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探究电池结构对CO电还原过程中铜催化剂重构的影响。

Exploring the influence of cell configurations on Cu catalyst reconstruction during CO electroreduction.

作者信息

Choi Woong, Chae Younghyun, Liu Ershuai, Kim Dongjin, Drisdell Walter S, Oh Hyung-Suk, Koh Jai Hyun, Lee Dong Ki, Lee Ung, Won Da Hye

机构信息

Clean Energy Research Center, Korea Institute of Science and Technology, Seoul, 02792, Republic of Korea.

Department of Energy Engineering, Gyeongsang National University, Jinju, 52725, Republic of Korea.

出版信息

Nat Commun. 2024 Sep 27;15(1):8345. doi: 10.1038/s41467-024-52692-w.

Abstract

Membrane electrode assembly (MEA) cells incorporating Cu catalysts are effective for generating C chemicals via the CO reduction reaction (CORR). However, the impact of MEA configuration on the inevitable reconstruction of Cu catalysts during CORR remains underexplored, despite its considerable potential to affect CORR efficacy. Herein, we demonstrate that MEA cells prompt a unique reconstruction of Cu, in contrast to H-type cells, which subsequently influences CORR outcomes. Utilizing three Cu-based catalysts, specifically engineered with different nanostructures, we identify contrasting selectivity trends in the production of C 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 CuO, resulting in altered Cu surfaces compared to those in H-type cells. Time-resolved CORR studies, supported by Operando analysis, further highlight that significant Cu reconstruction within MEA cells is a primary factor leading to the deactivation of CORR into C chemicals.

摘要

包含铜催化剂的膜电极组件(MEA)电池通过一氧化碳还原反应(CORR)生成含碳化学品的效率很高。然而,尽管MEA配置对CORR过程中铜催化剂不可避免的重构有相当大的影响CORR效率的潜力,但对此仍未进行充分探索。在此,我们证明,与H型电池相比,MEA电池会促使铜发生独特的重构,这随后会影响CORR结果。利用三种具有不同纳米结构的特定工程化铜基催化剂,我们确定了H型电池和MEA电池在含碳化学品生产中截然不同的选择性趋势。原位X射线吸收光谱以及两种电池类型的非原位分析表明,MEA电池有助于氧化铜的还原,与H型电池相比,这会导致铜表面发生变化。在原位分析的支持下,时间分辨CORR研究进一步强调,MEA电池内显著的铜重构是导致CORR转化为含碳化学品失活的主要因素。

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