Abstract
Organic-inorganic lead halide perovskites are a new class of semiconductor materials with great potential in photocatalytic hydrogen production, however, their development is greatly plagued by their low photocatalytic activity, instability of organic component and lead toxicity in particular. Herein, we report an anti-dissolution environmentally friendly Cs2SnI6 perovskite anchored with a new class of atomically dispersed Pt-I3 species (PtSA/Cs2SnI6) for achieving the highly efficient photocatalytic hydrogen production in HI aqueous solution at room temperature. Particularly, we discover that Cs2SnI6 in PtSA/Cs2SnI6 has a greatly enhanced tolerance towards HI aqueous solution, which is very important for achieving excellent photocatalytic stability in perovskite-based HI splitting system. Remarkably, the PtSA/Cs2SnI6 catalyst shows a superb photocatalytic activity for hydrogen production with a record turnover frequency of 70.6 h−1per Pt, about 176.5 times greater than that of Pt nanoparticles supported Cs2SnI6 perovskite, along with superior cycling durability. Charge-carrier dynamics studies in combination with theory calculations reveal that the dramatically boosted photocatalytic performance on PtSA/Cs2SnI6 originates from both unique coordination structure and electronic property of Pt-I3 sites, and strong metal-support interaction effect that can not only greatly promote the charge separation and transfer, but also substantially reduce the energy barrier for hydrogen production. This work opens a new way for stimulating more research on perovskite composite materials for efficient hydrogen production.
Highlights
Organic-inorganic lead halide perovskites are a new class of semiconductor materials with great potential in photocatalytic hydrogen production, their development is greatly plagued by their low photocatalytic activity, instability of organic component and lead toxicity in particular
Cs2SnI6 is insoluble in aqueous hydroiodic acid (HI) solution at room temperature (RT), confirmed by the fact that the solubility of Cs2SnI6 was zero at 25 °C, and slightly increased to 10.0 × 10−6 mol L−1 as the temperature was improved to 100 °C, still far lower than that of reported MAPbI3 (0.645 mol L−1 at 20 °C) (Fig. 1d)[25]
There is no change in the color of aqueous HI solution with or without Cs2SnI6 powder, which further verifies the insolubility for Cs2SnI6
Summary
Organic-inorganic lead halide perovskites are a new class of semiconductor materials with great potential in photocatalytic hydrogen production, their development is greatly plagued by their low photocatalytic activity, instability of organic component and lead toxicity in particular. We report an anti-dissolution environmentally friendly Cs2SnI6 perovskite anchored with a new class of atomically dispersed Pt-I3 species (PtSA/Cs2SnI6) for achieving the highly efficient photocatalytic hydrogen production in HI aqueous solution at room temperature. We demonstrate the first example on making a new class of single-atom Pt–I3 sites anchored on all-inorganic Cs2SnI6 perovskite (PtSA/Cs2SnI6) for efficient H2 evolution photocatalysis from HI splitting at RT via a facile and cost-effective strategy. Combining charge-carrier dynamics studies with theory calculations reveals that both unique coordination structure and electronic property of Pt–I3 sites and strong metal–support interaction (SMSI) effect are the main reasons in achieving the greatly enhanced photocatalytic performance in hydrogen production from HI aqueous solution
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