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Title: Spatial Molecular Layer Deposition of Ultrathin Polyamide To Stabilize Silicon Anodes in Lithium-Ion Batteries

Abstract

Cycling stability is central to implementing silicon (Si) anodes in next-generation high-energy lithium-ion batteries. However, challenges remain due to the lack of effective strategies to enhance the structural integrity of the anode during electrochemical cycling. Here, we develop a nanoscale polyamide coating, using spatial molecular layer deposition (MLD) of m-phenylenediamine and trimesoyl chloride precursors, to preserve the structural integrity of Si anodes. Poly(acrylic acid) (PAA) has been widely used in Si-based anodes as a binding agent due to its effective binding interactions with Si particles. However, the structural integrity of the anode is compromised by thermochemical decomposition of the poly(acrylic acid) binder, which can occur during electrode drying or during electrochemical cycling. Decomposition causes a 62% decrease in the elastic modulus of the Si anode, as measured by nanoindentation in electrolyte-soaked conditions. This study shows that an ultrathin polyamide coating counteracts this structural degradation, increases the elastic modulus of the degraded anode by 345%, and improves cohesion. Electrochemical analysis of polyamide-coated anodes reveals a film thickness dependence in cycling behavior. High overpotentials and fast capacity fading are observed for Si anodes with a 15 nm coating, whereas Si anodes with a 0.5 nm coating demonstrate stable cycling over 150 cyclesmore » with a capacity >1400 mAh g-1. Our findings identify polyamide as an effective electrode coating material to enhance structural integrity, leading to excellent cyclability with higher capacity retention. Furthermore, the use of the spatial MLD approach to deposit the coating enables short deposition time and a facile route to scale-up.« less

Authors:
 [1];  [1];  [2];  [3];  [1];  [4];  [5];  [2];  [1];  [4]
  1. University of Colorado
  2. University of Kentucky
  3. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  4. Virginia Polytechnic Institute and State University
  5. Yeungnam University
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1544540
Report Number(s):
NREL/JA-5K00-74359
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
ACS Applied Energy Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 6
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 33 ADVANCED PROPULSION SYSTEMS; molecular layer deposition; surface modification; polyamide; silicon anodes; lithium-ion batteries

Citation Formats

Wallas, Jasmine M., Welch, Brian C., Wang, Yikai, Liu, Jun, Hafner, Simon E., Qiao, Rui, Yoon, Taeho, Cheng, Yang-Tse, George, Steven M., and Ban, Chunmei. Spatial Molecular Layer Deposition of Ultrathin Polyamide To Stabilize Silicon Anodes in Lithium-Ion Batteries. United States: N. p., 2019. Web. doi:10.1021/acsaem.9b00326.
Wallas, Jasmine M., Welch, Brian C., Wang, Yikai, Liu, Jun, Hafner, Simon E., Qiao, Rui, Yoon, Taeho, Cheng, Yang-Tse, George, Steven M., & Ban, Chunmei. Spatial Molecular Layer Deposition of Ultrathin Polyamide To Stabilize Silicon Anodes in Lithium-Ion Batteries. United States. doi:10.1021/acsaem.9b00326.
Wallas, Jasmine M., Welch, Brian C., Wang, Yikai, Liu, Jun, Hafner, Simon E., Qiao, Rui, Yoon, Taeho, Cheng, Yang-Tse, George, Steven M., and Ban, Chunmei. Fri . "Spatial Molecular Layer Deposition of Ultrathin Polyamide To Stabilize Silicon Anodes in Lithium-Ion Batteries". United States. doi:10.1021/acsaem.9b00326.
@article{osti_1544540,
title = {Spatial Molecular Layer Deposition of Ultrathin Polyamide To Stabilize Silicon Anodes in Lithium-Ion Batteries},
author = {Wallas, Jasmine M. and Welch, Brian C. and Wang, Yikai and Liu, Jun and Hafner, Simon E. and Qiao, Rui and Yoon, Taeho and Cheng, Yang-Tse and George, Steven M. and Ban, Chunmei},
abstractNote = {Cycling stability is central to implementing silicon (Si) anodes in next-generation high-energy lithium-ion batteries. However, challenges remain due to the lack of effective strategies to enhance the structural integrity of the anode during electrochemical cycling. Here, we develop a nanoscale polyamide coating, using spatial molecular layer deposition (MLD) of m-phenylenediamine and trimesoyl chloride precursors, to preserve the structural integrity of Si anodes. Poly(acrylic acid) (PAA) has been widely used in Si-based anodes as a binding agent due to its effective binding interactions with Si particles. However, the structural integrity of the anode is compromised by thermochemical decomposition of the poly(acrylic acid) binder, which can occur during electrode drying or during electrochemical cycling. Decomposition causes a 62% decrease in the elastic modulus of the Si anode, as measured by nanoindentation in electrolyte-soaked conditions. This study shows that an ultrathin polyamide coating counteracts this structural degradation, increases the elastic modulus of the degraded anode by 345%, and improves cohesion. Electrochemical analysis of polyamide-coated anodes reveals a film thickness dependence in cycling behavior. High overpotentials and fast capacity fading are observed for Si anodes with a 15 nm coating, whereas Si anodes with a 0.5 nm coating demonstrate stable cycling over 150 cycles with a capacity >1400 mAh g-1. Our findings identify polyamide as an effective electrode coating material to enhance structural integrity, leading to excellent cyclability with higher capacity retention. Furthermore, the use of the spatial MLD approach to deposit the coating enables short deposition time and a facile route to scale-up.},
doi = {10.1021/acsaem.9b00326},
journal = {ACS Applied Energy Materials},
number = 6,
volume = 2,
place = {United States},
year = {2019},
month = {5}
}