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ÍÅÏÎËÍÎÅ ÎÊÈÑËÅÍÈÅ Ñ 3 -Ñ 4 ÍÀÑÛÙÅÍÍÛÕ ÓÃËÅÂÎÄÎÐÎÄÎÂ ÄÎ ÎÊÑÈÃÅÍÀÒÎÂ ÍÀ ÏÎËÈÎÊÑÈÄÍÛÕ ÊÀÒÀËÈÇÀÒÎÐÀÕ Äîñóìîâ Ê., Ìàñàëèìîâà Á.Ê., Òóíãàòàðîâà Ñ.À., Êóçåìáàé Ê.Ê. Èíñòèòóò îðãàíè÷åñêîãî êàòàëèçà è ýëåêòðîõèìèè èì. Ä.Â. Ñîêîëüñêîãî ÌÎÍ ÐÊ, Àëìàòû, Êàçàõñòàí E-mail: tungatarova58@mail.ru Èññëåäîâàíû ïîëèîêñèäíûå íàíåñåííûå êàòàëèçàòîðû íà îñíîâå Ìî è ïðèðîäíûõ ãëèí Êàçàõñòàíà â ïðîöåññå îêèñëèòåëüíîé êîíâåðñèè ïðîïàí-áóòàíîâîé ñìåñè â êèñëîðîäñîäåðæàùèå ñîåäèíåíèÿ è óãëåâîäîðîäû. Îïðåäåëåíî âëèÿíèå òåìïåðàòàòóðû ðåàêöèè, ñîñòàâà ðåàêöèîííîé ñìåñè, âðåìåíè êîíòàêòà, ñîäåðæàíèÿ êèñëîðîäà â èñõîäíîé ñìåñè, à òàêæå ñîñòàâà àêòèâíîé ôàçû êàòàëèçàòîðà. Ïî îöåíêàì ñïåöèàëèñòîâ ïðèðîäíûõ çàïàñîâ íåôòè õâàòèò íà íåáîëüøîé îòðåçîê âðåìåíè. Â ñâÿçè ñ ýòèì ïðîáëåìà áîëåå ïîëíîãî èñïîëüçîâàíèÿ ïðèðîäíîãî è ïîïóòíîãî ãàçîâ â êà÷åñòâå ñûðüÿ äëÿ õèìè÷åñêîé ïðîìûøëåííîñòè ÿâëÿåòñÿ àêòóàëüíîé. Ïåðåä ó÷åíûìè ñòîèò çàäà÷à ïî ïîèñêó ñïîñîáîâ ïðåâðàùåíèÿ ãàçîîáðàçíûõ óãëåâîäîðîäîâ â æèäêèå, ïîòðåáíîñòü â êîòîðûõ ïðîäèêòîâàíà áîëüøèì óäîáñòâîì è äåøåâèçíîé õðàíåíèÿ, òðàíñïîðòèðîâêè è èñïîëüçîâàíèÿ, ïîñêîëüêó íîðìàòèâíûå àêòû ïî çàùèòå îêðóæàþùåé ñðåäû, ïðèíÿòûå â ã. Êèîòî, ßïîíèÿ, ïðèâåäóò â áóäóùåì ê ðåçêîìó îãðàíè÷åíèþ èëè ïîëíîìó ïðåêðàùåíèþ ñæèãàíèÿ ãàçà â ôàêåëàõ. Øèðîêàÿ ôðàêöèÿ ëåãêèõ óãëåâîäîðîäîâ, îñíîâó êîòîðîé ñîñòàâëÿåò ïðîïàí è áóòàí, ÿâëÿåòñÿ öåííåéøèì ñûðüåì äëÿ íåôòåõèìèè è íåôòåïåðåðàáîòêè [1, 2]. Èññëåäîâàíèÿ ïðîâîäèëèñü íà óñòàíîâêå ïðîòî÷íîãî òèïà ïðè àòìîñôåðíîì äàâëåíèè â òðóá÷àòîì êâàðöåâîì ðåàêòîðå ñ ôèêñèðîâàííûì ñëîåì êàòàëèçàòîðà. Àíàëèç èñõîäíûõ âåùåñòâ è ïðîäóêòîâ ðåàêöèè îñóùåñòâëÿëñÿ ñ ïîìîùüþ õðîìàòîãðàôè÷åñêîãî ìåòîäà íà ïðèáîðå «Agilent Technologies». Êàòàëèçàòîðû