期刊
CHEMICAL ENGINEERING JOURNAL
卷 262, 期 -, 页码 1152-1160出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2014.10.071
关键词
Acetylene hydrochlorination; Au/AC; Nitrogen-modified; Urea
资金
- Natural Science Foundation of China (NSFC) [20976164, 21303163]
- National Basic Research Program of China (973 Program) [2011CB710800]
- Qianjiang Talent Project in Zhejiang Province [QJD1302011]
- Scientific Research Fund of Zhejiang Provincial Education Department [Y201328681]
Improving the durability of Au3+ catalyst is an important step in increasing its utility when performing catalyzed acetylene hydrochlorination. Using nitrogen-modified activated carbon (NAC) as support, Au/NAC1 catalyst demonstrated excellent activity and stability when compared with the undoped Au/AC1 under the conditions of 180 degrees C and 1480 h(-1) of gas hourly space velocity (C2H2 based). Moreover, the Au/NAC1 catalyst delivered a stable performance during a 300 h test with the conversion of acetylene and the selectivity of vinyl chloride both reaching more than 99.9% at C2H2 hourly space velocity 100 h(-1), which substantially exceeds the best results reported in previous literature. The removal of carboxylic groups from the activated carbon surface and the introduction of nitrogen atoms as anchor sites by thermal pretreatment with urea are preferential to stabilize the catalytic active Au3+ species and inhibit the reduction of Au3+ to Au-0 in the preparation process of Au/NAC1 catalysts. In addition, increasing the electron density of Au3+ via electron transfer from nitrogen atoms to the Au3+ center can increase the adsorption of hydrogen chloride and inhibit the reduction of Au3+ to Au-0 during acetylene hydrochlorination and hence improve the catalytic stability. The excellent catalytic performance of the Au/NAC1 catalyst demonstrated its potential as an alternative to mercury chloride catalysts for acetylene hydrochlorination. (C) 2014 Elsevier B.V. All rights reserved.
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