采用简单的水热/溶剂热法,经后续在氮气气氛中的热处理合成了三维花型 Co-Ni/C 双金属催化剂,它由交织炭片构成,金属纳米颗粒高度分散其中.随着 Co/Ni 摩尔比的增加,金属颗粒的粒径逐渐从26 nm 减至4 nm 左右.将该催化剂用于邻氯硝基苯选择性加氢制备邻氯苯胺反应,其催化活性最高为单金属催化活性的2倍.这是由于 Co 和 Ni 物种之间存在协同效应.氢气程序升温脱附结果显示, Co/Ni 合金的生成使得 Co50Ni50/C 催化剂产生了新的催化活性位,因而其活性显著提高.
Three dimensional flower-like Co-Ni/C bimetallic catalysts composed of interlaced carbon flakes with highly dispersed metal nanoparticles were synthesized by a facile hydrothermal/solvothermal process followed by a heat treatment in flowing N2. The sizes of the metal nanoparticles were from 26 to 4 nm, which became smaller as the Co/Ni molar ratio increased. The catalytic activities for the selective hydrogenation of o-chloronitrobenzene to o-chloroaniline were tested. The conversion of o-chloronitrobenzene over the bimetallic Co-Ni/C catalysts was increased by up to 200% compared with that over a mono-metallic Co/C catalyst, which was due to a synergistic interaction between the Co and Ni species. Hydrogen temperature-programmed desorption results showed that new active sites were formed in the Co50Ni50/C catalyst due to the formation of a Co-Ni alloy, which gave the improved activity of the Co50Ni50/C catalyst.
参考文献
[1] | Ferrando R;Jellinek J;Johuston R L .[J].Chemical Reviews,2008,108:845. |
[2] | Zafeiratos S;Piccinin S;Teschner D .[J].Catalysis Science and Technology,2012,2:1787. |
[3] | Sun K Q;Hong Y C;Zhang G R;Xu B Q .[J].ACS Catal,2011,1:1336. |
[4] | Lim B;Jiang M J;Camargo P H C;Cho E C Tao J Lu X M Zhu Y M Xia Y N .[J].Science,2009,324:1302. |
[5] | Francis S A;Bergens S H .[J].Journal of Power Sources,2011,196:7470. |
[6] | Yao K;Cheng Y F .[J].Journal of Power Sources,2007,173:96. |
[7] | Burc R .[J].Accounts of Chemical Research,1982,15:24. |
[8] | Maroun F;Ozanam F;Magnussen OM;Behm RJ .The role of atomic ensembles in the reactivity of bimetallicelectrocatalysts[J].Science,2001(5536):1811-1814. |
[9] | Li H S;Xu H;Wang J F .[J].Journal of Natural Gas Chemistry,2011,20:1. |
[10] | Xiang M L;Wu D D;Zou J;Li D B Sun Y H She X C .[J].Journal of Natural Gas Chemistry,2011,20:520. |
[11] | 孙海杰,郭伟,周小莉,陈志浩,刘仲毅,刘寿长.非晶态合金Ru基催化剂在苯选择加氢中的应用进展[J].催化学报,2011(01):1-16. |
[12] | Yang B.;Lu QY.;Wang Y.;Zhuang L.;Lu JT.;Liu PF. .Simple and low-cost preparation method for highly dispersed PtRu/C catalysts[J].Chemistry of Materials,2003(18):3552-3557. |
[13] | Nashner M S;Frenkel A I;Adler D L;Shapley J R Nuzzo R G .[J].Journal of the American Chemical Society,1997,119:7760. |
[14] | He C N;Zhao N Q .[J].Journal of Materials Chemistry,2012,22:1297. |
[15] | 李海涛,陈昊然,张因,高春光,赵永祥.炭包覆氧化铝负载镍催化剂的制备和表征及其催化加氢性能[J].催化学报,2011(01):111-117. |
[16] | Takanabe K;Nagaoka K;Nariai K;Aika K .[J].Journal of Catalysis,2005,232:268. |
[17] | 严新焕,孙军庆,徐颖华,杨建峰.Ni-Co-B非晶态合金催化剂用于氯代硝基苯液相加氢制氯代苯胺[J].催化学报,2006(02):119-123. |
[18] | Hossain MM;Sedor KE;de Lasa HI .Co-Ni/Al2O3 oxygen carrier for fluidized bed chemical-looping combustion: Desorption kinetics and metal-support interaction[J].Chemical Engineering Science,2007(18/20):5464-5472. |
[19] | Ishihara T;Eguchi K;Arai H .[J].Applied Catalysis,1987,30:225. |
[20] | Ishihara T;Horiuchi N;Inoue T;Eguchi K Takita Y Arai H .[J].Journal of Catalysis,1992,136:232. |
[21] | Li P;Liu J;Nag N;Crozier PA .In situ preparation of Ni-Cu/TiO2 bimetallic catalysts[J].Journal of Catalysis,2009(1):73-82. |
[22] | Xu L P;Ding Y S;Chen C H;Zhao L L Rimkus C Joesten R Suib S L .[J].Chemistry of Materials,2008,20:308. |
[23] | Guan J G;Liu L J;Xu L L;Sun Z G Zhang Y .[J].Crystal Engineering Communications,2011,13:2636. |
[24] | Ren Y;Gao L .[J].Journal of the American Ceramic Society,2010,93:3560. |
[25] | Xing L;Qiu J S;Liang C H;Wang C Mao L .[J].Journal of Catalysis,2007,250:369. |
[26] | Abdelsayed V;Aljarash A;El-Shall M S;Al Othman Z A Alghamdi A H .[J].Chemistry of Materials,2009,21:2825. |
[27] | 周敏,林国栋,张鸿斌.多壁碳纳米管负载铂的甲苯加氢脱芳催化剂[J].催化学报,2007(03):210-216. |
[28] | Zhang J G;Wang H;Dalai A K .[J].Journal of Catalysis,2007,249:300. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%