甲烷部分氧化制合成氣載體及助劑對Ni系催化劑活性的影響

第22卷第4期催化學(xué)報2001年7月Vol. 22 NO. 4Chinese Journal of CatalysisJuly 2001文章編號:0253-983X2001)403830甲烷部分氧化制合成氣載體及助劑對Ni系催化劑活性的影響余林,袁書(shū)華2,田久英2,王升2,儲偉(1汕頭大學(xué)化學(xué)系,汕頭515063;2四川大學(xué)化學(xué)學(xué)院,成都610064:3中國科學(xué)院成都有機化學(xué)研究所,成都610041)摘要:采用浸漬法制備了Ni系催化劑并用程序升溫還原和X射線(xiàn)衍射技術(shù)對催化劑進(jìn)行了表征用固定床微反裝置考察了催化劑的催化活性.活性考察結果表明在Ni擔載量為8%的N/y-A2ONV/-A2O3N/B-A2O3和κ/α-AO3四種催化劑上甲烷部分氧化制合成氣反應的活性及產(chǎn)物選擇性存在著(zhù)明顯的差異.在770℃下甲烷轉化率及CO和H的選擇性按Ni/yAl2O31.0%才能使催化劑的活性Zh, Xu h y et al. Chin/ Catal ), 2000,21(5): 415有明顯提高8季亞英,李文釗,徐恒泳等.催化學(xué)報(JiYY,LiW參考文獻Zh, Xuhyet al. Chin j Catal), 2000,21(6): 603曹立新,陳燕馨,李文釗.分子催倀( Cao L x, Chen y1嚴前古,高利珍,儲偉等.化學(xué)學(xué)報( Yan Q G,GaoLX, Li W Zh. J Mol Catal( China )) 1994, 85): 375Zh, Chu W et al. Acta Chim Sin ) 1998, 56( 10): 102110 Jacono M L, Schiavello M, Cimino A.J Phys Chem2 ZhouJP, Li ch y, Zhang Zh B, Shen sh K.催化學(xué)報1971,78):1044( Chin catal),1999,204):39111褚衍來(lái),李樹(shù)本,林景治等.分子催 Chuy l,LiSh3任杰,陳仰光,吳東,范文浩.分子催做RenJ,ChenB, Lin j Zh et al. J Mol Catal( China )) 1996,10G, Wu D, Fan W H. J Mol Catal( China )) 1994, 8(6):449(3):1814 Zhang yh, Xiong GⅩ, Liu sh l et al.催化學(xué)撇(Mm/12儲偉,劉晰,于作龍等.天然氣化工(ChuW,LiuxYu ZL et al. Natur Gas Chem Ind),1998, 233): 29Catal),1999,20(4):3933 Wang Sh B, Lu G Q. Appl Catal B, 1998, 19( 3/4):5 Gadalla A M, Bower B. Chem Eng Sci,1998, 43(11)26714 Slagtern A, Olsbye U, Blom R et al. Stud Surf Sci6張兆彬,余長(cháng)春,沈師孔.催化學(xué)報 Zhang Zh B,YuChCatal,1977,107:497Ch, Shen Sh K. Chin J Catal ) 2000, 21(1): 1415 Ji M, Zhou MJ, Bi Y L et al. J Mol Catal( China7季亞英,李文釗,徐恒泳等.催化學(xué)報(JiYY,LiW1997,1(1):13Partial Oxidation of Methane to SyngasEffects of Support and Promoter on Catalytic Performance of Ni/Al2O3 CatalystYU Lin'*, YUAN Shuhua, TIAN Jiuying, WANG Sheng, CHU Wei(1 Departent of Chemistry, Shantou University, Shantou 515063, china2 College of Chemistry Sichuan University, Chengdu 610064, china3 Chengdu Institute of Organic Chemistry, The Chinese Academy of Sciences Chengdu 610041, ChinaAbstract: The Ni catalyst samples, with y,a-,0-,or a-Al2O3 as a support and with Ceo as a promoterwere charaterized by TPR and XRD techniques and evaluated by the reaction of partial oxidation of methaneto syngas. The evaluation results showed that the catalytic activity of the catalyst samples and the productselectivity increase in the order of 8%Ni/y-AlO3 <8%Ni/8-Al2O3<8%Ni/0-Al2O38%Ni/a-Al,OWhen adding Ceo promoter into the catalyst samples the catalytic activity of 8%Ni/y-AlO3 and 8% Ni/8-Al2O, increased significantly while that of 8% Ni/0-Al2O3 and 8%Ni/a-Al2O3 had hardly changed. Thiscan be due to the depression of the formation of the low active crystalline phase Nial O4 when adding Ceo2promoter into 8%Ni/y-AlO3 and 8%Ni/8-ALO3 samples. The characterization results from TPR and XRDconfirmed the above viewpoint. For 8% Ni/B-Al2O3 and 8% Ni/a-AlO3 with low BET surface area,nocrystalline phase NialO4 was detecteey ords: nickel alumina supported catalyst methane partial oxidation syngas ceria, promoter(Ed WGzh中國煤化工CNMHG