Photocatalytic CO2 Reduction Coupled with Oxidation of Benzyl Alcohol over CsPbBr3@PANI Nanocomposites

J Phys Chem Lett. 2023 Dec 14;14(49):11008-11014. doi: 10.1021/acs.jpclett.3c02766. Epub 2023 Dec 4.

Abstract

Herein, we successfully prepare conductive polyaniline (PANI)-encapsulated CsPbBr3 perovskite nanocrystals (PNCs) that demonstrate much improved photocatalytic performance and stability toward the CO2 reduction reaction (CRR) coupled with oxidation of benzyl alcohol (BA) to benzaldehyde. Due to the acid-base interaction between CO2 and PANI, CO2 molecules are selectively adsorbed on PANI in the form of carbamate. As a result, the rate of production of CO (rCO) reaches 26.1 μmol g-1 h-1 with a selectivity of 98.1%, which is in good agreement with the rate of oxidation (∼27.0 μmol g-1 h-1) of BA. Such a high reduction/oxidation rate is enabled by the fast electron transfer (∼2.2 ps) from PNCs to PANI, as revealed by femtosecond transient absorption spectroscopy. Moreover, because of the benefit of the encapsulation of PANI, no significant decrease in rCO is observed in a 10 h CRR test. This work offers insight into how to simultaneously achieve improved photocatalytic performance and stability of CsPbX3 PNCs.