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

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

    Cite this: ACS Energy Lett. 2022, 7, 3, 1195–1201
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    https://doi.org/10.1021/acsenergylett.1c02762
    Published March 1, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    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.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.1c02762.

    • Methodologies for using high throughput experimentation systems used herein; molecular additive synthesis and characterization; further description of durability testing; combinatorial experiments for selecting electrode, illumination, and potential range; additional SEM, TEM, and XPS characterization of electrodes; and table of all electrolysis and corrosion results (PDF)

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    Cited By

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    This article is cited by 7 publications.

    1. Fábio Vieira, Pierre Marcasuzaa, Leonard Curet, Laurent Billon, Aurélien Viterisi, Emilio Palomares. Selectivity of a Copper Oxide CO2 Reduction Electrocatalyst Shifted by a Bioinspired pH-Sensitive Polymer. ACS Applied Materials & Interfaces 2024, 16 (34) , 45038-45048. https://doi.org/10.1021/acsami.4c11927
    2. Joy S. Zeng, Vineet Padia, Grace Y. Chen, Joseph H. Maalouf, Aditya M. Limaye, Alexander H. Liu, Michael A. Yusov, Ian W. Hunter, Karthish Manthiram. Nonidealities in CO2 Electroreduction Mechanisms Revealed by Automation-Assisted Kinetic Analysis. ACS Central Science 2024, 10 (7) , 1348-1356. https://doi.org/10.1021/acscentsci.3c01295
    3. Aisulu Aitbekova, Nicholas Watkins, Matthias H. Richter, Phillip Jahelka, Jonas C. Peters, Theodor Agapie, Harry A. Atwater. Molecular Additives Improve the Selectivity of CO2 Photoelectrochemical Reduction over Gold Nanoparticles on Gallium Nitride. Nano Letters 2024, 24 (4) , 1090-1095. https://doi.org/10.1021/acs.nanolett.3c03590
    4. Tariq Abbas, Hamdya Sabrina Mohidin Yahya, Nor Aishah Saidina Amin. Insights and Progress on Photocatalytic and Photoelectrocatalytic Reactor Configurations and Materials for CO2 Reduction to Solar Fuels. Energy & Fuels 2023, 37 (23) , 18330-18368. https://doi.org/10.1021/acs.energyfuels.3c02863
    5. Yongpeng Liu, Meng Xia, Dan Ren, Simon Nussbaum, Jun-Ho Yum, Michael Grätzel, Néstor Guijarro, Kevin Sivula. Photoelectrochemical CO2 Reduction at a Direct CuInGaS2/Electrolyte Junction. ACS Energy Letters 2023, 8 (4) , 1645-1651. https://doi.org/10.1021/acsenergylett.3c00022
    6. Huitong Du, Jiaju Fu, Li-Xia Liu, Shichao Ding, Zhaoyuan Lyu, Yu-Chung Chang, Xin Jin, Fredrick O. Kengara, Bing Song, Qianhao Min, Jun-Jie Zhu, Dan Du, Cheng Gu, Yuehe Lin, Jin-Song Hu, Wenlei Zhu. Recent progress in electrochemical reduction of carbon monoxide toward multi-carbon products. Materials Today 2022, 59 , 182-199. https://doi.org/10.1016/j.mattod.2022.08.012
    7. Ian Lorenzo E. Gonzaga, Candy C. Mercado. Copper ternary oxides as photocathodes for solar-driven CO 2 reduction. REVIEWS ON ADVANCED MATERIALS SCIENCE 2022, 61 (1) , 430-457. https://doi.org/10.1515/rams-2022-0043
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    ACS Energy Letters

    Cite this: ACS Energy Lett. 2022, 7, 3, 1195–1201
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsenergylett.1c02762
    Published March 1, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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