biostudies-literatureZhang YJiangsu Collaborative Innovation Center of Biomedical Functional MaterialsPriority Academic Program Development of Jiangsu Higher Education InstitutionsNational Natural Science Foundation of ChinaChina Postdoctoral Science FoundationNatural Science Research of Jiangsu Higher Education InstitutionsNatural Science Foundation of Jiangsu Province175-182https://www.ebi.ac.uk/biostudies/studies/S-EPMC7845012biostudies-literatureUnknown7(1)The sluggish kinetics and unclear mechanism have significantly hindered the development of Li-CO₂ batteries. Here, a Li-CO₂ battery cathode catalyst based on a porphyrin-based covalent organic framework (TTCOF-Mn) with single metal sites is reported to reveal intrinsic catalytic sites of aprotic CO₂ conversion from the molecular level. The battery with TTCOF-Mn exhibits a low overpotential of 1.07 V at 100 mA/g as well as excellent stability at 300 mA/g, which is one of the best Li-CO₂ battery cathode catalysts to date. The unique features of TTCOF-Mn including uniform single-Mn(II)-sites, fast Li⁺ transfer pathways, and high electron transfer efficiency contribute to effective CO₂ reduction and Li₂CO₃ ACS central scienceSingle Metal Site and Versatile Transfer Channel Merged into Covalent Organic Frameworks Facilitate High-Performance Li-CO₂ Batteries.PMC784501219KJB150011218711412018M63057221871142BK20171032217010852019M6518732190112217KJB150025Lu MLi SLDong LZZhang YLan YQZhong RLWang JHJiang CChen YGao GKfalseSingle Metal Site and Versatile Transfer Channel Merged into Covalent Organic Frameworks Facilitate High-Performance Li-CO₂ Batteries.The sluggish kinetics and unclear mechanism have significantly hindered the development of Li-CO₂ batteries. Here, a Li-CO₂ battery cathode catalyst based on a porphyrin-based covalent organic framework (TTCOF-Mn) with single metal sites is reported to reveal intrinsic catalytic sites of aprotic CO₂ conversion from the molecular level. The battery with TTCOF-Mn exhibits a low overpotential of 1.07 V at 100 mA/g as well as excellent stability at 300 mA/g, which is one of the best Li-CO₂ battery cathode catalysts to date. The unique features of TTCOF-Mn including uniform single-Mn(II)-sites, fast Li⁺ transfer pathways, and high electron transfer efficiency contribute to effective CO₂ reduction and Li₂CO₃ 2021-01-01T00:00:00Z2021 Jan2025-04-26T02:35:18.697Z2021-02-21T05:25:10ZS-EPMC78450123353257810.1021/acscentsci.0c01390