Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 117, Issue 48, Pages 30135-30141Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2001837117
Keywords
electrochemical interface; solid-electrolyte interphase; metallic anodes; functionalized reduced graphene oxide
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Funding
- Office of Vehicle Technologies of the US Department of Energy, through the Advanced Battery Materials Research Program (Battery500 Consortium) [DE-EE0008198]
- NSF [DMR-1952877]
- Army Research Laboratory [W911NF-12-2-0023]
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Metallic anodes (lithium, sodium, and zinc) are attractive for rechargeable battery technologies but are plagued by an unfavorable metal-electrolyte interface that leads to nonuniform metal deposition and an unstable solid-electrolyte interphase (SEI). Here we report the use of electrochemically labile molecules to regulate the electrochemical interface and guide even lithium deposition and a stable SEI. The molecule, benzenesulfonyl fluoride, was bonded to the surface of a reduced graphene oxide aerogel. During metal deposition, this labile molecule not only generates a metal-coordinating benzenesulfonate anion that guides homogeneous metal deposition but also contributes lithium fluoride to the SEI to improve Li surface passivation. Consequently, high-efficiency lithium deposition with a low nucleation overpotential was achieved at a high current density of 6.0 mA cm(-2). A LijLiCoO(2) cell had a capacity retention of 85.3% after 400 cycles, and the cell also tolerated low-temperature (-10 degrees C) operation without additional capacity fading. This strategy was applied to sodium and zinc anodes as well.
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