High-density oxygen-deficient CuO induced from structural reconstruction for efficient furfural oxidation coupled with hydrogen evolution

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry Pub Date : 2025-04-24 DOI:10.1016/j.jechem.2025.04.037

Hanshuai Xu , Yun Han , Qilong Wu , Hao Chen , Xinyi Shen , Mingming Zhan , Qingzhu Shu , Xin Wang , Huajun Zheng , Lingxia Zheng , Yi Jia

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引用次数: 0

Abstract

The electrocatalytic furfural oxidation reaction (FFOR) represents an economical and promising technology to replace conventional oxygen evolution reaction, enabling the co-production of high value chemicals and H₂. Regulating the adsorption of furfural (FF) and OH⁻ species holds paramount importance in enhancing the overall performance. Herein, we have developed a unique CuO catalyst enriched with oxygen vacancies (O_v-CuO) resulting from the electrochemical reconstruction of α-Cu₂S, which demonstrates exceptional FFOR performance, with a conversion of 95.3%, near-perfect selectivity and Faraday efficiency (FE) for furoic acid (FA) at 1.475 V vs. RHE. The study provides detailed comparison of the structural evolution of different sulfide precatalysts and their impact on FFOR. Furthermore, it delves into the structure-activity relationship through a combination of characterization and theoretical calculations. The O_v-CuO not only enhances OH⁻ adsorption, changes the rate-determining step, but also reduces the reaction energy barrier toward FFOR. Additionally, a much lower cell voltage is required to coproduce FA and hydrogen in the two-electrode co-electrolysis system. This work would provide valuable insights into the reaction mechanism of FFOR on Cu based catalysts and establish guidelines for designing defective electrocatalysts for biomass conversion.

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通过结构重构诱导高密度缺氧CuO进行高效的糠醛氧化和析氢

电催化糠醛氧化反应（FFOR）是替代传统析氧反应的一种经济而有前景的技术，可实现高价值化学品和氢气的联产。调节糠醛（FF）和OH -的吸附对提高整体性能至关重要。在此，我们开发了一种独特的富含氧空位的CuO催化剂（Ov-CuO），这是由α-Cu2S的电化学重构产生的，它具有出色的FFOR性能，转化率为95.3%，与RHE相比，在1.475 V下对呋喃酸（FA）具有近乎完美的选择性和法拉第效率（FE）。本研究详细比较了不同硫化物预催化剂的结构演变及其对FFOR的影响。此外，通过表征和理论计算的结合，深入研究了构效关系。Ov-CuO不仅增强了OH -的吸附，改变了反应的速率决定步骤，而且降低了反应的能垒。此外，在双电极共电解系统中，需要更低的电池电压来共同生产FA和氢。这项工作将为FFOR在Cu基催化剂上的反应机理提供有价值的见解，并为设计有缺陷的生物质转化电催化剂提供指导。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL

CiteScore

19.10

自引率

8.40%

发文量

3631

审稿时长

15 days

期刊介绍： The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy