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SINGLE SITE CATALYSTS – IDEAL MODELS FOR UNDERSTANDING STRUCTURE-FUNCTION RELATIONSHIPS Bell Alexis T. Department of Chemical Engineering University of California, Berkeley, USA E-mail: bell@cchem.berkeley.edu Most heterogeneous catalysts consist of nanoparticles of a metal, metal oxide, or metal sulfide dispersed on a support. Such catalysts are difficult to characterize precisely even with modern analytical tools because the particles have a range of particle sizes and shapes. As a consequence, unambiguous definition of what is meant by a catalytically active site is not possible. This difficulty is severely reduced when the active sites are in the form of isolated metal cations or metal oxo groups, since now virtually all sites are identical, i.e., the sites take on a “molecular” character. For such materials it both experimental and theoretical methods can be used to a clear perspective of the composition and structure of the active site and its catalytic properties. This talk will examine several examples of such single-site catalysts. The first illustration concerns Fe-porphyrin catalysts used for the epoxidation of olefins by H 2 O 2 . Careful analysis of this reaction system has revealed the role of the axial ligand in controlling the catalyst activity and the selectivity with respect to H 2 O 2 . The second example examines the role of extra-framework Fe cations in Fe-ZSM-5 on the decomposition of N 2 O and the effects of water vapor on this process. The third illustration examines with the properties of isolated Cu + cations supported on meosporous silica and exchanged into zeolites Y and ZSM-5 and the role of such cations in the oxidative carbonylation of methanol to dimethyl carbonate. 5
ÑÎÂÐÅÌÅÍÍÛÅ ÀÑÏÅÊÒÛ ÌÎËÅÊÓËßÐÍÎÃÎ ÄÈÇÀÉÍÀ ÀÊÒÈÂÍÛÕ ÖÅÍÒÐÎÂ ÊÀÒÀËÈÇÀÒÎÐÎÂ Ëèõîëîáîâ Â.À. Èíñòèòóò ïðîáëåì ïåðåðàáîòêè óãëåâîäîðîäîâ ÑÎ ÐÀÍ, Îìñê E-mail: val@incat.okno.ru 6
Page 1 and 2: Èíñòèòóò êàòàëèçà
Page 3 and 4: Îðãàíèçàòîðû êîíôå
Page 8 and 9: ÑÒÀÁÈËÈÇÈÐÎÂÀÍÍÛÅ
Page 10 and 11: ÈÇÓ×ÅÍÈÅ ÌÅÕÀÍÈÇÌÎ
Page 12 and 13: Ñðàâíåíèå äèíàìèêè
Page 14 and 15: ÐÎËÜ ÍÎÑÈÒÅËÅÉ Â ÔÎ
Page 16 and 17: ÒÐÈÈÇÎÁÓÒÈËÀËÞÌÈÍ
Page 18: ÏÐÎÃÐÅÑÑ Â ÎÁËÀÑÒÈ
Page 22 and 23: MOLECULAR DESIGN OF NEW TYPE OF CAT
Page 24 and 25: PALLADIUM AND COBALT CATALYZED OXID
Page 26 and 27: ÍÎÂÛÉ ÏÎÄÕÎÄ Ê ÔÎÐÌ
Page 28 and 29: Èîííûé îáìåí Al 2O 3 2+
Page 30 and 31: êîòîðûõ èììîáèëèçî
Page 32 and 33: ïðèâåäøàÿ ê ñîçäàí
Page 34 and 35: ÐÀÇÐÀÁÎÒÊÀ ÊÀÒÀËÈÇ
Page 36 and 37: ðàñïðåäåëåíèÿ ÷àñò
Page 38 and 39: ÷òî äåôåêòû ýòîãî â
Page 40 and 41: ÈÇÓ×ÅÍÈÅ ÔÎÐÌÈÐÎÂÀ
Page 42 and 43: Ñîäåðæàíèå äèîêñèä
Page 44 and 45: Òàáë. 1. Äàííûå õåìî
Page 46 and 47: ñëàáîñâÿçàííîì ñîñ
Page 48 and 49: ãèäðîãåíèçàöèè, âå
Page 50 and 51: ÑÅËÅÊÒÈÂÍÀß ÎÊÈÑËÈ
Page 52 and 53: ÌÎÄÈÔÈÖÈÐÎÂÀÍÈÅ ÀË
Page 54 and 55: ãèäðîîêèñüþ àëþìèí
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ïðîìûñëîâûõ ìèíè-Í
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ÏÎËÓ×ÅÍÈÅ ÆÈÄÊÈÕ Ó
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ÈÇÎÌÅÐÈÇÀÖÈß ÓÃËÅÂ
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ÊÀÒÀËÈÒÈ×ÅÑÊÈÅ ÏÐÅ
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îáðàçîâàíèÿ öèêëîï
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ïðåèìóùåñòâåííîå ï
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ÈÍÒÅÐÊÀËÈÐÎÂÀÍÍÛÅ
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ÊÐÅÊÈÍÃ Ñ 10 -Ñ 15 - ÀË
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Â ÈÊ- ñïåêòðàõ àäñî
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Ïî âëèÿíèþ íà êàòàë
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Ïðåîáëàäàþùèìè ïðè
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ÃÈÄÐÎÏÅÐÅÐÀÁÎÒÊÀ Í
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Ïîñëå ãèäðîïåðåðàá
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óñëîâèé ïðîöåññà î
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åå ðåàêöèè. Èìåííî
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í-C 4 H 8 + Pd II + Í 2 Î ⎯⎯
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ïðîäóêòîâ. Íàïðèìå
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×ÈÑËÎ È ÐÅÀÊÖÈÎÍÍÀ
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Äëÿ âñåõ ñèñòåì îïð
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ñèíäèîòàêòè÷åñêèé
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ñâÿçåé è ýêâèâàëåí
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ÝËÅÊÒÐÎÕÈÌÈ×ÅÑÊÈÉ
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ÑÒÅÍÄÎÂÛÅ ÄÎÊËÀÄÛ
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ÈÇÓ×ÅÍÈÅ ÌÅÕÀÍÈÇÌÀ
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Ðèñóíîê 2. Äèôôåðåí
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âòîðîé ïî èíòåíñèâ
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êîëåáàíèÿ â ìîñòèê
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ÑÒÐÓÊÒÓÐÍÎ-ÎÐÃÀÍÈÇ
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Òàáëèöà 2. Ðàñïðåäå
