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Ñêîðîñòü<br />
Ðåàëüíûé ñîñòàâ êèñëîé Cs<br />
îáðàçîâàíèÿ<br />
Îáðàçåö<br />
ñîëè<br />
ìåòèëàöåòàòà,<br />
10 -8 mol m -2 s -1<br />
1%Rh/Cs 1.5 H 1.5 PW 12 O 40 0.8H 3 PW 12 Î 40 /Cs 2.2 H 0.8 PW 12 Î 40 0.78<br />
1%Rh/Cs 2 HPW 12 O 40 0.5H 3 PW 12 Î 40 /Cs 2.5 H 0.5 PW 12 Î 40 0.42<br />
Ëèòåðàòóðà<br />
1. G.G. Volkova, L.M. Plyasova, A.N. Salanov, G.N. Kustova, T.M. Yurieva and<br />
V.A. Likholobov, Catal. Lett. 80 (2002) 175.<br />
2. G.G. Volkova, L.M. Plyasova, L.N. Shkuratova, A.A. Budneva, E.A. Paukshtis,<br />
M.N. Timofeeva, V.A. Likholobov, Stud. Sur. Sci. Catal. 147 (2004) 403.<br />
3. W.R. Wegman, European Patent 0353 722 (1989).<br />
114
50 Rate/10 -8 mol g -1 s -1 40 30 20 10 0 by-products methyl acetate Cs1 Cs1.5 Cs2 Cs2.5 SO4(1) SO4(2) WOx Ðèñ. 1. Àêòèâíîñòü è ñåëåêòèâíîñòü êàòàëèçàòîðîâ Rh/Cs x H 3-x PW 12 O 40 , Rh/SO 4 /ZrO 2 , Rh/WO x /ZrO 2 â ðåàêöèè êàðáîíèëèðîâàíèÿ äèìåòèëîâîãî ýôèðà â ìåòèëàöåòàò Ïðåäïîëàãàåòñÿ, ÷òî àêòèâàöèÿ ñâÿçè Ñ-Î â ìîëåêóëå äèìåòèëîâîãî ýôèðà è îáðàçîâàíèå ñâÿçè ìåòàëë-àëêèë ïðîèñõîäèò ñ ó÷àñòèåì ñèëüíûõ áðåíñòåäîâñêèõ öåíòðîâ, ðàáîòàþùèõ â ñî÷åòàíèè ñ êàðáîíèëüíûìè êîìïëåêñàìè ðîäèÿ, íà êîòîðûõ ïðîèñõîäèò âñòðàèâàíèå ìîëåêóëû ÑÎ è îáðàçîâàíèå àöåòàòà. Ìåòîäàìè ÐÔÀ, ßÌÐ, ÈÊÑ è ÑÝÌ èçó÷åíû îñîáåííîñòè ôîðìèðîâàíèÿ êèñëûõ öåçèåâûõ ñîëåé ôîñôîðâîëüôðàìîâîé ÃÏÊ, ïîêàçàíî, ÷òî • â îáëàñòè ñîñòàâîâ Ñs1-Cs2.5 íàáëþäàåòñÿ îáðàçîâàíèå äâóõ ôàç – êèñëîé öåçèåâîé ñîëè è êèñëîòû; • êèñëûå öåçèåâûå ñîëè èìåþò ñîñòàâ Cs2.1-Cs2.7, ñðåäíèå ñîëè ñîñòàâà Cs1-Cs1.5 íå îáðàçóþòñÿ, ðàçìåð ïåðâè÷íûõ ÷àñòèö 80-100 A. Êîëè÷åñòâî öåçèÿ, ââåäåííîãî â ñèñòåìó Cs x H 3-x PW 12 O 40 , îïðåäåëÿåò óäåëüíóþ ïîâåðõíîñòü êàòàëèçàòîðîâ. Äëÿ ýôôåêòèâíîãî êàòàëèçàòîðà áåçãàëîãåííîãî êàðáîíèëèðîâàíèÿ ÄÌÝ óäåëüíàÿ ïîâåðõíîñòü äîëæíà áûòü íå ìåíåå 60 ì 2 ã -1 . • ÃÏÊ íàõîäèòñÿ íà ïîâåðõíîñòè Cs ôàçû, êîòîðàÿ ÿâëÿåòñÿ íîñèòåëåì, êîëè÷åñòâî ÃÏÊ îïðåäåëÿåò ñóïåðêèñëîòíûå ñâîéñòâà è óíèêàëüíûå êàòàëèòè÷åñêèå ñâîéñòâà öåçèåâûõ ñèñòåì. Äëÿ ýôôåêòèâíîãî êàòàëèçàòîðà áåçãàëîãåííîãî êàðáîíèëèðîâàíèÿ ÄÌÝ ñîäåðæàíèå ÃÏÊ â îáðàçöå äîëæíî áûòü íå ìåíåå 0.5HPW/CsPW. 113
Ñêîðîñòü Ðåàëüíûé ñîñòàâ êèñëîé Cs îáðàçîâàíèÿ Îáðàçåö ñîëè ìåòèëàöåòàòà, 10 -8 mol m -2 s -1 1%Rh/Cs 1.5 H 1.5 PW 12 O 40 0.8H 3 PW 12 Î 40 /Cs 2.2 H 0.8 PW 12 Î 40 0.78 1%Rh/Cs 2 HPW 12 O 40 0.5H 3 PW 12 Î 40 /Cs 2.5 H 0.5 PW 12 Î 40 0.42 Ëèòåðàòóðà 1. G.G. Volkova, L.M. Plyasova, A.N. Salanov, G.N. Kustova, T.M. Yurieva and V.A. Likholobov, Catal. Lett. 80 (2002) 175. 2. G.G. Volkova, L.M. Plyasova, L.N. Shkuratova, A.A. Budneva, E.A. Paukshtis, M.N. Timofeeva, V.A. Likholobov, Stud. Sur. Sci. Catal. 147 (2004) 403. 3. W.R. Wegman, European Patent 0353 722 (1989). 114
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