Abstract

In the emerging Sb2 S3 -based solar energy conversion devices, a CdS buffer layer prepared by chemical bath deposition is commonly used to improve the separation of photogenerated electron-hole pairs. However, the cation diffusion at the Sb2 S3 /CdS interface induces detrimental defects but is often overlooked. Designing a stable interface in the Sb2 S3 /CdS heterojunction is essential to achieve high solar energy conversion efficiency. As a proof of concept, this study reports that the modification of the Sb2 S3 /CdS heterojunction with an ultrathin Al2 O3 interlayer effectively suppresses the interfacial defects by preventing the diffusion of Cd2+ cations into the Sb2 S3 layer. As a result, a water-splitting photocathode based on Ag:Sb2 S3 /Al2 O3 /CdS heterojunction achieves a significantly improved half-cell solar-to-hydrogen efficiency of 2.78% in a neutral electrolyte, as compared to 1.66% for the control Ag:Sb2 S3 /CdS device. This work demonstrates the importance of designing atomic interfaces and may provide a guideline for the fabrication of high-performance stibnite-type semiconductor-based solar energy conversion devices.

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