Hu Cheng, Hu Jingcong, Zhu Zijian, Lu Yue, Chu Shengqi, Ma Tianyi, Zhang Yihe, Huang Hongwei
Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Beijing, 100083, P. R. China.
Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, P. R. China.
Angew Chem Int Ed Engl. 2022 Oct 24;61(43):e202212397. doi: 10.1002/anie.202212397. Epub 2022 Sep 29.
Developing efficient piezocatalytic systems for two-electron water splitting (TEWS) with producing H and H O shows great promise to meet the industrial demand. Herein, Ag single atoms (SAs) and clusters are co-anchored on carbon nitride (Ag -CN) to serve as the multifunctional sites for efficient TEWS. The Ag SAs enhance the in-plane piezoelectric polarization of CN that is intimately modulated by the atomic coordination induced charge redistribution, and Ag clusters afford strong interfacial electric field to remarkably promote the out-of-plane migration of piezoelectrons from CN. Moreover, Ag -CN yields a larger piezoresistive effect that elevates carrier mobility under strain. Consequently, a superior H and H O evolution rate of 7.90 mmol g h and 5.84 mmol g h is delivered by Ag -CN, respectively, far exceeding that of the previously reported piezocatalysts. This work not only presents the SAs decoration as an available polarization enhancement strategy, but also sheds light on the superiority of multi-sites engineering in piezocatalysis.
开发用于双电子水分解（TEWS）以产生H和H₂O的高效压电催化系统，对于满足工业需求具有巨大潜力。在此，银单原子（SAs）和团簇共锚定在氮化碳（Ag-CN）上，作为高效TEWS的多功能位点。银单原子增强了CN的面内压电极化，这通过原子配位诱导的电荷重新分布得到密切调制，并且银团簇提供强界面电场以显著促进压电电子从CN的面外迁移。此外，Ag-CN产生更大的压阻效应，在应变下提高载流子迁移率。因此，Ag-CN分别实现了7.90 mmol g⁻¹ h⁻¹和5.84 mmol g⁻¹ h⁻¹的优异H₂和H₂O析出速率，远远超过先前报道的压电催化剂。这项工作不仅展示了单原子修饰作为一种可行的极化增强策略，而且还揭示了多位点工程在压电催化中的优越性。
