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Specific ion effects at graphitic interfaces

Author

Listed:
  • Cheng Zhan

    (Lawrence Livermore National Laboratory)

  • Maira R. Cerón

    (Lawrence Livermore National Laboratory)

  • Steven A. Hawks

    (Lawrence Livermore National Laboratory)

  • Minoru Otani

    (National Institute of Advanced Industrial Science and Technology (AIST))

  • Brandon C. Wood

    (Lawrence Livermore National Laboratory)

  • Tuan Anh Pham

    (Lawrence Livermore National Laboratory)

  • Michael Stadermann

    (Lawrence Livermore National Laboratory)

  • Patrick G. Campbell

    (Lawrence Livermore National Laboratory)

Abstract

Improved understanding of aqueous solutions at graphitic interfaces is critical for energy storage and water desalination. However, many mechanistic details remain unclear, including how interfacial structure and response are dictated by intrinsic properties of solvated ions under applied voltage. In this work, we combine hybrid first-principles/continuum simulations with electrochemical measurements to investigate adsorption of several alkali-metal cations at the interface with graphene and within graphene slit-pores. We confirm that adsorption energy increases with ionic radius, while being highly dependent on the pore size. In addition, in contrast with conventional electrochemical models, we find that interfacial charge transfer contributes non-negligibly to this interaction and can be further enhanced by confinement. We conclude that the measured interfacial capacitance trends result from a complex interplay between voltage, confinement, and specific ion effects-including ion hydration and charge transfer.

Suggested Citation

  • Cheng Zhan & Maira R. Cerón & Steven A. Hawks & Minoru Otani & Brandon C. Wood & Tuan Anh Pham & Michael Stadermann & Patrick G. Campbell, 2019. "Specific ion effects at graphitic interfaces," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12854-7
    DOI: 10.1038/s41467-019-12854-7
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