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

doi:10.11949/j.issn.0438-1157.20150861

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

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

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/Abstract

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

中图分类号:

TQ028.8

代斌, 张春丽, 康丽华, 朱明远. 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[J]. 化工学报, 2015, 66(9): 3476-3482.

DAI Bin, ZHANG Chunli, KANG Lihua, ZHU Mingyuan. Poisoning effect of H₂S on catalytic performance of AuCl₃/AC in acetylene hydrochlorination[J]. CIESC Journal, 2015, 66(9): 3476-3482.

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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

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

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