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Nitrogen-Triggered Amorphization Enables High-Performance Solid-State Electrolytes
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DOI：10.1039/D5EE05943G.png)
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Abstract
En 中文
Amorphous solid-state electrolytes (SSEs) hold great promise for advancing the application of all-solid-state batteries (ASSBs); owing to their favorable ionic conductivity; structural tunability; and promising electrochemical performance. However; the absence of universal design principles for amorphous SSEs limits their development. By fundamentally re-evaluating the amorphization-forming ability of amorphous SSE systems; this study establishes a nitrogen-driven universal strategy to convert diverse metal chlorides into amorphous xLi3N-MCly (0.3 ≤ 3x ≤ 1.9; M denotes a metal element; 2 ≤ y ≤ 5) SSE. Nitrogen synergistically disrupts crystalline order via distorted coordination polyhedra and N-bridged networks; while dynamic bond reorganization enables rapid Li+ migration; achieving ionic conductivity of 2.02 mS cm‒1 for 0.533Li3N-HfCl4 at 25 °C. Structural-property relationships reveal that high charge density and bridging capability of N3‒ enhance network disorder; shorten metal-coordinating atom distances; and optimize Li+ diffusion pathway connectivity. ASSBs employing 0.533Li3N-HfCl4 retain 81.87% capacity after 2000 cycles at 1; 000 mA g‒1 with high cathode loading (6.24 mg cm‒2); demonstrating engineering viability. This work provides a paradigm for rational design of high-performance amorphous SSEs.
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