Insights into Photogenerated Carrier Dynamics and Overall Water Splitting of the CrS3/GeSe Heterostructure

Xue-Qing Wan; Chuan-Lu Yang; Xiao-Hu Li; Mei-Shan Wang; Xiao-Guang Ma

doi:10.1021/acs.jpclett.3c01780

Insights into Photogenerated Carrier Dynamics and Overall Water Splitting of the CrS₃/GeSe Heterostructure

J Phys Chem Lett. 2023 Oct 12;14(40):9126-9135. doi: 10.1021/acs.jpclett.3c01780. Epub 2023 Oct 4.

Authors

Xue-Qing Wan¹, Chuan-Lu Yang^{1

2}, Xiao-Hu Li^{2

3}, Mei-Shan Wang¹, Xiao-Guang Ma¹

Affiliations

¹ School of Physics and Optoelectronic Engineering, Ludong University, Yantai 264025, China.
² Xinjiang Astronomical Observatory, Chinese Academy of Sciences, Urumqi 830011, China.
³ Key Laboratory of Radio Astronomy, Chinese Academy of Sciences, Urumqi 830011, China.

PMID: 37793127
DOI: 10.1021/acs.jpclett.3c01780

Abstract

Based on the nonadiabatic molecular dynamics (NAMD) simulations and the first-principles calculations, we explore the overall water-splitting schemes and the photogenerated carrier dynamics for two configurations (CG and C_yG) of the CrS₃/GeSe van der Waals heterostructures. The photocatalytic direct Z-schemes and carrier migration pathways for hydrogen and oxygen evolution reactions (HER/OER) are constructed based on the electronic properties. The solar-to-hydrogen efficiency (η'_STH values) of the schemes can reach 10.60% and 10.17% and further rise under tensile strain. The NAMD results demonstrate similar transfer times of the electron/hole for HER/OER and more rapid electron-hole recombination in CG enables it to be superior to C_yG in photocatalytic performance. Moreover, the Gibbs free energy indicates that both the HERs and OERs turn to spontaneously proceed with CG and C_yG at pH = 0-12.37 and pH = 2.55-11.01, respectively. These facts reveal that the CrS₃/GeSe heterostructure is promising in photocatalytic overall water splitting.