Amorphous materials are some of the most promising electrolyte candidates for lithium metal batteries. The mechanical, electrochemical, chemical, and thermal properties can be regulated by modifying the compositions and structures of amorphous materials. Through understanding the working principles of amorphous materials as electrolytes/electrodes as well as providing more insights into constructing compatible electrolyte-electrode interfaces, superior amorphous materials-based batteries can be developed in the future. This project has prepared a novel polymer-based solid-state electrolyte using a ZIF-62 glass as a functional filler. The polymer-glass electrolyte shows uniform distribution of the functional filler and improvements in both ionic conductivity and mechanical properties. Upon addition of an ionic liquid (IL), the obtained polymer glass-IL electrolyte delivers high ionic conductivity, large electrochemical stability window, high lithium-ion transference number, and excellent inhibition of lithium dendrites growth. Moreover, full batteries based on the polymer-glass-IL electrolyte exhibit superior rate capability and cycle performance. Atomistic simulations demonstrate that the superior performance of this new composite electrolyte is attributed to the uniformly distributed defects on the surface of the ZIF-62 glass, giving rise to stronger interactions with the IL, which in turn leads to the formation of a less confined environment that facilitates ionic conductivity. A novel strategy of synthetic ZIF-62 glass layer has been proposed as a solution to improve the reversible lithium plating/stripping and suppress dendrite growth in lithium metal batteries. Simulations show that lithium ions have faster diffusion rate and smoother diffusion channels in ZIF-62 glass compared to ZIF-62 crystal. The performed experiments confirm that the ZIF-62 glass layer enables uniform Li-ion transport, achieving the rapid Li-ion infiltration/extraction, and promoting isotropic Li nucleation and growth. The fabricated lithium metal anode can operate for 300 h in symmetric batteries. Both LiFePO4 and high-voltage LiCoO2 based full batteries reveal high reversible capacities, superior rate performances, and long cycling stability properties up to 1000 cycles.
The project's outcomes have been disseminated within the scientific community through various channels. First, the research findings have been submitted or prepared for publication in peer-reviewed journals: (1) Metal-Organic Framework Glass as a Functional Filler Enables Enhanced Performance of Solid-State Polymer Electrolytes for Lithium Metal Batteries (Advanced Science, published); (2) Amorphous Materials for Lithium-Ion and Post-Lithium-Ion Batteries (Small, published); (3) High-Performance Dendrite-Free Lithium Metal Anode Based on Metal-organic Framework Glass (under review); (4) Amorphous Materials Based Heterostructure and Heterointerface for Rechargeable Batteries (in preparation). These papers will or have been disseminated within the academic community through various channels, including social media. Furthermore, the research has been presented at two prominent national/international conferences: (1) Annual Meeting of the Danish Electrochemical Society (Copenhagen, 2023); and (2) The 41st Annual International Battery Seminar & Exhibit (Orlando, 2024).
