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ÐÀÇÐÀÁÎÒÊÀ ÊÀÒÀËÈÒÈ×ÅÑÊÈÕ ÑÈÑÒÅÌ ÍÀ ÎÑÍÎÂÅ Y õ Ce 1-x Zr y O 2 ÄËß ÐÅÀÊÖÈÈ ÑÅËÅÊÒÈÂÍÎÃÎ ÎÊÈÑËÅÍÈß ÑÎ Â ÈÇÁÛÒÊÅ ÂÎÄÎÐÎÄÀ Áåðåçèíà Ë.À., Ëþáóøêèí Ð.À., Áóðäåéíàÿ Ò.Í., Òðåòüÿêîâ Â.Ô. Èíñòèòóò íåôòåõèìè÷åñêîãî ñèíòåçà èì. À.Â. Òîï÷èåâà ÐÀÍ, Ìîñêâà Å-mail: l_berezina@mail.ru Ïðîâåäåíî ñðàâíèòåëüíîå èññëåäîâàíèå àêòèâíîñòè íàíåñ¸ííûõ Cu,Ñî/Y (x) Ce (y) Zr (1-x-y) O (2) êàòàëèòè÷åñêèõ ñèñòåì â ðåàêöèè íèçêîòåìïåðàòóðíîãî ñåëåêòèâíîãî îêèñëåíèÿ ÑÎ â èçáûòêå âîäîðîäà. Ïîêàçàíî, ÷òî äàííûå êàòàëèòè÷åñêèå ñèñòåìû îáåñïå÷èâàþò âûñîêèå çíà÷åíèÿ êîíâåðñèè ÑÎ è ñåëåêòèâíîñòè ïî Î 2 â èíòåðâàëå òåìïåðàòóð äî 150 î Ñ. Ïîëó÷åííûå ýêñïåðèìåíòàëüíûå äàííûå ïîêàçàëè, ÷òî íà ýòèõ êàòàëèçàòîðàõ ìîæíî äîñòè÷ü ñòåïåíü î÷èñòêè âîäîðîäà îò ÑÎ. Â íàñòîÿùåå âðåìÿ âî âñåì ìèðå ïðîâîäÿòñÿ èññëåäîâàòåëüñêèå ðàáîòû â îáëàñòè ñîçäàíèÿ íîâûõ âèäîâ ìîòîðíûõ òîïëèâ, îòâå÷àþùèõ òðåáîâàíèÿì ýêîëîãè÷íîñòè è âûñîêîé ýôôåêòèâíîñòè. Öåëüþ ýòèõ ðàáîò ÿâëÿåòñÿ ðàçðàáîòêà íàöèîíàëüíûõ êîíöåïöèé ïðîèçâîäñòâà è èñïîëüçîâàíèÿ àëüòåðíàòèâíûõ ìîòîðíûõ òîïëèâ è ñîçäàíèå ñîîòâåòñòâóþùèõ äâèãàòåëåé, îòâå÷àþùèõ ñàìûì æåñòêèì ìèðîâûì ñòàíäàðòàì. Â êà÷åñòâå ïåðñïåêòèâíîãî èñòî÷íèêà ýíåðãèè äëÿ çàìåíû äâèãàòåëåé âíóòðåííåãî ñãîðàíèÿ â àâòîìîáèëÿõ ðàññìàòðèâàþòñÿ ïîëèìåðíûå ìåìáðàííûå òîïëèâíûå ýëåìåíòû (PEMFC). Òîïëèâíûå ýëåìåíòû îòíîñÿòñÿ ê õèìè÷åñêèì èñòî÷íèêàì òîêà. Îíè îñóùåñòâëÿþò ïðÿìîå ïðåâðàùåíèå ýíåðãèè òîïëèâà â ýëåêòðè÷åñòâî. Îäíàêî èñïîëüçîâàíèå òîïëèâíûõ ýëåìåíòîâ ñâÿçàíî ñ ðÿäîì ñëîæíîñòåé, ãëàâíàÿ èç êîòîðûõ – õðàíåíèå âîäîðîäà íà áîðòó àâòîìîáèëÿ. Ïîýòîìó ïðåäëàãàåòñÿ ïîëó÷àòü âîäîðîä èç ìåòàíîëà, ïðè ýòîì îáðàçóåòñÿ ÑÎ, êîòîðûé ÿâëÿåòñÿ íå òîëüêî íåæåëàòåëüíûì êîìïîíåíòîì â âûõëîïíûõ ãàçàõ, íî è ÿäîì äëÿ àíîäà òîïëèâíîãî ýëåìåíòà. Ïîýòîìó, ïåðåä ïîäà÷åé ñìåñè â PEMFC íåîáõîäèìî ïðîâåäåíèå äîïîëíèòåëüíîé ðåàêöèè ñåëåêòèâíîãî êàòàëèòè÷åñêîãî îêèñëåíèÿ ÑÎ â èçáûòêå âîäîðîäà. Ðåçóëüòàòû èññëåäîâàíèÿ Co,Cu/Y-Ce-Zr îêñèäíûõ êàòàëèçàòîðîâ â ðåàêöèè ñåëåêòèâíîãî îêèñëåíèÿ ÑÎ â èçáûòêå Í 2 ïðåäñòàâëåíû íà ðèñ. 1. 151
Òåñòèðîâàíèå êàòàëèçàòîðîâ â ðåàêöèè ñåëåêòèâíîãî îêèñëåíèÿ ÑÎ ïðîâîäèëîñü íà óñòàíîâêå ïðîòî÷íîãî òèïà â èíòåðâàëå òåìïåðàòóð 20-240 î Ñ, äàâëåíèé 0.1-0.5 ÌÏà ïðè îáúåìíûõ ñêîðîñòÿõ w = (3.6-25.0) ·10 3 ÷ -1 íà ìîäåëüíîé ãàçîâîé ñìåñè ñîñòàâà (% îá.): ÑÎ-1.0, Î 2 -1.4, Í 2 -5, N 2 äî 100. 