基于NH_3-SCR的CeO_2-TiO_2复合氧化物催化剂:结构与脱硝性能
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摘要
以TiOSO_4·2H_2O和Ce(NO_3)_3·6H_2O为前驱体,采用共沉淀法制备了不同CeO_2含量的CeO_2-TiO_2复合氧化物催化剂.对样品结构进行了表征,考察了催化剂的NH_3-SCR(NH_3选择性催化还原)反应活性、N_2选择性和抗水抗硫性能.结果表明,随着催化剂中CeO_2含量的增加,催化剂的物相结构、晶粒尺寸及脱硝性能均出现规律性变化,这种改变与样品的酸碱性和氧化还原性能的变化有关.当样品中CeO_2的质量分数约为50%时,催化剂的结构呈无定形态,具有较大的比表面积和较多的氧空位,有利于反应物分子在催化剂表面的吸附和活化,拓宽了催化剂的低温活性窗口并提高了NO的转化率.
A series of CeO_2-TiO_2 mixed oxides catalysts prepared by Co-precipitation method was investigated on selective catalytic reduction(SCR) of NO_x with NH_3. The properties of the catalysts were characterized using XRD,BET,XRF,XPS,H_2-TPR,NH_3-TPD and NO+O_2-TPD techniques. The results indicated that the crystal structure,crystallite size and catalytic NH_3-SCR activity over the catalysts presented a regular change with the increase of CeO_2 concentration. Particularly,the 50 CeTi catalyst with amorphous structure of CeO_2-TiO_2 showed a higher BET surface area and a stronger surface acidity than other samples. Meanwhile,favorable Ce~(3+) and the surface adsorbed oxygen benefited the adsorption of NO_x and NH_3 molecules,which enhanced DeNO_x performance.
A series of CeO_2-TiO_2 mixed oxides catalysts prepared by Co-precipitation method was investigated on selective catalytic reduction(SCR) of NO_x with NH_3. The properties of the catalysts were characterized using XRD,BET,XRF,XPS,H_2-TPR,NH_3-TPD and NO+O_2-TPD techniques. The results indicated that the crystal structure,crystallite size and catalytic NH_3-SCR activity over the catalysts presented a regular change with the increase of CeO_2 concentration. Particularly,the 50 CeTi catalyst with amorphous structure of CeO_2-TiO_2 showed a higher BET surface area and a stronger surface acidity than other samples. Meanwhile,favorable Ce~(3+) and the surface adsorbed oxygen benefited the adsorption of NO_x and NH_3 molecules,which enhanced DeNO_x performance.
引文
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[3]Liu J.D.,Huang Z.G.,Li Z.,Guo Q.Q.,Li Q.Y.,Chem.J.Chinese Universities,2014,35(3),589—595(刘建东,黄张根,李哲,郭倩倩,李巧艳.高等学校化学学报,2014,35(3),589—595)
[4]Tang C.J.,Zhang H.L.,Dong L.,Catal.Sci.Technol.,2016,6,1248—1264
[5]Li Q.,Gu H.C.,Li P.,Zhou Y.H.,Liu Y.,Qi Z.N.,Xin Y.,Zhang Z.L.,Chin.J.Catal.,2014,35(8),1289—1298(李倩,谷华春,李萍,周钰浩,刘莹,齐中囡,辛颖,张昭良.催化学报,2014,35(8),1289—1298)
[6]Li Z.G.,Li J.H.,Liu S.X.,Ren X.N.,Ma J.,Su W.K.,Peng Y.,Catalysis Today,2015,258,11—16
[7]Yu M.,Li C.T.,Zeng G.M.,Zhou Y.,Zhang X.N.,Xie Y.,Applied Surface Science,2015,342,174—182
[8]Zhou A.Y.,Yu D.Q.,Yang L.,Sheng Z.Y.,Applied Surface Science,2016,378,167—173
[9]Chen L.,Si Z.C.,Wu X.D.,Weng D.,Appl.Mater.Interfaces,2014,6,8134—8145
[10]Liu J.,Li X.Y.,Zhao Q.D.,Ke J.,Xiao H.N.,Lv X.J.,Liu S.M.,TadéM.,Wang S.B.,Appl.Catal.B:Environ.,2017,200,297—308
[11]Luo M.F.,Chen J.,Chen L.S.,Lu J.Q.,Feng Z.C.,Li C.,Chem.Mater.,2001,13,197—202
[12]Gao X.,Jiang Y.,Zhong Yi.,Luo Z.Y.,Cen K.F.Journal of Hazardous Materials,2010,174,734—739
[13]Li P.,Xin Y.,Li Q.,Wang Z.P.,Zhang Z.L.,Zheng L.R.,Environ.Sci.Technol.,2012,46,9600—9605
[14]Wang H.Q.,Cao S.,Fang Z.,Yu F.X.,Liu Y.,Weng X.L.,Wu Z.B.,Applied Surface Science,2015,330,245—252
[15]Xiao X.,Xiong S.C.,Shi Y.J.,Shan W.P.,Yang S.J.,J.Phys.Chem.C,2016,120,1066—1076
[16]Song L.Y.,Zhan Z.C.,Liu X.J.,He H.,Qiu W.G.,Zi X.H.,Chin.J.Catal.,2014,35(7),1030—1035(宋丽云,展宗城,刘晓军,何洪,邱文革,訾学红.催化学报,2014,35(7),1030—1035)
[17]Chao J.D.,He H.,Song L.Y.,Fang Y.J.,Liang Q.M.,Zhang G.G.,Qiu W.G.,Zhang R.,Chem.J.Chinese Universities,2015,36(3),523—530(晁晶迪,何洪,宋丽云,房玉娇,梁全明,张桂臻,邱文革,张然.高等学校化学学报,2015,36(3),523—530)
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[19]Yan D.J.,Yu Y.,Huang X.M.,Liu S.J.,Liu Y.H.,J.Fuel.Chem.Technol.,2016,44(2),232—238
[20]Shi Z.N.,Yang P.,Tao F.,Zhou R.X.,Chem.Eng.J.,2016,295,99—108
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[23]Su Y.F.,Tang Z.C.,Han W.L.,Zhang P.,Song Y.,Lu G.X.,Cryst.Eng.Comm.,2014,16,5189—5197
[24]Ferrizz R.M.,Gorte R.J.,Vohs J.M.,Catal.Lett.,2002,82(1/2),123—129
[25]Bêche E.,Charvin P.,Perarnau D.,Abanades S.,Flamant G.,Surface&Interface Analysis,2008,40(3/4),264—267
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