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Photoanodes based on In 2 S 3 /ZnO heterojunction nanosheet arrays (NSAs) have been fabricated by atomic layer deposition of ZnO over In 2 S 3  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 In 2 S 3 /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 In 2 S 3 /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 In 2 S 3  NSAs, respectively. A detailed energy band edge analysis reveals the type-II band alignment of the In 2 S 3 /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.Electronic supplementary material  The online version of this article (10.1007/s40820-018-0199-z) contains supplementary material, which is available to authorized users.

Highly Enhanced Visible-Light-Driven Photoelectrochemical Performance of ZnO-Modified In2S3 Nanosheet Arrays by Atomic Layer Deposition