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Title: Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode

Here, the physiochemical properties of the solid-electrolyte interphase, primarily governed by electrolyte composition, have a profound impact on the electrochemical cycling of metallic lithium. Herein, we discover that the effect of nitrate anions on regulating lithium deposition previously known in ether-based electrolytes can be extended to carbonate-based systems, which dramatically alters the nuclei from dendritic to spherical, albeit extremely limited solubility. This is attributed to the preferential reduction of nitrate during solid-electrolyte interphase formation, and the mechanisms behind which are investigated based on the structure, ion-transport properties, and charge transfer kinetics of the modified interfacial environment. To overcome the solubility barrier, a solubility-mediated sustained-release methodology is introduced, in which nitrate nanoparticles are encapsulated in porous polymer gel and can be steadily dissolved during battery operation to maintain a high concentration at the electroplating front. As such, effective dendrite suppression and remarkably enhanced cycling stability are achieved in corrosive carbonate electrolytes.
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [1] ;  [2]
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE
OSTI Identifier:
1475484

Liu, Yayuan, Lin, Dingchang, Li, Yuzhang, Chen, Guangxu, Pei, Allen, Nix, Oliver, Li, Yanbin, and Cui, Yi. Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode. United States: N. p., Web. doi:10.1038/s41467-018-06077-5.
Liu, Yayuan, Lin, Dingchang, Li, Yuzhang, Chen, Guangxu, Pei, Allen, Nix, Oliver, Li, Yanbin, & Cui, Yi. Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode. United States. doi:10.1038/s41467-018-06077-5.
Liu, Yayuan, Lin, Dingchang, Li, Yuzhang, Chen, Guangxu, Pei, Allen, Nix, Oliver, Li, Yanbin, and Cui, Yi. 2018. "Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode". United States. doi:10.1038/s41467-018-06077-5. https://www.osti.gov/servlets/purl/1475484.
@article{osti_1475484,
title = {Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode},
author = {Liu, Yayuan and Lin, Dingchang and Li, Yuzhang and Chen, Guangxu and Pei, Allen and Nix, Oliver and Li, Yanbin and Cui, Yi},
abstractNote = {Here, the physiochemical properties of the solid-electrolyte interphase, primarily governed by electrolyte composition, have a profound impact on the electrochemical cycling of metallic lithium. Herein, we discover that the effect of nitrate anions on regulating lithium deposition previously known in ether-based electrolytes can be extended to carbonate-based systems, which dramatically alters the nuclei from dendritic to spherical, albeit extremely limited solubility. This is attributed to the preferential reduction of nitrate during solid-electrolyte interphase formation, and the mechanisms behind which are investigated based on the structure, ion-transport properties, and charge transfer kinetics of the modified interfacial environment. To overcome the solubility barrier, a solubility-mediated sustained-release methodology is introduced, in which nitrate nanoparticles are encapsulated in porous polymer gel and can be steadily dissolved during battery operation to maintain a high concentration at the electroplating front. As such, effective dendrite suppression and remarkably enhanced cycling stability are achieved in corrosive carbonate electrolytes.},
doi = {10.1038/s41467-018-06077-5},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {9}
}

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