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Covalent organic frameworks comprising cobalt porphyrins for catalytic CO <sub>2</sub> reduction in water

Song LinChemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USAChristian S. DiercksDepartment of Chemistry, University of California, Berkeley, CA 94720, USAYue‐Biao ZhangDepartment of Chemistry, University of California, Berkeley, CA 94720, USANikolay KornienkoDepartment of Chemistry, University of California, Berkeley, CA 94720, USAEva M. NicholsChemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USAYingbo ZhaoDepartment of Chemistry, University of California, Berkeley, CA 94720, USAAubrey R. ParisDepartment of Chemistry, University of California, Berkeley, CA 94720, USADohyung KimDepartment of Materials Science and Engineering, University of California, Berkeley, CA 94720, USAPeidong YangDepartment of Chemistry, University of California, Berkeley, CA 94720, USAOmar M. YaghiDepartment of Chemistry, University of California, Berkeley, CA 94720, USAChristopher J. ChangChemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA

2015en

ABI

Annotatsiya

Conversion of carbon dioxide (CO2) to carbon monoxide (CO) and other value-added carbon products is an important challenge for clean energy research. Here we report modular optimization of covalent organic frameworks (COFs), in which the building units are cobalt porphyrin catalysts linked by organic struts through imine bonds, to prepare a catalytic material for aqueous electrochemical reduction of CO2 to CO. The catalysts exhibit high Faradaic efficiency (90%) and turnover numbers (up to 290,000, with initial turnover frequency of 9400 hour(-1)) at pH 7 with an overpotential of -0.55 volts, equivalent to a 26-fold improvement in activity compared with the molecular cobalt complex, with no degradation over 24 hours. X-ray absorption data reveal the influence of the COF environment on the electronic structure of the catalytic cobalt centers.

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DOI: 10.1126/science.aac8343

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