Mo对猝冷Ni-Mo骨架催化剂结构和催化性能的影响

化学学报 ›› 2004, Vol. 62 ›› Issue (14): 1281-1286. 上一篇下一篇

Mo对猝冷Ni-Mo骨架催化剂结构和催化性能的影响

胡华荣¹, 王友臻¹, 乔明华¹, 范康年¹, 宗保宁², 张晓昕², 李和兴³

1. 复旦大学化学系, 上海市分子催化和创新材料重点实验室, 上海, 200433;
2. 石油化工科学研究院, 北京, 100083;
3. 上海师范大学化学系, 上海, 200233

投稿日期:2003-08-12 修回日期:2004-03-23 发布日期:2014-02-17
通讯作者: 范康年,E-mail:knfan@fudan.edu.cn;乔明华,E-mail:mhqiao@fudan.edu.cn E-mail:knfan@fudan.edu.cn;mhqiao@fudan.edu.cn
基金资助:
"973"国家重点基础研究发展规划(No.G2000048009)、国家自然科学基金(Nos.20203004,20073008)和上海市自然科学基金(No.02ZA14006)资助项目.

Effect of Mo on the Structure and Catalytic Behavior of the Rapidly Quenched Skeletal Ni-Mo Catalysts

HU Hua-Rong¹, WANG You-Zhen¹, QIAO Ming-Hua¹, FAN Kang-Nian¹, ZONG Bao-Ning², ZHANG Xiao-Xin², LI He-Xing³

1. Shanghai Key Laboratory of Molecular Catalysis & Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433;
2. Research Institute of Petroleum Processing, Beijing 100083;
3. Department of Chemistry, Shanghai Normal University, Shanghai 200233

Received:2003-08-12 Revised:2004-03-23 Published:2014-02-17

文章分享

摘要/Abstract

采用猝冷法制备了不同Mo含量的Ni-Mo-Al合金,经碱处理活化后得到猝冷Ni-Mo骨架催化剂.以ICP,N2物理吸附,XRD,H2-TPD等手段对合金及催化剂的物化性质进行了表征.结果表明,随着Mo含量的增加,合金中依次出现Ni₁₆Mo₁₀Al₇₄,MoAl₃物相,同时NiAl₃相减少,Ni₂Al₃相增加.Mo的存在使合金中更多的铝被抽提,减少了催化剂中残留的Ni₂Al₃物相,催化剂的比表面积、平均孔径、孔容和晶粒尺寸均随Mo含量增加而减小.将催化剂用于2-乙基蒽醌加氢反应,发现Mo加快了反应速率,同时抑制了降解产物的产生.在催化剂中Mo含量达到2.47 wt%时,双氧水的得率可达到100%.结合Ni晶粒大小、表面吸附氢状态、Mo的化学态,进一步讨论了Mo对猝冷Ni-Mo骨架催化性能的修饰作用.

关键词: 猝冷合金, Ni-Mo-Al, Ni-Mo, 2乙基蒽醌, H₂O₂

A series of rapidly quenched skeletal Ni-Mo catalysts with different Mo contents were prepared by alkali leaching of Ni-Mo-Al alloys derived from the single-roller melt-spinning method.It was revealed that the addition of Mo not only alters the phase compositions of the Ni-Mo-Al alloys, but also has pronounced influence on the physical characters of the leached Ni-Mo catalysts.In liquid phase hydrogenation of 2-ethylanthraquinone, it was found that Mo can accelerate the hydrogenation while depress the formation of the degradation products.The yield of H₂O₂ reaches as high as ca.100% at a Mo content of 2.47 wt% in the catalyst.The positive effect of Mo on the catalytic behavior was rationalized in terms of the nickel crystallite size, the population of the surface hydrogen species, and the chemical states of Mo.

Key words: rapidly quenched alloy, Ni-Mo-Al,Ni-Mo, 2-ethylanthraquinone, H₂O₂

引用此文

胡华荣, 王友臻, 乔明华, 范康年, 宗保宁, 张晓昕, 李和兴. Mo对猝冷Ni-Mo骨架催化剂结构和催化性能的影响[J]. 化学学报, 2004, 62(14): 1281-1286.

HU Hua-Rong, WANG You-Zhen, QIAO Ming-Hua, FAN Kang-Nian, ZONG Bao-Ning, ZHANG Xiao-Xin, LI He-Xing. Effect of Mo on the Structure and Catalytic Behavior of the Rapidly Quenched Skeletal Ni-Mo Catalysts[J]. Acta Chimica Sinica, 2004, 62(14): 1281-1286.

