电化学二氧化碳还原过程中铜催化剂上碳沉积的研究与缓解

Jing-Wen DuanMu, Zhi-Zheng Wu, Fei-Yue Gao, Peng-Peng Yang, Zhuang-Zhuang Niu, Yu-Cai Zhang, Li-Ping Chi and Min-Rui Gao*, 
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引用次数: 0

摘要

铜(Cu)被认为是将二氧化碳(CO2)电化学转化为高附加值碳氢化合物的最有效催化剂,但其稳定性仍面临相当大的挑战。在此,我们报告了二氧化碳还原过程中碳沉积对铜电极活性位点的毒害效应--这是一个经常被忽视的关键失活因素。我们发现,甲烷形成的中间体 *C 可在电极表面解吸形成碳物种。我们发现甲烷的形成与碳的沉积之间存在很强的相关性,有利于甲烷生成的反应条件会导致更多的碳沉积。沉积的碳会阻塞活性位点,从而导致催化性能迅速下降。我们进一步证明,可以通过增加电极的粗糙度和提高电解液的 pH 值来减轻碳沉积。这项工作为设计更稳定的二氧化碳还原催化剂提供了新的指导。
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Investigation and Mitigation of Carbon Deposition over Copper Catalyst during Electrochemical CO2 Reduction

Copper (Cu) is considered to be the most effective catalyst for electrochemical conversion of carbon dioxide (CO2) into value-added hydrocarbons, but its stability still faces considerable challenge. Here, we report the poisoning effect of carbon deposition during CO2 reduction on the active sites of Cu electrode─a critical deactivation factor that is often overlooked. We find that, *C, an intermediate toward methane formation, could desorb on the electrode surface to form carbon species. We reveal a strong correlation between the formation of methane and the carbon deposition, and the reaction conditions favoring methane production result in more carbon deposition. The deposited carbon blocks the active sites and consequently causes rapid deterioration of the catalytic performance. We further demonstrate that the carbon deposition can be mitigated by increasing the roughness of the electrode and increasing the pH of the electrolyte. This work offers a new guidance for designing more stable catalysts for CO2 reduction.

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来源期刊
Precision Chemistry
Precision Chemistry 精密化学技术-
CiteScore
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期刊介绍: Chemical research focused on precision enables more controllable predictable and accurate outcomes which in turn drive innovation in measurement science sustainable materials information materials personalized medicines energy environmental science and countless other fields requiring chemical insights.Precision Chemistry provides a unique and highly focused publishing venue for fundamental applied and interdisciplinary research aiming to achieve precision calculation design synthesis manipulation measurement and manufacturing. It is committed to bringing together researchers from across the chemical sciences and the related scientific areas to showcase original research and critical reviews of exceptional quality significance and interest to the broad chemistry and scientific community.
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