–‘”‡Žƒ–‹˜‡…‘–‡–‘ˆ†‹‡Ǧ
•‡Ž ƒ† ‰ƒ•‘Ž‹‡ǡ ”‡•’‡…–‹˜‡Ž›ǡ ‹ –Š‡ Ž‹“—‹† ’”‘†—…–Ǥ – Ž‡ƒ•–ǡ
–™‘ –‡•–• ™‡”‡ ’‡”ˆ‘”‡† –‘ ‡˜ƒŽ—ƒ–‡ –Š‡ …ƒ–ƒŽ›•–• ƒ† –Š‡
‡ƒ˜ƒŽ—‡•™‡”‡–ƒ‡™‹–Š–Š‡ƒ„•‘Ž—–‡†‹ˆˆ‡”‡…‡„‡–™‡‡
–Š‡–™‘’ƒ”ƒŽŽ‡Ž”‡•—Ž–•Ž‡••–ŠƒʹΨǤ
3. Resultsanddiscussion
3.1. Thecatalyticcrackingresultsoflightdieseloil
Š‡ ”‡•—Ž–• ‘ˆ –Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰ ‘ˆ Ž‹‰Š– †‹‡•‡Ž ‘˜‡”
Ǧͷ™‹–Š‘”™‹–Š‘—–‰‘Ž†‘†‹ˆ‹…ƒ–‹‘ƒ”‡Ž‹•–‡†‹ƒ„Ž‡ͳǡ
‹…Ž—†‹‰–Š‡ƒ…–—ƒŽ—Ž‘ƒ†‹‰ƒ†–Š‡”ƒ–‹‘‘ˆ™‡ƒƒ…‹†•‹–‡•
–‘•–”‘‰ƒ…‹†•‹–‡•ǡ™Š‹…Š™‡”‡„ƒ•‡†‘‘—”͵Ǧ‡ƒ•Ǧ
—”‡‡–•Ǥ  …‘’ƒ”‹•‘ ™‹–Š –Š‡ ’ƒ”‡– Ǧͷ …ƒ–ƒŽ›•–ǡ ‹– ‹•
…Ž‡ƒ” –Šƒ– –Š‡ ‹–”‘†—…–‹‘ ‘ˆ ‰‘Ž† ‹–‘ Ǧͷ ‹’”‘˜‡† –Š‡
’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ™‹–Š –Š‡ ‡š…‡’–‹‘ ‘ˆ –Š‡ —ȀǦͷǦƒ
…ƒ–ƒŽ›•–Ǥ‘™‡˜‡”ǡ–Š‡…ƒ–ƒŽ›–‹……”ƒ…‹‰ƒ…–‹˜‹–›”‡’”‡•‡–‡†„›
ƒ‹…”‘Ǧƒ…–‹˜‹–›‹†‡š™ƒ•‘Ž›‡Šƒ…‡†‘˜‡”–Š‡–Š”‡‡…ƒ–ƒǦ
Ž›•–•‘ˆ—ȀǦͷǦ†™‹–Š–Š‡‘”‡–‹…ƒŽ—Ž‘ƒ†‹‰•‘ˆͲǤͷǡͲǤͺƒ†
ͳǤͲ ™–ΨǤ Š‡ …‘””‡•’‘†‹‰ ‹…”‡ƒ•‡ ‹ ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–›
‘˜‡”–Š‡•‡–Š”‡‡…ƒ–ƒŽ›•–•™ƒ•ͺǤͺΨǡʹǤͻΨƒ†ʹ͵ǤʹΨǡ™Š‡”‡ƒ•
–Š‡ ‹…”‡ƒ•‡ ‹ –Š‡‹” ‹…”‘Ǧƒ…–‹˜‹–› ‹†‡š ȋȌ ™ƒ• ͹ǤͳΨǡ
ͶǤ͵Ψ ƒ† ͶǤͷΨǡ ”‡•’‡…–‹˜‡Ž›Ǥ Š‡ ”‡•—Ž–• •—‰‰‡•– –Šƒ– ƒ •ƒŽŽ
ƒ‘—–‘ˆ‰‘Ž†Šƒ•ƒ’‘•‹–‹˜‡‡ˆˆ‡…–‘–Š‡…ƒ–ƒŽ›–‹……”ƒ…‹‰‘ˆ
Ž‹‰Š– †‹‡•‡Ž ‘‹Ž –‘ ‹…”‡ƒ•‡ –Š‡ ’”‘†—…–‹‘ ‘ˆ ’”‘’›Ž‡‡ ƒ– ƒ
Ž‘™‡””‡ƒ…–‹‘–‡’‡”ƒ–—”‡‘ˆͶ͸ͲιǤ ‡…‡–Ž›ǡ
—‘‡–ƒŽǤȏ͵ͳǡ͵ʹȐˆ‘—†–Šƒ–ƒ•‡”‹‡•‘ˆ‹ȀŽ‘Ǧ
Ž‡…—Žƒ”•‹‡˜‡•†‡’‘•‹–‡†™‹–Š‰‘Ž†•Š‘™‡†Š‹‰Š‡”ƒ…–‹˜‹–›ƒ†ƒ
Ž‘™‡””‡ƒ…–‹‘–‡’‡”ƒ–—”‡–Šƒ–Š‘•‡™‹–Š‘—–‰‘Ž†‘†‹ˆ‹…ƒǦ
–‹‘ ˆ‘” ƒ”‘ƒ–‹œƒ–‹‘ǡ ‹•‘‡”‹œƒ–‹‘ ƒ† ƒŽ›Žƒ–‹‘ ”‡ƒ…–‹‘•
ƒ† …ƒ–ƒŽ›–‹… …”ƒ…‹‰ ‘ˆ ͵Ȃͻ Š›†”‘…ƒ”„‘•Ǥ Š‹• ˆ—”–Š‡”
•—’’‘”–•–Š‡’‘–‡–‹ƒŽƒ’’Ž‹…ƒ–‹‘‘ˆ‰‘Ž†‹–Š‡ˆ‹‡Ž†‘ˆ’‡–”‘Ǧ
Ž‡—…Š‡‹•–”›Ǥ
3.2. XRDmeasurements Fig.1. …Š‡ƒ–‹…†‹ƒ‰”ƒ‘ˆ–Š‡‹…”‘Ǧƒ…–‹˜‹–›‡ƒ•—”‡‡–Ǥ
‹‰Ǥ͵•Š‘™•–Š‡’ƒ––‡”•‘ˆǦͷƒ†–Š‡—ȀǦͷ
…ƒ–ƒŽ›•–•Ǥ…‘’ƒ”‹•‘™‹–Š–Š‡’ƒ”‡–Ǧͷǡ–Š‡’ƒ––‡”•‘ˆ
—ȀǦͷǦ„ǡ…ǡƒ††•‡‡–‘ƒ‹–ƒ‹–Š‡•ƒ‡•–”—…–—”‡ǡ„—–
ͳ͹ͷͲ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
Table1
”‘†—…–†‹•–”‹„—–‹‘•‘ˆ–Š‡…ƒ–ƒŽ›–‹……”ƒ…‹‰‘ˆŽ‹‰Š–†‹‡•‡Ž‘‹Žƒ–Ͷ͸Ͳι‘˜‡”–Š‡•–—†‹‡†…ƒ–ƒŽ›•–•Ǥ
”‘†—…–†‹•–”‹„—–‹‘ȋΨȌ
‘˜‡”•‹‘
”‘’›Ž‡‡•‡Ž‡…–‹˜‹–› —…‘–Ǥ„ Ȁ…
ȋΨȌ
ȋΨȌ
ȋΨȌ
ȋ™–ΨȌ
”›‰ƒ•Ϊ
ƒ
ƒ•‘Ž‹‡
‹‡•‡Ž‘‹Ž
Ǧͷ
ͶͲǤͶ
ͺǤ͸
ͷͳǤͲ
Ͷ͸ǤͲ
ͶͻǤͲ
ʹͻǤ͸
Ȅ
ͶǤ͸
ͳǤͲ™–Ψ—ȀǦͷǦƒ
͵͵Ǥ͹
ͳͲǤͲ
ͷ͸Ǥ͵
ʹͺǤͳ
͵ʹǤͳ
ʹ͹Ǥͻ
ͲǤ͸͹
Ͳ
ͳǤͲ™–Ψ—ȀǦͷǦ„
ʹ͸Ǥ͹
ͶǤͻ
͸ͺǤͶ
ͶͲǤͶ
Ͷ͵Ǥͺ
͵ͳǤͶ
ͲǤͲͺ
ʹʹǤͷ
ͳǤͲ™–Ψ—ȀǦͷǦ…
͵͵Ǥ͹
ͶǤ͹
͸ͳǤ͸
͵ͶǤͳ
͵ͺǤ͵
ͶͲǤͺ
ͲǤͻͳ
ʹǤ͵
ͲǤͷ™–Ψ—ȀǦͷǦ†
ͷͷǤͺ
͵Ǥͳ
ͶͳǤͳ
͸͹Ǥͳ
ͷ͸Ǥͳ
͵ͺǤͶ
ͲǤͳͲ
͵ǤͶ
