Covalent organic frameworks comprising cobalt porphyrins for catalytic CO2 reduction in water

Lin, S.; Diercks, C. S.; Zhang, Y. -B.; Kornienko, N.; Nichols, E. M.; Zhao, Y.; Paris, A. R.; Kim, D.; Yang, P.; Yaghi, O. M.; Chang, C. J.

doi:10.1126/science.aac8343

Covalent organic frameworks comprising cobalt porphyrins for catalytic CO₂ reduction in water

Journal Article · Thu Aug 20 00:00:00 EDT 2015 · Science

DOI:https://doi.org/10.1126/science.aac8343· OSTI ID:1370752

Lin, S.; Diercks, C. S.; Zhang, Y. -B.; Kornienko, N.; Nichols, E. M.; Zhao, Y.; Paris, A. R.; Kim, D.; Yang, P.; Yaghi, O. M.; Chang, C. J.

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.

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)

Sponsoring Organization:: USDOE SC Office of Basic Energy Sciences (SC-22)

DOE Contract Number:: SC0001015

OSTI ID:: 1370752

Journal Information:: Science, Journal Name: Science Journal Issue: 6253 Vol. 349; ISSN 0036-8075

Publisher:: AAAS

Country of Publication:: United States

Language:: English

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Covalent organic frameworks comprising cobalt porphyrins for catalytic CO2 reduction in water

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