Abstract

Photoanodes based on In2S3/ZnO heterojunction nanosheet arrays (NSAs) have been fabricated by atomic layer deposition of ZnO over In2S3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facile solvothermal process. The as-prepared photoanodes show dramatically enhanced performance for photoelectrochemical (PEC) water splitting, compared to single semiconductor counterparts. The optical and PEC properties of In2S3/ZnO NSAs have been optimized by modulating the thickness of the ZnO overlayer. After pairing with ZnO, the NSAs exhibit a broadened absorption range and an increased light absorptance over a wide wavelength region of 250–850 nm. The optimized sample of In2S3/ZnO-50 NSAs shows a photocurrent density of 1.642 mA cm−2 (1.5 V vs. RHE) and an incident photon-to-current efficiency of 27.64% at 380 nm (1.23 V vs. RHE), which are 70 and 116 times higher than those of the pristine In2S3 NSAs, respectively. A detailed energy band edge analysis reveals the type-II band alignment of the In2S3/ZnO heterojunction, which enables efficient separation and collection of photogenerated carriers, especially with the assistance of positive bias potential, and then results in the significantly increased PEC activity.

Highlights

  • Photoelectrochemical (PEC) water splitting is regarded as one of the most attractive approaches for producing hydrogen in a clean, renewable, and eco-friendly manner to store solar energy, which has aroused significant interest in the recent years [1,2,3,4,5]

  • To fabricate heterojunction nanosheet arrays (NSAs), the In2S3 nanosheets were conformably coated with ZnO overlayers through a thermal atomic layer deposition (ALD) process at 150 °C (Fig. 1a)

  • The results show that In2S3/ZnO-50 NSAs display the highest photocurrent density, which is significantly much higher than that of the pure In2S3

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Summary

Introduction

Photoelectrochemical (PEC) water splitting is regarded as one of the most attractive approaches for producing hydrogen in a clean, renewable, and eco-friendly manner to store solar energy, which has aroused significant interest in the recent years [1,2,3,4,5]. There is no single one material that can satisfy all the aforementioned requirements among more than about 130 types of semiconductor materials [6] To address these challenges, nanostructured architectures have been explored because of their various advantages compared to bulk materials [8,9,10,11]. Among the known nanostructured semiconductors, metal chalcogenides have attracted substantial attention as a group of highly efficient photocatalysts for PEC water splitting [15]. The defect spinel structure b-In2S3, which is an n-type semiconductor with a bandgap of 2.0–2.3 eV, has been reported to be a promising photoanode material for PEC water splitting under visible-light irradiation in all three different crystal structures owing to its relatively negative conduction band edge, moderate charge transport properties, stable chemical, and physical characteristics along with low toxicity [20,21,22]. BIn2S3 nanocrystals with various 2D morphologies, such as nanosheets, nanoplates, nanoflakes, and nanobelts, have been successfully synthesized by different methods as photoanode materials for PEC applications [23,24,25,26]

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