Activated carbon supported ternary gold-cesium(I)-indium(III) catalyst for the hydrochlorination of acetylene

被引:40
|
作者
Zhao, Jia [1 ]
Zhang, Tongtong [1 ]
Di, Xiaoxia [1 ]
Xu, Jiangtao [1 ]
Gu, Shanchuan [1 ]
Zhang, Qunfeng [1 ]
Ni, Jun [1 ]
Li, Xiaonian [1 ]
机构
[1] Zhejiang Univ Technol, Ind Catalysis Inst, State Key Lab Breeding Base Green Chem Synth Tech, Hangzhou 310014, Zhejiang, Peoples R China
基金
中国国家自然科学基金;
关键词
AU/C CATALYSTS; GOLD CATALYST; MERCURY; DEACTIVATION; REGENERATION; K2PDCL4; SURFACE; AUCL3; METAL;
D O I
10.1039/c5cy00663e
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Commercialization of acetylene hydrochlorination using AuCl3 catalysts has been impeded by its poor stability. We have been studying CsCl as a promoter, which can improve acetylene hydrochlorination activity and has resistance to catalytic deactivation. In-III added to the Au-Cs-I/AC catalysts worked as efficient catalysts for the hydrochlorination of acetylene to vinyl chloride. A series of trimetallic catalysts.1AuxIn(III)4Cs(I)/AC with x = 0.5, 1, 2, 3) were prepared and assessed for their ability to promote hydrochlorination of acetylene. The enhancement of stability observed for a Au/In-III/CsI weight ratio of 1 : 1 : 4 was particularly remarkable. It delivered stable performance within the conversion of acetylene, reaching more than 92.8%, and there was only 3.7% C2H2 conversion loss after running for 50 h under the reaction conditions of a temperature of 180 degrees C and a C2H2 hourly space velocity of 1480 h(-1). Moreover, the 1Au1In(III)4Cs(I)/AC catalyst delivered stable performance with an estimated lifetime exceeding 6520 h at a C2H2 hourly space velocity of 50 h(-1). H-2-TPR, TEM, HCl-TPD, C2H2-TPD, XPS and TGA techniques were further applied to reveal the structural information on the Au-In-III -Cs-I/AC catalysts. The results reveal that the addition of InCl3 increased the electron density of Au3+ species via electron transfer from the In atoms to the Au3+ center which can increase the adsorption of hydrogen chloride and therefore improve the catalytic stability. These results demonstrate that the addition of metal additives CsCl and InCl3 results in a synergistic effect to enhance the activity and the stability of Au-based catalysts. The excellent catalytic performance of the 1Au1In(III)4Cs(I)/AC catalyst demonstrated its potential as an alternative to mercury chloride catalysts for acetylene hydrochlorination.
引用
收藏
页码:4973 / 4984
页数:12
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