In-situ/operando study of Cu-based nanocatalysts for CO2 electroreduction using electrochemical liquid cell TEM.

IF 4.2 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Frontiers in Chemistry Pub Date : 2025-01-30 eCollection Date: 2025-01-01 DOI:10.3389/fchem.2025.1525245
Jiawei Wan, Qiubo Zhang, Ershuai Liu, Yi Chen, Jiana Zheng, Amy Ren, Walter S Drisdell, Haimei Zheng
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Abstract

The structure of a nanocatalyst during electrocatalytic reactions often deviates from its pristine structure due to intrinsic properties, or physical and chemical adsorption at the catalytic surfaces. Taking Cu-based catalysts for CO2 electroreduction reactions (CO2RR) as an example, they often experience segregation, leaching, and alloying during reactions. With the recent breakthrough development of high-resolution polymer electrochemical liquid cells, in-situ electrochemical liquid cell transmission electron microscopy (EC-TEM) alongside other advanced microscopy techniques, has become a powerful platform for revealing electrocatalysts restructuring at the atomic level. Considering the complex reactions involving electrified solid-liquid interfaces and catalyst structural evolution with intermediates, systematic studies with multimodal approaches are crucial. In this article, we demonstrate a research protocol for the study of electrocatalysts structural evolution during reactions using the in-situ EC-TEM platform. Using Cu and CuAg nanowire catalysts for CO2RR as model systems, we describe the experimental procedures and findings. We highlight the platform's crucial role in elucidating atomic-scale pathways of nanocatalyst restructuring and identifying catalytic active sites, as well as avoiding potential artifacts to ensure unbiased conclusions. Using the multimodal characterization toolbox, we provide the opportunity to correlate the structure of a working catalyst with its performance. Finally, we discuss advancements as well as the remaining gap in elucidating the structural-performance relationship of working catalysts. We expect this article will assist in establishing guidelines for future investigations of complex electrochemical reactions, such as CO₂RR and other catalytic processes, using the in-situ EC-TEM platform.

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利用电化学液体电池TEM对cu基纳米催化剂CO2电还原的原位/操作研究。
在电催化反应中,纳米催化剂的结构往往由于其固有性质或催化表面的物理和化学吸附而偏离其原始结构。以cu基催化剂用于CO2电还原反应(CO2RR)为例,它们在反应过程中经常发生偏析、浸出和合金化。随着高分辨率聚合物电化学液体电池的突破性发展,原位电化学液体电池透射电子显微镜(EC-TEM)与其他先进的显微镜技术一起,已经成为揭示电催化剂在原子水平上重组的强大平台。考虑到涉及带电固液界面和催化剂结构演变的复杂反应,采用多模态方法进行系统研究至关重要。在本文中,我们展示了一种利用原位EC-TEM平台研究反应过程中电催化剂结构演变的研究方案。以Cu和CuAg纳米线催化剂为模型体系,描述了实验过程和结果。我们强调该平台在阐明纳米催化剂重组的原子尺度途径和识别催化活性位点以及避免潜在的人工产物以确保公正的结论方面的关键作用。使用多模态表征工具箱,我们提供了将工作催化剂的结构与其性能相关联的机会。最后,我们讨论了在阐明工作催化剂的结构-性能关系方面的进展和仍然存在的差距。我们希望这篇文章将有助于为未来使用原位EC-TEM平台研究复杂的电化学反应(如CO₂RR和其他催化过程)建立指导方针。
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来源期刊
Frontiers in Chemistry
Frontiers in Chemistry Chemistry-General Chemistry
CiteScore
8.50
自引率
3.60%
发文量
1540
审稿时长
12 weeks
期刊介绍: Frontiers in Chemistry is a high visiblity and quality journal, publishing rigorously peer-reviewed research across the chemical sciences. Field Chief Editor Steve Suib at the University of Connecticut is supported by an outstanding Editorial Board of international researchers. This multidisciplinary open-access journal is at the forefront of disseminating and communicating scientific knowledge and impactful discoveries to academics, industry leaders and the public worldwide. Chemistry is a branch of science that is linked to all other main fields of research. The omnipresence of Chemistry is apparent in our everyday lives from the electronic devices that we all use to communicate, to foods we eat, to our health and well-being, to the different forms of energy that we use. While there are many subtopics and specialties of Chemistry, the fundamental link in all these areas is how atoms, ions, and molecules come together and come apart in what some have come to call the “dance of life”. All specialty sections of Frontiers in Chemistry are open-access with the goal of publishing outstanding research publications, review articles, commentaries, and ideas about various aspects of Chemistry. The past forms of publication often have specific subdisciplines, most commonly of analytical, inorganic, organic and physical chemistries, but these days those lines and boxes are quite blurry and the silos of those disciplines appear to be eroding. Chemistry is important to both fundamental and applied areas of research and manufacturing, and indeed the outlines of academic versus industrial research are also often artificial. Collaborative research across all specialty areas of Chemistry is highly encouraged and supported as we move forward. These are exciting times and the field of Chemistry is an important and significant contributor to our collective knowledge.
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