Regulating Intermediate Adsorption and Promoting Charge Transfer of CoCr-LDHs by Ce Doping for Enhancing Electrooxidation of 5-Hydroxymethylfurfural

IF 13 2区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Small Pub Date : 2025-01-14 DOI:10.1002/smll.202409343

Ling Ding, Zewen Shen, Hao Pan, Yana Chen, Yezi Hu, Guixia Zhao, Guangtong Hai, Xiubing Huang

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Abstract

Electrochemical oxidation of 5-hydroxymethylfurfural (HMFOR) to generate high-value chemicals under mild conditions acts as an energy-saving and sustainable strategy. However, it is still challenging to develop electrocatalysts with high efficiency and good durability. Here, nickel foam (NF) supported CoCrCe(7.5%)-LDH (layered double hydroxides) by doping Ce into CoCr-LDH show high 5-hydroxymethylfurfural (HMF) conversion (99%), 2,5-furandicarboxylic acid (FDCA) yield (99%), and Faraday efficiency (100%) at 1.4 V_RHE. The CoCrCe(7.5%)-LDH also exhibits remarkable stability with 97% conversion of HMF after 10 cycles. The X-ray absorption near-edge spectroscopy (XANES) and theoretical calculation show that Ce doping into CoCr-LDH is beneficial to the formation of high-valance Co and significantly facilitates the electron transfer, regulates the adsorption behavior of intermediates, reduces the Gibbs free energy barrier and accelerates the reaction rate. This work promotes the use of rare earth elements as electrocatalysts to promote the oxidation of HMF.

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在温和条件下对 5-羟甲基糠醛（HMFOR）进行电化学氧化以生成高价值化学品是一种节能和可持续发展的策略。然而，开发高效、耐用的电催化剂仍具有挑战性。在这里，通过在 CoCr-LDH 中掺杂 Ce，以泡沫镍 (NF) 为支撑的 CoCrCe(7.5%)-LDH（层状双氢氧化物）在 1.4 VRHE 下显示出较高的 5-hydroxymethylfurfural (HMF) 转化率（99%）、2,5-呋喃二甲酸 (FDCA) 产率（99%）和法拉第效率（100%）。CoCrCe(7.5%)-LDH 还表现出显著的稳定性，10 个循环后 HMF 的转化率达到 97%。X 射线吸收近边光谱（XANES）和理论计算表明，在 CoCr-LDH 中掺入 Ce 有利于形成高价位 Co，并能显著促进电子转移，调节中间产物的吸附行为，降低吉布斯自由能垒，加快反应速率。这项工作促进了稀土元素作为电催化剂在促进 HMF 氧化过程中的应用。

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来源期刊

Small 工程技术-材料科学：综合

CiteScore

17.70

自引率

3.80%

发文量

1830

审稿时长

2.1 months

期刊介绍： Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments. With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology. Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.