Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries
Abstract All-solid-state Li metal batteries (ASSLMBs) promise superior safety and energy density compared to conventional Li-ion batteries. However, their widespread adoption is hindered by detrimental interfacial reactions between solid-state electrolytes (SSEs) and the Li negative electrode, compr...
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Nature Portfolio
2025-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-58522-x |
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| author | Longyun Shen Zilong Wang Shengjun Xu Ho Mei Law Yanguang Zhou Francesco Ciucci |
| author_facet | Longyun Shen Zilong Wang Shengjun Xu Ho Mei Law Yanguang Zhou Francesco Ciucci |
| author_sort | Longyun Shen |
| collection | DOAJ |
| description | Abstract All-solid-state Li metal batteries (ASSLMBs) promise superior safety and energy density compared to conventional Li-ion batteries. However, their widespread adoption is hindered by detrimental interfacial reactions between solid-state electrolytes (SSEs) and the Li negative electrode, compromising long-term cycling stability. The challenges in directly observing these interfaces impede a comprehensive understanding of reaction mechanisms, necessitating first-principle simulations for designing novel interlayer materials. To overcome these limitations, we develop a database-supported high-throughput screening (DSHTS) framework for identifying stable interlayer materials compatible with both Li and SSEs. Using Li3InCl6 as a model SSE, we identify Li3OCl as a potential interlayer material. Experimental validation demonstrates significantly improved electrochemical performance in both symmetric- and full-cell configurations. A Li|Li3OCl|Li3InCl6|LiCoO2 cell exhibits an initial discharge capacity of 154.4 mAh/g (1.09 mA/cm2, 2.5–4.2 V vs. Li/Li+, 303 K) with 76.36% capacity retention after 1000 cycles. Notably, a cell with a conventional In-Li6PS5Cl interlayer delivers only 132.4 mAh/g and fails after 760 cycles. An additional interlayer-containing battery with Li(Ni0.8Co0.1Mn0.1)O2 as the positive electrode achieves an initial discharge capacity of 151.3 mAh/g (3.84 mA/cm2, 2.5–4.2 V vs. Li/Li+, 303 K), maintaining stable operation over 1650 cycles. The results demonstrate the promise of the DSHTS framework for identifying interlayer materials. |
| format | Article |
| id | doaj-art-67f2d77ff11f46a29b4abd177ad7ca2a |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-67f2d77ff11f46a29b4abd177ad7ca2a2025-08-20T02:28:10ZengNature PortfolioNature Communications2041-17232025-04-011611910.1038/s41467-025-58522-xHarnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteriesLongyun Shen0Zilong Wang1Shengjun Xu2Ho Mei Law3Yanguang Zhou4Francesco Ciucci5Division of Emerging Interdisciplinary Areas, The Hong Kong University of Science and Technology, Clear Water BayDepartment of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Clear Water BayChair of Electrode Design for Electrochemical Energy Systems, University of BayreuthChair of Electrode Design for Electrochemical Energy Systems, University of BayreuthDepartment of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Clear Water BayDepartment of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Clear Water BayAbstract All-solid-state Li metal batteries (ASSLMBs) promise superior safety and energy density compared to conventional Li-ion batteries. However, their widespread adoption is hindered by detrimental interfacial reactions between solid-state electrolytes (SSEs) and the Li negative electrode, compromising long-term cycling stability. The challenges in directly observing these interfaces impede a comprehensive understanding of reaction mechanisms, necessitating first-principle simulations for designing novel interlayer materials. To overcome these limitations, we develop a database-supported high-throughput screening (DSHTS) framework for identifying stable interlayer materials compatible with both Li and SSEs. Using Li3InCl6 as a model SSE, we identify Li3OCl as a potential interlayer material. Experimental validation demonstrates significantly improved electrochemical performance in both symmetric- and full-cell configurations. A Li|Li3OCl|Li3InCl6|LiCoO2 cell exhibits an initial discharge capacity of 154.4 mAh/g (1.09 mA/cm2, 2.5–4.2 V vs. Li/Li+, 303 K) with 76.36% capacity retention after 1000 cycles. Notably, a cell with a conventional In-Li6PS5Cl interlayer delivers only 132.4 mAh/g and fails after 760 cycles. An additional interlayer-containing battery with Li(Ni0.8Co0.1Mn0.1)O2 as the positive electrode achieves an initial discharge capacity of 151.3 mAh/g (3.84 mA/cm2, 2.5–4.2 V vs. Li/Li+, 303 K), maintaining stable operation over 1650 cycles. The results demonstrate the promise of the DSHTS framework for identifying interlayer materials.https://doi.org/10.1038/s41467-025-58522-x |
| spellingShingle | Longyun Shen Zilong Wang Shengjun Xu Ho Mei Law Yanguang Zhou Francesco Ciucci Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries Nature Communications |
| title | Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries |
| title_full | Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries |
| title_fullStr | Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries |
| title_full_unstemmed | Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries |
| title_short | Harnessing database-supported high-throughput screening for the design of stable interlayers in halide-based all-solid-state batteries |
| title_sort | harnessing database supported high throughput screening for the design of stable interlayers in halide based all solid state batteries |
| url | https://doi.org/10.1038/s41467-025-58522-x |
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