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Enabling a Durable Electrochemical Interface via an Artificial Amorphous Cathode Electrolyte Interphase for Hybrid Solid/Liquid Lithium-Metal Batteries |
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| Authors: | Jia-Yan Liang Dr. Xu-Dong Zhang Dr. Xian-Xiang Zeng Dr. Min Yan Prof. Ya-Xia Yin Prof. Sen Xin Wen-Peng Wang Dr. Xiong-Wei Wu Dr. Ji-Lei Shi Prof. Li-Jun Wan Prof. Yu-Guo Guo |
| Affiliation: | 1. CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence inMolecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMs), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China These authors contributed equally to this work.;2. CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence inMolecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMs), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China These authors contributed equally to this work.;3. School of Chemistry and Materials Science, Hunan Agricultural University, Changsha, 410128 P. R. China;4. CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence inMolecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMs), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China;5. CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence inMolecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMs), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China |
| Abstract: | A hybrid solid/liquid electrolyte with superior security facilitates the implementation of high-energy-density storage devices, but it suffers from inferior chemical compatibility with cathodes. Herein, an optimal lithium difluoro(oxalato)borate salt was introduced to build in situ an amorphous cathode electrolyte interphase (CEI) between Ni-rich cathodes and hybrid electrolyte. The CEI preserves the surface structure with high compatibility, leading to enhanced interfacial stability. Meanwhile, the space-charge layer can be prominently mitigated at the solid/solid interface via harmonized chemical potentials, acquiring promoted interfacial dynamics as revealed by COMSOL simulation. Consequently, the amorphous CEI integrates the bifunctionality to provide an excellent cycling stability, high Coulombic efficiency, and favorable rate capability in high-voltage Li-metal batteries, innovating the design philosophy of functional CEI strategy for future high-energy-density batteries. |
| Keywords: | Amorphe Phasen Grenzflächen-Elektrochemie Grenzflächenstabilität Hybrid-Fest/flüssig-Batterien Kathoden-Elektrolyt-Interphasen |