Insights into the electrochemical oxidation selectivity of hydroxymethylfurfural over humin-layered Au nanoparticles

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-05-07 DOI:10.1016/j.jcat.2024.115542

Bohyeon Kim , Kunli Yang , Kylie Park , Joseph Cline , Ryan Thorpe , Christopher J. Kiely , Steven McIntosh

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Abstract

Au nanoparticle catalysts are promising electrocatalysts for biomass upgrading. Starting from a pristine Au electrode, herein we demonstrate a simple route for the electrochemical preparation of Au NPs supported on thin layers of humin (Au/H). Utilizing an oxidized Au surface as a precursor, these electrocatalytic structures are formed upon reduction of 5-hydroxymethylfurfural (HMF) in alkaline media while performing a potential sweep. We subsequently utilize this Au/H structure for the electrochemical oxidation of ethanol and HMF in a rotating disk electrode (RDE) configuration and perform additional analysis via electrochemical surface-enhanced Raman Scattering (SERS). The RDE test reveals Au/H has different reaction kinetics towards alcohol and aldehyde functional groups, enabling a mechanistic understanding of the reaction pathway for HMF oxidation. The SERS experiment identifies the favorable reduction pathway from Au₂O₃ to gold, suggesting the possible active site on this catalyst for HMF oxidation.

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透视羟甲基糠醛在腐植酸层金纳米粒子上的电化学氧化选择性

金纳米粒子催化剂是一种很有前景的生物质升级电催化剂。从原始金电极开始，我们在本文中展示了一条在腐殖质薄层（Au/H）上支撑金纳米粒子的电化学制备的简单路线。利用氧化金表面作为前驱体，在碱性介质中还原 5-hydroxymethylfurfural (HMF)，同时进行电位扫描，就能形成这些电催化结构。随后，我们利用这种 Au/H 结构在旋转盘电极（RDE）配置中对乙醇和 HMF 进行电化学氧化，并通过电化学表面增强拉曼散射（SERS）进行了额外的分析。RDE 测试表明，Au/H 对醇和醛官能团具有不同的反应动力学，从而从机理上了解了 HMF 氧化的反应途径。SERS 实验确定了从 Au2O3 到金的有利还原途径，表明该催化剂上可能存在 HMF 氧化的活性位点。

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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.