TY - JOUR
T1 - Selective valorization of 5-hydroxymethylfurfural to 2,5-diformylfuran using atmospheric O2 and MAPBBr3 perovskite under visible light
AU - Zhang, Mo
AU - Li, Zheng
AU - Xin, Xing
AU - Zhang, Junhao
AU - Feng, Yeqin
AU - Lv, Hongjin
N1 - Publisher Copyright:
© 2020 American Chemical Society
PY - 2020/12/18
Y1 - 2020/12/18
N2 - 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 (MAPbBr3, MA = methylammonium) is utilized as a photocatalyst for selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) using atmospheric O2 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 O2, photogenerated electrons (e−), holes (h+), •O2−, and 1O2 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.
AB - 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 (MAPbBr3, MA = methylammonium) is utilized as a photocatalyst for selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) using atmospheric O2 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 O2, photogenerated electrons (e−), holes (h+), •O2−, and 1O2 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.
KW - 5-hydroxymethylfurfural
KW - Atmospheric O
KW - Heterogeneous photocatalysis
KW - Lead-halide perovskite
KW - Selective oxidation
KW - Visible-light irradiation
UR - http://www.scopus.com/inward/record.url?scp=85097756755&partnerID=8YFLogxK
U2 - 10.1021/acscatal.0c04330
DO - 10.1021/acscatal.0c04330
M3 - Article
AN - SCOPUS:85097756755
SN - 2155-5435
VL - 10
SP - 14793
EP - 14800
JO - ACS Catalysis
JF - ACS Catalysis
IS - 24
ER -
