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用于高活性、选择性、稳定性和可扩展性的CO电还原的表面钝化

Surface passivation for highly active, selective, stable, and scalable CO electroreduction.

作者信息

Zhu Jiexin, Li Jiantao, Lu Ruihu, Yu Ruohan, Zhao Shiyong, Li Chengbo, Lv Lei, Xia Lixue, Chen Xingbao, Cai Wenwei, Meng Jiashen, Zhang Wei, Pan Xuelei, Hong Xufeng, Dai Yuhang, Mao Yu, Li Jiong, Zhou Liang, He Guanjie, Pang Quanquan, Zhao Yan, Xia Chuan, Wang Ziyun, Dai Liming, Mai Liqiang

机构信息

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, Hubei, P. R. China.

Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.

出版信息

Nat Commun. 2023 Aug 3;14(1):4670. doi: 10.1038/s41467-023-40342-6.

Abstract

Electrochemical conversion of CO to formic acid using Bismuth catalysts is one the most promising pathways for industrialization. However, it is still difficult to achieve high formic acid production at wide voltage intervals and industrial current densities because the Bi catalysts are often poisoned by oxygenated species. Herein, we report a BiS nanowire-ascorbic acid hybrid catalyst that simultaneously improves formic acid selectivity, activity, and stability at high applied voltages. Specifically, a more than 95% faraday efficiency was achieved for the formate formation over a wide potential range above 1.0 V and at ampere-level current densities. The observed excellent catalytic performance was attributable to a unique reconstruction mechanism to form more defective sites while the ascorbic acid layer further stabilized the defective sites by trapping the poisoning hydroxyl groups. When used in an all-solid-state reactor system, the newly developed catalyst achieved efficient production of pure formic acid over 120 hours at 50 mA cm (200 mA cell current).

摘要

使用铋催化剂将CO电化学转化为甲酸是最有希望实现工业化的途径之一。然而,由于铋催化剂常常被含氧物种毒化,在宽电压区间和工业电流密度下仍难以实现高甲酸产量。在此,我们报道了一种BiS纳米线-抗坏血酸混合催化剂,其在高外加电压下同时提高了甲酸的选择性、活性和稳定性。具体而言,在高于1.0 V的宽电位范围内和安培级电流密度下,甲酸盐形成的法拉第效率超过了95%。观察到的优异催化性能归因于一种独特的重构机制,该机制形成了更多的缺陷位点,而抗坏血酸层通过捕获中毒的羟基进一步稳定了这些缺陷位点。当用于全固态反应器系统时,新开发的催化剂在50 mA cm(200 mA电池电流)下120多小时内实现了纯甲酸的高效生产。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/63d9/10400642/169054a38091/41467_2023_40342_Fig1_HTML.jpg

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