Constructing Hybrid Solid–Liquid Li+ Transport Networks for Fast-Charging Thick Electrodes
Jiacheng Zhu, Xuewei Gu, Hongmei Song, Defu Cao, Jiliang Qiu, Qi Yang, Huajun Li, Shuwei Li, Wenjun Li, Ziwei Wang, Qiu Fang, Cong Zhong, Zhaoxiang Wang, Byoungwoo Kang, Jizhou Li, Huigen Yu, Yejing Li, Hong Li, Tao Cheng, Xuefeng WangAbstract
Fast-charging technology for high-energy-density lithium-ion batteries remains constrained by high interfacial impedance and sluggish Li+ transport within electrodes. Herein, hierarchical-sized Li1.5Al0.5Ti1.5(PO4)3 (LATP, particle ranging from 5 to 500 nm) is used to construct a hybrid solid–liquid Li+ transport network in high-mass-loading cathodes (27 mg cm–2). A combination of different characterization techniques is employed to understand the underlying working principle of LATP from the particle to the electrode scale. LATP nanograins (∼10 nm) adsorbed onto cathode particle surfaces reduce Li+ desolvation energy (43.30 vs 52.97 kJ mol–1) and stabilize a thin CEI after cycling. Submicron LATP particles (320–480 nm) infiltrate pores of thick electrodes, forming interconnected networks that increase the Li+ diffusion coefficient. Furthermore, LATP increases the Li+ transference number of the liquid electrolyte within LATP-permeated regions. Consequently, LiNi0.8Co0.1Mn0.1O2||Li cells with LATP-blended cathodes deliver dramatically enhanced rate performance (102 vs 36 mAh g–1 at 0.75C and –10 °C).