Atomically dispersed Pd catalysts for the selective hydrogenation of succinic acid to γ-butyrolactone

被引:41
作者
Zhang, Chi [1 ]
Chen, Lifang [1 ]
Cheng, Hongye [1 ]
Zhu, Xuedong [1 ]
Qi, Zhiwen [1 ]
机构
[1] East China Univ Sci & Technol, State Key Lab Chem Engn, Sch Chem Engn, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金;
关键词
Atomically dispersed; Palladium; Selective hydrogenation; Succinic acid; Atom activity; AQUEOUS-PHASE HYDROGENATION; AEROBIC OXIDATION; PALLADIUM; CLUSTERS; ALUMINA; SURFACE; GOLD; 1,4-BUTANEDIOL; SUPPORTS; BIOMASS;
D O I
10.1016/j.cattod.2016.01.028
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Heterogeneous palladium catalysts with high atom-efficiency offer practical value for selective hydrogenation. Here, we prepared atomically dispersed Pd species supported on gamma-AlOOH nanosheets (Pd/gamma-AlOOH), which contain clusters and dominated single atoms. Even with an extremely low amount of Pd loading, the catalytic activity of 0.1 Pd/gamma-AlOOH leads to 50.3% of succinic acid conversion at 4h. At the time, the succinic acid conversion reaches 90.7% and 97.1%, and the selectivity to gamma-butyrolactone is high up to 96.9% and 93.8% over 0.5 Pd/gamma-AlOOH and 1.0 Pd/gamma-AlOOH , respectively. The supported Pd single atom (Pd-1/gamma-AlOOH ) Exhibits 30- and 1100-fold increase in the catalytic activity compared with the supported clusters Pd-13/gamma-AlOOH and Pd-55/gamma-AlOOH for the selective hydrogenation of succinic acid to gamma-butyrolactone, respectively. Analysis of the structural properties confirms that Pd single atoms on gamma-AlOOH (0 1 0) surface have high adsorption energy, which is in agreement with catalytic efficiency. In addition, Pd single atoms in the catalyst 0.2 Pd/gamma-AlOOH account for 86.6% of the overall catalytic activity and can serve as the most efficient catalytic active sites. (C) 2016 Published by Elsevier B.V.
引用
收藏
页码:55 / 61
页数:7
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