A First-Principles High-Throughput Search for Layered Sulfides for CO2 Reduction Photocatalysis

ORAL

Abstract

Artificial photosynthesis presents a promising opportunity to extract CO2 from the atmosphere and produce useful chemical fuels. While a wealth of water splitting photoanodes have been identified, efficient CO2 reduction calls for the discovery of new photocatalysts. In this work, we develop a high-throughput screening workflow using first-principles density functional theory (DFT) with van der Waals corrections to discover new CO2 reduction photocatalysts. The high valence bands, and hence high conduction bands, observed in low-band gap sulfides show promise for meeting the high redox potentials of CO2 reduction. We draw on the success of MoS2 as a CO2 reduction photocatalyst to motivate a search for layered sulfides with similar electronic, structural, and aqueous stability properties. With this workflow we analyze thousands of metal-sulfide compounds from the Materials Project database. We identify promising layered sulfides with DFT band gaps between 0-3 eV, minimal Pourbaix thermodynamic instability under CO2 reduction conditions and suitable band edge alignment to CO2 redox potentials.

*This work is supported by the Department of Energy via the Joint Center for Artificial Photosynthesis, Molecular Foundry, and NERSC.

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Presenters

  • Elizabeth Peterson

    • Department of Physics, University of California - Berkeley

Authors

  • Elizabeth Peterson

    • Department of Physics, University of California - Berkeley

  • Sebastian Reyes-Lillo

    • Departamento de Ciencias Físicas, Universidad Nacional Andre Bello
    • Departamento de Ciencias Fisicas, Universidad Andres Bello
    • Departamento de Ciencias Fisicas UNAB; Molecular Foundry LBNL

  • John Gregoire

    • Joint Center for Artificial Photosynthesis, Caltech

  • Jeffrey Neaton

    • Molecular Foundry, Lawrence Berkeley National Laboratory; Department of Physics, University of California, Berkeley; Kavli Energy Nanosciences Institute at Berkeley
    • Physics, University of California, Berkeley; Lawrence Berkeley National Laboratory
    • Department of Physics, University of California
    • Univ of California - Berkeley
    • Lawrence Berkeley Natl Lab
    • Materials Science Division, Lawrence Berkeley National Laboratory
    • Molecular Foundry, Lawrence Berkeley National Lab
    • Physics, University of California, Berkeley
    • Department of Physics UCB; Molecular Foundry LBNL; Kavli ENSI
    • Lawrence Berkeley National Laboratory
    • Department of Physics, Univ of California - Berkeley
    • Lawrence Berkeley National Lab and University of California - Berkeley