100 100 Êîíâåðñèÿ ÑÎ, % 80 60 40 20 2 1 3 4 5 Êîíâåðñèÿ ÑÎ , % 80 60 40 20 1 2 3 0 0 30 60 90 120 150 180 210 240 Òåìïåðàòóðà, îÑ a 0 0 30 60 90 120 150 180 210 240 270 Òåìïåðàòóðà, îÑ Ðèñ. 1. Òåìïåðàòóðíûå çàâèñèìîñòè êîíâåðñèè ÑÎ â ðåàêöèè ñåëåêòèâíîãî îêèñëåíèÿ ÑÎ íà (à) Cu-ñîäåðæàùèõ (1 – 1%Cu/CeO 2 ; 2 – 1% Cu/Y 0.06 Ce 0.44 Zr 0.5 O 2 ; 3 – 1% Cu/Ce 0.5 Zr 0.5 O 2 ; 4 – 1% Cu/Y 0.1 Ce 0.1 Zr 0.8 O 2 ; 5 – 1% Cu/ZrO 2 ) è (á) Ñî-ñîäåðæàùèõ (1 – 1% Co/CeO 2 ; 2 – 1% Co/Ce 0,5 Zr 0,5 O 2 ; 3 – 1% Co/ZrO 2 ) êàòàëèòè÷åñêèõ ñèñòåìàõ b Â òàáë. 1 ïðåäñòàâëåíû çíà÷åíèÿ òåìïåðàòóð 50 %-îé êîíâåðñèè ÑÎ è ñåëåêòèâíîñòè ïî êèñëîðîäó ïðè ýòîé òåìïåðàòóðå, ïîëó÷åííûå íà èññëåäîâàííûõ ñèñòåìàõ. Òàáëèöà 1. Òåìïåðàòóðà 50 %-îé êîíâåðñèè ÑÎ è ñåëåêòèâíîñòü ïî êèñëîðîäó â ðåàêöèè îêèñëåíèÿ ÑÎ â âîäîðîäñîäåðæàùåì ãàçå Îáðàçåö Ò 50 % , î Ñ S, % 1% Cu/CeO 2 95 94.6 1% Cu/Ce 0,5 Zr 0,5 O 2-? 108 96.4 1% Cu/Y 0,06 Ce 0,44 Zr 0,5 O 2-? 90 98.5 1%Cu/Y 0,1 Ce 0,1 Zr 0,8 O 2-? 141 71.1 1%Cu/ZrO 2 165 37.8 1%Co/CeO 2 132 24.6 1%Co/Ce 0,5 Zr 0,5 O 2-? 162 41.8 1%Co/ ZrO 2 176 32.1 152
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Èíñòèòóò êàòàëèçà
Page 3 and 4:
Îðãàíèçàòîðû êîíôå
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SINGLE SITE CATALYSTS - IDEAL MODEL
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ÑÒÀÁÈËÈÇÈÐÎÂÀÍÍÛÅ
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ÈÇÓ×ÅÍÈÅ ÌÅÕÀÍÈÇÌÎ
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Ñðàâíåíèå äèíàìèêè
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ÐÎËÜ ÍÎÑÈÒÅËÅÉ Â ÔÎ
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ÒÐÈÈÇÎÁÓÒÈËÀËÞÌÈÍ
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ÏÐÎÃÐÅÑÑ Â ÎÁËÀÑÒÈ
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MOLECULAR DESIGN OF NEW TYPE OF CAT
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PALLADIUM AND COBALT CATALYZED OXID
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ÍÎÂÛÉ ÏÎÄÕÎÄ Ê ÔÎÐÌ
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Èîííûé îáìåí Al 2O 3 2+
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êîòîðûõ èììîáèëèçî
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ïðèâåäøàÿ ê ñîçäàí
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ÐÀÇÐÀÁÎÒÊÀ ÊÀÒÀËÈÇ
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ðàñïðåäåëåíèÿ ÷àñò
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÷òî äåôåêòû ýòîãî â
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ÈÇÓ×ÅÍÈÅ ÔÎÐÌÈÐÎÂÀ
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Ñîäåðæàíèå äèîêñèä
