期刊
NATURE CATALYSIS
卷 5, 期 8, 页码 716-725出版社
NATURE PORTFOLIO
DOI: 10.1038/s41929-022-00826-y
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资金
- National Science Foundation (NSF) [CHE-1955074]
- NSF [TG-CHE120088]
- National Institutes of Health [S10 OK012245]
- NSF through the University of Wisconsin Materials Research Science and Engineering Center [DMR-1720415]
- Water Science and Engineering Laboratory at UW-Madison
- DOE Office of Science [DE-AC02-06CH11357]
This study establishes an efficient cathodic valorization method for glycerol into high-value chemicals using the electro-Fenton process at a stable NiSe2 cathode. The proof-of-concept linear paired electrochemical process achieves high selectivity and conversion of glycerol into the same oxidation products at both NiSe2 cathode and Pt anode.
Electrochemical valorization of surplus biomass-derived feedstocks, such as glycerol, into high-value chemicals offers a sustainable route for utilization of biomass resources and decarbonization of chemical manufacturing; however, glycerol is typically valorized solely via anodic oxidation, with lower-value products such as hydrogen gas generated at the cathode. Here, we establish the efficient cathodic valorization of glycerol to the desirable C-3 oxidation products via the electro-Fenton process at a stable NiSe2 cathode, built upon the theoretical understanding and experimental demonstration of the high selectivity and stability of NiSe2 toward acidic H2O2 electrosynthesis. A proof-of-concept linear paired electrochemical process for concurrent valorization of glycerol into the same oxidation products at both NiSe2 cathode and Pt anode achieves high selectivity for value-added C-3 products and high glycerol conversion with little external energy input needed, when the electro-Fenton generation of hydroxyl radicals is carefully controlled. This conceptual strategy of linear pairing is generalizable for enabling atom-efficient electro-refinery of diverse biomass-derived feedstocks.
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