Highly Selective Synthesis of 1,4-Butanediol via Hydrogenation of Succinic Acid with Supported Cu-Pd Alloy Nanoparticles

被引:52
作者
Le, Son D. [1 ]
Nishimura, Shun [1 ]
机构
[1] JAIST, Grad Sch Adv Sci & Technol, 1-1 Asahidai, Nomi, Ishikawa 9231292, Japan
关键词
1,4-butanediol; gamma-butyrolactone; hydrogenation; succinic acid; CuPd alloy; LEVULINIC ACID; AQUEOUS HYDROGENATION; BIMETALLIC CATALYSTS; GAMMA-BUTYROLACTONE; DIMETHYL OXALATE; PARTICLE-SIZE; HAP CATALYST; NO REDUCTION; HYDROXYAPATITE; BIOMASS;
D O I
10.1021/acssuschemeng.9b04447
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Hydroxyapatite (HAP)-supported Cu-Pd catalysts, denoted as Cu-Pd/HAP, have been discovered to be the efficient catalysts for hydrogenation of bioderived succinic acid in which the products are selectively tunable by adjusting the mixing ratio of Cu and Pd. Optimal performance toward 1,4-butanediol (BDO) is observed with Cu-Pd/HAP prepared with 8 wt %-Cu and 2 wt %-Pd, affording a selectivity of 82% at quantitative conversion. In contrast, the monometallic Cu and Pd catalysts are unable to produce BDO as the major product, but only gamma-butyrolactone (GBL) with a low yield of 16% and butyric acid (BA) with a considerable yield of 78%, respectively, is formed. The formation of well-dispersed bimetallic alloy nanoparticles is revealed by transmission electron microscopy with energy-dispersive spectroscopy, H-2-temperature programmed reduction, X-ray diffraction, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy studies. It is concluded that the fine alloying structure with high Cu contents is significant in favoring the formation of BDO via the ring-opening step of GBL rather than the hydrogenation of GBL to the nontarget product of BA. In addition, the CuPd alloy catalyst exhibits good recycling ability in four consecutive runs without significant loss in its activity.
引用
收藏
页码:18483 / 18492
页数:19
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