期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 7, 期 24, 页码 19556-19569出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b04645
关键词
Alloyed Cu-Ni/BC; HMF; Hydrodeoxygenation; Reaction pathway; Synergy
资金
- National Key R&D Program of China [2018YFB1501402]
- National Science Foundation of China [51576199, 51536009]
- Natural Science Foundation of Guangdong Province [2017A030308010]
- DNL Cooperation Fund, CAS [DNL180302]
- Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program [2017BT01N092]
Alloyed Cu-Ni encapsulated in carbon was prepared by loading Ni and Cu onto biochar (BC) through an initial wetness impregnation method under mild conditions. The bimetallic catalysts were exploited to perform selective hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF). 2,5-Dimethylfurfural (DMF), a promising liquid fuel/fuel additive, could be obtained from HMF with the highest yield of 93.5% under the optimized conditions. During HMF HDO, two key intermediates, 5-methylfurfural (MFF) and 2,5-dihydroxymethylfuran (DHMF), dominating two distinct conversion pathways were systematically investigated by Arrhenius kinetics analysis. In addition, the turnover frequencies (TOFs) of HDO reaction over Cu-Ni/BC corresponding with Cu amount were thoroughly discussed, finding that the electron transfer from Cu to Ni in the alloy structure was beneficial to the HDO reaction and the conversion pathways can be regulated by reaction temperature variation. Importantly, the synergy of HDO of HMF by alloyed Cu-Ni metal and Lewis acid sites from oxide NiOx were hence clarified by systematic catalyst characterizations. The Cu-Ni/BC catalyst is stable for at least five consecutive runs to obtain the stabilized 81.9% of DMF since the third run.
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