ͲǤͺ™–Ψ—ȀǦͷǦ†
ͶͶǤͻ
ͺǤͶ
Ͷ͸Ǥ͹
ͷͲǤͳ
ͷ͵Ǥ͵
͵ʹǤͷ
ͲǤͳʹ
͵Ǥ͵ͷ
ͳǤͲ™–Ψ—ȀǦͷǦ†
Ͷ͸Ǥ͹
͸Ǥͺ
Ͷ͸Ǥͷ
ͷͲǤͶ
ͷ͵Ǥͷ
ͷʹǤͺ
ͲǤͳ͹
͵Ǥͺ
ͳǤʹ™–Ψ—ȀǦͷǦ†
ʹͶǤʹ
ͳͳǤͳ
͸ͶǤ͹
͵ͲǤͻ
͵ͷǤ͵
ͶͳǤͶ
ͲǤʹͲ
ͶǤͲ͹
ͳǤͷ™–Ψ—ȀǦͷǦ†
ʹ͵Ǥͻ
ͳͲǤʹ
͸ͷǤͻ
ʹͻǤ͸
͵ͶǤͳ
͸ͺǤ͸
ͲǤʹͳ
ͶǤͷ
ƒ
‡ƒ•Ž‹“—‡ˆ‹‡†’‡–”‘Ž‡—‰ƒ•Ǥ„Š‡ƒ…–—ƒŽ—Ž‘ƒ†‹‰‡ƒ•—”‡†„›ǦƒƒŽ›•‹•Ǥ…Š‡”ƒ–‹‘‘ˆ™‡ƒƒ…‹†–‘•–”‘‰ƒ…‹†„ƒ•‡†‘͵Ǧ
‡ƒ•—”‡‡–•Ǥ
ƒ–ƒŽ›•–
–Š‡ ‹–‡•‹–› †‡…”‡ƒ•‡• ‰”ƒ†—ƒŽŽ› ˆ”‘ —ȀǦͷǦ† –‘
—ȀǦͷǦ…ƒ†–Š‡—ȀǦͷǦ„Ǥ‘˜‡”•‡Ž›ǡ—ǦǦƒ…‘Ǧ
’Ž‡–‡Ž› Ž‘•‡• –Š‡ •–”—…–—”‡ ‘ˆ –Š‡ ‘”‹‰‹ƒŽ ’ƒ––‡”Ǥ Š‡
—ȀǦͷǦ† •ƒ’Ž‡ ‡šŠ‹„‹–• –Š‡ –›’‹…ƒŽ ’‡ƒ• ‘ˆ Ǧͷ ™‹–Š
•‹‹Žƒ”‹–‡•‹–‹‡•ǡ‹†‹…ƒ–‹‰–Šƒ––Š‡•–”—…–—”‡”‡ƒ‹•‹–ƒ…–
ƒˆ–‡” –Š‡ ‘†‹ˆ‹…ƒ–‹‘Ǥ Š‡ ’ƒ––‡”• ‘ˆ —ȀǦͷǦ† ™‹–Š
˜ƒ”‹‘—•—Ž‘ƒ†‹‰•‘ˆͲǤͷΨȂͳǤͷΨȋ‘–•Š‘™Ȍˆ—”–Š‡”•—’’‘”–
–Š‡ ƒ‹–‡ƒ…‡ ‘ˆ –Š‡ Ǧͷ •–”—…–—”‡ –Š”‘—‰Š –Š‡ †Ǧ–›’‡
’”‡’ƒ”ƒ–‹‘’”‘…‡†—”‡Ǥ ‘” ƒŽŽ •ƒ’Ž‡• ™‹–Š ‰‘Ž† ‘†‹ˆ‹…ƒ–‹‘ǡ –Š‡ …Šƒ”ƒ…–‡”‹•–‹…
’‡ƒ•…‘””‡•’‘†‹‰–‘—ȋͳͳͳȌƒ†ȋʹͲͲȌ…”›•–ƒŽ’Žƒ‡•ƒ”‡
†‡–‡…–‡†ƒ–ʹɅα͵ͺǤʹ郐†ͶͶǤͶιǡ™Š‹…Š‡ƒ•–Šƒ––Š‡—’ƒ”Ǧ
–‹…Ž‡• ƒ”‡ ‘– ƒ• •ƒŽŽ ƒ• –Š‘•‡ –Šƒ– ™‡ ’”‡˜‹‘—•Ž› ’”‡’ƒ”‡†
‘˜‡”ƒƒŽ—‹ƒ•—’’‘”–ȏʹͻǡ͵ͲȐǤŠ‡‡ƒ•‹œ‡‘ˆ–Š‡—’ƒ”Ǧ
–‹…Ž‡•‘ƒŽ—‹ƒ™ƒ•‹–Š‡”ƒ‰‡‘ˆʹȂ͵ǤŠ‡†‹ƒ‡–‡”•‘ˆ
–Š‡—’ƒ”–‹…Ž‡•‡•–‹ƒ–‡†„›–Š‡…Š‡”‡”ˆ‘”—Žƒƒ”‡ƒ’’”‘šǦ
‹ƒ–‡Ž›ʹͲǤŠ‹•˜ƒŽ—‡‹•“—‹–‡”‘—‰Š„‡…ƒ—•‡–Š‡‹–‡•‹–‹‡•
‘ˆ — ’‡ƒ• ƒ”‡ ‘– ˜‡”› ˜‹•‹„Ž‡ ƒ† ˜ƒ”› ™‹–Š †‹ˆˆ‡”‡– •ƒǦ
’Ž‡•Ǥ
^ Au(200)
* Au(111)
2000
3.3. TEMobservations ‘‹˜‡•–‹‰ƒ–‡–Š‡†‹•’‡”•‹‘‘ˆ‰‘Ž†’ƒ”–‹…Ž‡•‹–Š‡Ǧͷǡ
–™‘•ƒ’Ž‡•‘ˆͲǤͷƒ†ͳǤͷ™–Ψ—ȀǦͷǦ†™‡”‡•‡Ž‡…–‡†–‘
ƒ‡‘„•‡”˜ƒ–‹‘•ǤŠ‡”‡’”‡•‡–ƒ–‹˜‡‹ƒ‰‡•‘ˆ–Š‡
ͳǤͷ ™–Ψ —ȀǦͷǦ† •ƒ’Ž‡ ƒ”‡ †‹•’Žƒ›‡† ‹ ‹‰Ǥ ͶǤ Š‡ •‹œ‡
†‹•–”‹„—–‹‘ ‘ˆ –Š‡ — ’ƒ”–‹…Ž‡• ˜ƒ”‹‡† ‹ ƒ ”ƒ–Š‡” Žƒ”‰‡ ”ƒ‰‡
ˆ”‘δͳͲ–‘δʹͲͲ”‡‰ƒ”†Ž‡••‘ˆ–Š‡—Ž‘ƒ†‹‰•ǤŠ‡†‡’‘Ǧ
•‹–‹‘‘ˆ—’ƒ”–‹…Ž‡•™ƒ•˜‡”›‹Š‘‘‰‡‡‘—•ǡ™‹–Šƒˆ‡™—
’ƒ”–‹…Ž‡• ‘ •‘‡ ’ƒ”–• ‘ˆ –Š‡ Ǧͷ •—„•–”ƒ–‡ ™Š‡”‡ƒ• ‘
‘–Š‡” ’ƒ”–• –ƒ…‹‰ —„‡”• ‘ˆ — ’ƒ”–‹…Ž‡•Ǥ ˆ‡™ •ƒŽŽ —
’ƒ”–‹…Ž‡•ǡ™Š‹…Šƒ”‡‘–‡ƒ•›–‘†‹•–‹‰—‹•Šǡƒ”‡‹†‹…ƒ–‡†„›”‡†
ƒ””‘™•‹–Š‡‹ƒ‰‡•Ǥ
”‘ –Š‡•‡ ”ƒ†‘Ž› †‹•’‡”•‡† — ’ƒ”–‹…Ž‡•ǡ ™‡ …ƒ •‡‡
–Šƒ– •‘‡ — ’ƒ”–‹…Ž‡• ˆ‘” ƒ ˆŽƒ– •Šƒ’‡ ƒ† •Š‘™ ƒ •–”‘‰‡”
‹–‡”ƒ…–‹‘ ™‹–Š –Š‡ •—„•–”ƒ–‡Ǥ —”–Š‡”‘”‡ǡ •‘‡ •ƒŽŽ‡” —
’ƒ”–‹…Ž‡• ƒ› „‡ ‡„‡††‡† ‹ •Ž‹–Ǧ’‘”‡• „‡–™‡‡ –Š‡ ˆŽƒ›
Ǧͷ ’ƒ”–‹…Ž‡•ǤŽ‡ƒ”‡”‹ƒ‰‡•‘ˆ–Š‹• ƒ”‡†‹•’Žƒ›‡†‹‹‰Ǥ ͷǡ
™Š‹…Š•Š‘™•–™‘‹ƒ‰‡•‘ˆͳǤͷ™–Ψ—ȀǦͷǦ†„‡ˆ‘”‡
ƒ†ƒˆ–‡”‹–‹•ƒ‰‡†‹•–‡ƒƒ–ͺͲͲιǤŠ‡•‡…ƒ•‡•ƒ”‡•—”‡Ž›
‘– ’‘’—Žƒ” ˆ‘” –Š‡ •–—†‹‡† •ƒ’Ž‡• ™‹–Š ‰‘Ž† ‘†‹ˆ‹…ƒ–‹‘Ǣ
Š‘™‡˜‡”ǡ‹–ƒ›ƒ……‘—–ˆ‘”–Š‡…‘–”‹„—–‹‘‘ˆ–Š‡•‡•ƒŽŽ—
’ƒ”–‹…Ž‡•‘–Š‡’‘”‡•‹œ‡†‹•–”‹„—–‹‘‘ˆ–Š‡’ƒ”‡–Ǧͷ•—„Ǧ
(1)
Intensity (a.u.)
