Molecular Coatings Improve the Selectivity and Durability of CO2 Reduction Chalcogenide Photocathodes

Lai, Yungchieh; Watkins, Nicholas B.; Muzzillo, Christopher; Richter, Matthias; Kan, Kevin; Zhou, Lan; Haber, Joel A.; Zakutayev, Andriy; Peters, Jonas C.; Agapie, Theodor; Gregoire, John M.

doi:10.1021/acsenergylett.1c02762

Title: Molecular Coatings Improve the Selectivity and Durability of CO₂ Reduction Chalcogenide Photocathodes

Journal Article · 28 February 2022 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.1c02762 · OSTI ID:1860329

Lai, Yungchieh ^[1]; Watkins, Nicholas B. ^[1];

^[2];

^[1]; Kan, Kevin ^[1]; Zhou, Lan ^[1];

^[1];

^[2];

^[1];

^[1]

California Institute of Technology (CalTech), Pasadena, CA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

The quest for solar-driven conversion of carbon dioxide to chemicals and fuels hinges upon the identification of an efficient, durable, and selective photocathode. Chalcogenide p-type semiconductors exemplified by chalcopyrite Cu(In,Ga)Se₂ (CIGS) have been effectively deployed as photocathodes. However, selectivity toward CO₂ reduction and durability of the commonly used CdS adlayer remain primary challenges. Here, we demonstrate that for the wide band gap CuGa₃Se₅ chalcopyrite absorber these challenges are well addressed by an organic coating generated in situ from an N,N'-(1,4-phenylene)bispyridinium ditriflate salt in the electrolyte. The molecular additive provides a 30-fold increase in selectivity toward CO2R products compared to the unmodified system and lowers Cd corrosion at least 10-fold. This dual functionality highlights the promise of hybrid solid-state-molecular photocathodes for enabling durable and efficient solar fuel systems.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); U.S. Department of Energy

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1860329

Report Number(s):: NREL/JA-5K00-81932; MainId:82705; UUID:3e66f44d-0fc0-4d6b-8dc8-3228877d8ae7; MainAdminID:64122

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 3 Vol. 7; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Molecular Coatings Improve the Selectivity and Durability of CO2 Reduction Chalcogenide Photocathodes

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Title: Molecular Coatings Improve the Selectivity and Durability of CO₂ Reduction Chalcogenide Photocathodes