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.

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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