1600
*
^
(2)
*
^
(3)
*
^
(4)
*
^
(5)
1200
800
400
0
10
20
30
40
50
2T/( o )
Fig. 3. ’ƒ––‡”• ‘ˆ Ǧͷ ȋͳȌǡ —ȀǦͷǦƒ ȋʹȌǡ —ȀǦͷǦ„ ȋ͵Ȍǡ
—ȀǦͷǦ…ȋͶȌǡƒ†—ȀǦͷǦ†ȋͷȌ…ƒ–ƒŽ›•–•Ǥ
Fig.4.‡’”‡•‡–ƒ–‹˜‡‹ƒ‰‡•‘ˆͳǤͷ™–Ψ—ȀǦͷǦ†•ƒ’Ž‡Ǥ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
Fig.5.‹ƒ‰‡•‘ˆͳǤͷ™–Ψ—ȀǦͷ„‡ˆ‘”‡ȋƒȌƒ†ƒˆ–‡”ȋ„Ȍƒ‰‡†
‹•–‡ƒƒ–ͺͲͲιǤ
•–”ƒ–‡ ƒ† Š‡…‡ ‡š‡”– •‘‡ ‹’ƒ…– ‘ –Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰
’‡”ˆ‘”ƒ…‡Ǥ
3.4. N2adsorptionǦdesorptionisothermsofZSMǦ5withand
withoutgoldmodification
‹‰Ǥ ͸ •Š‘™• –Š‡ ʹ ƒ†•‘”’–‹‘Ǧ†‡•‘”’–‹‘ ‹•‘–Š‡”• ‘ˆ
Ǧͷƒ†–Š‡ —ȀǦͷǦƒǡ „ǡ …ǡ † …ƒ–ƒŽ›•–•Ǥ Š‡‹•‘–Š‡”•‘ˆ
Ǧͷ ƒ† —ȀǦͷǦ… ƒ† —ȀǦͷǦ† ’”‡•‡– ƒ –›’‡ ‹•‘Ǧ
–Š‡” ™‹–Š ƒ Ͷ Š›•–‡”‡•‹• Ž‘‘’ǡ ™Š‹…Š ‹• –›’‹…ƒŽ ˆ‘” ‹Ǧ
…”‘’‘”‘—•ƒ–‡”‹ƒŽ• ™‹–Š•‘‡•Ž‹–ǦŽ‹‡ ’‘”‡• ƒ†‡•‘’‘”‡•Ǥ
Š‡ …ƒ’‹ŽŽƒ”› …‘†‡•ƒ–‹‘ ’Š‡‘‡‘ ƒ– Ž‘™‡” ”‡Žƒ–‹˜‡
’”‡••—”‡ ”ƒ‰‡ ‘ˆ ͲǤʹȂͲǤ͵ ˆ‘” –Š‡ •ƒ’Ž‡ ‘ˆ —ȀǦͷǦ… ‹†‹Ǧ
…ƒ–‡•–Š‡’”‡•‡…‡•‘‡†‹•‘”†‡”‡†’‘”‡•ǤŠ‡…‘””‡•’‘†‹‰
’‘”‡ •‹œ‡ †‹•–”‹„—–‹‘• …‘ˆ‹”‡† –Šƒ– –Š‡ ƒŒ‘”‹–› ‘ˆ –Š‡•‡
120
(4)
100
90
(1)
80
12
10
(3)
8
6
ZSM-5
0.5%
0.8%
1.0%
1.2%
1.5%
0.0015
0.0010
0.0005
0.0000
120
1
2
3
Pore size (nm)
110
4
90
(a)
80
70
120
110
0.0
(a)
0.2
0.4
0.6
0.8
1.0
0.0
0.2
0.4
0.6
0.8
1.0
100
90
80
4
70
70
0.0 0.2 0.4 0.6 0.8 1.0
Relative pressure (p/p0)
(b)
0.0020
Adsorbed amount (mL/g)
(5)
130
110
0.0025
100
(2)
Adsorbed amount (mL/g)
Adsorbed amount (mL/g)
140
0.0030
14
150
ͳ͹ͷͳ
’‘”‡•™‡”‡ƒ’’”‘š‹ƒ–‡Ž›ʹǡƒ••Š‘™‹‹‰Ǥ͹ˆ‘”–Š‡’‘”‡
•‹œ‡†‹•–”‹„—–‹‘•‘ˆǦͷƒ†ͳǤͲ™–Ψ—ȀǦͷǦ†ƒ•™‡ŽŽƒ•
‘–Š‡”•ƒ’Ž‡•Ǥ
‘˜‡”•‡Ž›ǡ –Š‡ ƒ†•‘”„‡† ƒ‘—– ‘ˆ Ž‹“—‹† ‹–”‘‰‡ ‘
—ȀǦͷǦƒ ƒ† —ȀǦͷǦ„ ‹• “—‹–‡ Ž‘™ǡ •Š‘™‹‰ ƒ –›’‡ ‹•‘–Š‡”™‹–Šƒ͵Š›•–‡”‡•‹•Ž‘‘’ǤŠ‡•‡ƒ”‡‘’‘”‘—•ƒ–‡Ǧ
”‹ƒŽ•–Šƒ–Šƒ˜‡Žƒ”‰‡”•Ž‹–ǦŽ‹‡’‘”‡•ƒ‘‰•–ƒ…‡†ˆŽƒ›’ƒ”–‹Ǧ
…Ž‡•Ǥ Š‡ ’ƒ––‡”• ‹†‹…ƒ–‡ –Šƒ– —ȀǦͷǦƒ ƒ†
—ȀǦͷǦ„ ƒŽ‘•– Ž‘•‡ –Š‡ ‘”‹‰‹ƒŽ •–”—…–—”‡ ‘ˆ –Š‡
ǦͷǤ Š‹• ƒ› ‡š’Žƒ‹ –Š‡‹” Ž‘™‡” •‡Ž‡…–‹˜‹–› ˆ‘” ’”‘’›Ž‡‡
’”‘†—…–‹‘ǡƒ••Š‘™‹ƒ„Ž‡ͳǤ
ʹƒ†•‘”’–‹‘Ǧ†‡•‘”’–‹‘‹•‘–Š‡”•ƒ†’‘”‡•‹œ‡†‹•–”‹„—Ǧ
–‹‘ …—”˜‡• ‘ˆ Ǧͷ ƒ† ˆ‹˜‡ —ȀǦͷǦ† •ƒ’Ž‡• ™‹–Š ˜ƒ”‹Ǧ
‘—• — Ž‘ƒ†‹‰• ƒ”‡ †‹•’Žƒ›‡† ‹ ‹‰Ǥ ͹Ǥ ‹‹Žƒ” –‘ –Šƒ– ‘ˆ –Š‡
’ƒ”‡– Ǧͷǡ –Š‡ ‹•‘–Š‡”• ‘ˆ ƒŽŽ –Š‡ •ƒ’Ž‡• …‘–ƒ‹‹‰ —
ƒ”‡ –›’‹…ƒŽ –›’‡ ‹•‘–Š‡”• ™‹–Š ƒ Ͷ Š›•–‡”‡•‹• Ž‘‘’ǡ ™Š‹…Š
‡ƒ•–Šƒ––Š‡•‡‹…”‘’‘”‘—•ƒ–‡”‹ƒŽ•Šƒ˜‡ƒ…‘„‹ƒ–‹‘‘ˆ
•‘‡ •Ž‹–ǦŽ‹‡ ’‘”‡• ƒ† ‡•‘’‘”‡•Ǥ Š‡ †‹ˆˆ‡”‡…‡ „‡–™‡‡
