Efficient Methanol Oxidation Kinetics Enabled by an Ordered Heterocatalyst with Dual Electric Fields.

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of the American Chemical Society Pub Date : 2025-02-12 Epub Date: 2025-01-30 DOI:10.1021/jacs.4c16885
Tian Liu, Qing-Xia Chen, Zhen He, Jin-Long Wang, Si-Zhe Sheng, Jian-Wei Liu, Shu-Hong Yu
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Abstract

Induced by a sharp-tip-enhanced electric field, periodical nanoassemblies can regulate the reactant flux on the electrode surface, efficiently optimizing the mass transfer kinetics in electrocatalysis. However, when the nanoscale building blocks in homoassemblies are arranged densely, it results in the overlap and reduction of the local electric field. Herein, we present a comprehensive kinetic heteromodel that simultaneously couples the sharp-tip-enhanced electric field and charge transfer electric field between different building blocks with any arrangement densities. The dual electric fields drive the diffusion of reactants from the bulk solution to the electrode surface, significantly enhancing mass transfer kinetics along the horizontal and longitudinal directions, which promotes the electrocatalytic activity significantly. Moreover, the wide generality of the model is further confirmed by electrochemical experiments involving various electrocatalytic systems and catalysts. Therefore, this work highlights the significant role of dual electric fields in electrocatalysis, which is expected to facilitate the development of customized and outstanding catalysts in the future.

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双电场有序异催化剂实现甲醇高效氧化动力学。
在尖尖增强电场的诱导下,周期性纳米组件可以调节电极表面的反应物通量,有效地优化电催化过程中的传质动力学。然而,当纳米级结构块在同质组装体中密集排列时,会导致局部电场的重叠和减小。在此,我们提出了一个综合的异质动力学模型,该模型可以同时耦合任何排列密度的不同构建块之间的尖尖增强电场和电荷转移电场。双电场驱动反应物从本体溶液向电极表面扩散,显著增强了横向和纵向传质动力学,显著提高了电催化活性。此外,涉及各种电催化体系和催化剂的电化学实验进一步证实了该模型的广泛性。因此,这项工作强调了双电场在电催化中的重要作用,有望促进未来定制和优秀催化剂的开发。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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