Rowan R. Katzbaer¹, Simon Gelin², Monica J. Theibault³, Mohammed M. Khan², Cierra Chandler², Nicola Colonna^4,5, Zhiqiang Mao^1,6, Héctor D. Abruña^3*, Ismaila Dabo^2,6,7*, Raymond E. Schaak^1,7,8*

1 Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

2 Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

3 Department of Chemistry, Cornell University, Cornell, New York 14850, United States

4 Laboratory for Materials Simulations, Paul Scherrer Institute, 5232 Villigen, Switzerland

5 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

6 Department of Physics, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

7 Materials Research Institute, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

8 Department of Chemical Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States

* Corresponding authors emails: hda1@cornell.edu, dabo@psu.edu, res20@psu.edu

DOI10.24435/materialscloud:yd-cz [version v1]

Publication date: Jan 10, 2025

How to cite this record

Rowan R. Katzbaer, Simon Gelin, Monica J. Theibault, Mohammed M. Khan, Cierra Chandler, Nicola Colonna, Zhiqiang Mao, Héctor D. Abruña, Ismaila Dabo, Raymond E. Schaak, Data-intensive exploration of the photoelectrochemical responses of main-group metal sulfides, Materials Cloud Archive 2025.7 (2025), https://doi.org/10.24435/materialscloud:yd-cz

Description

Materials that efficiently promote the thermodynamically uphill water-splitting reaction under solar illumination are essential for generating carbon-free (“green”) hydrogen. Mapping out the combinatorial space of potential photocatalysts for this reaction can be expedited using data-intensive materials exploration. The calculated band gaps and band alignments can serve as key indicators and metrics to computationally screen photoactive materials. Ternary main-group metal sulfides containing p- and s-block elements represent a promising, albeit underexplored, class of photocatalysts. Here, we computationally screen 86 candidate ternary main-group metal sulfides containing p- and s-block elements. By validating electronic structure predictions against experimental band gaps and band edges for synthetically accessible materials, we propose eight potential photocatalysts. Using computed Pourbaix diagrams, we further narrowed the candidate pool to four materials based on the predicted aqueous stability. We then synthesized and characterized these four materials and experimentally screened them for photoresponsiveness under photocatalytically relevant conditions. We also characterized their experimental band gaps and band edge positions and compared them with computational predictions. Based on the experimental screening protocols, we identify MgIn₂S₄ and BaSn₂S₅ as photoresponsive materials with sufficient aqueous stability to be considered in greater depth as potential photocatalysts for overall water-splitting. This record contains the computational predictions for the four candidates discussed in our manuscript.

Materials Cloud sections using this data

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File name	Size	Description
archive.tar.gz MD5md5:8b8d0c611f2f277f65e26a8eee6c197f	3.0 MiB	This record contains the computational predictions for the four candidates discussed in our manuscript: DFT, DFT+U, DFT+U+SOC, and HSE06 calculations.

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External references

Keywords

Photocatalysts Sulfides Water Splitting