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

IF 5.1 Q1 POLYMER SCIENCE ACS Macro Letters Pub Date : 2024-09-12 DOI:10.1016/j.scib.2024.09.013

Yuanqing He, Chongyang Ma, Shiheng Mo, Chung-Li Dong, Wei Chen, Shuo Chen, Huan Pang, Ren Zhi Ma, Shuangyin Wang, Yuqin Zou

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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.

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单釉质 MnO2 纳米片与脉冲电催化相结合，用于中性电解质中的生物质电氧化。

在碱性电解质中对 5-hydroxymethylfurfural (HMFOR) 进行电化学氧化是从生物质衍生物中生产高价值化学品的一种可行策略。然而，在强碱性条件下醛基的歧化以及 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。使用中性电解质为电解提供了另一种环境，但电解质中缺乏 OH- 离子往往导致电流密度低和 FDCA 产率低。在本研究中，一种夹层结构催化剂（由封闭在单酰胺MnO2纳米片（S-Ru/MnO2）之间的Ru团簇组成）与电化学脉冲法结合使用，在中性电解质中实现了5-羟甲基糠醛到FDCA的电化学转化。脉冲电解以及 Ru 簇和 MnO2 纳米片之间的强电子传递有助于将 Ru 保持在低氧化态，从而确保高活性。由于 *OH 生成量增加，与可逆氢电极 (RHE) 相比，在 1.55 V 电压下的电流密度达到了突破性的 47 mA/cm2，在中性电解质中的 FDCA 产率高达 98.7%。这项研究提供了一种将电催化剂设计与电解技术相结合的策略，从而在中性 HMFOR 中实现了卓越的性能。

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来源期刊

ACS Macro Letters 化学-

CiteScore

10.40

自引率

3.40%

发文量

209

审稿时长

1 months

期刊介绍： ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.