Li Siqi, Li Wei, Li Yizhen, Fan Guoli, Li Feng
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Beijing Yanshan Petrochemical High-Tech Co., Ltd., Sinopec Group, Beijing, 102500, P. R. China.
Chempluschem. 2017 Feb;82(2):270-279. doi: 10.1002/cplu.201600500. Epub 2016 Nov 29.
A facile and economical strategy to synthesize high surface area Mg-doped ZnAl O spinels is developed. These materials are employed as catalyst supports to prepare supported gold catalysts for the aerobic oxidation of benzyl alcohol by using molecular oxygen in the absence of additional alkali. The as-fabricated supported Au catalyst with the Mg/(Mg+Zn) molar ratio of 0.15 was found to show good catalytic activity with high benzaldehyde selectivity (>99 %) and a high turnover frequency of 5382 h . The relationship between the surface properties of the supported Au catalysts and their catalytic performances reveals that the high catalytic efficiency is mainly attributable to surface cooperative effects between the abundant basic sites and favorable active Au species, including metallic Au and cationic Au ions. A possible mechanism for selective oxidation of benzyl alcohol is tentatively proposed. Moreover, the as-fabricated supported Au catalyst could be reused at least four times without significant loss of its catalytic performance. The present finding provides a new route for designing high-performance supported noble or non-noble metal catalysts by using high surface area ZnAl O -based spinels.
开发了一种简便且经济的策略来合成高比表面积的镁掺杂锌铝氧化物尖晶石。这些材料被用作催化剂载体，以制备用于在无额外碱的情况下利用分子氧对苯甲醇进行有氧氧化的负载型金催化剂。发现所制备的镁/（镁+锌）摩尔比为0.15的负载型金催化剂表现出良好的催化活性，具有高苯甲醛选择性（>99%）和5382 h⁻¹的高周转频率。负载型金催化剂的表面性质与其催化性能之间的关系表明，高催化效率主要归因于丰富的碱性位点与有利的活性金物种（包括金属金和阳离子金离子）之间的表面协同效应。初步提出了苯甲醇选择性氧化的可能机理。此外，所制备的负载型金催化剂可以重复使用至少四次而其催化性能无明显损失。本研究结果为利用高比表面积的锌铝氧化物基尖晶石设计高性能负载型贵金属或非贵金属催化剂提供了一条新途径。
