期刊
CHEMSUSCHEM
卷 15, 期 13, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202102444
关键词
2; 5-hexanedione; furan aldehydes; heterogeneous catalysis; hydrogenolysis; ring-opening
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]
This study successfully modulated the intimacy between hydrogenation sites and acidic sites using iodine(I)-modified Pd-supported catalysts, leading to improved selectivity and yield in the synthesis of 2,5-hexanedione. Additionally, the selective synthesis of 2,5-hexanedione from 5-hydroxymethylfurfural via hydrogenolysis and subsequent ring-opening route was reported for the first time.
Currently, low intimacy between hydrogenation sites and acidic sites causes unsatisfactory catalytic activity and selectivity for the synthesis of 2,5-hexanedione from C-6 furan aldehydes (5-methylfurfural, 5-hydroxymethylfurfural). Herein, iodine(I) modification of Pd-supported catalysts (such as PdI/Al2O3 and PdI/SiO2) was investigated to modulate the hydrogenation sites and acidic sites. Unlike Pd catalysts that produced 71.4 % yield of 2-hydroxymethyl-5-methyl tetrahydrofuran via an overhydrogenation route of 5-methylfurfural, PdI catalysts showed a high efficiency for 2,5-hexanedione with 93.7 % yield by a hydrogenative ring-opening route. More importantly, the selective synthesis of 2,5-hexanedione from 5-hydroxymethylfurfural with a high yield of 50.2 % by the hydrogenolysis and subsequent ring-opening route was reported for the first time. I-modified Pd nanoparticles produced in-situ hydrogen spillover, which promoted the selective C=O hydrogenation and ring-opening steps by regulating the adsorption configuration of the reactants and the transformation of Lewis to Bronsted acidity, respectively.
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