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Unlocking Thermodynamic-Kinetic Synergy via Rh/Co Dual Sites and Ordered Interfacial Hydrogen-Bond Network for Efficient Biomass Electrooxidation

delete2026-07-10
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OA
AI
D
Dezhao Zhang
H
Haoyu Zhan
L
Lingling Fang
Y
Yankun Lu
Z
Zhenyu Zhao
J
Junyu Zhong
X
Xingshuai Lv
P
Pei Zhao
马兆玲 (Zhaoling Ma)
P
Peng Zhou *
张立学 cover
张立学 (Lixue Zhang)
DOI:10.1002/cey2.70310delete
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Abstract

Abstract

En 中文
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) offers a sustainable route to bio-based polymer monomers, yet its efficiency is constrained by sluggish adsorption and proton-coupled electron transfer (PCET) kinetics. Herein, we report a composite catalyst comprising amorphous RhOx anchored on cobalt-deficient Co3O4 (RhOx-Vco) that synergistically optimizes both thermodynamics and kinetics. Combined experiments and theoretical calculations unveil that RhOx and Co defects collaboratively upshift the d-band center of Co and create Rh/Co dual sites, cooperatively enhancing HMF and OH− adsorption. Concurrently, this strengthened OH− adsorption guides preferential parallel alignment of interfacial water molecules, fostering a highly connected hydrogen-bond network that accelerates PCET kinetics. Benefiting from this multi-level synergy, RhOx-Vco achieves a seven-fold higher current density at 1.40 V than pristine Co3O4, along with a high FDCA yield of 95.8% in three-electrode system. Remarkably, when integrated into a membrane electrode assembly flow electrolyzer, the system maintains excellent performance with 93.4% FDCA yield, 85.6% Faradaic efficiency, and robust cycling stability, demonstrating its practical viability. This work establishes a design paradigm integrating defect and interface engineering to coordinately regulate multi-step reaction processes, offering broad insights for advancing biomass and PCET-related electrocatalysis.
Keywords:
adsorption regulation
biomass
electrocatalysis
hydrogen bond network
synergy
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Carbon Energy cover
Carbon Energy
IF:
24.2
Papers:
925
Citations:
8.9K

Organization

O
ocean university of china
Scholars:
3.0W
Papers: 1.9W
Citations: 21
G
guangxi normal university
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1.4K
Papers: 485
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Q
qingdao university
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Papers: 1.5K
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