Construction of highly dispersed Au active sites by ice photochemical polishing for efficient acetylene hydrochlorination

被引:4
|
作者
Yao, Lisha [1 ]
Zhang, Haiyang [1 ]
Li, Yanqin [1 ]
Zhang, Miaomiao [1 ]
Li, Feng [1 ]
Li, Linfeng [1 ]
Zhang, Jinli [1 ,2 ]
机构
[1] Shihezi Univ, Key Lab Green Proc Chem Engn Xinjiang Bingtuan, Sch Chem & Chem Engn, Shihezi 832000, Peoples R China
[2] Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
VINYL-CHLORIDE MONOMER; GRAPHITIC CARBON; GOLD CATALYSTS; PERFORMANCE; STABILITY;
D O I
10.1039/d1nj05120b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Considering the economic and environmental advantages of water as a solvent and the drawbacks of Au catalysts prepared in an aqueous solution for acetylene hydrochlorination, such as easy aggregation of active components, insufficient active sites, and serious carbon deposition, supported gold catalysts were prepared by using an ice photochemical method (liquid nitrogen freezing and UV light irradiation). The appropriate ice-photochemical treatment results in ice lattice formation, which inhibits gold nuclei formation during the catalyst preparation and catalytic reaction. In addition, it limits the crystal phase change and aggregation of active species. The freezing and the energy absorbed by the gold component under irradiation at the exact wavelengths may produce a plasma effect on the surface of the Au component and promote the excitation of outer electrons of the Au nucleus to Cl, suppressing the transition of the dispersed atomic active species with a high valence state to the inert Au-0 clusters. Therefore, the superior activity of the prepared catalysts Au/AC-F1I1 is probably caused by the synergistic adsorption and activation of reactants by the highly dispersed AuClx-like multi-sites, facilitating the rapid electrophilic addition reaction and impeding the carbon deposition, thus promoting the continuous exposure of active sites. The significantly improved activity and stability, and the environment-friendly preparation strategy provide new inspiration for the design and application of Au-based catalysts for acetylene hydrochlorination.
引用
收藏
页码:3738 / 3746
页数:9
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