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弥合二氧化碳电还原中分批式和流动反应器配置之间的活性差距。

Bridging activity gaps between batch and flow reactor configurations in the electroreduction of carbon dioxide.

作者信息

Sun Qiwen, Fu Linke, Chang Xiaoxia, Xu Bingjun

机构信息

College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.

出版信息

Sci Adv. 2024 Nov 22;10(47):eadp5697. doi: 10.1126/sciadv.adp5697.

Abstract

To date, the understanding of various modes of CO mass transport remains incomplete, impeding the transfer of catalysts identified in the more accessible electrochemical batch cells to high-performance flow cells. In this work, we demonstrate that the meniscus region formed between the electrode and the convex liquid level due to the electrowetting of the catalyst plays a vital role in the CORR in batch cells. CORR in the meniscus region in batch cells exhibits similar performance with that in flow cells, and the performance disparity between these two configurations largely disappears when conducting CORR primarily in the meniscus region. An assembled double-sided gas diffusion electrode with a gas channel is developed to maximize the meniscus-like region, achieving a CORR partial current density of 640 mA/cm on commercial Cu in the KHCO electrolyte. This performance represents the highest CORR activity in neutral buffered media.

摘要

迄今为止,对一氧化碳传质的各种模式的理解仍不完整,这阻碍了在更易操作的电化学间歇式电池中鉴定出的催化剂向高性能流通池的转移。在这项工作中,我们证明了由于催化剂的电润湿作用,在电极和凸液面之间形成的弯月面区域在间歇式电池的一氧化碳还原反应(CORR)中起着至关重要的作用。间歇式电池中弯月面区域的CORR表现出与流通池中相似的性能,并且当主要在弯月面区域进行CORR时,这两种配置之间的性能差异在很大程度上消失了。开发了一种带有气体通道的组装式双面气体扩散电极,以最大化弯月面状区域,在KHCO电解液中的商业铜上实现了640 mA/cm的CORR分电流密度。这一性能代表了中性缓冲介质中最高的CORR活性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/70ab/11584008/db0accde8943/sciadv.adp5697-f1.jpg

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