–Š‡‹•”‡ˆŽ‡…–‡†ǡ–‘•‘‡‡š–‡–ǡ‹–Š‡‹”’‘”‡•‹œ‡†‹•–”‹„—–‹‘
…—”˜‡•Ǥ Š‡ —ȀǦͷǦ† •ƒ’Ž‡ ™‹–Š ͲǤͷ ™–Ψ ‘‹ƒŽ —
Ž‘ƒ†‹‰•Š‘™‡†–Š‡ƒ””‘™‡•–’‘”‡•‹œ‡†‹•–”‹„—–‹‘ǡˆ‘ŽŽ‘™‡†
„› –Š‡ •ƒ’Ž‡ ™‹–Š ͳǤͲ ™–Ψ — Ž‘ƒ†‹‰Ǥ Š‡ •ƒ’Ž‡ ™‹–Š ͲǤͺ
™–Ψ—•Š‘™‡†ƒ•‹‹Žƒ”’‘”‡•‹œ‡†‹•–”‹„—–‹‘”ƒ‰‡–‘–Šƒ–‘ˆ
–Š‡’ƒ”‡–Ǧͷǡ•Ž‹‰Š–Ž›™‹†‡”–Šƒ–Š‡•ƒ’Ž‡™‹–ŠͳǤͲ™–Ψ
—ƒ†ƒ””‘™‡”–Šƒ–Š‡•ƒ’Ž‡™‹–ŠͳǤʹ™–Ψ—ǤŠ‡•ƒ’Ž‡
™‹–Š ͳǤͷ ™–Ψ — Šƒ† –Š‡ ™‹†‡•– ’‘”‡ •‹œ‡ †‹•–”‹„—–‹‘Ǥ Š‡
™‹†–Š‘ˆ–Š‡’‘”‡•‹œ‡†‹•–”‹„—–‹‘…‘—Ž†„‡•‘”–‡†ƒ•ˆ‘ŽŽ‘™•ǣ
Š‡•ƒ’Ž‡™‹–ŠͳǤͷ™–Ψ—εε–Š‡•ƒ’Ž‡™‹–ŠͳǤʹ™–Ψ—ε
–Š‡’ƒ”‡–Ǧͷγ–Š‡•ƒ’Ž‡™‹–ŠͲǤͺ™–Ψ—ε–Š‡•ƒ’Ž‡
Pore volume (mL/g)
0.0 0.2 0.4 0.6 0.8 1.0
Relative pressure (p/p0)
Fig. 6. ʹ ƒ†•‘”’–‹‘Ǧ†‡•‘”’–‹‘ ‹•‘–Š‡”• ‘ˆ Ǧͷ ȋͳȌ ƒ†
—ȀǦͷǦƒȋʹȌǡ—ȀǦͷǦ„ȋ͵Ȍǡ—ȀǦͷǦ…ȋͶȌƒ†—ȀǦͷǦ†ȋͷȌ
…ƒ–ƒŽ›•–•Ǥ
Relative pressure (p/p0)
Fig.7.ʹƒ†•‘”’–‹‘Ǧ†‡•‘”’–‹‘ ‹•‘–Š‡”•ȋƒȌƒ† ’‘”‡ •‹œ‡†‹•–”‹„—Ǧ
–‹‘…—”˜‡•ȋ„Ȍ‘ˆǦͷƒ†ˆ‹˜‡—ȀǦͷǦ†•ƒ’Ž‡•™‹–Š†‹ˆˆ‡”‡–—
Ž‘ƒ†‹‰•Ǥ
ͳ͹ͷʹ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
™‹–Š ͳǤͲ ™–Ψ — ε –Š‡ •ƒ’Ž‡ ™‹–Š ͲǤͷ ™–Ψ —Ǥ ‘–ƒ„Ž›ǡ –Š‡
–Š”‡‡•ƒ’Ž‡•–Šƒ–Šƒ˜‡ƒƒ””‘™‡”’‘”‡•‹œ‡†‹•–”‹„—–‹‘–Šƒ
–Š‡ ’ƒ”‡– Ǧͷ •Š‘™ ƒ ‡Šƒ…‡‡– ‹ „‘–Š ’”‘’›Ž‡‡
•‡Ž‡…–‹˜‹–›ƒ†‹…”‘Ǧƒ…–‹˜‹–›Ǥ
20
Intensity (mV)
3.5. NH3ǦTPDmeasurements
3.6. Discussion
 ‰‡‡”ƒŽǡ •‘‡ ‹ʹ ƒ† Žʹ͵ ‹ –Š‡ œ‡‘Ž‹–‡ …ƒ „‡ †‹•Ǧ
•‘Ž˜‡†‹ƒ„ƒ•‹…•‘Ž—–‹‘ǡŽ‡ƒ†‹‰–‘–Š‡Ž‘••‘ˆ–Š‡•–”‘‰ƒ…‹†
•‹–‡•ƒ†–Š‡’ƒ”–‹ƒŽ†‡•–”—…–‹‘‘ˆ–Š‡•–”—…–—”‡Ǥ™‡ƒ„ƒ•‡
…‘—Ž† †‹••‘Ž˜‡ ƒ •ƒŽŽ ƒ‘—– ‘ˆ •‹Ž‹…ƒ ƒ† ƒŽ—‹ƒǡ ˆ‘”‹‰
•‘‡ ‡•‘’‘”‡• „› ‡š–‡†‹‰ –Š‡ ‹…”‘’‘”‡•Ǥ •–”‘‰ „ƒ•‡
…‘—Ž††‡•–”‘›–Š‡ …”›•–ƒŽ •–”—…–—”‡‘ˆ–Š‡‘Ž‡…—Žƒ” •‹‡˜‡ ƒ†
–—”–Š‡‘Ž‡…—Žƒ”•‹‡˜‡‹–‘ƒƒ‘”’Š‘—•‘Ǧƒ…‹†‹…ƒ–‡”‹Ǧ
ƒŽ ™‹–Š „‹‰ Š‘Ž‡• ȏ͵ͶȐǤ Š‡ †‡•–”—…–‹‘ ‘ˆ –Š‡ •–”—…–—”‡ ‘ˆ
—ȀǦͷǦƒ ƒ† —ȀǦͷǦ„ ‹• ’‘••‹„Ž› ”‡Žƒ–‡† –‘ –Š‡ —•‡ ‘ˆ
ƒͶ ‹ –Š‡ ’”‡’ƒ”ƒ–‹‘ ’”‘…‡†—”‡ǡ ™Š‹…Š ‹• ‹ ƒ‰”‡‡‡–
™‹–Š–Š‡”‡•—Ž–•‹‡ˆǤȏ͵ͷȐǤ –Š‹••–—†›ǡƒ•‘Ž—–‹‘™ƒ•—•‡†–‘ƒ†Œ—•––Š‡’‘ˆƒ
—ŽͶ•‘Ž—–‹‘–‘ͻƒ†–Š‡–Š‡†”‹‡†’”‡…—”•‘”™ƒ••‘ƒ‡†
‹ƒ‘‹ƒ•‘Ž—–‹‘ƒ–’αͳͲˆ‘”ʹͶŠ„‡ˆ‘”‡–Š‡ˆ‹ƒŽ•–‡’–‘
12
8
4
0
-4
-8
16
Intensity (mV)
Š‡ ƒ…‹† •‹–‡• ‘ˆ œ‡‘Ž‹–‡• ƒ”‡ ‘ˆ–‡ …Šƒ”ƒ…–‡”‹œ‡† „›
͵ǦǤ‰‡‡”ƒŽǡ–Š‡”‡ƒ”‡–™‘™‡ŽŽ”‡•‘Ž˜‡†’‡ƒ•ˆ‘”œ‡‘Ǧ
Ž‹–‡•ǡ ™Š‹…Š ƒ”‡ ”‡ˆ‡””‡† –‘ ƒ• –Š‡ Ž‘™ –‡’‡”ƒ–—”‡ ȋȌ ’‡ƒ
ƒ†–Š‡Š‹‰Š–‡’‡”ƒ–—”‡ȋȌ’‡ƒǡ…‘””‡•’‘†‹‰–‘–Š‡–‘–ƒŽ
—„‡” ‘ˆ ™‡ƒ ƒ…‹† •‹–‡• ƒ† •–”‘‰ ƒ…‹† •‹–‡•ǡ ”‡•’‡…–‹˜‡Ž›Ǥ
Š‡ •–”‘‰ ƒ…‹†•‹–‡•…‘–”‹„—–‡–‘–Š‡ †‡…‘’‘•‹–‹‘‘ˆͶΪ
