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Vast bulk recombination of photo-generated carriers and sluggish surface oxygen evolution reaction (OER) kinetics severely hinder the development of photoelectrochemical water splitting. Herein, through constructing a vertically ordered ZnInS nanosheet array with an interior gradient energy band as photoanode, the bulk recombination of photogenerated carriers decreases greatly. We use the atomic layer deposition technology to introduce Fe-In-S clusters into the surface of photoanode. First-principles calculations and comprehensive characterizations indicate that these clusters effectively lower the electrochemical reaction barrier on the photoanode surface and promote the surface OER reaction kinetics through precisely affecting the second and third steps (forming processes of O* and OOH*) of the four-electron reaction. As a result, the optimal photoanode exhibits the high performance with a significantly enhanced photocurrent of 5.35 mA cm −2  at 1.23 V RHE  and onset potential of 0.09 V RHE . Present results demonstrate a robust platform for controllable surface modification, nanofabrication, and carrier transport.

Atomic layer deposition triggered Fe-In-S cluster and gradient energy band in ZnInS photoanode for improved oxygen evolution reaction