TY - JOUR
T1 - Pd4S3Se3, Pd4S3Te3, and Pd4Se3Te3: Candidate Two-Dimensional Janus Materials for Photocatalytic Water Splitting
AU - Luo, Yi
AU - Sun, Minglei
AU - Yu, Jin
AU - Schwingenschlögl, Udo
N1 - KAUST Repository Item: Exported on 2021-06-07
Acknowledgements: We gratefully acknowledge funding from the Scientific Research Foundation of the Graduate School of Southeast University. The research reported in this publication was supported by funding from King Abdullah University of Science and Technology (KAUST).
PY - 2021/5/17
Y1 - 2021/5/17
N2 - The anisotropic Janus materials Pd4S3Se3, Pd4S3Te3, and Pd4Se3Te3 are demonstrated to be stable based on the cohesive energy, the phonon spectrum, and ab initio molecular dynamics simulation. They are semiconductors with indirect band gaps of 1.25, 0.78, and 1.32 eV, respectively, and exhibit ultrahigh carrier mobilities of up to 9455 cm2 V–1 s–1. Band edges enclosing the redox potentials of water enable photocatalytic water splitting. Importantly, the large intrinsic electric fields of the Janus structures facilitate the migration of photo-generated carriers, which enhances the carrier utilization and, therefore, the solar-to-hydrogen efficiency. The obtained efficiencies of 30.1% for Pd4S3Se3, 38.6% for Pd4S3Te3, and 23.8% for Pd4Se3Te3 surpass the conventional theoretical limit of 18%. In addition, the materials are predicted to catalyze the hydrogen and oxygen evolution reactions. Application potential is identified in electronics, optoelectronics, and photocatalytic water splitting.
AB - The anisotropic Janus materials Pd4S3Se3, Pd4S3Te3, and Pd4Se3Te3 are demonstrated to be stable based on the cohesive energy, the phonon spectrum, and ab initio molecular dynamics simulation. They are semiconductors with indirect band gaps of 1.25, 0.78, and 1.32 eV, respectively, and exhibit ultrahigh carrier mobilities of up to 9455 cm2 V–1 s–1. Band edges enclosing the redox potentials of water enable photocatalytic water splitting. Importantly, the large intrinsic electric fields of the Janus structures facilitate the migration of photo-generated carriers, which enhances the carrier utilization and, therefore, the solar-to-hydrogen efficiency. The obtained efficiencies of 30.1% for Pd4S3Se3, 38.6% for Pd4S3Te3, and 23.8% for Pd4Se3Te3 surpass the conventional theoretical limit of 18%. In addition, the materials are predicted to catalyze the hydrogen and oxygen evolution reactions. Application potential is identified in electronics, optoelectronics, and photocatalytic water splitting.
UR - http://hdl.handle.net/10754/669408
UR - https://pubs.acs.org/doi/10.1021/acs.chemmater.1c00812
U2 - 10.1021/acs.chemmater.1c00812
DO - 10.1021/acs.chemmater.1c00812
M3 - Article
SN - 0897-4756
JO - Chemistry of Materials
JF - Chemistry of Materials
ER -
