采用3种不同的浸渍过程制备了系列 WO3改性 MnOx/TiO2催化剂,并采用 BET 比表面积测试、X 射线衍射、拉曼光谱、H2程序升温还原、高分辨扫描电镜和原位红外光谱等技术进行表征.结果显示,一步浸渍法和先钨后锰的分布浸渍法制备的催化剂中, Mn 和 W 的协同作用提高了活性组分的分散状态,并阻止了钛载体的转晶;在所有的 Mn 基催化剂中, Mn 物种主要以Mn2O3形式存在,但在15%MnOx-5%WO3/TiO2中出现了少量的 MnO2; WO3的加入大大增强了催化剂的还原能力,提高了其表面酸位尤其是 B 酸的数量与强度,并促进了活性中间物(-NH2)的生成.表面 Lewis 酸在低温 SCR 反应起主要作用,并且发现-NH2也是活性很高的物种.在 NH3低温催化还原 NO 的反应中,一步浸渍法制备的催化剂活性最高.
参考文献
[1] | Phil HH;Reddy MP;Kumar PA;Ju LK;Hyo JS .SO2 resistant antimony promoted V2O5/TiO2 catalyst for NH3-SCR of NOx at low temperatures[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2008(3/4):301-308. |
[2] | Schneider H;Scharf U;Wokaun A;Baiker A .[J].Journal of Catalysis,1994,146:545. |
[3] | 郭静,李彩亭,路培,崔华飞,彭敦亮,文青波.CeO2改性MnOx/Al2O3的低温SCR法脱硝性能及机制研究[J].环境科学,2011(08):2240-2246. |
[4] | 侯亚芹,黄张根,马建蓉,郭士杰.V_2O_5/ACF催化剂低温下选择性催化还原NO的机理[J].催化学报,2009(10):1007-1011. |
[5] | Zhao Q S;Sun L S;Liu Y;Su S Xiang J Hu S .[J].J Central South Univ of Technol,2011,18:1883. |
[6] | Ramis G;Yi L;Busca G;Turco M Kotur E Willey R J .[J].Journal of Catalysis,1995,157:523. |
[7] | Irfan M F;Qurashi A;Alam M W .[J].Arabian Journal For Science and Engineering,2010,35:79. |
[8] | Fabrizioli P;Burgi T;Baiker A .[J].Journal of Catalysis,2002,206:143. |
[9] | Richter M;Trunschke A;Bentrup U;Brzezinka K W Schreier E Schneider M Pohland M M Fricke R .[J].Journal of Catalysis,2002,206:98. |
[10] | Morales MR;Barbero BP;Cadus LE .Combustion of volatile organic compounds on manganese iron or nickel mixed oxide catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(1/2):1-10. |
[11] | Pe?a D A;Uphade B S;Smirniotis P G .[J].Journal of Catalysis,2004,221:421. |
[12] | Kapteijn F;Singoredjo L;Andreini A;Moulijn T A .[J].Applied Catalysis B:Environmental,1994,3:173. |
[13] | 徐海涛,金保昇,张亚平,孙克勤,汪小蕾.MnOx/TiO2催化剂的制备及其低温NH3选择性催化还原NO性能[J].东南大学学报(自然科学版),2012(03):463-467. |
[14] | Wu Z B;Jiang B Q;Liu Y;Zhao W R Guan B H .[J].Journal of Hazardous Materials,2007,145:488. |
[15] | Qi G S;Yang R T;Chang R .[J].Catalysis Letters,2003,87:67. |
[16] | 唐晓龙,郝吉明,易红宏,宁平,李俊华.活性炭改性整体催化剂上低温选择性还原NOx[J].中国环境科学,2007(06):845-850. |
[17] | Shen B X;Liu T;Zhao N;Ma J Hao X C .[J].Advances in Materials Research,2011,383-390:1945. |
[18] | Chen Z H;Wang F R;Li H;Yang Q Wang L F Li X H .[J].Industrial and Engineering Chemistry Research,2012,51:202. |
[19] | Liu F D;He H;Ding Y;Zhang C B .[J].Applied Catalysis B:Environmental,2009,93:194. |
[20] | 李雪辉,李华,高翔,陈志航,杨青,王芙蓉,王乐夫.共沉淀法制备Cr-Mn复合氧化物及其低温催化还原NOx性能[J].催化学报,2011(03):477-482. |
[21] | Wu Z B;Jiang B Q;Liu Y .Appl Catal B,2008,79:34722陈志航,李雪辉,高翔,江燕斌,吕扬效,王芙蓉,王乐夫[J].催化学报,2009,30:4. |
[22] | Wu B J;Liu X Q;Xiao P;Wang S G .[J].Chemical Research in Chinese Universities,2008,24:615. |
