In Situ Reconstructed Hydroxyl‐Rich Atomic‐Thin Bi2O2CO3 Enables Ampere‐Scale Synthesis of Formate from CO2 with Activated Water Dissociation

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Advanced Materials Pub Date : 2024-12-23 DOI:10.1002/adma.202415639
Qizheng Huang, Zhengyi Qian, Na Ye, Yingjun Tan, Menggang Li, Mingchuan Luo, Shaojun Guo
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引用次数: 0

Abstract

Renewable electricity‐driven CO2 electroreduction provides a promising route toward carbon neutrality and sustainable chemical production. Nevertheless, the viability of this route faces constraints of catalytic efficiency and durability in near‐neutral electrolytes at industrial‐scale current densities, mechanistically originating from unfavorable accommodation of *H species from water dissociation. Herein, a new strategy is reported to accelerate water dissociation by the rich surface hydroxyl on bismuth subcarbonate nanosheets in situ electrochemical transformed from bismuth hydroxide nanotube precursors. This catalyst enables the electrosynthesis of formate at current densities up to 1000 mA cm−2 with >96% faradaic efficiencies in flow cells, and a 200 h durable membrane electrode assembly in a dilute near‐neutral environment. Combined kinetic studies, in situ characterizations, and theoretical calculations reveal that the atomic thickness strengthens the hydroxyl adsorption, and with a highly localized electron configuration, the hydroxyl‐functionalized surface is more affinitive to oxygenated species, thus lowering the barrier for water dissociation and the crucial hydrogenation step in the proton‐coupled electron transfer from *OCHO to *HCOOH.

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来源期刊
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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