Liang Zuozhong, Kong Ningning, Yang Chenxi, Zhang Wei, Zheng Haoquan, Lin Haiping, Cao Rui
Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China.
Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China.
Angew Chem Int Ed Engl. 2021 Jun 1;60(23):12759-12764. doi: 10.1002/anie.202101562. Epub 2021 Apr 13.
Nitrogen-doped graphene could catalyze the electrochemical reduction and evolution of oxygen, but unfortunately suffers from sluggish catalytic kinetics. Herein, for the first time, we report an onion-like carbon coated Co, N-doped carbon (OLC/Co-N-C) material, which possesses multilayers of highly curved nanostructures that form mesoporous architectures. These unique nanospheres are produced when surfactant micelles are introduced to synthesis precursors. Owing to the combined electronic effect and nanostructuring effect, our OLC/Co-N-C materials exhibit high bifunctional oxygen reduction/evolution reaction (ORR/OER) activity, showing a promising application in rechargeable Zn-air batteries. Experimental results are rationalized by theoretical calculations, showing that the curvature of graphitic carbon plays a vital role in promoting activities of meta-carbon atoms near graphitic N and ortho/meta carbon atoms close to pyridinic N.
氮掺杂石墨烯能够催化氧的电化学还原和析出,但遗憾的是其催化动力学较为迟缓。在此,我们首次报道了一种洋葱状碳包覆的钴、氮掺杂碳(OLC/Co-N-C)材料,它具有多层高度弯曲的纳米结构,形成了介孔结构。当将表面活性剂胶束引入合成前驱体时会产生这些独特的纳米球。由于电子效应和纳米结构效应的共同作用,我们的OLC/Co-N-C材料表现出高的双功能氧还原/析出反应(ORR/OER)活性,在可充电锌空气电池中显示出有前景的应用。理论计算对实验结果进行了合理的解释,表明石墨碳的曲率在促进石墨氮附近的间位碳原子以及靠近吡啶氮的邻位/间位碳原子的活性方面起着至关重要的作用。