The ligand coordination approach for improving the stability of low-mercury catalyst in the hydrochlorination of acetylene

doi:10.1016/j.cjche.2016.12.003

›› 2017, Vol. 25 ›› Issue (9): 1217-1221.DOI: 10.1016/j.cjche.2016.12.003

• Catalysis, kinetics and reaction engineering • 上一篇下一篇

The ligand coordination approach for improving the stability of low-mercury catalyst in the hydrochlorination of acetylene

Xiaolong Xu, Haihua He, Jia Zhao, Bailin Wang, Shanchuan Gu, Xiaonian Li

Institute of Industrial Catalysis of Zhejiang University of Technology, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Hangzhou 310032, China

收稿日期:2016-09-12 修回日期:2016-12-05 出版日期:2017-09-28 发布日期:2017-10-11
通讯作者: Xiaonian Li,E-mail:xnli@zjut.edu.cn
基金资助:
Supported by the National Natural Science Foundation of China (21476207) and the China Postdoctoral Science Foundation (2016M592015).

The ligand coordination approach for improving the stability of low-mercury catalyst in the hydrochlorination of acetylene

Xiaolong Xu, Haihua He, Jia Zhao, Bailin Wang, Shanchuan Gu, Xiaonian Li

Institute of Industrial Catalysis of Zhejiang University of Technology, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Hangzhou 310032, China

Received:2016-09-12 Revised:2016-12-05 Online:2017-09-28 Published:2017-10-11
Supported by:
Supported by the National Natural Science Foundation of China (21476207) and the China Postdoctoral Science Foundation (2016M592015).

摘要/Abstract

摘要： Mercuric chloride supported on activated carbon (HgCl₂/AC) is used as an industrial catalyst for the hydrochlorination of acetylene. Loss of HgCl₂ by sublimating from the surface of activated carbon causes the irreversible deactivation of mercury catalyst and environmental pollution. In this work, a ligand coordination approach based on the Principle of Hard and Soft Acids and Bases (HSAB) was employed to design more stable lowmercury catalyst. The low-mercury catalysts (4% HgCl₂ loading) were prepared by using HgCl₂ and potassium halides (KX, X=Cl, I) as precursors. The HgCl₂-4KI/AC catalyst showed best catalytic stability than HgCl₂/AC and HgCl₂-4KCl/AC in the hydrochloriantion of acetylene. HgCl₂ could form more stable complex with KI, K₂HgI₄ as the main active component of the HgCl₂-4KI/AC catalyst. The characterizations of XRD and EDX analysis illustrated that the active component of HgCl₂-4KI/AC was highly dispersed on the surface of activated carbon. The sublimation rates of HgCl₂ from the catalysts verified that the active component with larger stability constant had better thermal stability. Using Hg(Ⅱ) complexes with high stability constant as the active component may be the research direction of developing highly stable low-mercury catalyst for the hydrochlorination of acetylene.

关键词: Low-mercury catalyst, Sublimation, K₂HgI₄, Ligand coordination, Acetylene hydrochlorination

Abstract: Mercuric chloride supported on activated carbon (HgCl₂/AC) is used as an industrial catalyst for the hydrochlorination of acetylene. Loss of HgCl₂ by sublimating from the surface of activated carbon causes the irreversible deactivation of mercury catalyst and environmental pollution. In this work, a ligand coordination approach based on the Principle of Hard and Soft Acids and Bases (HSAB) was employed to design more stable lowmercury catalyst. The low-mercury catalysts (4% HgCl₂ loading) were prepared by using HgCl₂ and potassium halides (KX, X=Cl, I) as precursors. The HgCl₂-4KI/AC catalyst showed best catalytic stability than HgCl₂/AC and HgCl₂-4KCl/AC in the hydrochloriantion of acetylene. HgCl₂ could form more stable complex with KI, K₂HgI₄ as the main active component of the HgCl₂-4KI/AC catalyst. The characterizations of XRD and EDX analysis illustrated that the active component of HgCl₂-4KI/AC was highly dispersed on the surface of activated carbon. The sublimation rates of HgCl₂ from the catalysts verified that the active component with larger stability constant had better thermal stability. Using Hg(Ⅱ) complexes with high stability constant as the active component may be the research direction of developing highly stable low-mercury catalyst for the hydrochlorination of acetylene.

Key words: Low-mercury catalyst, Sublimation, K₂HgI₄, Ligand coordination, Acetylene hydrochlorination

Xiaolong Xu, Haihua He, Jia Zhao, Bailin Wang, Shanchuan Gu, Xiaonian Li. The ligand coordination approach for improving the stability of low-mercury catalyst in the hydrochlorination of acetylene[J]. , 2017, 25(9): 1217-1221.

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The ligand coordination approach for improving the stability of low-mercury catalyst in the hydrochlorination of acetylene

The ligand coordination approach for improving the stability of low-mercury catalyst in the hydrochlorination of acetylene

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