糠醛
催化作用
化学
双功能
环戊酮
羟甲基
有机化学
路易斯酸
药物化学
作者
Qiang Deng,Ru Zhou,Yongchao Zhang,Xiang Li,Jiahui Li,Shaobo Tu,Guan Sheng,Jun Wang,Zheling Zeng,Tatchamapan Yoskamtorn,Edman Tsang
标识
DOI:10.1002/anie.202211461
摘要
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., Ti3 AlC2 , Ti2 AlC, Ti3 SiC2 ) supporting Pd catalysts were fabricated, which showed high catalytic activity; Pd/Ti3 AlC2 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 °C.
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