Aqueous Photoelectrochemical CO2 Reduction to CO and Methanol over a Silicon Photocathode Functionalized with a Cobalt Phthalocyanine Molecular Catalyst

Bo Shang, Conor L. Rooney*, David J. Gallagher, Bernie T. Wang, Andrey Krayev, Hadar Shema, Oliver Leitner, Nia J. Harmon, Langqiu Xiao, Colton Sheehan, Samuel R. Bottum, Elad Gross, James F. Cahoon, Thomas E. Mallouk, Hailiang Wang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

We report a precious-metal-free molecular catalyst-based photocathode that is active for aqueous CO2 reduction to CO and methanol. The photoelectrode is composed of cobalt phthalocyanine molecules anchored on graphene oxide which is integrated via a (3-aminopropyl)triethoxysilane linker to p-type silicon protected by a thin film of titanium dioxide. The photocathode reduces CO2 to CO with high selectivity at potentials as mild as 0 V versus the reversible hydrogen electrode (vs RHE). Methanol production is observed at an onset potential of −0.36 V vs RHE, and reaches a peak turnover frequency of 0.18 s−1. To date, this is the only molecular catalyst-based photoelectrode that is active for the six-electron reduction of CO2 to methanol. This work puts forth a strategy for interfacing molecular catalysts to p-type semiconductors and demonstrates state-of-the-art performance for photoelectrochemical CO2 reduction to CO and methanol.

Original languageAmerican English
Article numbere202215213
JournalAngewandte Chemie - International Edition
Volume62
Issue number4
DOIs
StatePublished - 23 Jan 2023

Bibliographical note

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

Keywords

  • CO Reduction
  • Methanol
  • Molecular Catalyst
  • Photoelectrochemical Reaction
  • Silicon Photocathode

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