H2S预处理对Ni2P/SiO2催化剂结构及氯苯加氢脱氯性能的影响

doi:10.1016/S1872-2067(12)60595-6

催化学报 ›› 2013, Vol. 34 ›› Issue (6): 1201-1207.DOI: 10.1016/S1872-2067(12)60595-6

H₂S预处理对Ni₂P/SiO₂催化剂结构及氯苯加氢脱氯性能的影响

杨庆^a, 代吉才^b, 李克伦^a, 陈吉祥^a

a 天津大学化工学院催化科学与工程系, 天津300072;
b 河北泊头职业学院, 河北泊头062150

收稿日期:2012-12-27 修回日期:2013-04-02 出版日期:2013-06-07 发布日期:2013-06-09
通讯作者: 陈吉祥
基金资助:
天津市自然科学基金(12JCYBJC13200).

Effect of H₂S pre-treatment on structure and activity of Ni₂P/SiO₂ catalyst for hydrodechlorination of chlorobenzene

YANG Qing^a, DAI Jicai^b, LI Kelun^a, CHEN Jixiang^a

a Department of Catalysis Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
b Hebei Botou Vocational College, Botou 062150, Hebei, China

Received:2012-12-27 Revised:2013-04-02 Online:2013-06-07 Published:2013-06-09
Supported by:
This work was supported by the Natural Science Foundation of Tianjin (12JCYBJC13200).

摘要/Abstract

摘要：

采用10% H₂S/H₂对Ni₂P/SiO₂催化剂进行预处理,利用X射线衍射、电感耦合等离子发射光谱、X射线光电子能谱、CO化学吸附、H₂程序升温脱附、NH₃程序升温脱附及活性评价等方法研究了H₂S预处理对催化剂结构和氯苯加氢脱氯反应性能的影响.结果表明,即使在873K进行H₂S预处理,Ni₂P/SiO₂催化剂体相结构及Ni₂P晶粒大小没有发生变化,但导致Ni₂P晶粒表面形成了磷硫镍相(NiP_xS_y),同时使表面溢流氢数量增加.硫物种的存在不仅阻塞了部分镍中心,使催化剂表面镍中心密度降低,也导致镍中心的缺电子性进一步增加.经H₂S预处理后Ni₂P/SiO₂催化剂上氯苯加氢脱氯反应的转化频率(TOF)明显提高,这可能与催化剂表面Ni物种的缺电子性增强及溢流氢数量增多有关.

关键词: 磷化镍, 硫化氢, 电子结构, 溢流氢, 氯苯, 加氢脱氯

Abstract:

The effect of 10% H₂S/H₂ treatment on the structure of Ni₂P/SiO₂ and its activity for the hydrodechlorination of chlorobenzene was investigated using X-ray diffraction, inductively coupled plasma atomic emission spectroscopy, X-ray photoelectron spectroscopy, CO chemisorption, H₂ temperature-programmed desorption, NH₃ temperature-programmed desorption, and activity tests. The H₂S/H₂ treatment did not change the Ni₂P phase or crystallite size even at temperatures as high as 873 K. However, S species were incorporated in the surface of the Ni₂P crystallites to form surface phosphosulfide (NiP_xS_y) species, which blocked the Ni sites and induced their further electron-deficiency. H₂S/H₂ treatment also led to an increase of spilt-over hydrogen species. The treated Ni₂P/SiO₂ catalyst had higher turnover frequencies in the hydrodechlorination of chlorobenzene than the untreated catalyst. This was ascribed to the increased electron-deficiency of Ni site and a greater amount of spilt-over hydrogen species.

Key words: Nickel phosphide, Hydrogen sulfide, Electron structure, Spilt-over hydrogen, Chlorobenzene, Hydrodechlorination

杨庆, 代吉才, 李克伦, 陈吉祥. H₂S预处理对Ni₂P/SiO₂催化剂结构及氯苯加氢脱氯性能的影响[J]. 催化学报, 2013, 34(6): 1201-1207.

YANG Qing, DAI Jicai, LI Kelun, CHEN Jixiang. Effect of H₂S pre-treatment on structure and activity of Ni₂P/SiO₂ catalyst for hydrodechlorination of chlorobenzene[J]. Chinese Journal of Catalysis, 2013, 34(6): 1201-1207.

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H₂S预处理对Ni₂P/SiO₂催化剂结构及氯苯加氢脱氯性能的影响

Effect of H₂S pre-treatment on structure and activity of Ni₂P/SiO₂ catalyst for hydrodechlorination of chlorobenzene

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