Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects

Chang-Wei Bai; Lian-Lian Liu; Jie-Jie Chen; Fei Chen; Zhi-Quan Zhang; Yi-Jiao Sun; Xin-Jia Chen; Qi Yang; Han-Qing Yu

doi:10.1038/s41467-024-49046-x

Nature Communications (Jun 2024)

Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects

Chang-Wei Bai,
Lian-Lian Liu,
Jie-Jie Chen,
Fei Chen,
Zhi-Quan Zhang,
Yi-Jiao Sun,
Xin-Jia Chen,
Qi Yang,
Han-Qing Yu

Affiliations

Chang-Wei Bai: Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University
Lian-Lian Liu: CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China
Jie-Jie Chen: CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China
Fei Chen: Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University
Zhi-Quan Zhang: Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University
Yi-Jiao Sun: Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University
Xin-Jia Chen: Key Laboratory of the Three Gorges Reservoir Region’s Eco-Environment, Ministry of Education, College of Environment and Ecology, Chongqing University
Qi Yang: Key Laboratory of Environmental Biology and Pollution Control, Ministry of Education, College of Environmental Science and Engineering, Hunan University
Han-Qing Yu: CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science and Technology of China

DOI: https://doi.org/10.1038/s41467-024-49046-x
Journal volume & issue: Vol. 15, no. 1
pp. 1 – 16

Abstract

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Abstract Artificial photosynthesis using carbon nitride (g-C3N4) holds a great promise for sustainable and cost-effective H2O2 production, but the high carrier recombination rate impedes its efficiency. To tackle this challenge, we propose an innovative method involving multispecies iodine mediators (I−/I3 −) intercalation through a pre-photo-oxidation process using potassium iodide (suspected deteriorated “KI”) within the g-C3N4 framework. Moreover, we introduce an external electric field by incorporating cationic methyl viologen ions to establish an auxiliary electron transfer channel. Such a unique design drastically improves the separation of photo-generated carriers, achieving an impressive H2O2 production rate of 46.40 mmol g−1 h−1 under visible light irradiation, surpassing the most visible-light H2O2-producing systems. Combining various advanced characterization techniques elucidates the inner photocatalytic mechanism, and the application potential of this photocatalytic system is validated with various simulation scenarios. This work presents a significative strategy for preparing and applying highly efficient g-C3N4-based catalysts in photochemical H2O2 production.

Published in Nature Communications

ISSN: 2041-1723 (Online)
Publisher: Nature Portfolio
Country of publisher: United Kingdom
LCC subjects: Science
Website: https://www.nature.com/ncomms/

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