Abstract
All-solid-state batteries (ASSBs) with Li metal anodes or Si anodes are promising candidates to achieve high energy density and improved safety, but they suffer from undesirable lithium dendrite growth or huge volume expansion, respectively. Here we synthesize a hard-carbon-stabilized Li–Si alloy anode in which sintering of Si leads to the transformation of micro-metre particles into dense continuum. A 3D ionic-electronic-conductive network composed of plastically deformable Li-rich phases (Li15Si4 and LiC6) that enlarges active area and relieves stress concentration is created in the anode, leading to improved electrode kinetics and mechanical stability. With the hard-carbon-stabilized Li-Si anode, full cells using LiCoO2 or LiNi0.8Co0.1Mn0.1O2 cathodes and Li6PS5Cl electrolyte achieve favourable rate capability and cycle stability. In particular, the ASSB with LiNi0.8Co0.1Mn0.1O2 at high loading of 5.86 mAh cm−2 delivers 5,000 cycles at 1 C (5.86 mA cm−2), demonstrating the potential of using hard-carbon-stabilized Li–Si alloy anodes for practical applications of ASSBs.
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Acknowledgements
This work is supported by Outstanding Youth Fund Project by the Department of Science and Technology of Jiangsu Province (grant number BK20220045), Key R&D Project funded by Department of Science and Technology of Jiangsu Province (grant number BE2020003), Key Program-Automobile Joint Fund of the National Natural Science Foundation of China (grant number U1964205), General Program of the National Natural Science Foundation of China (grant number 51972334), General Program of National Natural Science Foundation of Beijing (grant number 2202058), cultivation project of leading innovative experts in Changzhou City (CQ20210003), National Overseas High-level Expert Recruitment Program (grant number E1JF021E11), Talent Program of the Chinese Academy of Sciences, ‘Scientist Studio Program Funding’ from Yangtze River Delta Physics Research Center and Tianmu Lake Institute of Advanced Energy Storage Technologies (grant number TIES-SS0001) and Science and Technology Research Institute of China Three Gorges Corporation (grant number 202103402).
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W.Y. and F.W. conceived and designed the experimental work. W.Y. prepared samples and carried out experiments. Z.M., Y.X. and S.S. performed the simulation using phase field simulation. M.Y., T.M. and X.Z. assisted with sample preparation. Y.H. and Y.W. assisted with characterization. W.Y., Z.M. and F.W. wrote the paper. D.W., Y.H. and P.L. helped with visualization. Z.W., J.L., J.X., P.L., F.W., H.L. and L.C. discussed the results and revised or commented on the manuscript. F.W. acquired funding and supervised/managed the whole project.
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Z.M., Y.X. and S.S. are employed by ByteDance Research. The other authors declare no competing interests.
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Nature Energy thanks Felix Hippauf, Dong-Wan Kim and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Cycle test data and rate test data.
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Battery test source data and phase field simulation data.
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Cycle test data, rate test data, XRD source data and surface area source data.
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Rate test data and comparison data.
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Cycle test data and comparison data.
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Charge–discharge test source data, cycle test data, fast discharge test data and comparison data.
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XRD and XPS data.
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Yan, W., Mu, Z., Wang, Z. et al. Hard-carbon-stabilized Li–Si anodes for high-performance all-solid-state Li-ion batteries. Nat Energy 8, 800–813 (2023). https://doi.org/10.1038/s41560-023-01279-8
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DOI: https://doi.org/10.1038/s41560-023-01279-8
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