Triggering photocatalytic performance of La 2 Co x Mn 2-x O 6 via heat activation

Author:

Chen Cheng123ORCID,Wu Mingge13,Chen Bolei4ORCID,Ma Chunyan12ORCID,Song Maoyong123ORCID,Jiang Guibin23

Affiliation:

1. Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China

2. State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China

3. University of Chinese Academy of Sciences, Beijing 100049, China

4. Hubei Key Laboratory of Environmental and Health Effects of Persistent Toxic Substances, Jianghan University, Wuhan 430056, China

Abstract

The La-based perovskite (LaBO 3 ) exhibits excellent optical properties. However, its valence band (VB) potential is not sufficiently positive to reach the oxidation potential required for the cleavage of chemical bonds (such as benzylic C–H), limiting its application in photocatalysis. Herein, we report the unconventional effects of heat activation on the reduction of the dissociation energy of benzylic C–H and aqueous H–O, thereby triggering the photocatalytic activity of La 2 Co x Mn 2-x O 6 perovskites. Additionally, we demonstrate that photocatalysis is the main contributor to substrate conversion in the selective oxidation of toluene and reduction of CO 2 . Particularly, La 2 Co 1.5 Mn 0.5 O 6 shows excellent performance with a product yield of 550.00 mmol g cat −1 and a toluene conversion of 22,866.67 μmol g cat −1 h −1 . To the best of our knowledge, this is the highest reported product yield for the selective oxidation of benzylic C–H bond of toluene. Our findings provide insight into the specific role of heat activation in photocatalysis, which is crucial for breaking and overcoming the VB barrier to realize challenging reactions.

Funder

National Natural Science Foundation of China

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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