Data-Intensive Exploration of the Photoelectrochemical Responses of Main-Group Metal Sulfides
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.
WOS:001230357900001
2024-05-23
REVIEWED
Funder | Grant 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 | |
Swiss National Science Foundation (SNSF) through its National Centre of Competence in Research (NCCR) MARVEL | |