期刊
ACS CATALYSIS
卷 10, 期 24, 页码 14793-14800出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04330
关键词
lead-halide perovskite; heterogeneous photocatalysis; atmospheric O-2; 5-hydroxymethylfurfural; selective oxidation; visible-light irradiation
资金
- National Natural Science Foundation of China [21871025, 21831001]
- Recruitment Program of Global Experts (Young Talents)
- BIT Excellent Young Scholars Research Fund
Selective production of value-added platform chemicals from renewable biomass feedstocks and their derivatives has attracted tremendous attention with high potential in addressing global problems of energy and sustainability. In this work, a lead-halide perovskite ( MAPbBr(3), MA = methylammonium) is utilized as a photocatalyst for selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) using atmospheric O-2 upon visible-light irradiation. Under minimally optimized conditions, the photocatalytic conversion of HMF in acetonitrile solvent reaches 100% with a DFF selectivity of over 90%, achieving an overall furanic carbon yield of over 96%. A detailed catalytic mechanism was proposed based on various spectroscopic and experimental results, revealing that the atmospheric O-2, photogenerated electrons (e(-)), holes (h(+)), O-center dot(2)-, and O-1(2) species together play crucial roles in the effective and selective photo-oxidation of HMF to DFF. In addition, our present photocatalytic system is also applicable for photo-oxidation of benzyl alcohol with approximately 100% conversion and benzaldehyde selectivity, providing insights for future exploration of the present catalytic system.
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