Reaction Mechanism of Photocatalytic Hydrogen Production at Water/Tin Halide Perovskite Interfaces
Journal article, 2022
While instability in aqueous environment has long impeded employment of metal halide perovskites for heterogeneous photocatalysis, recent reports have shown that some particular tin halide perovskites (THPs) can be water-stable and active in photocatalytic hydrogen production. To unravel the mechanistic details underlying the photocatalytic activity of THPs, we compare the reactivity of the water-stable and active DMASnBr3 (DMA = dimethylammonium) perovskite against prototypical MASnI3 and MASnBr3 compounds (MA = methylammonium), employing advanced electronic-structure calculations. We find that the binding energy of electron polarons at the surface of THPs, driven by the conduction band energetics, is cardinal for photocatalytic hydrogen reduction. In this framework, the interplay between the A-site cation and halogen is found to play a key role in defining the photoreactivity of the material by tuning the perovskite electronic energy levels. Our study, by elucidating the key steps of the reaction, may assist in development of more stable and efficient materials for photocatalytic hydrogen reduction.
Author
Damiano Ricciarelli
Consiglo Nazionale Delle Richerche
University of Perugia
Waldemar Kaiser
Consiglo Nazionale Delle Richerche
E. Mosconi
Consiglo Nazionale Delle Richerche
Julia Wiktor
Chalmers, Physics, Condensed Matter and Materials Theory
Muhammad Waqar Ashraf
Prince Mohammad Bin Fahd University
Lorenzo Malavasi
Universita degli studi di Pavia
Francesco Ambrosio
Istituto Italiano di Tecnologia
Consiglo Nazionale Delle Richerche
University of Salerno
F. De Angelis
University of Perugia
Prince Mohammad Bin Fahd University
Consiglo Nazionale Delle Richerche
ACS Energy Letters
23808195 (eISSN)
1308-1315Subject Categories
Physical Chemistry
Chemical Engineering
DOI
10.1021/acsenergylett.2c00122