Plasma induced grain boundaries to boost electrochemical reduction of CO2 to formate

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外文摘要：Bismuth-based catalysts are highly promising for the electrochemical carbon dioxide reduction reaction(eCO2RR)to formate product.However,achieving high activity and selectivity towards formate and ensuring long-term stability remains challenging.This work reports the oxygen plasma inducing strategy to construct the abundant grain boundaries of Bi/BiOx on ultrathin two-dimensional Bi nanosheets.The oxygen plasma-treated Bi nanosheet(OP-Bi)exhibits over 90％Faradaic efficiency(FE)for formate at a wide potential range from-0.5 to-1.1 V,and maintains a great stability catalytic performance without significant decay over 30 h in flow cell.Moreover,membrane electrode assembly(MEA)device with OP-Bi as catalyst sustains the robust current density of 100 mA cm-2 over 50 h,maintaining a formate FE above 90％.In addition,rechargeable Zn-CO2 battery presents the peak power density of 1.22 mW cm-2 with OP-Bi as bifunctional catalyst.The mechanism experiments demonstrate that the high-density grain boundaries of OP-Bi provide more exposed active sites,faster electron transfer capac-ity,and the stronger intrinsic activity of Bi atoms.In situ spectroscopy and theoretical calculations further elucidate that the unsaturated Bi coordination atoms between the grain boundaries can effectively acti-vate CO2 molecules through elongating the C-O bond,and reducing the formation energy barrier of the key intermediate(*OCOH),thereby enhancing the catalytic performance of eCO2RR to formate product.

外文关键词：

CO2 electroreductionBi nanosheetGrain boundaryUnsaturation Bi atomsMEA device

作者：

Guan Wang、Shengtao Zhong、Xiaoqian Xiong、Jing Li、Fangyuan Wang、Li Huo、Daoxiong Wu、Xingqi Han、Zhitong Wang、Qi Chen、Xinlong Tian、Peilin Deng

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作者单位：

School of Marine Science and Engineering,State Key Laboratory of Marine Resource Utilization in South China Sea,Hainan University,Haikou 570228,Hainan,China

基金：

Hainan Province Science and Technology Special FundHainan Province Science and Technology Special FundHainan Province Science and Technology Special FundNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaStartup Research Foundation of Hainan UniversityStartup Research Foundation of Hainan UniversityStartup Research Foundation of Hainan UniversityStartup Research Foundation of Hainan UniversityStartup Research Foundation of Hainan Universitycollaborative Innovation Center of Marine Science and Technology,Hainan Universitycollaborative Innovation Center of Marine Science and Technology,Hainan UniversityInnovative Research Projects for Graduate Students of Hainan ProvinceInnovative Research Projects for Graduate Students of Hainan ProvinceInnovative Research Projects for Graduate Students of Hainan ProvinceScientific Research Program Funded by Shaanxi Provincial Education Departmentspecific research fund of The Innovation Platform for Academicians of Hainan Province

项目编号：

ZDYF2024SHFZ074ZDYF2024SHFZ072ZDYF2022SHFZ2992210903522202053521640285227429722309037KYQDZR-2000820083200842112523035XTCX2022HYC04XTCX2022HYC05Qhyb2022-89Qhyb2022-87Qhys2022-17423JK0439YSPTZX202315

出版年：

2024

DOI：

10.1016/j.jechem.2024.04.026

能源化学

中国科学院大连化学物理研究所中国科学院成都有机化学研究所

能源化学

CSTPCDEI

影响因子：0.654

ISSN：2095-4956

年,卷(期)：2024.95(8)