Dual Channel H2O2 Photosynthesis in Pure Water over S‐Scheme Heterojunction Cs3PMo12/CC Boosted by Proton and Electron Reservoirs

Author:

Wei Chong1,Zhang Yu1,Qu Yunteng23ORCID,Hua Wenbo1,Jia Zixian4ORCID,Lu Jiangbo5,Xie Gang13,Xiao Jianming6,Hu Huaiming1,Yang Ying13,Liu Ji‐Quan13ORCID,Bai Jinbo7,Xue Ganglin1

Affiliation:

1. Key Laboratory of Synthetic and Natural Functional Molecule Chemistry College of Chemistry & Materials Science Northwest University 1 Xuefu Ave. Xi'an 710127 China

2. State Key Laboratory of Photoelectric Technology and Functional Materials International Collaborative Center on Photoelectric Technology and Nano Functional Materials Institute of Photonics & PhotonTechnology Northwest University Xi'an 710069 China

3. Shaanxi Key Laboratory for Carbon Neutral Technology Northwest University Xi'an 710127 China

4. SINOPEC Dalian Research Institute of Petroleum and Petrochemicals Co., Ltd Dalian 116045 China

5. School of Physics & Information Technology Shaanxi Normal University Xi'an Shaanxi 710062 China

6. Department College of Materials Science and Engineering Xi'an University of Architecture and Technology Xi'an 710055 China

7. CentraleSupélec, ENS Paris‐Saclay CNRS, LMPS‐Laboratoire de Mécanique Paris‐Saclay, Université Paris‐Saclay 8–10 rue Joliot‐Curie Gif‐sur‐Yvette 91190 France

Abstract

AbstractDual channel photo‐driven H2O2 production in pure water on small‐scale on‐site setups is a promising strategy to provide low‐concentrated H2O2 whenever needed. This process suffers, however, strongly from the fast recombination of photo‐generated charge carriers and the sluggish oxidation process. Here, insoluble Keggin‐type cesium phosphomolybdate Cs3PMo12O40 (abbreviated to Cs3PMo12) is introduced to carbonized cellulose (CC) to construct S‐scheme heterojunction Cs3PMo12/CC. Dual channel H2O2 photosynthesis from both H2O oxidation and O2 reduction in pure water has been thus achieved with the production rate of 20.1 mmol L−1 gcat.−1 h−1, apparent quantum yield (AQY) of 2.1% and solar‐to‐chemical conversion (SCC) efficiency of 0.050%. H2O2 accumulative concentration reaches 4.9 mmol L−1. This high photocatalytic activity is guaranteed by unique features of Cs3PMo12/CC, namely, S‐scheme heterojunction, electron reservoir, and proton reservoir. The former two enhance the separation of photo‐generated charge carriers, while the latter speeds up the torpid oxidation process. In situ experiments reveal that H2O2 is formed via successive single‐electron transfer in both channels. In real practice, exposing the reaction system under natural sunlight outdoors successfully results in 0.24 mmol L−1 H2O2. This work provides a key practical strategy for designing photocatalysts in modulating redox half‐reactions in photosynthesis.

Funder

China Postdoctoral Science Foundation

National Natural Science Foundation of China

Publisher

Wiley

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