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Title: A High-Rate Aqueous Proton Battery Delivering Power Below -78 °C via an Unfrozen Phosphoric Acid

Abstract

Lithium-sulfur batteries are attractive for automobile and grid applications due to their high theoretical energy density and the abundance of sulfur. Despite the significant progress in cathode development, lithium metal degradation and the polysulfide shuttle remain two critical challenges in the practical application of Li-S batteries. Development of advanced electrolytes has become a promising strategy to simultaneously suppress lithium dendrite formation and prevent polysulfide dissolution. Here, a new class of concentrated siloxane-based electrolytes, demonstrating significantly improved performance over the widely investigated ether-based electrolytes are reported in terms of stabilizing the sulfur cathode and Li metal anode as well as minimizing flammability. Through a combination of experimental and computational investigation, it is found that siloxane solvents can effectively regulate a hidden solvation-ion-exchange process in the concentrated electrolytes that results from the interactions between cations/anions and solvents. As a result, it could invoke a quasi-solid-solid lithiation and enable reversible Li plating/stripping and robust solid-electrolyte interphase chemistries. The solvation-ion-exchange process in the concentrated electrolytes is a key factor in understanding and designing electrolytes for other high-energy lithium metal batteries.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [3];  [2]; ORCiD logo [2];  [1]
+ Show Author Affiliations
  1. Oregon State University, Corvallis, OR (United States)
  2. Argonne National Laboratory (ANL), Lemont, IL (United States)
  3. Hewlett‐Packard Company, Corvallis, OR (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1658599
Alternate Identifier(s):
OSTI ID: 1632241
Grant/Contract Number:  
AC02-06CH11357; AC02‐06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 10; Journal Issue: 28; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Aqueous electrolyte; battery; low temperature; phosphoric acid; proton

Citation Formats

Jiang, Heng, Shin, Woochul, Ma, Lu, Hong, Jessica J., Wei, Zhixuan, Liu, Yusung, Zhang, Suoying, Wu, Xianyong, Xu, Yunkai, Guo, Qiubo, Subramanian, Mas A., Stickle, William F., Wu, Tianpin, Lu, Jun, and Ji, Xiulei. A High-Rate Aqueous Proton Battery Delivering Power Below -78 °C via an Unfrozen Phosphoric Acid. United States: N. p., 2020. Web. doi:10.1002/aenm.202000968.
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Jiang, Heng, Shin, Woochul, Ma, Lu, Hong, Jessica J., Wei, Zhixuan, Liu, Yusung, Zhang, Suoying, Wu, Xianyong, Xu, Yunkai, Guo, Qiubo, Subramanian, Mas A., Stickle, William F., Wu, Tianpin, Lu, Jun, & Ji, Xiulei. A High-Rate Aqueous Proton Battery Delivering Power Below -78 °C via an Unfrozen Phosphoric Acid. United States. https://doi.org/10.1002/aenm.202000968
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Jiang, Heng, Shin, Woochul, Ma, Lu, Hong, Jessica J., Wei, Zhixuan, Liu, Yusung, Zhang, Suoying, Wu, Xianyong, Xu, Yunkai, Guo, Qiubo, Subramanian, Mas A., Stickle, William F., Wu, Tianpin, Lu, Jun, and Ji, Xiulei. Mon . "A High-Rate Aqueous Proton Battery Delivering Power Below -78 °C via an Unfrozen Phosphoric Acid". United States. https://doi.org/10.1002/aenm.202000968. https://www.osti.gov/servlets/purl/1658599.
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@article{osti_1658599,
title = {A High-Rate Aqueous Proton Battery Delivering Power Below -78 °C via an Unfrozen Phosphoric Acid},
author = {Jiang, Heng and Shin, Woochul and Ma, Lu and Hong, Jessica J. and Wei, Zhixuan and Liu, Yusung and Zhang, Suoying and Wu, Xianyong and Xu, Yunkai and Guo, Qiubo and Subramanian, Mas A. and Stickle, William F. and Wu, Tianpin and Lu, Jun and Ji, Xiulei},
abstractNote = {Lithium-sulfur batteries are attractive for automobile and grid applications due to their high theoretical energy density and the abundance of sulfur. Despite the significant progress in cathode development, lithium metal degradation and the polysulfide shuttle remain two critical challenges in the practical application of Li-S batteries. Development of advanced electrolytes has become a promising strategy to simultaneously suppress lithium dendrite formation and prevent polysulfide dissolution. Here, a new class of concentrated siloxane-based electrolytes, demonstrating significantly improved performance over the widely investigated ether-based electrolytes are reported in terms of stabilizing the sulfur cathode and Li metal anode as well as minimizing flammability. Through a combination of experimental and computational investigation, it is found that siloxane solvents can effectively regulate a hidden solvation-ion-exchange process in the concentrated electrolytes that results from the interactions between cations/anions and solvents. As a result, it could invoke a quasi-solid-solid lithiation and enable reversible Li plating/stripping and robust solid-electrolyte interphase chemistries. The solvation-ion-exchange process in the concentrated electrolytes is a key factor in understanding and designing electrolytes for other high-energy lithium metal batteries.},
doi = {10.1002/aenm.202000968},
journal = {Advanced Energy Materials},
number = 28,
volume = 10,
place = {United States},
year = {2020},
month = {6}
}
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https://doi.org/10.1002/aenm.202000968
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