期刊
CHINESE JOURNAL OF CATALYSIS
卷 39, 期 10, 页码 1599-1607出版社
SCIENCE PRESS
DOI: 10.1016/S1872-2067(18)63105-5
关键词
Levulinic acid; gamma-valerolactone; Bimetallic catalyst; Hydrogenation; Dual-catalytic functionality
资金
- National Natural Science Foundation of China [51502297, 51372248, 51432009]
- Instrument Developing Project of the Chinese Academy of Sciences [yz201421]
Bimetallic nanostructures have attracted great interest as efficient catalyst to enhance activity, selectivity and stability in catalytical conversion. Herein, we report a facile one-pot carbothermal route to in-situ controllable synthesize heterogeneous bimetallic Ni3Fe NPs@C nanocatalyst. The X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy and N-2 adsorption-description results reveal that the Ni3Fe alloy nanoparticles are evenly embedded in carbon matrix. The as-prepared Ni3Fe NPs@C catalyst shows excellent selective hydrogenation catalytic performance toward the conversion of levulinic acid (LA) to gamma-valerolactone (GVL) via both direct hydrogenation (DH) and transfer hydrogenation (TH). In DH of LA, the bimetallic catalyst achieved a 93.8% LA conversion efficiency with a 95.5% GVL selectivity and 38.2 mmol g(-1) h(-1) GVL productivity (under 130 degrees C, 2MPa H-2 within 2 h), which are 6 and 40 times in comparison with monometallic Ni NPs@C and Fe NPs@C catalysts, respectively. In addition, the identical catalyst displayed a full conversion of LA with almost 100% GVL selectivity and 167.1 mmol g(-1) h(-1) GVL productivity at 180 degrees C within 0.5 h in TH of LA. Under optimal reaction conditions, the DH and TH catalytic performance of 500-Ni3Fe NPs@C(3:1) catalyst for converting LA to GVL is comparable to the state-of-the-art noble-based catalysts. The demonstrated capability of bimetallic catalyst design approach to introduce dual-catalytic functionality for DH and TH reactions could be adoptable for other catalysis processes. (C) 2018, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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