期刊
ACS CATALYSIS
卷 -, 期 -, 页码 7926-7935出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02068
关键词
ethyl levulinate; gamma-valerolactone; Ni3P catalyst; hydrogenation; in situ FTIR
资金
- National Natural Science Foundation of China [22178195]
- National Key Research and Development Program of China [2018YFB0604804]
- Petro-China Innovation Foundation [2016D-5007-0507]
- Tsinghua National Laboratory for Information Science and Technology
Developing non-noble metal catalysts with high activity and selectivity for biomass conversion is important yet challenging. In this study, a series of Ni-xP/Al2O3 catalysts with different P/Ni molar ratios were prepared for the conversion of ethyl levulinate to gamma-valerolactone. The developed Ni-0.38P/Al2O3 catalyst exhibited 5.4 times higher activity than the conventional Ni/Al2O3 catalyst and outperformed existing non-noble metal catalysts. The unique catalytic performance was attributed to the formation of Ni3P phase, as identified through various characterizations.
It is important but challenging to develop non-noble metal catalysts with high activity and selectivity for biomass conversion. The activation of C=O bond is a crucial step in biomass upgradation. Herein, a series of Ni-xP/Al2O3 catalysts with different P/Ni molar ratios were prepared for the conversion of ethyl levulinate to gamma-valerolactone. The developed Ni-0.38P/Al2O3 catalyst was 5.4 times more active than conventional Ni/Al2O3 based on turnover frequency and significantly outperformed the state-of-the-art non-noble metal catalysts. The unique catalytic performance was ascribed to the formation of Ni3P phase, which was identified by several characterizations. The results of DFT calculation and characterization by XPS and CO-FTIR revealed that electron was transferred from Ni to P with the formation of Ni delta+ sites. In situ FTIR for the surface reaction indicated that Ni delta+ acted as a new active site to activate the C=O bond, which rendered the high intrinsic activity of Ni3P for the C=O hydrogenation of EL.
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