Molecularly Engineered Artificial Solid Electrolyte Interphase with Tailored Lithiophilicity and Solvent-Phobicity for Stable Lithium Metal Batteries
Yeong Hun Jeong
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
Search for more papers by this authorGwangbin Won
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
Search for more papers by this authorSeunghyeon Kim
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
Search for more papers by this authorDaun Jeong
Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, MN, 55455 USA
Search for more papers by this authorDa-Sol Kwon
Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul, 02841 Republic of Korea
Energy Storage Research Center, Korea Institute of Science and Technology (KIST), 14 Gil 5 Hwarang-ro, Seongbuk-gu, Seoul, 02792 Republic of Korea
Search for more papers by this authorDa Kyoung Yong
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorJaehyuk Choi
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorHyun Woo Ahn
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorSulkyung Kim
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorMiso Lim
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorCorresponding Author
Jimin Shim
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
E-mail: [email protected]
Search for more papers by this authorYeong Hun Jeong
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
Search for more papers by this authorGwangbin Won
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
Search for more papers by this authorSeunghyeon Kim
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
Search for more papers by this authorDaun Jeong
Department of Chemical Engineering and Materials Science, University of Minnesota, Minneapolis, MN, 55455 USA
Search for more papers by this authorDa-Sol Kwon
Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul, 02841 Republic of Korea
Energy Storage Research Center, Korea Institute of Science and Technology (KIST), 14 Gil 5 Hwarang-ro, Seongbuk-gu, Seoul, 02792 Republic of Korea
Search for more papers by this authorDa Kyoung Yong
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorJaehyuk Choi
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorHyun Woo Ahn
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorSulkyung Kim
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorMiso Lim
Kolon Industries, Inc., Seoul, 07793 Republic of Korea
Search for more papers by this authorCorresponding Author
Jimin Shim
Department of Chemistry Education, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul, 08826 Republic of Korea
E-mail: [email protected]
Search for more papers by this authorAbstract
Lithium (Li) metal is recognized as a promising anode material for rechargeable batteries primarily due to its high specific capacity and energy density. However, a major challenge persists in uncontrolled Li electrodeposition and irregular solid electrolyte interphase (SEI) formation during cycling, leading to premature cell failure and safety hazards. Herein, an artificial SEI is presented for Li metal with tailored lithiophilicity and solvent-phobicity to address these critical issues. As a model system for the artificial SEI, a series of polyethyleneimine (PEI) substituted by 1,2-epoxyhexane (EH) (PEI-EH) is introduced, consisting of lithiophilic, nitrogen-rich PEI, which promotes Li ion solvation and regulates uniform ion flux. The abundant amine groups in PEI are partially substituted with solvent-phobic hexyl groups to reduce electrolyte swelling and prevent solvent decomposition. By systematically modulating the physical properties of PEI-EH, including polarity and mechanical characteristics, an optimized artificial protective layer for Li metal that effectively suppresses Li dendrite growth and irregular SEI formation is identified. This study highlights the importance of molecular engineering in the design of artificial SEIs for achieving dendrite-free, long-lasting Li metal batteries.
Conflict of Interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available in the supplementary material of this article.
Supporting Information
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