‹‘•ˆ‘”‡†‘˜‡”•–”‘‰”ސ•–‡†ƒ…‹†•‹–‡•Ǥ••Š‘™‹‹‰Ǥͺǡ
‘‡…Ž‡ƒ”’‡ƒƒ†‘‡•ƒŽŽ’‡ƒƒ”‡‘„•‡”˜‡†Ǥš…‡’–
ˆ‘”—ȀǦͷǦƒƒ†—ȀǦͷǦ„‹™Š‹…Š–Š‡•–”—…–—”‡‹•†‡Ǧ
•–”‘›‡†ǡ –Š‡ — ‘†‹ˆ‹…ƒ–‹‘ †”ƒƒ–‹…ƒŽŽ› ‹…”‡ƒ•‡• –Š‡ –‘–ƒŽ
ƒ…‹† †‡•‹–›ǡ ƒ† ‡•’‡…‹ƒŽŽ› ƒ •‹‰‹ˆ‹…ƒ– ‹…”‡ƒ•‡ ‹ –Š‡ ™‡ƒ
ƒ…‹† ‹–‡•‹–› ™‹–Š ƒ ‹…”‡ƒ•‡ ‹ ‰‘Ž† Ž‘ƒ†‹‰Ǥ Š‹• …‘—Ž† „‡
…‘””‡Žƒ–‡† –‘ –Š‡ ‹…”‡ƒ•‡ ‹ •‡Ž‡…–‹˜‹–› ˆ‘” –Š‡ •›–Š‡•‹• ‘ˆ
’”‘’›Ž‡‡Ǥ ‘™‡˜‡”ǡ ‘Ž› –Š‡ –Š”‡‡ …ƒ–ƒŽ›•–• ͲǤͷǡ ͲǤͺ ƒ† ͳǤͲ
™–Ψ—ȀǦͷǦ†‡šŠ‹„‹–‡†‰‘‘†’‡”ˆ‘”ƒ…‡‹„‘–Š’”‘’›ŽǦ
‡‡•‡Ž‡…–‹˜‹–›ƒ†‹…”‘Ǧƒ…–‹˜‹–›‹†‡šǡƒ••Š‘™‹ƒ„Ž‡ͳǤ–
Šƒ• „‡‡ ”‡’‘”–‡† –Šƒ– ”‡Žƒ–‹˜‡Ž› ‹Ž† ƒ…‹†‹–› •–”‡‰–Š ƒ† ƒ
”‡ƒ•‘ƒ„Ž‡ —„‡” ‘ˆ •–”‘‰ ƒ…‹† •‹–‡• ˆƒ˜‘” ’”‘’›Ž‡‡ ’”‘Ǧ
†—…–‹‘ȏ͵͵ȐǤƒ‹‰‹–‘ƒ……‘—––Š‡’‘”‡•‹œ‡†‹•–”‹„—–‹‘ǡ–Š‡
”ƒ–‹‘‘ˆ™‡ƒƒ…‹†•‹–‡•–‘•–”‘‰ƒ…‹†•‹–‡•…ƒŽ…—Žƒ–‡†ˆ”‘–Š‡
͵Ǧ…—”˜‡•ȋƒ„Ž‡ͳȌ•—‰‰‡•–•–Šƒ––Š‡”‡‹•ƒ•›‡”‰›„‡Ǧ
–™‡‡–Š‡ƒ…‹†’”‘’‡”–›ƒ†’‘”‡•‡Ž‡…–‹˜‹–›‹’”‘’›Ž‡‡’”‘Ǧ
†—…–‹‘Ǥ Š‡”‡ ƒ”‡ ‘ „‹‰ †‹ˆˆ‡”‡…‡• ‹ –Š‡ ”ƒ–‹‘ ‘ˆ ™‡ƒ –‘
•–”‘‰ ƒ…‹† •‹–‡• ˆ‘” –Š‡ …ƒ–ƒŽ›•–• –Šƒ– ƒ‹–ƒ‹ –Š‡ Ǧͷ
•–”—…–—”‡Ǥ
0.5%
0.8%
1.0%
1.2%
1.5%
ZSM-5
16
ZSM-5
a
b
c
d
12
8
4
0
-4
-8
0
100
200
300
400
Temperature (oC)
500
Fig.8.͵Ǧ…—”˜‡•‘ˆ–Š‡’ƒ”‡–Ǧͷƒ†ƒŽŽ–Š‡•ƒ’Ž‡•‘ˆ—
‘†‹ˆ‹‡†ǦͷǤ
’”‡’ƒ”‡ˆ‹˜‡—ȀǦͷǦ†…ƒ–ƒŽ›•–•™‹–Š‘‹ƒŽ—Ž‘ƒ†‹‰•‘ˆ
ͲǤͷǡͲǤͺǡͳǤͲǡͳǤʹƒ†ͳǤͷ™–ΨǤ‘‡˜ƒŽ—ƒ–‡–Š‡‹ˆŽ—‡…‡‘ˆ–Š‡
–™‘ „ƒ•‡• —•‡† ‹ –Š‡ ’”‡’ƒ”ƒ–‹‘ ‘ˆ –Š‡ …ƒ–ƒŽ›•– ‘ –Š‡ …ƒ–ƒǦ
Ž›–‹……”ƒ…‹‰”‡ƒ…–‹‘ǡ–™‘‡™•ƒ’Ž‡•™‡”‡’”‡’ƒ”‡†™‹–ŠǦ
‘—–‹–”‘†—…‹‰‰‘Ž†ƒ†–‡•–‡†—†‡”–Š‡•ƒ‡”‡ƒ…–‹‘…‘†‹Ǧ
–‹‘•Ǥ Š‡ ˆ‹”•– •ƒ’Ž‡ ™ƒ• ’”‡’ƒ”‡† „› ”‡’Žƒ…‹‰ –Š‡ —ŽͶ
•‘Ž—–‹‘™‹–ŠƒŽ•‘Ž—–‹‘ȋ•ƒ‡ƒ‘—–‘ˆŽȌƒ†ƒ†Œ—•–‹‰
–Š‡’‘ˆ–Š‡Ž•‘Ž—–‹‘–‘ͻ„›—•‹‰ƒ•‘Ž—–‹‘„‡ˆ‘”‡
–Š‡‹’”‡‰ƒ–‹‘‘ˆ–Š‡’ƒ”‡–ǦͷǤŠ‡†”‹‡†’”‡…—”•‘”™ƒ•
–Š‡•‘ƒ‡†‹ƒ‘‹ƒ•‘Ž—–‹‘ȋ’αͳͲȌˆ‘”ʹͶŠˆ‘ŽŽ‘™‡†
„› ™ƒ•Š‹‰ǡ †”›‹‰ ƒ† …ƒŽ…‹ƒ–‹‘Ǥ Š‡ •‡…‘† •ƒ’Ž‡ ™ƒ•
†‹”‡…–Ž› •‘ƒ‡† ‹ –Š‡ ’ƒ”‡– Ǧͷ ‹ ƒ ƒ‘‹ƒ •‘Ž—–‹‘
ȋ’ α ͳͲȌ ˆ‘” ʹͶ Š ƒ† –Š‡ ™ƒ•Š‡†ǡ †”‹‡† ƒ† …ƒŽ…‹‡†Ǥ Š‡
…ƒ–ƒŽ›–‹… …”ƒ…‹‰ –‡•–‹‰ ”‡•—Ž–• ƒ– Ͷ͸Ͳ ι –‘‰‡–Š‡” ™‹–Š –Š‡
…‘””‡•’‘†‹‰ ”‡•—Ž–• ‘ –Š‡ ’ƒ”‡– Ǧͷ ’‡”ˆ‘”‡† ƒ– –Š‡
•ƒ‡–‹‡ƒ”‡•Š‘™‹ƒ„Ž‡ʹǤŠ‡’ƒ”‡–Ǧͷ—•‡†Š‡”‡
™ƒ•ˆ”‘ƒ‘–Š‡”„ƒ–…Šǡ™Š‹…Š™ƒ•’—”…Šƒ•‡†ˆ”‘–Š‡•ƒ‡
…‘’ƒ› ƒ† Šƒ† –Š‡ •ƒ‡ ‹ȀŽ ”ƒ–‹‘ ƒ† ƒ •‹‹Žƒ” •—”ˆƒ…‡
ƒ”‡ƒ–‘–Š‡‘‡‹ƒ„Ž‡ ͳǤƒŽŽ †‹ˆˆ‡”‡…‡•‹–‡•–‹‰”‡•—Ž–•
…ƒ„‡ˆ‘—†‘˜‡”–™‘’ƒ”‡–•‘ˆǦͷǤ
– ‹• …Ž‡ƒ” –Šƒ– •‹‹Žƒ” ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ƒ† ‹Ǧ
…”‘Ǧƒ…–‹˜‹–›ƒ”‡‘„–ƒ‹‡†ˆ‘”–Š‡–™‘„ƒ•‡Ǧ–”‡ƒ–‡†•ƒ’Ž‡•ǡ™‹–Š
