探索二氧化碳电还原过程中电池配置对铜催化剂重构的影响

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2024-09-27 DOI:10.1038/s41467-024-52692-w
Woong Choi, Younghyun Chae, Ershuai Liu, Dongjin Kim, Walter S. Drisdell, Hyung-suk Oh, Jai Hyun Koh, Dong Ki Lee, Ung Lee, Da Hye Won
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摘要

采用铜催化剂的膜电极组件(MEA)电池可通过二氧化碳还原反应(CO2RR)有效生成 C2+ 化学品。然而,MEA 配置对 CO2RR 过程中 Cu 催化剂不可避免的重构所产生的影响仍未得到充分探索,尽管其对 CO2RR 的功效具有相当大的潜在影响。在此,我们证明了与 H 型电池相比,MEA 电池能促使 Cu 发生独特的重构,进而影响 CO2RR 的结果。我们利用三种基于铜的催化剂(特别设计了不同的纳米结构),确定了 H 型细胞和 MEA 细胞在生产 C2+ 化学品方面截然不同的选择性趋势。操作X射线吸收光谱以及两种细胞类型的原位分析表明,与H型细胞相比,MEA细胞促进了Cu2O的还原,从而改变了Cu表面。通过 Operando 分析支持的时间分辨 CO2RR 研究进一步突出表明,MEA 细胞内大量的铜重构是导致 CO2RR 失活转化为 C2+ 化学品的主要因素。
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Exploring the influence of cell configurations on Cu catalyst reconstruction during CO2 electroreduction

Membrane electrode assembly (MEA) cells incorporating Cu catalysts are effective for generating C2+ chemicals via the CO2 reduction reaction (CO2RR). However, the impact of MEA configuration on the inevitable reconstruction of Cu catalysts during CO2RR remains underexplored, despite its considerable potential to affect CO2RR efficacy. Herein, we demonstrate that MEA cells prompt a unique reconstruction of Cu, in contrast to H-type cells, which subsequently influences CO2RR outcomes. Utilizing three Cu-based catalysts, specifically engineered with different nanostructures, we identify contrasting selectivity trends in the production of C2+ chemicals between H-type and MEA cells. Operando X-ray absorption spectroscopy, alongside ex-situ analyses in both cell types, indicates that MEA cells facilitate the reduction of Cu2O, resulting in altered Cu surfaces compared to those in H-type cells. Time-resolved CO2RR studies, supported by Operando analysis, further highlight that significant Cu reconstruction within MEA cells is a primary factor leading to the deactivation of CO2RR into C2+ chemicals.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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