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Tuning the Solid Electrolyte Interphase for Selective Li‐ and Na‐Ion Storage in Hard Carbon
Authors:Fernando A. Soto  Pengfei Yan  Mark H. Engelhard  Asma Marzouk  Chongmin Wang  Guiliang Xu  Zonghai Chen  Khalil Amine  Jun Liu  Vincent L. Sprenkle  Fedwa El‐Mellouhi  Perla B. Balbuena  Xiaolin Li
Affiliation:1. Department of Chemical Engineering, Texas A&M University, College Station, TX, USA;2. Pacific Northwest National Laboratory, Richland, WA, USA;3. Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, Doha, Qatar;4. Chemical Sciences and Engineering Division, Argonne National Laboratory, Argonne, IL, USA
Abstract:Solid‐electrolyte interphase (SEI) films with controllable properties are highly desirable for improving battery performance. In this paper, a combined experimental and theoretical approach is used to study SEI films formed on hard carbon in Li‐ and Na‐ion batteries. It is shown that a stable SEI layer can be designed by precycling an electrode in a desired Li‐ or Na‐based electrolyte, and that ionic transport can be kinetically controlled. Selective Li‐ and Na‐based SEI membranes are produced using Li‐ or Na‐based electrolytes, respectively. The Na‐based SEI allows easy transport of Li ions, while the Li‐based SEI shuts off Na‐ion transport. Na‐ion storage can be manipulated by tuning the SEI layer with film‐forming electrolyte additives, or by preforming an SEI layer on the electrode surface. The Na specific capacity can be controlled to < 25 mAh g?1; ≈ 1/10 of the normal capacity (250 mAh g?1). Unusual selective/preferential transport of Li ions is demonstrated by preforming an SEI layer on the electrode surface and corroborated with a mixed electrolyte. This work may provide new guidance for preparing good ion‐selective conductors using electrochemical approaches.
Keywords:Li‐ion batteries  Na‐ion batteries  selective ion transfer  solid‐electrolyte interphase
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