One single-atom Mn doping strategy enabling two functions of oxygen reduction reaction and pseudocapacitive performance

Abstract

Single-atom metal species as highly effective active sites are crucial for enhancing energy storage and conversion properties. However, achieving the simultaneous construction of single-atom sites and the regulation of matrix structures to enable their application in both energy storage and conversion remains a challenge. Here, we have successfully developed unique MnN2C2 active sites, atomically dispersed on N-doped mesoporous graphitic carbon sheets (MnSAs/NMC). This is accomplished through the strategic utilization of MnCl2 salt, which serves dual roles of a pore-forming agent and a template. The MnSAs/NMC catalyst demonstrates compelling electrocatalytic activity for the oxygen reduction reaction (ORR), with an impressive half-wave potential (E1/2 = 0.90 V), alongside superior capacitance reaching 444 F g-1 at 0.5 A g-1 for supercapacitors. Crucially, both experimental and theoretical simulations validate that the single-atom dispersed MnN2C2 optimizes the adsorption energy of reactants and intermediates in the ORR process and pseudocapacitive behavior, leading to excellent ORR activity and capacitive performance. Interestingly, MnSAs/NMC-based Zn-air batteries exhibit concurrently high-power density derived from capacitive property and high energy density enhanced by ORR process. This study presents a novel preparation method for single-atom catalysts, which paves the way for the commercial application of super energy storage and conversion devices.