Alternative solvent to aqua regia to activate Au/AC catalysts for the hydrochlorination of acetylene

催化作用 化学 王水 X射线光电子能谱 乙炔 水溶液 无机化学 溶剂 吸附 解吸 核化学 金属 化学工程 有机化学 工程类
作者
Jia Zhao,Bolin Wang,Xiaolong Xu,Yi Yu,Shuxia Di,Hao Xu,Yuanyuan Zhai,Haihua He,Lingling Guo,Zhiyan Pan,Xiao‐Nian Li
出处
期刊:Journal of Catalysis [Elsevier BV]
卷期号:350: 149-158 被引量:69
标识
DOI:10.1016/j.jcat.2017.02.027
摘要

In this paper, we demonstrate that the less toxic, relatively safe, and recyclable organic aqua regia (OAR) can be employed as a greener alternative solvent to conventional aqua regia to activate Au/AC catalysts for the hydrochlorination of acetylene. We show that Au-based catalysts prepared with HAuCl4 as precursor can be prepared initially in water (Au(H2O)/AC). Although catalysts prepared from aqueous HAuCl4 showed poor activity, it can be significantly enhanced by catalyst activation in OAR (Au(H2O)/AC(OAR)). In contrast to the catalyst activation procedure using aqua regia (Au(aq)/AC), we demonstrate that the new activation procedure leads to both improved activity and stability of the resulting Au(H2O)/AC(OAR) catalyst. Further analyses of X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) show that the variations of Au particle size and chemical state caused by OAR treatment promote Au oxidation and high dispersion. In addition, temperature-programmed reduction (TPR) and temperature-programmed desorption (TPD) indicated that the presence of residual sulfur and nitrogen species may help stabilize the cationic Au3+ species and generate a catalyst less prone to deactivation by increasing the reduction temperature of the Au3+ species and enhancing the adsorption of hydrogen chloride over the Au(H2O)/AC(OAR) catalyst. These results suggest that OAR can be substituted for conventional solvents to activate Au/AC catalysts for the hydrochlorination of acetylene.
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