Construction of PdSe2/ZnIn2S4 heterojunctions with covalent interface for highly efficient photocatalytic hydrogen evolution

Wei Guan; Ruiming Jia; Lin Zhang; Ming Meng; Peng Wang; Ying Wang; Haoyu Wang; Xingchen Dong; Lina Sui; Zhixing Gan; Lifeng Dong; Liyan Yu

doi:10.1016/j.jcis.2023.06.130

Construction of PdSe₂/ZnIn₂S₄ heterojunctions with covalent interface for highly efficient photocatalytic hydrogen evolution

J Colloid Interface Sci. 2023 Nov:649:685-693. doi: 10.1016/j.jcis.2023.06.130. Epub 2023 Jun 19.

Authors

Wei Guan¹, Ruiming Jia¹, Lin Zhang¹, Ming Meng², Peng Wang¹, Ying Wang¹, Haoyu Wang¹, Xingchen Dong¹, Lina Sui¹, Zhixing Gan³, Lifeng Dong⁴, Liyan Yu⁵

Affiliations

¹ College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China.
² School of Physics and Telecommunication Engineering, Zhoukou Normal University, Zhoukou 466001, PR China.
³ College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China; Center for Future Optoelectronic Functional Materials, School of Computer and Electronic Information/School of Artificial Intelligence, Nanjing Normal University, Nanjing 210023, PR China. Electronic address: zxgan@njnu.edu.cn.
⁴ College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China. Electronic address: donglifeng@qust.edu.cn.
⁵ College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China. Electronic address: liyanyu@qust.edu.cn.

PMID: 37385033
DOI: 10.1016/j.jcis.2023.06.130

Abstract

Constructing semiconductor heterojunctions can enable novel schemes for highly efficient photocatalytic activity. However, introducing strong covalent bonding at the interface remains an open challenge. Herein, ZnIn₂S₄ (ZIS) with abundant sulfur vacancies (Sv) is synthesized with the presence of PdSe₂ as an additional precursor. The sulfur vacancies of Sv-ZIS are filled by Se atoms of PdSe₂, leading to the Zn-In-Se-Pd compound interface. Our density functional theory (DFT) calculations reveal the increased density of states at the interface, which will increase the local carrier concentration. Moreover, the length of the Se-H bond is longer than that of the SH bond, which is good for the evolution of H₂ from the interface. In addition, the charge redistribution at the interface results in a built-in field, providing the driving force for efficient separation of photogenerated electron-hole. Therefore, the PdSe₂/Sv-ZIS heterojunction with strong covalent interface exhibits an excellent photocatalytic hydrogen evolution performance (4423 μmol g^-1h^-1) with an apparent quantum efficiency (λ > 420 nm) of 9.1 %. This work will provide new inspirations to improve photocatalytic activity by engineering the interfaces of semiconductor heterojunctions.

Keywords: Interface; Photocatalytic hydrogen evolution; Photogenerated carriers; Semiconductor heterojunctions.