文献类型：期刊文献

英文题名：Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis

作者：Sun, Ji Wei[1];Wu, Xuefeng[1];Liu, Peng Fei[1];Chen, Jiacheng[2];Liu, Yuanwei[1];Lou, Zhen Xin[1];Zhao, Jia Yue[1];Yuan, Hai Yang[1];Chen, Aiping[1];Wang, Xue Lu[3,4];Zhu, Minghui[2];Dai, Sheng[5,6];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Engn Res Ctr Hierarch Nanomat, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Normal Univ, Sch Phys & Elect Sci, Phys Dept, 3663 North Zhongshan Rd, Shanghai 200062, Peoples R China;[4]East China Normal Univ, Sch Phys & Elect Sci, Shanghai Key Lab Magnet Resonance, 3663 North Zhongshan Rd, Shanghai 200062, Peoples R China;[5]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2023

卷号：14

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000971817200001)】；

基金：This work was financially supported by the Science and Technology Commission of Shanghai Municipality (21DZ1207101, 22ZR1416400, 22ZR1415700), the Key Program of National Natural Science Foundation of China (22239001), the National Natural Science Funds for Distinguished Young Scholars (51725201), the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the National Natural Science Foundation of China (22072045), the Innovation Program of Shanghai Municipal Education Commission (E00014), Shanghai Rising-star Program (20QA1402400), and Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400). The authors acknowledge the Fundamental Research Funds for the Central Universities and the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry. The authors also thank the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) and the 1W1B beamline of the Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses. Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

摘要：Practical electrochemical CO2-to-CO conversion requires a non-precious catalyst to react at high selectivity and high rate. Atomically dispersed, coordinatively unsaturated metal-nitrogen sites have shown great performance in CO2 electroreduction; however, their controllable and large-scale fabrication still remains a challenge. Herein, we report a general method to fabricate coordinatively unsaturated metal-nitrogen sites doped within carbon nanotubes, among which cobalt single-atom catalysts can mediate efficient CO2-to-CO formation in a membrane flow configuration, achieving a current density of 200 mA cm(-2) with CO selectivity of 95.4% and high full-cell energy efficiency of 54.1%, outperforming most of CO2-to-CO conversion electrolyzers. By expanding the cell area to 100 cm(2), this catalyst sustains a high-current electrolysis at 10 A with 86.8% CO selectivity and the single-pass conversion can reach 40.4% at a high CO2 flow rate of 150 sccm. This fabrication method can be scaled up with negligible decay in CO2-to-CO activity. In situ spectroscopy and theoretical results reveal the crucial role of coordinatively unsaturated metal-nitrogen sites, which facilitate CO2 adsorption and key *COOH intermediate formation. Scalable fabrication of coordinatively unsaturated metal-nitrogen is challenging. Here the authors report a general method for synthesize such material for CO2 electrochemical conversion at a high catalytic current of 10 A for more than 60 h stability using a 100 cm2 membrane flow cell.