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50 Rate/10 -8 mol g -1 s -1 40 30 2
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ÐÀÇÐÀÁÎÒÊÀ È ÈÑÑËÅ
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êèñëîðîäó øïèíåëè C
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èçîìåðèçàöèè í-ãåê
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ÃÅÍÅÇÈÑ ÔÀÇÎÂÎÃÎ Ñ
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óïëîòíåíèÿ çàïîëíÿ
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Ïðèðîäà èñõîäíûõ ñ
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ÏÎËÈÌÅÐÍÛÅ ÐÎÄÈÉÑÎ
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ïðîìîòîðîâ. Â ðàáîò
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ôîðìàëüäåãèä, äè- è
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Äàëüíåéøàÿ äåãèäðî
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ÌÅÒÎÄÛ ÐÅÃÓËÈÐÎÂÀÍ
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ÑÈÍÒÅÇ È ÈÑÑËÅÄÎÂÀ
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ÂËÈßÍÈÅ ÎÁÐÀÁÎÒÎÊ
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Íàðÿäó ñ óâåëè÷åíè
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îáîðîòîâ êàòàëèçàò
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Íàìè ðàçðàáîòàí ïð
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äî 0,5 ÌÏà. Ôîðìû çàâ
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Î ÏÐÎÖÅÑÑÀÕ ÏÐÅÄÎÒ
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ÐÀÇÐÀÁÎÒÊÀ ÊÀÒÀËÈÒ
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ÏÐÅÂÐÀÙÅÍÈß ÑÒÈÐÎË
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ÆÈÄÊÎÔÀÇÍÀß ÈÇÎÌÅÐ
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ÍÅÏÎËÍÎÅ ÎÊÈÑËÅÍÈÅ
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ÍÀÍÎÑÒÐÓÊÒÓÐÍÛÅ ÊÀ
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ÃÈÄÐÎÊÎÍÂÅÐÑÈß Í-Ã
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ðàñòåò ñ ïîâûøåíèå
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Èíäèâèäóàëüíàÿ àäñ
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â ÑÍÃ ñíèæàåò òåìïå
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Ïðîöåññ áèôîðìèíãà
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ÈÑÏÎËÜÇÎÂÀÍÈÅ ÊÀÒÀ
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Ïîâûøåíèå äàâëåíèÿ
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Èç ïðèðîäíîãî öåîë
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ÄÅÃÈÄÐÈÐÎÂÀÍÈÅ ËÅÃ
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ðîäèåâûå è ðóòåíèå
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Òàáëèöà 1. Âëèÿíèå ï
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ÈÑÑËÅÄÎÂÀÍÈÅ ÏÐÎÖÅ
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ÏÅÐÅÐÀÁÎÒÊÀ ÄÈÑÒÈË
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ÃÈÄÐÎÏÅÐÅÐÀÁÎÒÊÀ í
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ÊÐÅÊÈÍÃ ÒßÆÅËÎÃÎ Í
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óãëåðîäà â äèîêñèä
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ïîäà÷è ñûðüÿ 1,0-1,5 ÷
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ëîêàëèçîâàííûå íà
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CÓËÜÔÎÊÀÒÈÎÍÈÒÛ ÍÀ
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Ïðè íàëè÷èè â ñèñòå
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ãåêñàäåêàíîë-2 (ïðè
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óñëîâèÿ îêèñëåíèÿ
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ãàçîâ òåðìîäåñîðáö
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ïîëèìåðèçàöèè ýòèë
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ÊÀÒÀËÈÇÈÐÓÅÌÎÅ ÏÀË
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ÈÑÑËÅÄÎÂÀÍÈÅ ÂËÈßÍ
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ÄÈÌÅÐÈÇÀÖÈß ÝÒÈËÅÍ
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ÈÇÓ×ÅÍÈÅ ÏÐÎÖÅÑÑÎÂ
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ÐÀÑÏÐÅÄÅËÅÍÈÅ ÂÍÓÒ
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ÃÎÌÎ - È ÑÎÏÎËÈÌÅÐÈ
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ÏÎËÈÌÅÐÈÇÀÖÈß ÝÒÈË
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Ñ ïðèìåíåíèåì ìåòî
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àìîðôíûìè è êðèñòà
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ÑÏÈÑÎÊ ÀÄÐÅÑÎÂ Ó×À
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ÃÐÈÃÎÐÜÅÂÀ Íåëëè Ã
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ÊÀÐÛÌÎÂÀ Ðàøèäà Õà
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ÌÓÍØÈÅÂÀ Ìèíà Êåðè
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ÓÑÌÀÍÎÂÀ Ìàíçóðà Ì
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ÑÎÄÅÐÆÀÍÈÅ ÊËÞ×ÅÂÛ
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Ñåêöèÿ II Êàòàëèç â
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CÄ-I-3 CÄ-I-4 CÄ-I-5 CÄ-I-6 CÄ
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CÄ-II-10 Çàêèðîâà À.Ã.,
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CÄ-III-4 Ìèêåíàñ T.Á., Å
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