电化学表面增强拉曼光谱揭示的用于定制反应途径的核壳结构电催化剂的自我重构

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Zhixuan Lu, Yajun Huang, Ningyu Chen, Chuan Liu, Xiang Wang* and Bin Ren*, 
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引用次数: 0

摘要

电催化剂在电催化反应过程中会发生结构重构,并伴随着催化活性和选择性的显著变化。然而,要同时跟踪原位结构演变和反应过程,以进一步弄清表面重构的起源及其与电催化性能的相关性,仍然具有挑战性。我们利用参与甲酸电氧化反应(FAER)的物种作为探针分子,采用电化学表面增强拉曼光谱(EC-SERS)揭示了金核铂壳纳米粒子(Au@Pt NPs)的表面重构过程。通过电位依赖性拉曼特征,我们清楚地揭示了在 FAER 过程中,金核中的金原子可以迁移到超薄铂壳中。重要的是,原位 SERS 光谱显示,Au@Pt NPs 的重构源于电催化过程中产生的 CO。我们进一步发现,这种结构转变降低了 CO 在铂表面的结合强度,并调整了 FAER 的反应路径,从而使甲酸直接脱氢为 CO2 的路径缩短了 2.6 倍。这项工作证明了电催化剂在反应过程中的结构演变对催化性能的重要性,为设计高效、稳健的电催化剂提供了启示。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Self-Reconstruction of Core–Shell Structured Electrocatalysts for Tailoring Reaction Pathways Revealed by Electrochemical Surface-Enhanced Raman Spectroscopy

Self-Reconstruction of Core–Shell Structured Electrocatalysts for Tailoring Reaction Pathways Revealed by Electrochemical Surface-Enhanced Raman Spectroscopy

Self-Reconstruction of Core–Shell Structured Electrocatalysts for Tailoring Reaction Pathways Revealed by Electrochemical Surface-Enhanced Raman Spectroscopy

The electrocatalysts undergo structural reconstruction during electrocatalytic reactions, accompanied by significant variations in the catalytic activity and selectivity. However, it is still challenging to track in situ structural evolution and reaction process simultaneously to further figure out the origin of the surface reconstruction and its correlation to the electrocatalytic performance. By utilizing the species involved in formic acid electrooxidation reaction (FAER) as probe molecules, we employed electrochemical surface-enhanced Raman spectroscopy (EC-SERS) to reveal that the surface reconstruction process occurred on Au core-Pt shell nanoparticles (Au@Pt NPs). Via potential-dependent Raman features, we clearly revealed that the Au atoms from the Au core can migrate to the ultrathin Pt shell during FAER. Importantly, in situ SERS spectra showed that the reconstruction of Au@Pt NPs originated from the CO produced during the electrocatalytic process. We further showed that this structural transformation reduces the CO binding strength on Pt surfaces and tailors the reaction pathways of the FAER, thus facilitating the pathway of direct dehydrogenation of formic acid to CO2 by 2.6 times. This work demonstrates the importance of structural evolution of electrocatalysts during the reaction process to the catalytic performance, providing insight for designing highly efficient and robust electrocatalysts.

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来源期刊
ACS Catalysis
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.
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