Regulating electronic structure of CoN4 with axial Co—S for promoting oxygen reduction and Zn-air battery performance
Chang Chen, Zhiqiang Chen, Junxi Zhong, Xin Song, Dongfang Chen, Shoujie Liu, Weng‐Chon Cheong, Jiazhan Li, Xin Tan, Chang He, Jiaqi Zhang, Di Liu, Qiuhua Yuan, Chen Chen, Qing Peng, Yadong Li
Abstract
Regulating the coordination environment of transition-metal based materials in the axial direction with heteroatoms has shown great potential in boosting the oxygen reduction reaction (ORR). The coordination configuration and the regulation method are pivotal and elusive. Here, we report a combined strategy of matrix-activization and controlled-induction to modify the CoN4 site by axial coordination of Co—S (Co1N4-S1), which was validated by the aberration-corrected electron microscopy and X-ray absorption fine structure analysis. The optimal Co1N4-S1 exhibits an excellent alkaline ORR activity, according to the half-wave potential (0.897 V vs. reversible hydrogen electrode (RHE)), Tafel slope (24.67 mV/dec), and kinetic current density. Moreover, the Co1N4-S1 based Zn-air battery displays a high power density of 187.55 mW/cm2 and an outstanding charge—discharge cycling stability for 160 h, demonstrating the promising application potential. Theoretical calculations indicate that the better regulation of CoN4 on electronic structure and thus the highly efficient ORR performance can be achieved by axial Co—S.