îõàðàêòåðèçîâàíû ìåòîäàìè ÐÔÀ, îñóùåñòâëåíî îïðåäåëåíèå ïîâåðõíîñòè, ïîðèñòîñòè è ýëåìåíòíîãî ñîñòàâà îáðàçöîâ. Â êà÷åñòâå êàòàëèçàòîðîâ èñïîëüçîâàíû íàíåñåííûå ïîëèîêñèäíûå êîíòàêòû íà îñíîâå Mo, Bi, Ce, Ni, W, Sb, Mn, Fe, Ga, Cr. Â êà÷åñòâå íîñèòåëåé èñïîëüçîâàíû ïðèðîäíûå ãëèíû Êàçàõñòàíà. Ïðîöåññ îñóùåñòâëÿëñÿ ïðè òåìïåðàòóðàõ 300-600 °C ïðè îáúåìíîé ñêîðîñòè 7500-15000 ÷ -1 . Óñòàíîâëåíî, ÷òî îñíîâíûìè æèäêèìè ïðîäóêòàìè ÿâëÿþòñÿ àöåòîí, ìåòàíîë, àöåòàëüäåãèä. Â ãàçîâîé ôàçå ïðåîáëàäàåò ýòèëåí. Îïòèìàëüíûìè 157
òåìïåðàòóðàìè ïî ìåòàíîëó è àöåòàëüäåãèäó ÿâëÿþòñÿ 300-350 °Ñ, ïî àöåòîíó - 450-500 °Ñ, ïî óêñóñíîé êèñëîòå - 500-600 °Ñ (Ðèñ. 1). Ñ ïîâûøåíèåì òåìïåðàòóðû ñîäåðæàíèå ýòèëåíà â îòõîäÿùåì ãàçå ïðè 500-600 °Ñ óâåëè÷èâàåòñÿ ñ 5 äî 17 %. Ñîäåðæàíèå â êàòàëèçàòå % , 45 40 35 30 25 20 15 10 5 0 ÑÍ 3ÎÍ (ÑÍ 3 ) 2 ÑÎ ÑÍ 3 ÑÎÎÍ Ñ 2 Í 4 ÑÍ 3 ÑÍÎ 300 350 400 450 500 550 600 Òåìïåðàòóðà, îÑ Ðèñ. 1. Âëèÿíèå òåìïåðàòóðû ðåàêöèè íà íàïðàâëåíèå îêèñëèòåëüíîãî ïðåâðàùåíèÿ ïðîïàí-áóòàíîâîé ñìåñè íà ÌîCrGa/Òîðãàéñêàÿ ãëèíà. Ñ 3 Í 8 +Ñ 4 Í 10 – 60,0 %, Î 2 – 8,4 %, N 2 – 31,6 %, W – 7500 ÷ -1 . Èñïûòàíèÿ ïðèðîäíûõ ãëèí ìåòîäîì ÐÔÀ ïîêàçàëè, ÷òî îñíîâíûå ôàçû Òîðãàéñêîé áåëîé ãëèíû – êàîëèíèò Al 2 [OH] 4 Si 2 O 5 (ASTM-29-1488) è α-êâàðö SiO 2 , à Òîðãàéñêàÿ êðàñíàÿ ãëèíà îòëè÷àåòñÿ îò áåëîé íàëè÷èåì ãåìàòèòà Fe 2 O 3 è îòñóòñòâèåì α-êâàðöà. Ñîîòíîøåíèå SiO 2 /Al 2 O 3 (êðåìíèåâûé ìîäóëü) ñîñòàâëÿåò 5-0,4. Ïîñëå êèñëîòíîé îáðàáîòêè êðåìíèåâûé ìîäóëü âîçðàñòàåò. Îáðàáîòêà ñîðáåíòîâ 10 % HCl ñïîñîáñòâîâàëà ðàçðàáîòêå è óâåëè÷åíèþ ðàäèóñà ïîð. Êèñëîòíàÿ îáðàáîòêà îáðàçöîâ êàòàëèçàòîðîâ ïðèâîäèëà ê óâåëè÷åíèþ ñîäåðæàíèÿ àöåòîíà â êàòàëèçàòå, òàêèå æå çàêîíîìåðíîñòè íàáëþäàëèñü è äëÿ îñòàëüíûõ êèñëîðîäñîäåðæàùèõ ñîåäèíåíèé. Âàðüèðîâàíèå îáúåìíîé ñêîðîñòè è ñîîòíîøåíèÿ êîìïîíåíòîâ â ðåàêöèîííîé ñìåñè ïîêàçàëî, ÷òî îïòèìàëüíîé äëÿ ïîëó÷åíèÿ àöåòîíà è ìåòàíîëà ÿâëÿåòñÿ îáúåìíàÿ ñêîðîñòü 7500 ÷ -1 ïðè 450-500 î Ñ è 300-350 î Ñ, ñîîòâåòñòâåííî, à äëÿ ñèíòåçà ýòèëåíà áëàãîïðèÿòíû îáúåìíûå ñêîðîñòè â èíòåðâàëå 7500-9000 ÷ -1 . Ñ ïîâûøåíèåì ñîäåðæàíèÿ êèñëîðîäà â èñõîäíîé ñìåñè êîëè÷åñòâî àöåòîíà è ìåòàíîëà â êàòàëèçàòå óâåëè÷èâàëîñü. Àíàëèç ñîñòàâà ïðîäóêòîâ ïîêàçàë, ÷òî ïðîöåññ ïðîòåêàåò ïî ñëîæíîìó ìåõàíèçìó, âêëþ÷àþùåìó ïðîöåññû îêèñëåíèÿ è îêèñëèòåëüíîãî äåãèäðèðîâàíèÿ. Ëèòåðàòóðà 1. Â.Í. Ïàðìîí. Êàòàëèç â ïðîìûøëåííîñòè. 2 (2002) 9-10. 2. À.À. Ïåòðîâ. Êàòàëèç â ïðîìûøëåííîñòè. 2 (2002) 11-15. 158
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Èíñòèòóò êàòàëèçà
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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
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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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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
Page 146 and 147: Íàìè ðàçðàáîòàí ïð
Page 148 and 149: äî 0,5 ÌÏà. Ôîðìû çàâ
Page 150 and 151: Î ÏÐÎÖÅÑÑÀÕ ÏÐÅÄÎÒ
Page 152 and 153: ÐÀÇÐÀÁÎÒÊÀ ÊÀÒÀËÈÒ
Page 154 and 155: ÏÐÅÂÐÀÙÅÍÈß ÑÒÈÐÎË
Page 156 and 157: ÆÈÄÊÎÔÀÇÍÀß ÈÇÎÌÅÐ
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
Page 168 and 169: â ÑÍÃ ñíèæàåò òåìïå
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
Page 202 and 203: ãåêñàäåêàíîë-2 (ïðè
Page 204 and 205: óñëîâèÿ îêèñëåíèÿ
Page 206 and 207: 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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ÐÐ¾Ð»ÐµÐºÑÐ»ÑÑÐ½ÑÐ¹ Ð´Ð¸Ð·Ð°Ð¹Ð½ ÐºÐ°ÑÐ°Ð»Ð¸Ð·Ð°ÑÐ¾ÑÐ¾Ð² Ð¸ ÐºÐ°ÑÐ°Ð»Ð¸Ð· Ð² Ð¿ÑÐ¾ÑÐµÑÑÐ°Ñ...