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Title: Mechanistic analysis of multiple processes controlling solar-driven H2O2 synthesis using engineered polymeric carbon nitride
Authors: Zhao, Yubao
Zhang, Peng
Yang, Zhenchun
Li, Lina
Gao, Jingyu
Chen, Sheng
Xie, Tengfeng
Diao, Caozheng 
Xi, Shibo 
Xiao, Beibei
Hu, Chun
Choi, Wonyong
Issue Date: 17-Jun-2021
Publisher: Nature Research
Citation: Zhao, Yubao, Zhang, Peng, Yang, Zhenchun, Li, Lina, Gao, Jingyu, Chen, Sheng, Xie, Tengfeng, Diao, Caozheng, Xi, Shibo, Xiao, Beibei, Hu, Chun, Choi, Wonyong (2021-06-17). Mechanistic analysis of multiple processes controlling solar-driven H2O2 synthesis using engineered polymeric carbon nitride. Nature Communications 12 (1) : 3701. ScholarBank@NUS Repository.
Rights: Attribution 4.0 International
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 ?mol 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. © 2021, The Author(s).
Source Title: Nature Communications
ISSN: 2041-1723
DOI: 10.1038/s41467-021-24048-1
Rights: Attribution 4.0 International
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