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Title: Tuning the Solid Electrolyte Interphase for Selective Li- and Na-Ion Storage in Hard Carbon

Abstract

Solid-electrolyte interphase (SEI) with controllable properties are highly desirable to improve battery performance. In this paper, we use a combined experimental and simulation approach to study the SEI formation on hard carbon in Li and Na-ion batteries. We show that with proper additives, stable SEI can be formed on hard carbon by pre-cycling the electrode materials in Li or Na-ion electrolyte. Detailed mechanistic studies suggest that the ion transport in the SEI layer is kinetically controlled and can be tuned by the applied voltage. Selective Na and Li-ion SEI membranes are produced using the Na or Li-ion based electrolytes respectively. The large Na ion SEI allows easy transport of Li ions, while the small Li ion SEI shuts off the Na-ion transport. Na-ion storage can be manipulated by tuning the SEI with film-forming electrolyte additives or preforming a SEI on the electrodes’ surface. The Na specific capacity can be controlled to <25 mAh/g, ~1/10 of the normal capacity (250 mAh/g). Unusual selective/preferential transport of Li-ion is demonstrated by preforming a SEI on the electrode’s surface and corroborated with a mixed electrolyte. This work may provide new guidance for preparing good ion selective conductors using electrochemical approaches in the future.

Authors:
 [1];  [2];  [2];  [3];  [2];  [4];  [4];  [4];  [2];  [2];  [3];  [1];  [2]
  1. Department of Chemical Engineering, Texas A&M University, College Station TX 77843-3122 USA
  2. Pacific Northwest National Laboratory, 902 Battelle Boulevard Richland WA 99354 USA
  3. Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, P.O. Box 5825 Doha Qatar
  4. Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue Argonne IL 60439 USA
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE Office of Electricity Delivery and Energy Reliability (OE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1372989
Report Number(s):
PNNL-SA-121033
Journal ID: ISSN 0935-9648; 48877; TE1400000
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 18; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Environmental Molecular Sciences Laboratory

Citation Formats

Soto, Fernando A., Yan, Pengfei, Engelhard, Mark H., Marzouk, Asma, Wang, Chongmin, Xu, Guiliang, Chen, Zonghai, Amine, Khalil, Liu, Jun, Sprenkle, Vincent L., El-Mellouhi, Fedwa, Balbuena, Perla B., and Li, Xiaolin. Tuning the Solid Electrolyte Interphase for Selective Li- and Na-Ion Storage in Hard Carbon. United States: N. p., 2017. Web. doi:10.1002/adma.201606860.
Soto, Fernando A., Yan, Pengfei, Engelhard, Mark H., Marzouk, Asma, Wang, Chongmin, Xu, Guiliang, Chen, Zonghai, Amine, Khalil, Liu, Jun, Sprenkle, Vincent L., El-Mellouhi, Fedwa, Balbuena, Perla B., & Li, Xiaolin. Tuning the Solid Electrolyte Interphase for Selective Li- and Na-Ion Storage in Hard Carbon. United States. doi:10.1002/adma.201606860.
Soto, Fernando A., Yan, Pengfei, Engelhard, Mark H., Marzouk, Asma, Wang, Chongmin, Xu, Guiliang, Chen, Zonghai, Amine, Khalil, Liu, Jun, Sprenkle, Vincent L., El-Mellouhi, Fedwa, Balbuena, Perla B., and Li, Xiaolin. Tue . "Tuning the Solid Electrolyte Interphase for Selective Li- and Na-Ion Storage in Hard Carbon". United States. doi:10.1002/adma.201606860.
@article{osti_1372989,
title = {Tuning the Solid Electrolyte Interphase for Selective Li- and Na-Ion Storage in Hard Carbon},
author = {Soto, Fernando A. and Yan, Pengfei and Engelhard, Mark H. and Marzouk, Asma and Wang, Chongmin and Xu, Guiliang and Chen, Zonghai and Amine, Khalil and Liu, Jun and Sprenkle, Vincent L. and El-Mellouhi, Fedwa and Balbuena, Perla B. and Li, Xiaolin},
abstractNote = {Solid-electrolyte interphase (SEI) with controllable properties are highly desirable to improve battery performance. In this paper, we use a combined experimental and simulation approach to study the SEI formation on hard carbon in Li and Na-ion batteries. We show that with proper additives, stable SEI can be formed on hard carbon by pre-cycling the electrode materials in Li or Na-ion electrolyte. Detailed mechanistic studies suggest that the ion transport in the SEI layer is kinetically controlled and can be tuned by the applied voltage. Selective Na and Li-ion SEI membranes are produced using the Na or Li-ion based electrolytes respectively. The large Na ion SEI allows easy transport of Li ions, while the small Li ion SEI shuts off the Na-ion transport. Na-ion storage can be manipulated by tuning the SEI with film-forming electrolyte additives or preforming a SEI on the electrodes’ surface. The Na specific capacity can be controlled to <25 mAh/g, ~1/10 of the normal capacity (250 mAh/g). Unusual selective/preferential transport of Li-ion is demonstrated by preforming a SEI on the electrode’s surface and corroborated with a mixed electrolyte. This work may provide new guidance for preparing good ion selective conductors using electrochemical approaches in the future.},
doi = {10.1002/adma.201606860},
journal = {Advanced Materials},
issn = {0935-9648},
number = 18,
volume = 29,
place = {United States},
year = {2017},
month = {3}
}

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