Ni Single Atom Decorated Porous Hollow Carbon Nanosphere‐Based Electrodes for High Performance Symmetric Solid‐State Supercapacitors

Abstract

Ni single atom containing hollow carbon nanospheres with nitrogen doping has been synthesized by carbonization of Ni(NO3)2/phloroglucinol‐formaldehyde polymer/silica composite. The samples have been characterized by powder X‐ray diffraction, nitrogen adsorption/desorption, electron microscopic, Raman and X‐ray photoelectron spectroscopic studies. The microstructure and surface area vary with the amount of Ni(NO3)2 employed in the syntheses and the carbonization environment. An optimized amount of nickel and argon as the carbonization gas afford Ni‐1.0@N@HCN‐Ar which possesses overall superior features. The uniformly dispersed Ni single atoms within the hollow porous carbon framework fully utilize all the electroactive sites thereby improving the supercapacitive performance. The specific capacitance of Ni‐1.0@N@HCN‐Ar reaches 777 F∙g‐1 at 1 A∙g‐1 with a Coulombic efficiency of 98.4% and excellent recyclability. The energy and power density of Ni‐1.0@N@HCN‐Ar are found to be high; at 1 A∙g‐1 its energy density is 155.4 Wh∙kg‐1 with a power density of 600.3 W∙kg‐1. At a high current density of 10 A∙g‐1 the material shows a high energy density of 118.4 Wh∙kg‐1 with excellent power density of 6003.4 W∙kg‐1. A symmetric solid‐state supercapacitor assembled with this material, Ni‐1.0@N@HCN‐Ar//Ni‐1.0@N@HCN‐Ar using H2SO4/PVA gel electrolyte shows a superior energy density value of 30 Wh∙kg‐1 at a power density of 1200 W∙kg‐1.