采用程序升温脱附、在线质谱和原位漫反射红外光谱等手段,比较了NO和NO_2在V_2O_5及V_2O_5/AC催化剂表而的选择催化还原(SCR)反应行为.结果表明,氨以质子态NH_4~+和共价态NH_3分子两种形态吸附于纯V_2O_5表面,V=O为氨的主要吸附活性位.无氧状态下,NO和NO_2皆可与吸附于V_2O_5表面的NH_3反应,并且NO_2与吸附态NH_2的反应活性高于NO.但在V_2O_5/AC催化剂表面,同样在无氧条件下,NO几乎不与吸附态NH_3反应,而NO_2却可以反应并生成N_2.在V_2O_5/AC表面,NO很容易被气相O_2氧化为NO_2,然后参与SCR反应.可见,NO_2是NO在V_2O_5/AC表面发生SCR反应的中间体.
Temperature-programmed desorption, on-line mass spectroscopy, and in situ diffuse reflectance infrared Fourier transform spec-troscopy were preformed to study selective catalytic reduction (SCR) of NO and NO_2 with NH_3 over V_2O_5 and activated carbon (AC)-supported V_2O_5 (V_2O_5/AC). The results show that both protonated (NH4+) and molecularly coordinated (NH_3) ammonia species form on the V_2O_5 surface and V=O bond is the primary active site. Both NO_2 and NO can react with the adsorbed ammonia in the absence of oxy-gen, but the activity of NO_2 is superior to that of NO. On the V_2O_5/AC surface, NO_2 still can react with the adsorbed NH_3 species to form N_2, but NO shows little activity unless oxygen is present. SCR of NO on V_2O_5/AC proceeds through oxidation of NO to NO_2 by oxygen on the AC surface followed by reaction of NO_2 with NH_3 species adsorbed and activated on the V_2O_5 surface .
参考文献
[1] | Ramis G;Busca G;Bregani F;Forzatti P .[J].Applied Catalysis,1990,64:259. |
[2] | Ramis G;Yi L;Busca G;Tureo M Kotur E Willey R J .[J].Journal of Catalysis,1995,157:523. |
[3] | Centeno M A;Carrizosa I;Odoriozola J A .[J].Applied Catalysis B:Environmental,2001,29:307. |
[4] | Parvulescu VI.;Boghosian S.;Parvulescu V.;Jung SM.;Grange P. .Selective catalytic reduction of NO with NH3 over mesoporous V2O5-TiO2-SiO2 catalysts[J].Journal of Catalysis,2003(1):172-185. |
[5] | Bosch H;Janssen F .[J].Catalysis Today,1988,2:369. |
[6] | Forzatti P .[J].Catalysis Today,2000,62:51. |
[7] | Qi G;Yang R T .[J].Journal of Catalysis,2003,217:434. |
[8] | Zhu Z P;Liu Z Y;Liu S J;Niu H X .[J].Applied Catalysis B:Environmental,1999,23:L229. |
[9] | Lazaro MJ;Galvez ME;Ruiz C;Juan R;Moliner R .Vanadium loaded carbon-based catalysts for the reduction of nitric oxide[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2006(3/4):130-138. |
[10] | Zhu Z P;Liu Z Y;Niu H X;Liu S J .[J].Journal of Catalysis,1999,187:245. |
[11] | Zhu Z P;Liu Z Y;Liu S J;Niu H X .[J].Applied Catalysis B:Environmental,2001,30:267. |
[12] | 马建蓉,刘振宇,黄张根,刘清雅.NH3在V2O5/AC催化剂表面的吸附与氧化[J].催化学报,2006(01):91-96. |
[13] | 刘清雅,刘振宇,李成岳.NH3在选择性催化还原NO过程中的吸附与活化[J].催化学报,2006(07):636-646. |
[14] | Mochida I;Kisamori S;Hironaka M;Kawano S Matsumura Y Yoshikawa M .[J].Energy and Fuels,1994,8:1341. |
[15] | Zawadzki J;Wisniewski M;Skowronska K .[J].CARBON,2003,41:235. |
[16] | Juntgen H;Richter E;Kuhl H .[J].Fuel,1988,67:775. |
[17] | Shiraham N;Mochida I;Korai Y;Choi K H Enjoji T Shimahara T Yasutake A .[J].Applied Catalysis B:Environmental,2005,57:237. |
[18] | Tang X;Hao J;Yi H;Li J .[J].Catalysis Today,2007,126:406. |
[19] | Mochida I.;Shirahama M.;Kawano S.;Hada T.;Seo Y.;Yoshikawa M.;Yasutake A.;Korai Y. .Removal of SOx and NOx over activated carbon fibers[J].Carbon: An International Journal Sponsored by the American Carbon Society,2000(2):227-239. |
[20] | Busca G;Lietti L;Ramis G;Berti F .[J].Applied Catalysis B:Environmental,1998,18:1. |
[21] | Galvez M E;Boyano A;Lazaro M J;Moliner R .[J].Chemical Engineering Journal,2008,144:10. |
[22] | Huang B;Huang R;Jin D;Ye D .[J].Catalysis Today,2007,126:279. |
[23] | Jung S M;Grange P .[J].Applied Catalysis B:Environmental,2002,36:325. |
[24] | Ramis G;Busca G;Lorenzelli V;Forzatti P .[J].Applied Catalysis,1990,64:243. |
[25] | Zhu Z P;Liu Z Y;Liu S J;Niu H X .[J].Fuel,2000,79:651. |
[26] | Richter E .[J].Catalysis Today,1990,7:93. |
[27] | Kijlstra WS.;Poels EK.;Bliek A.;Brands DS. .MECHANISM OF THE SELECTIVE CATALYTIC REDUCTION OF NO BY NH3 OVER MNOX/AL2O3 .1. ADSORPTION AND DESORPTION OF THE SINGLE REACTION COMPONENTS[J].Journal of Catalysis,1997(1):208-218. |
[28] | Qi G;Yang R .[J].Journal of Physical Chemistry B,2004,108:15738. |
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