Highly Durable Ruthenium Silicon Nanoalloy Robust for Electrocatalytic Reduction of Biomass-Derived Aldehydes

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-09-05 DOI:10.1021/acscatal.5c01181

Man Zhang, Nadaraj Sathishkumar, Wenhao Luo, Jinlu He, Juan Zhang, Yanheng Hao, Ke Li, Yuchen Wang, Bin Liu, Huixia Luo, Guoqing Guan*, Qian He and Kai Yan*,

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引用次数: 0

Abstract

The electrocatalytic reduction (ECR) of biomass-derived feedstocks to value-added chemicals offers a promising solution for harnessing renewable electricity and biomass-based resources. Herein, we demonstrate the development of high-performing and stable silicon-based nanoalloy catalysts for the ECR of biomass-derived aldehydes. Ruthenium silicon (RuSi) nanoalloy electrocatalysts are prepared via a solvent-free microwave pyrolysis strategy (denoted as M-RuSi) achieve nearly perfect conversion of 5-hydroxymethylfurfural (HMF) with an unprecedented 2,5-dihydroxymethylfuran selectivity of 99% at −0.6 V_RHE over 200 h durability. In situ attenuated total reflectance Fourier transform infrared spectroscopy and theoretical calculations reveal that H* active species with high coverage are generated on M-RuSi nanoalloy, and the rate-determining step is HMF adsorption (F-CHO* → F-CH₂O*) for ECR, which effectively suppresses the competing hydrogen evolution reaction. This M-RuSi nanoalloy can robustly catalyze a series of biomass aldehydes, suggesting promising practical applications.

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高度耐用的钌硅纳米合金，用于电催化还原生物质衍生的醛

生物质原料的电催化还原（ECR）为利用可再生电力和生物质资源提供了一个有前途的解决方案。在此，我们展示了高性能和稳定的硅基纳米合金催化剂的发展，用于生物质衍生醛的ECR。钌硅（RuSi）纳米合金电催化剂采用无溶剂微波热解策略制备（M-RuSi），在−0.6 VRHE条件下实现了5-羟甲基糠醛（HMF）近乎完美的转化，2,5-二羟甲基糠醛的选择性达到了前所未有的99%，耐久性超过200 h。原位衰减全反射傅立叶变换红外光谱和理论计算表明，M-RuSi纳米合金表面产生了高覆盖的H*活性物质，其速率决定步骤是对ECR的HMF吸附（F-CHO*→F-CH2O*），有效抑制了竞争性析氢反应。该M-RuSi纳米合金可以催化一系列生物质醛，具有良好的实际应用前景。

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

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.