[23] | 张亚平,赵晓媛,孙克勤,沈凯,徐海涛,周长城.负载型钼氧化物催化剂NH3选择性催化还原NOx[J].东南大学学报(自然科学版),2011(05):1030-1035. |
[24] | Nova I;Lietti L;Tronconi E;Forzatti P .[J].Catalysis Today,2000,60:73. |
[25] | Chen J P;Yang R T .[J].Applied Catalysis A:General,1992,80:135. |
[26] | 张亚平,汪小蕾,孙克勤,沈凯,徐海涛,周长城.W03对MnOx/TiO2低温脱硝SCR催化剂的改性研究[J].燃料化学学报,2011(10):782-786. |
[27] | Zhang Y P;Zhao X Y;Xu H T;Shen K Zhou C C Jin B S Sun K Q .[J].Journal of Colloid and Interface Science,2011,361:212. |
[28] | Kenevey K;Morris M A;Cunningham J;Ferrand G .[J].Key Engineering Materials,1996,118-119:303. |
[29] | Qi G S;Yang R T;Chang R .[J].Applied Catalysis B:Environmental,2004,51:93. |
[30] | Wu Z B;Jiang B Q;Liu Y;Wang H Q Jin R B .[J].Environmental Science and Technology,2007,41:5812. |
[31] | Li J H;Chen J J;Ke R;Luo C K Hao J M .[J].Catalysis Communications,2007,8:1896. |
[32] | Sun C Z;Zhu J;Lv Y Y;Qi L Liu B Gao F Sun K Q Dong L Chen Y .[J].Applied Catalysis B:Environmental,2011,103:206. |
[33] | Naito N;Katada N;Niwa M .[J].Journal of Physical Chemistry B,1999,103:7206. |
[34] | Larrubia M A;Ramis G;Busca G .[J].Applied Catalysis B:Environmental,2000,27:145. |
[35] | Alejandre A G;Ramirez J;Busca G .[J].Langmuir,1998,14:630. |
[36] | Lietti L;Ramis G;Berti F;Toledo G Robba D Busca G Forzatti P .[J].Catalysis Today,1998,42:101. |
[37] | Tsiganenko A A;Pozdnyakov D V;Filimonv V N .[J].Journal of Molecular Structure,1975,29:299. |
[38] | Ramis G;Busca G;Bregani F;Forzatti P .[J].Applied Catalysis,1990,64:259. |
[39] | Lietti L;Aemany J L;Forzatti P;Busca G Ramis G Giamello E Bregani F .[J].Catalysis Today,1996,29:143. |
[40] | Busca G;Lietti L;Ramis G;Berti F .[J].Applied Catalysis B:Environmental,1998,18:1. |
[41] | Kobayashi M;Miyoshi K .WO3-TiO2 monolithic catalysts for high temperature SCR of NO by NH3: Influence of preparation method on structural and physico-chemical properties, activity and durability[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2007(3/4):253-261. |
[42] | Vittadini A;Casarin M;Selloni A .[J].Journal of Physical Chemistry B,2005,109:1652. |
[43] | Tops?e N Y;Tops?e H;Dumesic J A .[J].Journal of Catalysis,1995,151:226. |
[44] | Schneider H;Tschudin S;Schneider M;Wokaun A Baiker A .[J].Journal of Catalysis,1994,147:5. |
[45] | Zhu J;Gao F;Dong L H;Yu W J Qi L Wang Z Dong L Chen Y .[J].Applied Catalysis B:Environmental,2010,95:144. |
[46] | 陈亮,李俊华,葛茂发,马磊,常化振.CeO2-WO3复合氧化物催化剂的NH3-SCR反应机理[J].催化学报,2011(05):836-841. |
[47] | Kijlstra WS.;Smit HI.;Poels EK.;Bliek A.;Brands DS. .MECHANISM OF THE SELECTIVE CATALYTIC REDUCTION OF NO BY NH3 OVER MNOX/AL2O3 .2. REACTIVITY OF ADSORBED NH3 AND NO COMPLEXES[J].Journal of Catalysis,1997(1):219-230. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%