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  4. Data-Intensive Exploration of the Photoelectrochemical Responses of Main-Group Metal Sulfides
 
research article

Data-Intensive Exploration of the Photoelectrochemical Responses of Main-Group Metal Sulfides

Katzbaer, Rowan R.
•
Gelin, Simon
•
Theibault, Monica J.
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May 23, 2024
Journal Of Physical Chemistry C

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.

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Type
research article
DOI
10.1021/acs.jpcc.4c00341
Web of Science ID

WOS:001230357900001

Author(s)
Katzbaer, Rowan R.
Gelin, Simon
Theibault, Monica J.
Khan, Mohammed M.
Chandler, Cierra
Colonna, Nicola  
Mao, Zhiqiang
Abruna, Hector D.
Dabo, Ismaila
Schaak, Raymond E.
Date Issued

2024-05-23

Publisher

Amer Chemical Soc

Published in
Journal Of Physical Chemistry C
Subjects

Physical Sciences

•

Technology

•

Energy

•

Refinement

•

Mgin2S4

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
FunderGrant Number

, Division of Materials Research

DMR-2011839

National Science Foundation through the Penn State Materials Research Science and Engineering Center (MRSEC)

DMREF-1729338

DMREF and INFEWS programs of the National Science Foundation

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Available on Infoscience
June 5, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/208446
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