ƒ ‹…”‡ƒ•‡ ‹ –Š‡ ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ƒ† ƒ †‡…”‡ƒ•‡ ‹ –Š‡
‹…”‘Ǧƒ…–‹˜‹–› ‹ …‘’ƒ”‹•‘ ™‹–Š –Š‘•‡ ‘ˆ –Š‡ ’ƒ”‡– ǦͷǤ
Table2
Š‡…ƒ–ƒŽ›–‹……”ƒ…‹‰”‡•—Ž–•‘˜‡”Ǧͷ–”‡ƒ–‡†„›„ƒ•‡•Ǥ
ƒ–ƒŽ›•–
Ǧͷ
Ǧͷ–”‡ƒ–‡†„›„ƒ•‡•ȋͳȌ
Ǧͷ–”‡ƒ–‡†„›„ƒ•‡•ȋʹȌ
”‘†—…–†‹•–”‹„—–‹‘ȋΨȌ
”›‰ƒ•Ϊ
ƒ
ƒ•‘Ž‹‡
‹‡•‡Ž‘‹Ž
ͶͶǤͲ
͸Ǥʹ
ͶͻǤͺ
͵ͷǤͷ
͸Ǥ͸
ͷ͹Ǥͻ
͵͹Ǥ͹
͸ǤͲ
ͷ͸Ǥ͵
‘˜‡”•‹‘ ȋΨȌ
Ͷ͹Ǥ͸
͵ͻǤͳ
ͶͲǤ͹
ȋΨȌ
ͷͲǤ͵
ͶʹǤʹ
Ͷ͵Ǥ͹
”‘’›Ž‡‡•‡Ž‡…–‹˜‹–›
ȋΨȌ
͵ͳǤͶ
ͶͺǤʹ
ͶͻǤͷ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
ͳ͹ͷ͵
‘” –Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰ ”‡ƒ…–‹‘ǡ ƒ…‹† …ƒ–ƒŽ›•‹• ‹• †‘‹Ǧ
ƒ–Ǥ—”–Š‡””‡•‡ƒ”…Š‹•‡‡†‡†–‘…‘ˆ‹”–Š‡ƒ„‘˜‡…‘…Ž—Ǧ
•‹‘• ƒ† ‰ƒ‹ ƒ „‡––‡” —†‡”•–ƒ† ‘ˆ –Š‡ ”‘Ž‡ ‘ˆ ƒ‘‰‘Ž† ‹
•—…ŠŠƒ”•Š”‡ƒ…–‹‘…‘†‹–‹‘•Ǥ
Š‹• ‹’Ž‹‡• –Šƒ– ƒ› †‹ˆˆ‡”‡…‡ ‹ –Š‡ ƒ‘—–• ‘ˆ ”‡•‹†—ƒŽ ƒ† Ž ‹ –Š‡ ˆ‹˜‡ —ȀǦͷǦ† …ƒ–ƒŽ›•–• ™‹–Š ˜ƒ”‹‘—• — Ž‘ƒ†Ǧ
‹‰•†‘‡•‘– •‹‰‹ˆ‹…ƒ–Ž›‹ˆŽ—‡…‡–Š‡…ƒ–ƒŽ›–‹… ’‡”ˆ‘”ƒ…‡
—†‡” –Š‡ –‡•–‡† …‘†‹–‹‘•Ǥ ƒ‹‰ ‹–‘ ƒ……‘—– –Š‡ †ƒ–ƒ
•Š‘™‹ƒ„Ž‡ͳǡ™‡…ƒ…‘…Ž—†‡–Šƒ–‰‘Ž†‡Šƒ…‡•–Š‡’”‘Ǧ
’›Ž‡‡ •‡Ž‡…–‹˜‹–› ƒ† ‹…”‘Ǧƒ…–‹˜‹–› ‘ˆ –Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰
”‡ƒ…–‹‘‘ˆŽ‹‰Š–†‹‡•‡Ž‘‹ŽǡƒŽ–Š‘—‰Š‹–…ƒ‘–•‹’Ž›–ƒ‡ƒ•—„Ǧ
–”ƒ…–‹‘‘ˆ„ƒ•‡•‡ˆˆ‡…–™Š‹…Š™ƒ•‹˜‘Ž˜‡†‹’”‡’ƒ”ƒ–‹‘’”‘Ǧ
…‡••Ǥ Š‡ ‘„•‡”˜ƒ–‹‘• •Š‘™ –Šƒ– –Š‡ — ’ƒ”–‹…Ž‡• ‹ –Š‡
•–—†‹‡† —ȀǦͷ …ƒ–ƒŽ›•– ƒ”‡ ’”‡†‘‹ƒ–Ž› †‹•–”‹„—–‡† ‘
–Š‡‘—–‡”•—”ˆƒ…‡‘ˆ–Š‡‘Ž‡…—Žƒ”•‹‡˜‡™‹–Šƒ—‡˜‡†‹•’‡”Ǧ
•‹‘ƒ†•‹œ‡Ǥ‘™‡˜‡”ǡ–Š‡‡„‡††‹‰‘ˆƒˆ‡™•ƒŽŽ—’ƒ”–‹Ǧ
…Ž‡• ‹•‹†‡ –Š‡ ‘Ž‡…—Žƒ” •‹‡˜‡ ’‘”‡• …ƒ‘– „‡ ”—Ž‡† ‘—–Ǥ •
‡˜‹†‡…‡† „› –Š‡ ʹ ƒ†•‘”’–‹‘Ǧ†‡•‘”’–‹‘ ‡ƒ•—”‡‡–ǡ
–Š”‡‡ •ƒ’Ž‡• ™‹–Š ͲǤͷǡ ͲǤͺǡ ƒ† ͳǤͲ ™–Ψ — Ž‘ƒ†‹‰•ǡ ™Š‹…Š
Šƒ˜‡ ƒ””‘™‡” ’‘”‡ •‹œ‡ †‹•–”‹„—–‹‘ –Šƒ –Š‡ ’ƒ”‡– Ǧͷǡ
‡šŠ‹„‹– ƒ ‡Šƒ…‡‡– ‹ „‘–Š ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ƒ† ‹Ǧ
…”‘Ǧƒ…–‹˜‹–›Ǥ
……‘”†‹‰ –‘ –Š‡ Ž‹–‡”ƒ–—”‡ǡ –Š‡”‡ ƒ”‡ –™‘ ’”‘…‡••‡• ‹Ǧ
˜‘Ž˜‡†‹–Š‡ˆ‘”ƒ–‹‘‘ˆ’”‘’›Ž‡‡ǣȾǦ•…‹••‹‘ƒ†ƒ’”‘–‡‘ŽǦ
›•‹•‡…Šƒ‹•‘–Š‡ƒ…‹†•‹–‡•‘ˆ–Š‡œ‡‘Ž‹–‡ȏ͵͸ȐǤ
‡‡”ƒŽŽ›ǡ
–Š‡ ‡–ƒŽ •‹–‡• ƒˆˆ‡…– –Š‡ •‡…‘† ˆ‘”‹‰ …ƒ”„‡‹— •’‡…‹‡•
–Šƒ–…ƒ’”‘†—…‡Ž‹‰Š–‘Ž‡ˆ‹•‘”ސ•–‡†ƒ…‹†•‹–‡•ǤŠ‡”‡ˆ‘”‡ǡ
–Š‡ ”ސ•–‡† ƒ…‹† •‹–‡• ƒ”‡ ˜‡”› ‹’‘”–ƒ– ˆ‘” –Š‡ …ƒ–ƒŽ›–‹…
…”ƒ…‹‰”‡ƒ…–‹‘Ǥ‘™‡˜‡”ǡ”‡’‘”–•ƒ„‘—–Š‘™–‘‹…”‡ƒ•‡–Š‡
—„‡”‘ˆ”ސ•–‡†ƒ…‹†•‹–‡•‘ˆǦͷ„›‡–ƒŽ‘†‹ˆ‹…ƒ–‹‘
–‘’”‘‘–‡Ž‹‰Š–‘Ž‡ˆ‹•’”‘†—…–‹‘ƒ”‡”ƒ”‡ȏ͵͹ȐǤ
Š‡͵Ǧ”‡•—Ž–••Š‘™‡†–Šƒ–—‘†‹ˆ‹…ƒ–‹‘‘ˆǦͷ
”‡•—Ž–‡†‹‘”‡ƒ…‹†•‹–‡•–Šƒ‹Ǧͷ‹–•‡Žˆƒˆ–‡”–Š‡’”‘…‡••
