Agglomeration-Free and Air-Inert Garnet for Upgrading PEO/Garnet Composite Solid State Electrolyte
Jun Cheng,
Hongqiang Zhang,
Deping Li,
Yuanyuan Li,
Zhen Zeng,
Fengjun Ji,
Youri Wei,
Xiao Xu,
Qing Sun,
Shang Wang,
Jingyu Lu,
Lijie Ci
Affiliations
Jun Cheng
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Hongqiang Zhang
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Deping Li
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Yuanyuan Li
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Zhen Zeng
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Fengjun Ji
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Youri Wei
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Xiao Xu
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Qing Sun
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Shang Wang
State Key Laboratory of Advanced Welding and Joining, Harbin Institute of Technology, Harbin 150001, China
Jingyu Lu
School of Science, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Lijie Ci
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China
Due to the intrinsically high ionic conductivity and good interfacial stability towards lithium, garnet-type solid electrolytes are usually introduced into polymer electrolytes as fillers to prepare polymer/garnet composite electrolytes, which can improve the ionic conductivity and enhance the mechanical strength to suppress Li dendrites. However, the surface Li2CO3 and/or LiOH passive layers which form when garnet is exposed to the air greatly reduce the enhancement effect of garnet on the composite electrolyte. Furthermore, compared with micro-size particles, nano-size garnet fillers exhibit a better effect on enhancing the performance of composite solid electrolytes. Nevertheless, inferior organic/inorganic interphase compatibility and high specific surface energy of nanofillers inevitably cause agglomeration, which severely hinders the effect of nanoparticles for promoting composite solid electrolytes. Herein, a cost-effective amphipathic 3-Aminopropyltriethoxysilane coupling agent is introduced to modify garnet fillers, which effectively expands the air stability of garnet and greatly improves the dispersion of garnet fillers in the polymer matrix. The well-dispersed garnet filler/polymer interface is intimate through the bridging effect of the silane coupling agent, resulting in boosted ionic conductivity (0.72 × 10−4 S/cm at room temperature) of the composite electrolyte, enhanced stability against lithium dendrites (critical current density > 0.5 mA/cm2), and prolonged cycling life of LFP/Li full cells.