Structure-property relationships of copper modified mesoporous TiO2 materials on alkyne homocoupling reactions

被引:22
作者
Luo, Zhu [1 ]
Cetegen, Shaylin A. [2 ]
Miao, Ran [3 ]
Jiang, Ting [2 ]
Chen, Sheng-Yu [3 ]
Jafari, Tahereh [1 ]
Zhang, Yashan [3 ]
Suib, Steven L. [1 ,2 ,3 ]
机构
[1] Univ Connecticut, Inst Mat Sci, U-3136, Storrs, CT 06269 USA
[2] Univ Connecticut, Dept Chem & Biomol Engn, Storrs, CT 06269 USA
[3] Univ Connecticut, Dept Chem, U-3060, Storrs, CT 06269 USA
关键词
UCT mesoporous TiO2; Heterogeneous catalysis; Homocoupling; Supported materials; TERMINAL ALKYNES; VISIBLE-LIGHT; CATALYSTS; NANOPARTICLES; PALLADIUM; OXIDATION; HYDROXIDE; DESIGN; ROUTE; FILMS;
D O I
10.1016/j.jcat.2016.03.009
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
Three different modification (doping, solvent free, and impregnation) methods were used to obtain a series of mesoporous Cu-TiO2 materials with various copper loading amounts (0-15 mol%). The influence of the modification procedure on the physico-chemical properties was characterized by PXRD, N-2 sorption, SEM, EDX elemental mapping, and XPS techniques. The presence of copper species has been detected either in the TiO2 lattice as Cu+ (via doping methods) or on the surface of TiO2 as CuO species (via solvent free and impregnation methods). With the modification of Cu, the surface area of mesoporous Cu-TiO2 materials can be increased up to 128 m(2)/g. The catalytic activities of Cu-TiO2 materials were investigated using the alkyne-alkyne homocoupling reaction with air as the sole oxidant under mild reaction conditions without any additives. The doped Cu-TiO2 materials show the highest catalytic activity (1,4-diphenyl-1,3-butadiyne yields > 99%). The different catalytic mechanisms, active sites, and structure-property relationships of all the catalysts are discussed. Definitive features affecting the catalytic performance of the obtained Cu-TiO2 materials are the loading amounts and the states of Cu, surface area, and pore size distributions. Reusability tests were conducted on the collected sample without washing, and 74% yield was achieved even after three cycles. (C) 2016 Elsevier Inc. All rights reserved.
引用
收藏
页码:94 / 103
页数:10
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