湖南大学邹雨芹团队报道了单层二氧化锰纳米片约束钌簇结合脉冲电催化，在中性电解质中的生物质电氧化。相关研究成果于2024年9月12日发表在国际顶尖学术期刊《科学通报》。

在碱性电解质中，电化学氧化5-羟甲基糠醛（HMFOR）是从生物质衍生物中，生产高价值化学品的一种有前景的策略。然而，在强碱性条件下，醛基的歧化和HMF的聚合形成腐殖质，会影响2,5-呋喃二甲酸（FDCA）产品的纯度。中性电解质的使用为电解提供了一种替代环境，但电解质中缺乏OH离子通常会导致电流密度低和FDCA产量低。

该文中，结合使用一种由限制在单层MnO₂纳米片（S-Ru/MnO₂）之间的Ru簇，组成的三明治结构催化剂与电化学脉冲法，在中性电解质中实现了5-羟甲基糠醛向FDCA的电化学转化。脉冲电解和Ru簇和MnO₂纳米片之间的强电子转移，有助于将Ru保持在低氧化态，确保高活性。与可逆氢电极（RHE）相比，增加的*OH生成导致1.55 V下突破性的电流密度为47 mA/cm²，中性电解质中FDCA的产率高达98.7%。

该项工作提供了一种将电催化剂设计与电解技术相结合的策略，以在中性HMFOR中实现卓越的性能。

附：英文原文

Title: Unilamellar MnO2 nanosheets confined Ru-clusters combined with pulse electrocatalysis for biomass electrooxidation in neutral electrolytes

Author: Huan Pang, Yuqin Zou

Issue&Volume: 2024/09/12

Abstract: The electrochemical oxidation of 5-hydroxymethylfurfural (HMFOR) in alkaline electrolyte is a promising strategy for producing high-value chemicals from biomass derivatives. However, the disproportionation of aldehyde groups under strong alkaline conditions and the polymerization of HMF to form humic substances can impact the purity of 2,5-furandicarboxylic acid (FDCA) products. The use of neutral electrolytes offers an alternative environment for electrolysis, but the lack of OH ions in the electrolyte often leads to low current density and low yields of FDCA. In this study, a sandwich-structured catalyst, consisting of Ru clusters confined between unilamellar MnO2 nanosheets (S-Ru/MnO2), was used in conjunction with an electrochemical pulse method to realize the electrochemical conversion of 5-hydroxymethylfurfural into FDCA in neutral electrolytes. Pulse electrolysis and the strong electron transfer between Ru clusters and MnO2 nanosheets help maintain Ru in a low oxidation state, ensuring high activity. The increased *OH generation led to a groundbreaking current density of 47 mA/cm2 at 1.55 V vs. reversible hydrogen electrode (RHE) and an outstanding yield rate of 98.7% for FDCA in a neutral electrolyte. This work provides a strategy that combines electrocatalyst design with an electrolysis technique to achieve remarkable performance in neutral HMFOR.

DOI: 10.1016/j.scib.2024.09.013

Source: https://www.sciencedirect.com/science/article/abs/pii/S2095927324006479