期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 8, 期 31, 页码 11477-11490出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c00335
关键词
Levulinic acid/ester; Hydrogenation; 2-Methyltetrahydrofuran; Bimetallic copper/nickel catalyst; Nonpolar solvent
资金
- Natural Science Foundation of Jiangsu Province [BK20191391]
- Qing Lan Project of Jiangsu Province
- Fundamental Research Funds for the Central Universities [JZ2018HGBZ0100]
A highly efficient bimetallic Cu-Ni catalytic system for selective hydrogenation of levulinic acid/ester to 2-methyltetrahydrofuran (2-MTHF) promoted by the solvent was presented. A 98% yield of 2-MTHF was achieved with optimal 10Cu-SNi/Al2O3 catalyst at a mild temperature in the presence of nonpolar organic solvent n-hexane and molecular hydrogen. A mechanistic study revealed a synergistic effect between Cu and Ni nanoparticles, wherein Ni primarily activated H-2 and hydrogenated levulinic acid/ester to GVL and Cu facilitated the hydrogenation of GVL to 2-MTHF. Detailed studies on solvent effects revealed that the n-hexane possessed higher H 2 dissolvability and enhanced adsorption of GVL on the catalyst surface to facilitate its conversion to 2-MTHF, providing a lower apparent activation energy barrier of 48.9 kJ/mol for the rate-determining step. DFT calculations also indicated a highest adsorption energy of GVL with Al2O3 over other substrates and solvent molecules, further highlighting the promotion effect of nonpolar n-hexane solvent.
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