Lattice interconversion of 1D ferrocene-based perovskite induced by solvent molecules for selectively photocatalytic toluene oxidation

Abstract

Metal halide perovskites (MHPs) have attracted enormous attention in the field potential applications of optoelectronics and photocatalysis due to their excellent optoelectronic performances, such as broad light absorption range, high charge mobility and long carrier diffusion length. However, using MHPs as photocatalysts for photocatalytic toluene oxidation is rare and the underlying mechanisms affecting toluene oxidation are still unclear. In this article, we constructed two novel one dimensional (1D) Ferrocene-based Perovskites catalysts, (C13H17FeNH)PbI3 and (C13H17FeNH)PbI3•DEF, in which (C13H17FeNH)PbI3 can photocatalyze the oxidation of toluene to benzaldehyde effectively. It's interesting that the crystal lattice of (C13H17FeNH)PbI3 and (C13H17FeNH)PbI3•DEF can be converted to each other through the gain and loss of solvent molecules, which not only regulates the electronic band structure, but also increases the separation efficiency of photogenerated carriers. These results were confirmed by the steady-state photoluminescence (PL), the time-resolved photoluminescence (TRPL) spectra, transient photocurrent responses measurements and density functional theory (DFT) calculations. In addition, the lower exciton binding energy (43.2 meV) of (C13H17FeNH)PbI3 further demonstrates its effective carriers’ separation efficiency. Furthermore, the selective adsorption of (C13H17FeNH)PbI3 on toluene and benzaldehyde provides a prerequisite for the efficient selective oxidation of toluene. Finally, (C13H17FeNH)PbI3 exhibited excellent catalytic activity for the photocatalytic oxidation of toluene to benzaldehyde with conversion of 28.5% and the selectivity (95.3%) towards benzaldehyde.