导出引用 EndNote|Reference Manager|ProCite|BibTeX|RefWorks

分享此文

参考文献

[1] Robertson, S. D.; Anderson, R. B. J. Catal. 1976, 41,405.
[2] Lee, H. K.; Jung, E. E.; Lee, J. S. Mater. Chem. Phys.1998, 55, 89.
[3] Masson, J.; Cividino, P.; Court, J. Appl. Catal. A 1997,161, 191.
[4] Montgomery, S. R. In Catalysis of Organic Reactions, Marcel Dekker, New York, 1981, p. 393.
[5] Gallezot, P.; Cerino, P. J.; Blanc, B.; Fleche, G.; Fuertes, P. J. Catal. 1994, 146, 93.
[6] Gros, J.; Hamer-Thibault, S.; Joud, J. C. J. Mater. Sci. 1989, 24, 2987.
[7] Liu, B.; Qiao, M. H.; Deng, J. F.; Fan, K. N.; Zhang, X. X.; Zong, B. N. J. Catal. 2001, 204, 512.
[8] Hu, H.-R.; Pei, Y.; He, Y.-G.; Xie, S.-H.; Jiang, H.W.; Fan, K.-N.; Qiao, M.-H.; Zong, B.-N.; Zhang, X.-X. J. Fudan Univ. 2002, 41,466 (in Chinese).(胡华荣,裴燕,何永根,谢颂海,姜慧文,范康年,乔明华,宗保宁,张晓昕,复旦大学学报,2002,41,466.)
[9] Wang, D.-L.; Wang, X.-K.; Ba, F.-H.; Shen, N.-F. J.Zhengzhou Univ. Technol. 2000, 21, 37 (in Chinese).(王东立,王西科,巴发海,沈宁福,郑州工业大学学报,2000, 21, 37. )
[10] Lei, H.; Song, Z.; Tan, D.-L.; Bao, X.-H.; Mu, X.-H.; Zong, B.-N.; Min, E.-Z. Chem. J. Chin. Univ. 2002, 23,2121 (in Chinese).(雷浩,宋真,谭大力,包信和,慕旭宏,宗保宁,闵恩泽,高等学校化学学报,2002,23,2121.)
[11] Zhang, H.-F.; Li, J.; Song, Q.-H.; Wang, J.-T. Mater. Sci. Prog. 1993, 7, 225 (in Chinese).(张海峰,李杰,宋启洪,王景唐,材料科学进展,1993,7,225. )
[12] Lu, Z.-L.; Wang, R.; Ke, J.; Chen, H.; Mu, X.-H.; Zong, B.-N. Chin. J. Catal. 1997, 18, 110 (in Chinese).(陆致龙,王蓉,柯俊,陈桦,慕旭宏,宗保宁,催化学报,1997,18,110.)
[13] Chen, X.-M.; Zhang, G.-S.; Wang, X.-K.; Shen, N.-F. J. Zhengzhou Univ. Technol. 1999, 20, 57 (in Chinese).(陈向明,张国胜,王西科,沈宁福,郑州工业大学学报,1999,20,57.)
[14] Highfield, J. G.; Oguro, K.; Grushko, B. Electrochim. Acta 2001, 47, 465.
[15] Taylor, A.; Doyle, N. J. J. Appl. Crystallogr. 1972, 5,210.
[16] Liu, B. Ph. D. Dissertation, Fudan University, Shanghai, 2003(in Chinese).(刘波,博士学位论文,复旦大学,上海,2003.)
[17] Serra, M.; Salagre, P.; Cesteros, Y.; Medina, F.; Sueiras, J.E. J. Catal. 2002, 209,202.
[18] Mikhailenko, S. D.; Khodareva, T. A.; Leongardt, E. V.; Lyashenko, A. I.; Fasman, A. B. J. Catal. 1993, 141,688.
[19] Wang, B.; Yang, L.-M.; Suo, J.-S. Acta Chim. Sinica 2003, 61, 285 (in Chinese).(王波,杨立明,索继栓,化学学报,2003,61,285.)
[20] Dai, W.-L.; Yu, H.-K.; Deng, J.-F.; Jiang, A.-R. ActaChim. Sinica 1995, 53, 188 (in Chinese).(戴维林,俞宏坤,邓景发,蒋安仁,化学学报,1995,53,188. )
[21] Drelinkiewicz, A. J. Mol. Catal. A 1995, 101, 61.
[22] Mikailenko, S. D.; Fasman, A. B.; Maksinova, N. A.; Leongard, E. V. Appl. Catal. 1984, 12, 141.