Affiliation:
1. School of Material Science and Engineering, Shanghai Institute of Technology, Shanghai 201418, China
2. School of Chemical and Environment Engineering, Shanghai Institute of Technology, Shanghai 201418, China
Abstract
To gain insight into photocatalytic behavior, transient absorption spectroscopy (TAS) was used to study LaCoxMn1−xO3, LaMnxNi1−xO3 and LaNixCo1−xO3 (x = 0, 0.2, 0.4, 0.6, 0.8 and 1.0) on a microsecond time scale. The results show that the electron lifetime is key to determining the photocatalytic reduction of CO2. This is the first time that the photogenerated electron lifetime in perovskite has been proposed to express the performance of the photocatalytic reduction of CO2 with H2O into CH4. In all cases, the decay curve can be well explained by two consecutive first-order kinetics, indicating that the electron exists within two major populations: one with a short lifetime and the other one with a long lifetime. The long-lived electrons are the rate-limiting species for the photocatalytic reaction and are related to the activity of the photocatalytic reduction of CO2 with H2O to produce CH4. For different photocatalysts, we find that the longer the electron decay lifetime is, the stronger the electron de-trapping ability is, and the electrons perform more activity. In this paper, TAS can not only detect the micro-dynamics process of carriers, but it is also demonstrated to be an easy and effective method for screening the most active catalyst in various catalysts for the photocatalytic reduction of CO2 with H2O accurately and quickly.
Funder
National Key R&D Program of China
Shanghai Technical Service Center for Advanced Ceramics Structure Design and Precision Manufacturing
Subject
Physical and Theoretical Chemistry,Catalysis,General Environmental Science