Zhang Canhui, Wang Xingkun, Ma Zhentao, Yao Hanxu, Liu Hengjun, Li Cheng, Zhou Jian, Xu Ren, Zheng Xusheng, Wang Huanlei, Li Qiang, Gu Meng, Jiang Heqing, Huang Minghua
School of Materials Science and Engineering, Ocean University of China, Qingdao 266100, China.
School of Materials Science and Engineering, Ocean University of China, Qingdao 266100, China; Qingdao Key Laboratory of Functional Membrane Material and Membrane Technology, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.
Sci Bull (Beijing). 2023 Sep 30;68(18):2042-2053. doi: 10.1016/j.scib.2023.07.049. Epub 2023 Jul 31.
Breakthrough in developing cost-effective Fe-based catalysts with superior oxygen reduction reaction (ORR) activities and ultra-long-term stability for application in Zn-air batteries (ZABs) remain a priority but still full of challenges. Herein, the neighboring NiN single-metal-atom and FeN dual-metal-atoms on the N-doped hollow carbon sphere (Fe/Ni-NHCS) were deliberately constructed as the efficient and robust ORR catalyst for ZABs. Both theory calculations and magnetic measurements demonstrate that the introduction of NiN provides a significant role on optimizing the electron spin state of FeN sites and reducing the energy barrier for the adsorption and conversion of the oxygen-containing intermediates, enabling the Fe/Ni-NHCS with excellent ORR performance and ultralow byproduct HO yield (0.5%). Impressively, the ZABs driven by Fe/Ni-NHCS exhibit unprecedented long-term rechargeable stability over 1200 h. This work paves a new venue to manipulate the spin state of active sites for simultaneously achieving superior catalytic activities and ultra-long-term stability in energy conversion technologies.
开发具有卓越氧还原反应（ORR）活性和超长期稳定性、适用于锌空气电池（ZABs）的高性价比铁基催化剂方面的突破仍然是一个优先事项，但仍充满挑战。在此，在氮掺杂空心碳球（Fe/Ni-NHCS）上特意构建了相邻的NiN单金属原子和FeN双金属原子，作为用于锌空气电池的高效且稳定的氧还原反应催化剂。理论计算和磁性测量均表明，NiN的引入在优化FeN位点的电子自旋状态以及降低含氧中间体吸附和转化的能垒方面发挥了重要作用，使得Fe/Ni-NHCS具有优异的氧还原反应性能和超低的副产物HO产率（0.5%）。令人印象深刻的是，由Fe/Ni-NHCS驱动的锌空气电池在超过1200小时内展现出前所未有的长期可充电稳定性。这项工作为在能量转换技术中操纵活性位点的自旋状态以同时实现卓越的催化活性和超长期稳定性开辟了一条新途径。