‘ˆŠ‹‰Š–‡’‡”ƒ–—”‡•–‡ƒ–”‡ƒ–‡–ǡ‹†‹…ƒ–‹‰–Šƒ–‰‘Ž†•—’Ǧ
’”‡••‡† –Š‡ †‡ǦƒŽ—‹ƒ–‹‘ –‘ •‘‡ ‡š–‡–Ǥ Ž–Š‘—‰Š –Š‡ —
’ƒ”–‹…Ž‡•†‹•’‡”•‡†”ƒ†‘Ž›‘–Š‡Ǧͷ•—„•–”ƒ–‡ǡ•‘‡‘ˆ
–Š‡ — ’ƒ”–‹…Ž‡• •–”‘‰Ž› ‹–‡”ƒ…–‡† ™‹–Š Ǧͷ •—„•–”ƒ–‡ „›
ˆ‘”‹‰ƒˆŽƒ–•Šƒ’‡ǤŠ‹•ƒ›Ž‡ƒ†–‘ƒ’ƒ”–‹ƒŽ‡Ž‡…–”‘–”ƒ•ˆ‡”
ˆ”‘‡–ƒŽŽ‹…—–‘ȋ‹ŽȌȋȌmǡ‹…”‡ƒ•‹‰–Š‡‘„‹Ž‹–›‘ˆ–Š‡
’”‘–‘ ‹ –Š‡ Š›†”‘š›Ž ‰”‘—’• ƒ† –Š—• ‡Šƒ…‹‰ –Š‡ ƒ…‹†
‹–‡•‹–›ǤŠ‡‡Ž‡…–”‘–”ƒ•ˆ‡”™‹ŽŽ„‡‡ˆ‹––Š‡…ƒ”„‡‹—‹‘
‡…Šƒ‹•Ǥ  ƒ††‹–‹‘ǡ –Š‡ —ȀǦͷ •ƒ’Ž‡ Šƒ• •–”‘‰‡”
–‘–ƒŽ ™‡ƒ ƒ…‹† •‹–‡• ȋ ”‡‰‹‘ȌǤ Š‡ •–”‘‰‡” ƒ…‹† •‹–‡• ‰‹˜‡
–Š‡ …ƒ”„‡‹— ‹‘• ƒ Ž‘‰‡” Ž‹ˆ‡–‹‡ –‘ —†‡”‰‘ •‡…‘†ƒ”›
–”ƒ•ˆ‘”ƒ–‹‘•ȏ͵ͺȐǤ 4. Conclusions
Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰ ”‡ƒ…–‹‘ ‘ˆ Ž‹‰Š– †‹‡•‡Ž ‘˜‡” Ǧͷ
™‹–Š‘”™‹–Š‘—–‰‘Ž†‘†‹ˆ‹…ƒ–‹‘™ƒ•‹˜‡•–‹‰ƒ–‡†ǤŠ‡—•‡‘ˆ
ƒͶ‹–Š‡’”‡’ƒ”ƒ–‹‘’”‘…‡••†‡•–”‘›•–Š‡•–”—…–—”‡‘ˆ
–Š‡ Ǧͷ •—„•–”ƒ–‡ ƒ† ”‡•—Ž–• ‹ ™‘”•‡ …ƒ–ƒŽ›–‹… ’‡”ˆ‘”Ǧ
ƒ…‡Ǥ ‘Ž† ‘†‹ˆ‹…ƒ–‹‘ ‡Šƒ…‡• –Š‡ ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–›ǡ
ƒŽ–Š‘—‰Š–Š‡…‘–”‹„—–‹‘ˆ”‘–Š‡„ƒ•‡•ȋƒ†ƒ‘‹ƒȌ
—•‡††—”‹‰–Š‡’”‡’ƒ”ƒ–‹‘…ƒ‘–„‡‡‰Ž‡…–‡†ǤŠ‡•‹—Ž–ƒǦ
‡‘—• ‡Šƒ…‡‡– ‘ˆ –Š‡ ’”‘’›Ž‡‡ •‡Ž‡…–‹˜‹–› ƒ† ‹…”‘Ǧ
ƒ…–‹˜‹–›‹†‡š‹•‘Ž›‘„–ƒ‹‡†‘˜‡”–Š‡—ȀǦͷ…ƒ–ƒŽ›•–•–Šƒ–
ƒ‹–ƒ‹‡†–Š‡‹”•–”—…–—”‡ƒ†Šƒ†•ƒŽŽ—’ƒ”–‹…Ž‡•™‹–Š
ƒ ƒ””‘™ ’‘”‡ •‹œ‡ †‹•–”‹„—–‹‘ǡ ”‡Žƒ–‹˜‡Ž› ‹Ž† ™‡ƒ ƒ…‹†‹–›
•–”‡‰–Š ƒ† ƒ ”‡ƒ•‘ƒ„Ž‡ —„‡” ‘ˆ •–”‘‰ ƒ…‹† •‹–‡•Ǥ Š‡•‡
”‡•—Ž–••—‰‰‡•––Šƒ–ƒ•ƒŽŽƒ‘—–‘ˆ‰‘Ž†Šƒ•ƒ’‘•‹–‹˜‡‡ˆˆ‡…–
‘ –Š‡ …ƒ–ƒŽ›–‹… …”ƒ…‹‰ ‘ˆ Ž‹‰Š– †‹‡•‡Ž ‘‹Ž ƒ† ‹…”‡ƒ•‡† ’”‘Ǧ
’›Ž‡‡’”‘†—…–‹‘ƒ–ƒŽ‘™‡””‡ƒ…–‹‘–‡’‡”ƒ–—”‡‘ˆͶ͸ͲιǤ
Acknowledgments Š‡ƒ—–Š‘”•˜‡”›—…Šƒ’’”‡…‹ƒ–‡”‘ˆ‡••‘”‹ˆ‡‰ƒˆ‘”
–Š‡ƒ••‹•–ƒ…‡‹͵Ǧ‡ƒ•—”‡‡–•ƒ†–Š‡•—’’Ž›‘ˆ–Š‡
’ƒ”‡–‘ˆǦͷ„›–Š‡‡–”‘…Š‡‹…ƒŽ ‡•‡ƒ”…Š•–‹–—–‡ǡ ‡–Ǧ
”‘Š‹ƒ‘Ǥ‹‹–‡†Ǥ
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Au/ZSM-5 ۢौࡸۢौ㻸ौ䖱Ḫ⋯ཐӝя✥
㡏⤫㻝*, 㶖䊧㻝, Ⰲ㾃㲯, 㯶⿼㉋
䁭㲉⫔䁈⿐䁈⿐⹅䁈䊛, 㩞Ⰼ㬂⿧㆑⹅⧭ゝ㭖䁱㈠䐱㾥 (⹅䄖䇇䇤), 㩞Ⰼ䁭㲉264005
᪎㾷: 㓿䗷йॱཊᒤⲴ⹄ウоᔰਁ, 䠁ۜॆᐢᓄ⭘ࡠ⧟ຳ⊑ḃ⋫⨶о᧗ࡦǃ㋮㓶ॆᐕਸᡀ઼㜭Ⓚㅹ亶ฏ, ⎹৺Ⲵॆᆖ৽ᓄ
ӾㆰঅⲴ CO ≗ॆ઼щ✟⧟≗ॆㅹᢙኅࡠ࣐≒ǃ㗠ॆ઼㕙ਸㅹ਴㊫ᴹᵪਸᡀ৽ᓄ, ⹄ウ亶ฏӾཊ⴨ۜॆࡠ൷⴨ۜॆԕ৺‫ݹ‬
ۜॆㅹ. ❦㘼䠁ۜॆᡰ᧒㍒Ⲵ৽ᓄཊ൘䖳⑙઼Ⲵ৽ᓄᶑԦл䘋㹼, ሩҾ䟽⋩ۜॆ㻲䀓䘉㊫儈⑙઼༽ᵲ␧ਸ৽ᓄ⢙փ㌫Ⲵ
⹄ウࠐѾᰐӪ䰞⍕. ۜॆ㻲ॆ(FCC) 䗷〻⭡Ҿާᴹ㜭㙇䖳վǃ৏ᯉվᓹ৺㻵㖞䘲ᓄ㜭࣋ᕪㅹՈ⛩, ൘໎ӗщ✟ᯩ䶒ਁᥕ⵰
䟽㾱֌⭘. ⭡Ҿ⢩↺ᆄ㔃ᶴⲴᤙᖒᙗǃ䖳ᕪⲴ䞨ᙗ઼վⲴ≒䖜〫⍫ᙗԕ৺㢟ྭⲴ≤✝っᇊᙗ, ZSM-5 ࠶ᆀㆋᱟⴞࡽᓄ⭘Ҿ
FCC ཊӗщ✟ۜॆࡲ઼ࣙࡲᴰѪᒯ⌋Ⲵ䟽㾱㓴࠶. ٬ᗇ⌘᜿Ⲵᱟ, ⴞࡽഭ޵ཆᔰਁⲴ᭩ᙗ ZSM-5 ᰐ䇪ᱟሩ C4 ⛳㊫઼⸣
㝁⋩ㅹۜॆ㻲䀓ᡆ֌Ѫࣙࡲ⭘Ҿ FCC ໎ӗщ✟൷ᴹ〟ᶱ֌⭘, ն৽ᓄ⑙ᓖ䖳儈 (བྷҾ 510 oC); ᖃ䱽վ৽ᓄ⑙ᓖਾ, ަ໎ӗ
щ✟Ⲵ㜭࣋ሶਇࡠᶱབྷ䲀ࡦ.