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Òàáë. 1. Äàííûå õåìî
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ñëàáîñâÿçàííîì ñîñ
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ãèäðîãåíèçàöèè, âå
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ÑÅËÅÊÒÈÂÍÀß ÎÊÈÑËÈ
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ÌÎÄÈÔÈÖÈÐÎÂÀÍÈÅ ÀË
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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
Page 102 and 103: ÈÇÓ×ÅÍÈÅ ÌÅÕÀÍÈÇÌÀ
Page 104 and 105: Ðèñóíîê 2. Äèôôåðåí
Page 106 and 107: âòîðîé ïî èíòåíñèâ
Page 108 and 109: êîëåáàíèÿ â ìîñòèê
Page 110 and 111: ÑÒÐÓÊÒÓÐÍÎ-ÎÐÃÀÍÈÇ
Page 112 and 113: Òàáëèöà 2. Ðàñïðåäå
Page 114 and 115: 50 Rate/10 -8 mol g -1 s -1 40 30 2
Page 116 and 117: ÐÀÇÐÀÁÎÒÊÀ È ÈÑÑËÅ
Page 118 and 119: êèñëîðîäó øïèíåëè C
Page 120 and 121: èçîìåðèçàöèè í-ãåê
Page 122 and 123: ÃÅÍÅÇÈÑ ÔÀÇÎÂÎÃÎ Ñ
Page 124 and 125: óïëîòíåíèÿ çàïîëíÿ
Page 126 and 127: Ïðèðîäà èñõîäíûõ ñ
Page 128 and 129: ÏÎËÈÌÅÐÍÛÅ ÐÎÄÈÉÑÎ
Page 130 and 131: ïðîìîòîðîâ. Â ðàáîò
Page 132 and 133: ôîðìàëüäåãèä, äè- è
Page 134 and 135: Äàëüíåéøàÿ äåãèäðî
Page 136 and 137: ÌÅÒÎÄÛ ÐÅÃÓËÈÐÎÂÀÍ
Page 138 and 139: ÑÈÍÒÅÇ È ÈÑÑËÅÄÎÂÀ
Page 140 and 141: ÂËÈßÍÈÅ ÎÁÐÀÁÎÒÎÊ
Page 142 and 143: Íàðÿäó ñ óâåëè÷åíè
Page 144 and 145: îáîðîòîâ êàòàëèçàò
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Page 148 and 149: äî 0,5 ÌÏà. Ôîðìû çàâ
Page 150 and 151: Î ÏÐÎÖÅÑÑÀÕ ÏÐÅÄÎÒ
Page 154 and 155: ÏÐÅÂÐÀÙÅÍÈß ÑÒÈÐÎË
Page 156 and 157: ÆÈÄÊÎÔÀÇÍÀß ÈÇÎÌÅÐ
Page 158 and 159: ÍÅÏÎËÍÎÅ ÎÊÈÑËÅÍÈÅ
Page 160 and 161: ÍÀÍÎÑÒÐÓÊÒÓÐÍÛÅ ÊÀ
Page 162 and 163: ÃÈÄÐÎÊÎÍÂÅÐÑÈß Í-Ã
Page 164 and 165: ðàñòåò ñ ïîâûøåíèå
Page 166 and 167: Èíäèâèäóàëüíàÿ àäñ
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Page 170 and 171: Ïðîöåññ áèôîðìèíãà
Page 172 and 173: ÈÑÏÎËÜÇÎÂÀÍÈÅ ÊÀÒÀ
Page 174 and 175: Ïîâûøåíèå äàâëåíèÿ
Page 176 and 177: Èç ïðèðîäíîãî öåîë
Page 178 and 179: ÄÅÃÈÄÐÈÐÎÂÀÍÈÅ ËÅÃ
Page 180 and 181: ðîäèåâûå è ðóòåíèå
Page 182 and 183: Òàáëèöà 1. Âëèÿíèå ï
Page 184 and 185: ÈÑÑËÅÄÎÂÀÍÈÅ ÏÐÎÖÅ
Page 186 and 187: ÏÅÐÅÐÀÁÎÒÊÀ ÄÈÑÒÈË
Page 188 and 189: ÃÈÄÐÎÏÅÐÅÐÀÁÎÒÊÀ í
Page 190 and 191: ÊÐÅÊÈÍÃ ÒßÆÅËÎÃÎ Í
Page 192 and 193: óãëåðîäà â äèîêñèä
Page 194 and 195: ïîäà÷è ñûðüÿ 1,0-1,5 ÷
Page 196 and 197: ëîêàëèçîâàííûå íà
Page 198 and 199: CÓËÜÔÎÊÀÒÈÎÍÈÒÛ ÍÀ
Page 200 and 201: 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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