Mechanistic analysis of multiple processes controlling solar-driven H2O2 synthesis using engineered polymeric carbon nitride

Yubao Zhao (), Peng Zhang, Zhenchun Yang, Lina Li, Jingyu Gao, Sheng Chen, Tengfeng Xie, Caozheng Diao, Shibo Xi, Beibei Xiao, Chun Hu and Wonyong Choi ()
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Yubao Zhao: Guangzhou University
Peng Zhang: Guangzhou University
Zhenchun Yang: Guangzhou University
Lina Li: Guangzhou University
Jingyu Gao: Guangzhou University
Sheng Chen: Nanjing University of Science and Technology
Tengfeng Xie: Jilin University
Caozheng Diao: National University of Singapore
Shibo Xi: National University of Singapore
Beibei Xiao: Jiangsu University of Science and Technology
Chun Hu: Guangzhou University
Wonyong Choi: Pohang University of Science and Technology (POSTECH)

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Solar-driven hydrogen peroxide (H2O2) production presents unique merits of sustainability and environmental friendliness. Herein, efficient solar-driven H2O2 production through dioxygen reduction is achieved by employing polymeric carbon nitride framework with sodium cyanaminate moiety, affording a H2O2 production rate of 18.7 μmol h −1 mg−1 and an apparent quantum yield of 27.6% at 380 nm. The overall photocatalytic transformation process is systematically analyzed, and some previously unknown structural features and interactions are substantiated via experimental and theoretical methods. The structural features of cyanamino group and pyridinic nitrogen-coordinated soidum in the framework promote photon absorption, alter the energy landscape of the framework and improve charge separation efficiency, enhance surface adsorption of dioxygen, and create selective 2e− oxygen reduction reaction surface-active sites. Particularly, an electronic coupling interaction between O2 and surface, which boosts the population and prolongs the lifetime of the active shallow-trapped electrons, is experimentally substantiated.

Date: 2021
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DOI: 10.1038/s41467-021-24048-1

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