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

doi:10.11949/j.issn.0438-1157.20150861

Abstract

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

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

CLC Number:

TQ028.8

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.

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.

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

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

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