In Situ Synthesis of Lead-Free Halide Perovskite Cs2AgBiBr6 Supported on Nitrogen-Doped Carbon for Efficient Hydrogen Evolution in Aqueous HBr Solution

ACS Appl Mater Interfaces. 2021 Mar 3;13(8):10037-10046. doi: 10.1021/acsami.0c21588. Epub 2021 Feb 19.

Abstract

Lead halide perovskites have shown great potential in photovoltaic and photocatalytic fields. However, the toxicity of lead impedes their wide application. Herein composites of lead-free halide perovskite Cs2AgBiBr6 supported on nitrogen-doped carbon (N-C) materials were synthesized successfully through a facile one-pot method for the first time. Without deposition of noble metals as the cocatalyst, the optimal composite Cs2AgBiBr6/N-C (Cs2AgBiBr6/N-C-140) exhibits outstanding photocatalytic performance with a high hydrogen evolution rate of 380 μmol g-1 h-1 under visible light irradiation (λ ≥ 420 nm), which is about 19 times faster than that of pure Cs2AgBiBr6 and 4 times faster than that of physically mixed Cs2AgBiBr6/N-C-140, respectively. The Cs2AgBiBr6/N-C-140 composite also displays high stability with no significant decrease after six cycles of repeated hydrogen evolution experiments. The addition of N-C with a high surface area helps to prevent aggregation of Cs2AgBiBr6 NPs and provides more pathways for the migration of photoinduced carriers. The nitrogen dopant can facilitate photoinduced electron transfer from Cs2AgBiBr6 to N-C to result in spatially separated electrons and holes with prolonged electron time and greatly enhance the photocatalytic performance. This study indicates that Cs2AgBiBr6-based perovskite materials are promising candidates for photocatalytic hydrogen evolution.

Keywords: HBr splitting; composite; electron transfer; hydrogen evolution; lead-free perovskite Cs2AgBiBr6; nitrogen-doped carbon.