化工学报 ›› 2015, Vol. 66 ›› Issue (9): 3476-3482.DOI: 10.11949/j.issn.0438-1157.20150861

• 催化、动力学与反应器 • 上一篇    下一篇

H2S为毒物对乙炔氢氯化反应中AuCl3/AC催化剂催化活性的影响

代斌, 张春丽, 康丽华, 朱明远   

  1. 石河子大学化学化工学院, 新疆兵团化工绿色过程重点实验室, 新疆 石河子 832003
  • 收稿日期:2015-06-09 修回日期:2015-07-06 出版日期:2015-09-05 发布日期:2015-09-05
  • 通讯作者: 代斌
  • 基金资助:

    国家自然科学基金项目(21366027)。

Poisoning effect of H2S on catalytic performance of AuCl3/AC in acetylene hydrochlorination

DAI Bin, ZHANG Chunli, KANG Lihua, ZHU Mingyuan   

  1. School of Chemistry and Chemical Engineering of Shihezi University, Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi 832003, Xinjiang, China
  • Received:2015-06-09 Revised:2015-07-06 Online:2015-09-05 Published:2015-09-05
  • Supported by:

    supported by the National Natural Science Foundation of China (21366027).

摘要:

采用等体积浸渍法制备了1% AuCl3/AC催化剂,探究了硫化氢(H2S)为毒物对乙炔氢氯化反应中催化剂催化活性的影响及失活机理。催化活性测试结果表明,以H2S为毒物可导致乙炔氢氯化反应中的AuCl3/AC催化剂的失活,且是一个不可逆过程;程序升温还原(TPR)和X射线光电子能谱(XPS)分析结果表明,H2S的加入可有效地加快Au3+还原为Au0;透射电镜能谱(TEM-EDX)观测分析形成的Au-S化合物也可导致催化剂失活,即随着H2S量的增大,更多的Au3+被还原为Au0,且形成的Au-S化合物覆盖在活性位点,使有效的活性组分降低进而导致AuCl3/AC催化剂失活。

关键词: H2S, AuCl3/AC, 催化, 失活机理, 乙炔氢氯化

Abstract:

A study about poisoning effect of hydrogen sulfide (H2S) on the catalytic performance of AuCl3/AC during acetylene hydrochlorination deactivation is described and discussed. 1% AuCl3/AC catalyst is prepared by an incipient wetness impregnation technique. The activity tests demonstrate that H2S poisoning results in the rapid and irreversible deactivation of AuCl3/AC catalyst in acetylene hydrochlorination. Temperature-programmed reduction (TPR) and X-ray photoelectron spectra (XPS) show that H2S addition can effectively accelerate active Au3+ reduction to metallic Au0. The formation of metal sulfide may also be another reason for catalyst deactivation in the presence of H2S, which is supported by transmission electron microscopy (TEM) and energy dispersion X-ray spectrometer (EDX) techniques. In other words, with the increase of H2S added to the feed gases, the content of Au3+ is greatly reduced to metallic Au0. Moreover, the active sites are covered with Au-S compound. Both of them could reduce the effective active component, leading to the deactivation of the AuCl3/AC catalyst.

Key words: H2S, AuCl3/AC, catalysis, deactivation mechanism, acetylene hydrochlorination

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