Transient Metal Centers at the Covalent Heterointerface Favor Photocatalytic Hydrogen Evolution

ACS Appl Mater Interfaces. 2023 Jul 5;15(26):31364-31374. doi: 10.1021/acsami.3c02662. Epub 2023 Jun 22.

Abstract

Semiconductor heterostructures effectively promote the transfer and separation of interfacial photoinduced charges for the photocatalytic process. Herein, we constructed a direct Z-scheme SnSe2/CdS heterojunction photocatalyst. N-type SnSe2 semiconductors are suitable candidate materials for oxidation half-reactions in Z-scheme heterojunctions. The intimate atomic-level interfacial contact through Cd-Se bonds provides a better interfacial charge transport channel for the photoinduced charges. Moreover, the transient Sn4+/Sn0 centers caused by the photoredox process boost the interfacial charge transport/separation at the interface. Besides, the presence of S vacancies acting as electron enrichment centers further enhances the redox ability for hydrogen production. Therefore, the SnSe2/CdS heterostructure showed a superior visible-light photocatalytic H2-production activity of 13.6 mmol·g-1·h-1 using ascorbic acid as a sacrificial agent, which is 9.7 times higher than that of pristine CdS. The apparent quantum yield reaches 10.5% at λ = 420 nm. This work provides a useful way to improve charge transfer in the Z-scheme heterojunction photocatalyst for hydrogen production.

Keywords: Cd−Se bond; H2 production; SnSe2; direct Z-scheme system; photocatalysis; transient metal centers.