期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202211461
关键词
Acidity; Frustrated Lewis Pairs; Hydrogenation; MAX Phases; Synergistic Reactions
资金
- National Natural Science Foundation of China [22178158, 52162014, 22065024, 21878138]
- Cultivating Project for Academic and Technical Leader of Key Discipline of Jiangxi Province [20212BCJ23038]
- Interdisciplinary Innovation Fund of Natural Science, NanChang University [9167-27060003-YB2101]
A series of partially oxidized MAX phase supported Pd catalysts showed excellent catalytic performance in the conversion of biomass-derived furfurals to ketones. Detailed studies revealed that in situ hydrogen spillover generates Frustrated Lewis H+-H- pairs, which play a crucial role in promoting selective C=O hydrogenation and ring opening reactions.
Currently, less favorable C=O hydrogenation and weak concerted acid catalysis cause unsatisfactory catalytic performance in the upgrading of biomass-derived furfurals (i.e., furfural, 5-methyl furfural, and 5-hydroxymethyl furfural) to ketones (i.e., cyclopentanone, 2,5-hexanedione, and 1-hydroxyl-2,5-hexanedione). A series of partially oxidized MAX phase (i.e., Ti3AlC2, Ti2AlC, Ti3SiC2) supporting Pd catalysts were fabricated, which showed high catalytic activity; Pd/Ti3AlC2 in particular displayed high performance for conversion of furfurals into targeted ketones. Detailed studies of the catalytic mechanism confirm that in situ hydrogen spillover generates Frustrated Lewis H+-H- pairs, which not only act as the hydrogenation sites for selective C=O hydrogenation but also provide acid sites for ring opening. The close intimate hydrogenation and acid sites promote bifunctional catalytic reactions, substantially reducing the reported minimum reaction temperature of various furfurals by at least 30-60 degrees C.
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