期刊
JOURNAL OF CATALYSIS
卷 365, 期 -, 页码 153-162出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2018.06.030
关键词
Green preparation; H2O2/HCl mixture; Au/AC; Surface chemistry; Ethyne hydrochlorination
资金
- National Natural Science Foundation of China (NSFC) grant No. 21606199, 21476207) [21606199, 21476207]
Gold on activated carbon (Au/AC) materials are promising alternative catalysts for ethyne hydrochlorination. The preparation of active, stable Au/AC catalysts without aqua regia for ethyne hydrochlorination remains a significant challenge. A novel catalyst preparation protocol involving impregnation using a H2O2/HCl mixture is established for highly active Au/AC catalysts comprising primarily of single-site cationic Au species, as identified by systematic X-ray photoelectron spectroscopy (XPS), temperature programmed reduction (TPR) analyses and transmission electron microscopy (TEM) imaging. In addition, evaluation of the Au-C interface by temperature-programmed desorption (TAD) analyses showed that the oxidation of activated carbon by the H2O2/HCl mixture, which creates surface oxygen-containing functional groups (SOGs), is a crucial step for the formation of active Au/AC catalysts. The structure determination and comprehensive experimental evidence allow density functional theory (DFT) to predict that single-site cationic AuCl species stabilized by SOGs via -O- linkages are efficient active sites for Au-catalyzed ethyne hydrochlorination. In addition, these catalysts can be reused for several times with negligible changes in performance after treatment with the H2O2/HCl mixture. The H2O2/HCl mixture is thus envisioned as a viable, green alternative to toxic aqua regia for the preparation of Au/AC catalysts for ethyne hydrochlorination. (C) 2018 Elsevier Inc. All rights reserved.
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