ᵜ᮷࡙⭘㓣㊣䠁վ⑙ۜॆ⍫ᙗ儈Ⲵ⢩⛩, 䟷⭘᭩䘋Ⲵ⊹〟⊹⏰ (DP) ᯩ⌅, 䙊䗷䈳ਈࡦ༷৲ᮠ઼䠁䖭䟿, ࡦ༷Ҷ㌫ࡇ䠁
‫؞‬侠Ⲵ ZSM-5 ۜॆࡲ, 㘳ሏҶަሩ䖫Ḥ⋩ۜॆ㻲䀓ཊӗщ✟Ⲵۜॆᙗ㜭. 䟷⭘ X ሴ㓯㹽ሴ (XRD)ǃN2 ੨䱴-㝡䱴ǃ≘〻ᒿ
ॷ⑙㝡䱴 (NH3-TPD)ǃ䘿ሴ⭥䮌 (TEM) ઼䈡ሬ㙖ਸㅹ⿫ᆀփ‫ݹ‬䉡 (ICP-AES) ㅹ᡻⇥⹄ウҶ㓣㊣䠁Ⲵ࠶ᮓ⣦ߥ৺ަሩ
ZSM-5 ⢙⨶ॆᆖ㔃ᶴⲴ䈳ਈ.
㔃᷌ਁ⧠, ൘ 460 oC Ⲵ䖳վ৽ᓄ⑙ᓖл, оᗞ㊣ ZSM-5 ⇽փ⴨∄, 䟷⭘ᑨ㿴 DP ⌅ࡦ༷Ⲵ㓿䗷└⍇⏔ਾᵚ⭘ NaBH4 䘈
৏㘼ᱟ൘ 300 oC лオ≄ѝ❉✗, ⨶䇪䠁䖭䟿࠶࡛Ѫ 0.5, 0.8 ઼ 1.0 wt% Ⲵйњ㓣㊣䠁ۜॆࡲⲴᗞ৽⍫ᙗ઼щ✟䘹ᤙᙗ൷໎
࣐. ަѝщ✟䘹ᤙᙗ࠶࡛ᨀ儈Ҷ 8.8%, 2.9%઼ 23.2%, ᗞ৽⍫ᙗᤷᮠ࠶࡛ᨀ儈Ҷ 7.1%, 4.3%઼ 4.5%. 䘉㺘᰾ቁ䟿䠁Ⲵᕅ‫ޕ‬
ᴹ࡙Ҿ൘䖳վ৽ᓄ⑙ᓖлۜॆ㻲ॆ䖫Ḥ⋩໎ӗщ✟, ৽᱐Ҷަۜॆ㻲䀓⛳㊫ॆਸ⢙Ⲵ㜭࣋.
TEM 㿲ሏ㺘᰾, Au/ZSM-5 ۜॆࡲѝ䠁㋂ᖴ࠶ᐳ䶎ᑨн൷र (< 10 nm – < 200 nm). ❦㘼ަѝаӋ䠁㋂ᆀо䖭փ੸ᡱᒣ
ᔿ᧕䀖, ᱮ⽪Ҷє㘵䰤䖳ᕪⲴ⴨ӂ֌⭘. ਖཆаӋ䖳ሿⲴ䠁㋂ᆀਟ㜭፼‫⤝ࡠޕ‬㕍⡷⣦ ZSM-5 仇㋂ѻ䰤Ⲵᆄ䳉ѝ, 䘉ਟ㜭൘
аᇊ〻ᓖкᖡ૽Ҷ⇽փ ZSM-5 Ⲵᆄ㔃ᶴ࠶ᐳ৺ަۜॆ㻲ॆᙗ㜭. XRD, N2 ੨䱴-㝡䱴઼ NH3-TPD 㔃᷌㺘᰾, 䠁ᕅ‫༷ࡦޕ‬
৲ᮠ৺ަ䖭䟿Ⲵਈॆሬ㠤Ҷ⇽փ ZSM-5 䖭փⲴ MFI 㔃ᶴǃᆄ㔃ᶴ࠶ᐳ৺ᕪᕡ䞨䟿Ⲵਈॆ. к䘠щ✟䘹ᤙᙗ઼ᗞ৽⍫ᙗഐ
CaixiaQietal./ChineseJournalofCatalysis37(2016)1747–1755
ͳ͹ͷͷ
䠁Ⲵ‫؞‬侠㘼਼ᰦᨀ儈Ⲵйњ䠁ۜॆࡲ, สᵜ‫؍‬ᤱҶᆼᮤⲴ ZSM-5 Ⲵ MFI 㔃ᶴ, ᒦфަᆄ࠶ᐳ∄ ZSM-5 ゴ. 䠁Ⲵᕅ‫ޕ‬᰾ᱮ
ᨀ儈Ҷ ZSM-5 ⇽փⲴ䞨ᙗቔަᱟվ⑙ᕡ䞨Ⲵ䞨ᕪᓖ, ❦㘼, 㔬ਸᙗ㜭Ո㢟Ⲵۜॆࡲަᕪᕡ䞨䟿Ⲵ∄ֻ⴨䘁. ഐ↔, 䠁‫؞‬侠
ሬ㠤ᗞ৽⍫ᙗ઼щ✟䘹ᤙᙗⲴ਼ᰦᨀ儈ਆߣҾ᭩ᙗۜॆࡲⲴ MFI 㔃ᶴǃᆄ࠶ᐳԕ৺ᕪᕡ䞨∄ֻⲴॿ਼֌⭘, 㘼䠁䖭䟿઼
䠁㋂ᆀቪረⲴᖡ૽н᰾ᱮ.
а㡜ᶕ䇢, ‫؞‬侠Ⲵ䠁኎ѫ㾱䙊䗷ᖒᡀ↓⻣⿫ᆀ㘼൘ B 䞨սк⭏ᡀ䖫✟⛳. 儈⑙≤⊭㘱ॆ䈅傼ਾ, 䠁‫؞‬侠Ⲵ ZSM-5 ∄ᵚ
‫؞‬侠ⲴZSM-5‫⮉؍‬ҶᴤཊⲴ䞨ս, 䈤᰾䠁൘аᇊ〻ᓖкᣁࡦҶ僘ᷦ䬍Ⲵ㝡䲔. ᡱᒣ⣦࠶ᐳ൘⇽փкⲴ䠁㋂ᆀо⇽փ䰤䖳ᕪ
Ⲵ⴨ӂ֌⭘ਟ㜭ሬ㠤䜘࠶⭥ᆀӾ䠁኎ᘱ䠁䖜〫ࡠ (SiAl)O(OH)m к, ໎࣐Ҷ㗏สѝ䍘ᆀⲴ⍱ࣘᙗ㘼ᨀ儈Ҷ᭩ᙗ࠶ᆀㆋⲴ䞨
ᙗ, ᴹ࡙Ҿ↓⻣⿫ᆀⲴᖒᡀ.
ީ䭤䈃: ۜॆ㻲ॆ; ZSM-5; 䠁‫؞‬侠; щ✟䘹ᤙᙗ; ᗞ৽⍫ᙗ⍻䈅
㬶ⷆ㦶㠻: 2016-05-17. ㅴ㬽㦶㠻: 2016-06-28. ⨗⟇㦶㠻: 2016-10-05.
*㵉䁗㑋㻖㦬. ⮈⿑/⪌䎇: (0535)6911732; ⮈䓴㾦㼅: [email protected]
〚㆑㎕䊕: 㩞Ⰼ㬂㲊㩞䁈䎀⼮䁭㲉㬱㯌➺ェ⿏; 㩞Ⰼ㬂䓵㦜㋧䁈〚㆑ (ZR2015BM006).
⡟㸥⭥䇃㸥⮈䓴⟇䇪Elsevier⨗⟇㪈䊻ScienceDirect㩰⨗⟇(http://www.sciencedirect.com/science/journal/18722067).