A stable covalent organic framework for photocatalytic carbon dioxide reduction

Zhiwei Fu, Xiaoyan Wang, Adrian M. Gardner, Xue Wang, Samantha Y. Chong, Gaia Neri, Alexander J. Cowan, Lunjie Liu, Xiaobo Li, Anastasia Vogel, Rob Clowes, Matthew Bilton, Linjiang Chen, Reiner Sebastian Sprick, Andrew I. Cooper

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

Photocatalytic conversion of CO2 into fuels is an important challenge for clean energy research and has attracted considerable interest. Here we show that tethering molecular catalysts - a rhenium complex, [Re(bpy)(CO)3Cl] - together in the form of a crystalline covalent organic framework (COF) affords a heterogeneous photocatalyst with a strong visible light absorption, a high CO2 binding affinity, and ultimately an improved catalytic performance over its homogeneous Re counterpart. The COF incorporates bipyridine sites, allowing for ligation of the Re complex, into a fully π-conjugated backbone that is chemically robust and promotes light-harvesting. A maximum rate of 1040 μmol g-1 h-1 for CO production with 81% selectivity was measured. CO production rates were further increased up to 1400 μmol g-1 h-1, with an improved selectivity of 86%, when a photosensitizer was added. Addition of platinum resulted in production of syngas, hence, the co-formation of H2 and CO, the chemical composition of which could be adjusted by varying the ratio of COF to platinum. An amorphous analog of the COF showed significantly lower CO production rates, suggesting that crystallinity of the COF is beneficial to its photocatalytic performance in CO2 reduction.

Original languageEnglish
Pages (from-to)543-550
Number of pages8
JournalChemical Science
Volume11
Issue number2
Early online date21 Nov 2019
DOIs
Publication statusPublished - 14 Jan 2020

Keywords

  • photocatalytic conversion
  • carbon dioxide reduction
  • clean energy research

Fingerprint Dive into the research topics of 'A stable covalent organic framework for photocatalytic carbon dioxide reduction'. Together they form a unique fingerprint.

  • Cite this

    Fu, Z., Wang, X., Gardner, A. M., Wang, X., Chong, S. Y., Neri, G., Cowan, A. J., Liu, L., Li, X., Vogel, A., Clowes, R., Bilton, M., Chen, L., Sprick, R. S., & Cooper, A. I. (2020). A stable covalent organic framework for photocatalytic carbon dioxide reduction. Chemical Science, 11(2), 543-550. https://doi.org/10.1039/c9sc03800k