Retreat in Order to Advance: Dual-Electrode Refinery of 5-Hydroxymethylfurfural toward 2,5-Furandicarboxylic Acid with High Carbon Efficiency

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-03-27 DOI:10.1021/acscatal.5c01243

Zhuxin Gui, Yingshuai Jia, Wenbiao Zhang, Ying Liang, Yizhong Chen, Tianlan Yan, Qingsheng Gao, Yahong Zhang, Yi Tang

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Abstract

Electro-refinery of 5-hydroxymethylfurfural (HMF) is an ecofriendly route to upgrade biomass feedstock under ambient conditions, producing high-value-added 2,5-furandicarboxylic acid (FDCA) and 2,5-bis(hydroxymethyl)furan (BHMF). However, FDCA electrosynthesis suffers from serious carbon loss due to HMF self-polymerization in the conventional alkaline electrolyte, emphasizing the protection of HMF via hydrogenation to robust BHMF for subsequent oxidation. Herein, dual-electrode HMF tandem refinery (DEHTR) integrated via cathodic protection and anodic oxidation, as the strategy of “retreat in order to advance” for FDCA electrosynthesis, was proposed. We developed a series of Cu-based cathodic/anodic catalysts by the alternating electrochemical treatments of copper foam, precisely regulating the active site amount/structure to accomplish the efficient HMF electro-hydrogenation (90.3% HMF conversion, 94.3% BHMF selectivity, and 86.3% FE) as well as BHMF electro-oxidation (99.3% FDCA yield and 95.5% FE). On this basis, DEHTR was finely constructed over an optimized Cu-based cathode/anode, which was expanded to a membrane-free flow electrolysis system, acquiring a higher FDCA yield and a carbon balance of 95.1% (vs 65.2% in direct HMF electro-oxidation) even at a large HMF concentration (100 mM). Moreover, gram-scale FDCA powder with 99.1% purity was simply separated from the DEHTR flow system. This work sheds light on the development of biomass electro-refinery with high carbon efficiency by collaboratively integrating dual-electrode procedures on cost-efficient electrocatalysts.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.