Ru nanoparticles deposited on ultrathin TiO2 nanosheets as highly active catalyst for levulinic acid hydrogenation to γ-valerolactone

被引：59
|
作者：
Gao, Xiaoqing [1 ,2 ]
Zhu, Shanhui [1 ]
Dong, Mei [1 ]
Wang, Jianguo [1 ]
Fan, Weibin [1 ]
机构：
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100039, Peoples R China
来源：
APPLIED CATALYSIS B-ENVIRONMENTAL | 2019年 / 259卷
基金：
中国国家自然科学基金;
关键词：
Ru; TiO2; nanosheets; Levulinic acid; Hydrogenation; gamma-Valerolactone; AQUEOUS-PHASE HYDROGENATION; SELECTIVE HYDROGENATION; TEMPERATURE HYDROGENATION; RUTHENIUM CATALYSTS; ANATASE TIO2; CONVERSION; SUPPORT; EFFICIENT; CU; FABRICATION;
D O I：
10.1016/j.apcatb.2019.118076
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：
Highly efficient synthesis of valuable y-valerolactone (GVL) by levulinic acid (LA) hydrogenation is still a challenge for Ru-based catalysts under mild condition. In this work, we have reported that ultrathin TiO2 nanosheets supported Ru nanoparticles showed extraordinarily high catalytic activity, GVL yield (99.1%) and reusability owing to the formation of Ru-O-Ti interfacial structure. The turnover frequency (TOF) reached as high as 19,045 h(-1) at 100 degrees C, much higher than those of Ru/SiO2, Ru/GO, Ru/MoS2, and commercial Ru/C. DFT calculation elucidates that the dominant reaction pathway of LA hydrogenation to GVL is preferentially hydrogenated to CH3CHOCH2CH2COOH*, followed by cyclization to CH3(OH)C4OH4OH* (GVL - OH) and final dehydroxylation, irrespective of surface structure. Compared to Ru (0 0 2) facet, Ru/TiO2 interfacial structure changes the rate-determining step from initial hydrogenation to cyclization, which greatly declines the activation barrier from 0.81 eV to 0.48 eV.
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页数：8
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