Ionic liquids modified electrochemical interfaces for enhanced biomass valorization

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2025-07-17 DOI:10.1016/j.jcat.2025.116330

Xinyu Liu, Jiansong Wang, He Li, Xiaoliang Qu, Yipu Xu, Liu-Liu Shen, Gui-Rong Zhang, Donghai Mei

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引用次数: 0

Abstract

Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) offers a sustainable route for biomass valorization. The technoeconomic viability of this promising route, however, hinges on developing efficient electrocatalysts. Moving beyond conventional structural engineering of catalysts, we introduce a surface modification strategy using a small amount of hydrophobic ionic liquids (ILs) to adjust the local electrochemical microenvironment. Specifically, by modifying a porous conductive metal organic framework (Ni-HHTP) with [MTBD][NTf₂], the FDCA yield and Faradaic efficiency (FE) are significantly enhanced to 99.9% and 97.0%, respectively, along with a threefold increase in FDCA production rate compared to the unmodified catalyst. Mechanistic studies reveal that the ILs facilitate HMF enrichment at the catalyst surface while preventing water-induced blockage of active sites. This work highlights the transformative potential of interfacial engineering with ILs as a versatile strategy for advancing electrocatalytic systems in biomass conversion applications.

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离子液体修饰电化学界面以增强生物质增值

5-羟甲基糠醛（HMF）的电化学氧化生成2,5-呋喃二羧酸（FDCA）为生物质增值提供了一条可持续的途径。然而，这条有前途的路线的技术经济可行性取决于开发高效的电催化剂。超越传统的催化剂结构工程，我们引入了一种使用少量疏水离子液体（ILs）来调整局部电化学微环境的表面改性策略。具体来说，通过用[MTBD][NTf2]修饰多孔导电金属有机骨架（Ni-HHTP）， FDCA产率和法拉第效率（FE）分别显著提高到99.9%和97.0%，FDCA产率比未修饰的催化剂提高了三倍。机理研究表明，ILs促进HMF在催化剂表面的富集，同时防止水引起的活性位点堵塞。这项工作强调了界面工程的变革潜力，作为推进生物质转化应用中的电催化系统的通用策略。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.