Anion-intercalation lithium metal batteries (AILMBs) are appealing due to their low cost and fast intercalation/de-intercalation kinetics of graphite cathodes. However, the safety and cycliability of existing AILMBs are constrained by the scarcity of compatible electrolytes. Herein, we showcase that a difluoroester can be applied as electrolyte solvent to realize high-performance AILMBs, which not only endows high oxidation resistance, but also efficiently tunes the solvation shell to enable highly reversible and kinetically fast cathode reaction beyond the trifluoro counterpart. The difluoroester-based electrolyte demonstrates nonflammability, high ionic conductivity, and electrochemical stability, along with excellent electrode compatibility. The Li| |graphite AILMBs reach a high durability of 10000 cycles with only a 0.00128% capacity loss per cycle under fast-cycling of 1 A g, and retain ~63% of room-temperature capacity when discharging at -65 °C, meanwhile supply stable power output under deformation and overcharge conditions. The electrolyte design paves a promising path toward fast-rate, low-temperature, durable, and safe AILMBs.
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http://dx.doi.org/10.1038/s41467-024-49795-9 | DOI Listing |
Micromachines (Basel)
October 2024
Department of Chemical, Biological, and Battery Engineering, Gachon University, Seongnam-si 13120, Gyeonggi-do, Republic of Korea.
The demand for safer, sustainable, and economical energy storage devices has motivated the development of lithium dual-ion batteries (Li_DIBs) for large-scale storage applications. For the Li_DIBs, expanded graphite (EG) cathodes are valuable as anion intercalation host frameworks to fabricate safer and more cost-effective devices. In this study, three different carbon cathode materials, including microwave-treated expanded graphite (MW-EG), ball-milled expanded graphite (BM-EG), and high-temperature-carbonized carbon nanoflakes (CNFs), were developed by different synthesis methods.
View Article and Find Full Text PDFLangmuir
November 2024
Key Laboratory of UV-Emitting Materials and Technology, Northeast Normal University, Ministry of Education, Changchun 130024, China.
Intercalation of anions unlocks graphite as a positive material in energy storage devices, and the performance could be affected by solvents in solutions. In this context, it is vital to investigate the role of solvents in anion intercalation. Herein, a hierarchical intercalation phenomenon, in which different graphite intercalation compounds are generated in the same solution, is studied in lithium tetrafluoroborate (LiBF) solutions of carboxylate ester solvents γ-butyrolactone (GBL) and methyl acetate (MA).
View Article and Find Full Text PDFNat Commun
June 2024
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, China.
Adv Sci (Weinh)
July 2024
Department of Chemical System Engineering, School of Engineering, The University of Tokyo, Hongo 7-3-1, Bunkyo-ku, Tokyo, 113-8656, Japan.
This review article discusses the hidden or often overlooked negative issues of large-capacity cathodes, high-voltage systems, concentrated electrolytes, and reversible lithium metal electrodes in high-energy-density lithium batteries and provides some feasible solutions that can realize the construction of realistic rechargeable batteries with higher energy densities. Similar objective discussion of the negative aspects of lithium-air batteries, multi-valent shuttles, anion shuttles, sulfur cathode systems, and all-solid ceramic batteries can help fabricate more realistic batteries.
View Article and Find Full Text PDFAdv Mater
November 2023
Department of Chemistry, Division of Advanced Materials Science, Pohang University of Science and Technology (POSTECH), Pohang, 37673, Republic of Korea.
Advanced energy-storage devices are indispensable for expanding electric mobility applications. While anion intercalation-type redox chemistry in graphite cathodes has opened the path to high-energy-density batteries, surpassing the limited energy density of conventional lithium-ion batteries , a significant challenge remains: the large volume expansion of graphite upon anion intercalation. In this study, a novel polymeric binder and cohesive graphite cathode design for dual-ion batteries (DIBs) is presented, which exhibits remarkable stability even under high voltage conditions (>5 V).
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