期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 318, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121842
关键词
Biomass conversion; Biobased fuel; Hydrogenolysis; Supported Pd catalyst; 5-(Chloromethyl)furfural (CMF)
资金
- National Key R & D Pro- gram of China [2021YFC2101604]
- National Natural Science Foundation of China [21978248]
- Guangdong Provincial Key Research and Development Program [2020B0101070001]
- Natural Science Foundation of Fujian Province of China [2019J06005]
The synthesis of renewable transportation fuel 2,5-dimethylfuran (DMF) from biomass was studied. It was found that the in-situ generation of acidic species and Pd-Cl active sites showed high selectivity and activity towards hydrogenolysis of biomass-derived 5-(chloromethyl)furfural (CMF) to DMF. The method achieved a 92% DMF yield from CMF in 15 minutes, with a space-time-yield at least one order of magnitude higher than previous literature using 5-hydroxymethylfurfural (HMF) as substrate.
The synthesis of renewable transportation fuel 2,5-dimethylfuran (DMF) from biomass is a promising solution for efficient alleviating the dependence on the petroleum-derived commodities. Here, we found that in-situ gener-ation of acidic species and Pd-Cl active sites bring high selectivity and activity towards hydrogenolysis of biomass-derived 5-(chloromethyl)furfural (CMF) to DMF. Gratifyingly, 92% DMF yield was achieved from CMF for 15 min, which indicates that space-time-yield is at least one order of magnitude higher than previous literature employed 5-hydroxymethylfurfural (HMF) as substrate. Kinetic studies showed that the in-situ formed acid has ignorable negative effect on polymerization of substrate to humins. DFT explicitly elucidate that the decorated Pd nanoparticles by Cl species provided lower adsorption energy and energy of C-O cleavage than Pd sites. Furthermore, the strategy of in-situ formation of homogeneous acid and halogen-modified metal is also efficient for catalytic conversion of other chlorinated carboxides to hydrocarbons with the ring intact.
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