Journal Article

Doping‐Induced Electronic/Ionic Engineering to Optimize the Redox Kinetics for Potassium Storage: A Case Study of Ni‐Doped CoSe2

Shan, Hui, Wang, Jingjing, Sari, Hirbod Maleki Kheimeh, Yang, Huijuan, Luo, Yangyang, Li, Wenbin, Li, Xifei, Xiao, Wei, Qin, Jian, Lei, Li, Xie, Chong, Zhang, Gaini

2022

Overview

Heteroatom doping effectively tunes the electronic conductivity of transition metal selenides (TMSs) with rapid K+ accessibility in potassium ion batteries (PIBs). Although considerable efforts are dedicated to investigating the relationship between the doping strategy and the resulting electrochemistry, the doping mechanisms, especially in view of the ion and electronic diffusion kinetics upon cycling, are seldom elucidated systematically. Herein, the crystal structure stability, charge/ion state, and bandgap of the active materials are found to be precisely modulated by favorable heteroatom doping, resulting in intrinsically fast kinetics of the electrode materials. Based on the combined mechanisms of intercalation and conversion reactions, electron and K+ ion transfer in Ni‐doped CoSe2 embedded in carbon nanocomposites (Ni‐CoSe2@NC) can be significantly enhanced via electronic engineering. Benefiting from the synthetic controlled Ni grains, the heterointerface formed by the intermediate products of electrochemical reactions in Ni‐CoSe2@NC strengthens the conversion kinetics and interdiffusion process, developing a low‐barrier mesophase with optimized potassium storage. Overall, an electronic tuning strategy can offer deeper atomic insights into the conversion reaction of TMSs in PIBs. Heteroatom doping has a significant impact on boosting the performance of secondary battery systems. By engineering the electrodes with controllable composites, ionic and electronic diffusion kinetics are simultaneously obtained. The underlying electrochemical K storage mechanisms based on the intercalation/deintercalation and conversion reactions are illustrated in detail by electrochemical kinetic analysis, theoretical calculations, and X‐ray absorption spectroscopy.

• Publisher: John Wiley & Sons, Inc,John Wiley and Sons Inc,Wiley
• Subject: Adsorption / Carbon / diffusion dynamics / doping / electronic engineering / Nanocomposites / Nanoparticles / Pore size / Potassium / potassium‐ion batteries / Scanning electron microscopy / transition metal selenides / Transmission electron microscopy