Single-atomic-site platinum steers photogenerated charge carrier lifetime of hematite nanoflakes for photoelectrochemical water splitting.

Gao, Rui-Ting; Zhang, Jiangwei; Nakajima, Tomohiko; He, Jinlu; Liu, Xianhu; Zhang, Xueyuan; Wang, Lei; Wu, Limin · Nat Commun · 2023

basic_science · Level V

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Abstract

Although much effort has been devoted to improving photoelectrochemical water splitting of hematite (α-Fe<sub>2</sub>O<sub>3</sub>) due to its high theoretical solar-to-hydrogen conversion efficiency of 15.5%, the low applied bias photon-to-current efficiency remains a huge challenge for practical applications. Herein, we introduce single platinum atom sites coordination with oxygen atom (Pt-O/Pt-O-Fe) sites into single crystalline α-Fe<sub>2</sub>O<sub>3</sub> nanoflakes photoanodes (SAs Pt:Fe<sub>2</sub>O<sub>3</sub>-Ov). The single-atom Pt doping of α-Fe<sub>2</sub>O<sub>3</sub> can induce few electron trapping sites, enhance carrier separation capability, and boost charge transfer lifetime in the bulk structure as well as improve charge carrier injection efficiency at the semiconductor/electrolyte interface. Further introduction of surface oxygen vacancies can suppress charge carrier recombination and promote surface reaction kinetics, especially at low potential. Accordingly, the optimum SAs Pt:Fe<sub>2</sub>O<sub>3</sub>-Ov photoanode exhibits the photoelectrochemical performance of 3.65 and 5.30 mA cm<sup>-2</sup> at 1.23 and 1.5 V<sub>RHE</sub>, respectively, with an applied bias photon-to-current efficiency of 0.68% for the hematite-based photoanodes. This study opens an avenue for designing highly efficient atomic-level engineering on single crystalline semiconductors for feasible photoelectrochemical applications.