Zhao Yubao, Zhang Peng, Yang Zhenchun, Li Lina, Gao Jingyu, Chen Sheng, Xie Tengfeng, Diao Caozheng, Xi Shibo, Xiao Beibei, Hu Chun, Choi Wonyong
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education & Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou, P. R. China.
Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Korea.
Nat Commun. 2021 Jun 17;12(1):3701. doi: 10.1038/s41467-021-24048-1.
Solar-driven hydrogen peroxide (HO) production presents unique merits of sustainability and environmental friendliness. Herein, efficient solar-driven HO production through dioxygen reduction is achieved by employing polymeric carbon nitride framework with sodium cyanaminate moiety, affording a HO production rate of 18.7 μmol h mg 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 O and surface, which boosts the population and prolongs the lifetime of the active shallow-trapped electrons, is experimentally substantiated.
太阳能驱动的过氧化氢（HO）生产具有可持续性和环境友好性等独特优点。在此，通过使用带有氰胺钠部分的聚合氮化碳框架实现了通过双氧还原高效太阳能驱动的HO生产，在380nm处的HO生产率为18.7μmol h mg，表观量子产率为27.6%。系统地分析了整个光催化转化过程，并通过实验和理论方法证实了一些以前未知的结构特征和相互作用。框架中氰胺基和吡啶氮配位钠的结构特征促进了光子吸收，改变了框架的能量格局，提高了电荷分离效率，增强了双氧的表面吸附，并创造了选择性的2e氧还原反应表面活性位点。特别是，通过实验证实了O与表面之间的电子耦合相互作用，该相互作用增加了活性浅俘获电子的数量并延长了其寿命。
