Electron-ion conjugation sites co-constructed by defects and heteroatoms assisted carbon electrodes for high-performance aqueous energy storage

Abstract

Rapid preparation strategies of carbon-based materials with a high power density and energy density are crucial for the large-scale application of carbon materials in energy storage. However, achieving these goals quickly and efficiently remains challenging. Herein, the rapid redox reaction of concentrated H2SO4 and sucrose was employed as a means to destroy the perfect carbon lattice to form defects and insert large numbers of heteroatoms into the defects to rapidly form electron-ion conjugated sites of carbon materials at room temperature. Among prepared samples, CS-800-2 showed an excellent electrochemical performance (377.7 F g−1, 1 A g−1) and high energy density in 1 M H2SO4 electrolyte owing to its large specific surface area and a significant number of electron-ion conjugated sites. Additionally, CS-800-2 exhibited desirable energy storage performance in other aqueous electrolytes containing various metal ions. The theoretical calculation results revealed increased charge density near the carbon lattice defects, and the presence of heteroatoms effectively reduced the adsorption energy of carbon materials toward cations. Accordingly, the constructed “electron-ion” conjugated sites comprising defects and heteroatoms on the super-large surface of carbon-based materials accelerated the pseudo-capacitance reactions on the material surface, thereby greatly enhancing the energy density of carbon-based materials without sacrificing power density. In sum, a fresh theoretical perspective for constructing new carbon-based energy storage materials was provided, promising for future development of high-performance energy storage materials and devices.