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Constructing Superionic Heterointerface via Multiphase Engineering to Achieve Stable Oxyhalide-Based All-Solid-State Batteries
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DOI：10.1002/anie.1909915.png)
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Abstract
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Amorphous oxyhalides attract great interest as solid-state electrolytes (SSEs) in all-solid-state batteries (ASSBs) because of their oxidative stability, low cost, and mechanical deformability. But the limited room-temperature ionic conductivity and the parasitic reactions on cathode/halide interfaces impede their practical applications. Herein, we adopt a facile multiphase regulation strategy by incorporating ZrB2 and ZrN into an amorphous 1.3Li2O-ZrCl4 (LZCO) matrix to simultaneously enhance Li+ transport and interfacial stability. ZrB2 and ZrN regulate the bridging-oxygen/non-bridging-oxygen ratio to promote amorphization and create superionic heterointerfaces, which enables a more continuous Li+ conduction network while preserving overall electronic insulation. The multiphase architecture mitigates the interfacial side reactions, improves the interface compatibility due to the formation of B-O and N-O bonds, and homogenizes electron transport pathways in the composite cathode. As a result, 1.3Li2O-0.8ZrCl4-0.1ZrB2-0.1ZrN (LZCOBN0.1) shows a high room-temperature ionic conductivity of 2.41 mS cm−1, compared with 1.3 mS cm−1 for pristine LZCO. ASSBs employing LZCOBN0.1 and LiNi0.90Co0.05Mn0.05O2 deliver a high initial capacity of 210 mAh g−1 at 0.1 C and retain 82.7% capacity after 2000 cycles at 3 C, demonstrating ultrahigh cycling stability. This work highlights the potential of phase engineering regulation in developing high-performance amorphous oxyhalide-based ASSBs.
Keywords:
all-solid-state batteries
amorphization
halide solid electrolytes
oxyhalides
superionic heterointerface
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