Ni/SiO2 catalysts derived from carbothermal reduction of nickel phyllosilicate in the hydrogenation of levulinic acid to ?-valerolactone: The efficacy of nitrogen decoration

被引:21
作者
Li, Cheng-Chia [1 ]
Hsieh, Chou-Hsun [1 ]
Lin, Yu-Chuan [1 ]
机构
[1] Natl Cheng Kung Univ, Dept Chem Engn, 1 Univ Rd, Tainan 70101, Taiwan
来源
MOLECULAR CATALYSIS | 2022年 / 523卷
关键词
Carbothermal reduction; Hydrogenation; Levulinic acid; Nickel phyllosilicate; Nitrogen; SELECTIVE HYDROGENATION; GAMMA-VALEROLACTONE; NI; AMMONIA; CONVERSION; SPECTRA; COBALT; SITES;
D O I
10.1016/j.mcat.2021.111720
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
Ni catalysts derived from the carbothermal reduction of nickel phyllosilicate were investigated and their application in the hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL) was revealed. The most effective catalyst (S3M1.5@NiPS-600) was prepared by using a sucrose-melamine mixture (molar ratio = 2:1) as the reducing agent with a proper thermal treatment (maintained at 600 degrees C for 2 h). By using S3M1.5@NiPS-600, a high GVL productivity (1387 mmol GVL/g surface Ni/h), good recyclability (4.9% loss of initial activity in five cycles), and a negligible deactivation rate were observed. The promising outcome was attributed to grafted carbon and nitrogen species on the carbothermally reduced Ni/SiO2 catalyst. Grafted carbon species improve catalyst stability whereas immobilized nitrogen species induce Ni delta+ (delta>2) with a strong Lewis acidity. Paired Ni delta+ and Ni0 sites are active in the reduction of the ketone group of LA, thereby enhancing the production of GVL.
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页数:12
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