Synergistic Regulation of Intrinsic Lithiophilicity and Mass Transport Kinetics of Non-Lithium-Alloying Nucleation Sites for Stable Operation of Low N/P Ratio Lithium Metal Batteries |
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Authors: | Minjun Bae Sung-Joon Park Minki Kim Eunji Kwon Seungho Yu Juhyung Choi Yujin Chang Yonghwan Kim Yoon Jeong Choi Hwichan Hong Liwei Lin Wang Zhang Seungman Park Ji Young Maeng Jungjin Park Seung-Yong Lee Seung-Ho Yu Yuanzhe Piao |
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Institution: | 1. Department of Applied Bioengineering, Graduate School of Convergence Science and Technology, Seoul National University, 145 Gwanggyo-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do, 16229 Republic of Korea;2. Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul, 02841 Republic of Korea;3. Division of Materials Science and Engineering, Hanyang University, 222 Wangshimni-ro, Seongdong-gu, Seoul, 04763 Republic of Korea;4. Energy Storage Research Center, Korea Institute of Science and Technology, Seoul, 02792 Republic of Korea;5. Department of Transdisciplinary Studies, Graduate School of Convergence Science and Technology, Seoul National University, 145 Gwanggyo-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do, 16229 Republic of Korea;6. Department of Applied Bioengineering, Graduate School of Convergence Science and Technology, Seoul National University, 145 Gwanggyo-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do, 16229 Republic of Korea
School of Chemistry and Chemical Engineering, Yangzhou University, Jiangsu, 225009 P. R. China |
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Abstract: | Constructing functional materials on a 3D host is an efficient strategy to tackle issues of lithium (Li) metal anodes. Although non-Li-alloying materials provide structural stability during cycling due to reduced lattice distortions, low lithiophilicity and sluggish mass transport kinetics limit their functionality. Herein, a synergistic strategy is proposed to improve intrinsic lithiophilicity and mass transport kinetics of non-Li-alloying nucleation sites and demonstrate its remarkable efficacy. Two carbon fiber (CF) hosts coated by non-Li-alloying nanosheets with and without oxygen-enriched carbon filler (OCF) as lithiophilicity and mass transport booster (OCF-DSC@CF and DSC@CF, respectively) are constructed and their physiochemical properties are systematically evaluated to reveal the efficacy of OCF. By advanced characterization techniques, including 3D tomography and location-dependent electron energy loss spectroscopies, the complex heterostructure of OCF-DSC@CF with distinctive roles of each constituent is clearly identified. As verified by theoretical and electrochemical analyses, the incorporation of OCF endows OCF-DSC@CF with substantially improved lithiophilicity and mass transport kinetics. Moreover, OCF-DSC@CF induces a multifunctional SEI enriched with LiF and LiCx, which exhibits well-balanced electrical resistivity and ionic conductivity. Benefiting from these attributes, OCF-DSC@CF exhibits an unprecedented cyclability under a low N/P ratio of 1.8, achieving 700 cycles at 0.5C with an exceptional capacity retention of 97.8%. |
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Keywords: | intrinsic lithiophilicity lithium metal battery low N/P ratio mass transport kinetic synergistic regulation |
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