4.6 Article

Linear paired electrochemical valorization of glycerol enabled by the electro-Fenton process using a stable NiSe2 cathode

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NATURE CATALYSIS
卷 5, 期 8, 页码 716-725

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NATURE PORTFOLIO
DOI: 10.1038/s41929-022-00826-y

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资金

  1. National Science Foundation (NSF) [CHE-1955074]
  2. NSF [TG-CHE120088]
  3. National Institutes of Health [S10 OK012245]
  4. NSF through the University of Wisconsin Materials Research Science and Engineering Center [DMR-1720415]
  5. Water Science and Engineering Laboratory at UW-Madison
  6. DOE Office of Science [DE-AC02-06CH11357]

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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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