第二金属组分对Ni/SiC催化剂CO_2甲烷化性能的影响
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摘要
采用共浸渍法制备了Fe,Co,Cu或Mn促进的系列SiC担载的Ni基双金属催化剂,采用XRD、TEM、H_2-TPR对其进行表征,并在固定床微型反应器装置上考察第二金属组分对Ni/SiC在CO_2甲烷化反应中的催化性能的影响。结果表明,Mn的添加提高了Ni/SiC催化剂中Ni的分散度,增强了NiO与SiC之间的相互作用,从而提高了催化剂的活性和稳定性;而Fe,Co,Cu的添加降低了Ni/SiC催化剂的活性,其中添加Cu的催化剂活性最差。
Fe, Co, Cu or Mn modified Ni/SiC catalysts were prepared by co-impregnation, and characterized by XRD, TEM and H_2-TPR, while their catalytic performances for CO_2 methanation were investigated in a fixed-bed micro reactor. Results showed that the addition of Mn could increase the dispersion of Ni and strengthen the interaction between Ni O and Si C and thus improve the activity and stability of Ni/Si C catalyst. On the contrary, the addition of Fe, Co, Cu reduced the activity of Ni/Si C catalyst, and the Ni-Cu/Si C had the lowest activity among them.
Fe, Co, Cu or Mn modified Ni/SiC catalysts were prepared by co-impregnation, and characterized by XRD, TEM and H_2-TPR, while their catalytic performances for CO_2 methanation were investigated in a fixed-bed micro reactor. Results showed that the addition of Mn could increase the dispersion of Ni and strengthen the interaction between Ni O and Si C and thus improve the activity and stability of Ni/Si C catalyst. On the contrary, the addition of Fe, Co, Cu reduced the activity of Ni/Si C catalyst, and the Ni-Cu/Si C had the lowest activity among them.
引文
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[29]Guo J J,Lou H,Zhao H,et al.Dry reforming of methane over nickel catalysts supported on magnesium aluminate spinels[J].Appl Catal A,2004,273:75-82.
[2]高建国,丁剑秋,杨芳芳,等.二氧化碳催化加氢甲烷化研究进展[J].贵州化工,2009,34(3):23-25.
[3]许文娟,马丽萍,黄彬,等.CO2催化加氢研究进展[J].化工进展,2009,28(s1):284-289.
[4]Weatherbee G D,Bartholomew C H.Hydrogenation of CO2on group VIII metals:I.Speciic activity of Ni/Si O2[J].J Catal,1981,68:67-76.
[5]孙卫中,莫若飞,靳国强,等.不同载体的镍基催化剂在甲烷部分氧化反应中的催化行为[J].天然气化工(C1化学与化工),2006,31(6):1-5.
[6]Shang R J,Sun W Z,Wang Y Y,et al.Silicon nitride supported nickel catalyst for partial oxidation of methane to syngas[J].Catal Commun,2008,9:2103-2106.
[7]李旭,图雅,双成,等.制备条件对Au/La-Mn-O催化剂低温氧化CO性能的影响[J].内蒙古师范大学学报,2010,39(5):521-524.
[8]魏旭芳,陈维民.浸渍还原法对DMFC阳极催化剂的影响[J].沈阳理工大学学报,2011,30(2):36-39.
[9]王定博,王斌,王焕如.碳四烯烃制丙烯催化剂的稳定性[J].工业催化,2011,19(6):54-57.
[10]谢有畅,钱民协,唐有祺.添加剂La2O3对甲烷化催化剂中镍的分散度和热稳定性的影响[J].中国科学B,1983,(9):788-795.
[11]Zhi G J,Guo X N,Wang Y Y,et al.Effect of La2O3modiication on the catalytic performance of Ni/Si C for methanation of carbon dioxide[J].Catal Commun,2011,16:56-59.
[12]魏蓉,刘家强,李志华.Mn助剂对甲醇合成Cu-Zn-A1催化剂的影响[J].山东师范大学学报,2009,24(3):54-56.
[13]职国娟,王英勇,靳国强,等.镍盐前躯体对CO2甲烷化Ni/Si C催化剂性能的影响[J].天然气化工(C1化学与化工),2012,37(4):10-14+42.
[14]李丽波,魏树权,徐国林.第二金属组分对CO2甲烷化沉淀型镍基催化剂的影响[J].天然气化工(C1化学与化工),2004,29(4):27-31.
[15]江琦.负载型镍催化剂上CO2加氢甲烷化研究[J].天然气化工(C1化学与化工),2000,25(4):9-14.
[16]常丽萍,钟顺和,谢克昌.二氧化碳催化氢化—Ni、Cu间的相互作用及不同担体的影响[J].燃料化学学报,1994,22(2):170-174.
[17]Osaki T,Mori T.Kinetic studies of CO2dissociation on supported Ni catalysts[J].React Kinet Catal Lett,2006,87:149-156.
[18]Sinfelt J H.Bimetallic Catalyst[M].New York:John Wiley and Sons,1983:77-92.
[19]李想,孟明,姚金松,等.Mn/Ce/La/Al2O3催化剂中锰物种的精细结构研究[J].无机化学学报,2007,23(2):211-216.
[20]高晓庆,王永钊,李海涛,等.Mn助剂对Ni/γ-Al2O3催化剂CO2甲烷化性能的影响[J].分子催化,2011,25(1):49-54.
[21]Martínez R,Romero E,Guimon C,et al.CO2reforming of methane over coprecipitated Ni-Al catalysts modified with lanthanum[J].Appl Catal A,2004,274:139-149.
[22]Yang R Q,Xing C,Lv C X,et al.Promotional effect of La2O3and Ce O2on Ni/γ-Al2O3catalysts for CO2reforming of CH4[J].Appl Catal A,2010,385:92-100.
[23]Seok S H,Han S H,Lee J S.The role of Mn O in Ni/Mn O-Al2O3catalysts for carbon dioxide reforming of methane[J].Appl Catal A,2001,215:31-38.
[24]郭建忠,侯昭胤,高静,等.不同粒径的Ni/Si O2催化剂上CH4和CO2吸附活化的漫反射傅里叶变换红外光谱研究[J].催化学报,2007,28(1):22-26.
[25]Krylov O V,Mamedov A K,Mirzabekova S R.Interaction of carbon dioxide with methane on oxide catalysts[J].Catal Today,1998,42:211-215.
[26]Nandini A,Pant K K,Dhingra S C.K-,Ce O2-,and Mnpromoted Ni/Al2O3catalysts for stable CO2reforming of methane[J].Appl Catal A,2005,290:166-174.
[27]Wang W,Gong J L.Methanation of carbon dioxide:An overview[J].Front Chem Sci Eng,2011,5:2-10.
[28]Burattin P,Che M,Louis C.Metal particle size in Ni/Si O2materials prepared by deposition-precipitation:influence of the nature of the Ni(II)phase and of its interaction with the support[J].J Phys Chem B,1999,103:6171-6178.
[29]Guo J J,Lou H,Zhao H,et al.Dry reforming of methane over nickel catalysts supported on magnesium aluminate spinels[J].Appl Catal A,2004,273:75-82.