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Title: Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells

Abstract

Lithium/Sulfur (Li/S) cells are a promising chemistry with potential to deliver a step-change in energy density compared to state-of-the-art Li-ion batteries. To minimize the environmental impact of the Li/S cell manufacturing and to compete with Li-ion cells in both performance and cost, electrodes cast using an aqueous process are highly desirable. Here we describe the discovery and application of a lithiated redox-mediating supramolecular binder based on the well-known n-type semiconductor, perylene bisimide, that forms high-fidelity sulfur electrodes from water-processed slurries. A 1.4-fold improvement in sulfur utilization at 3.0 C and 58% increase in capacity retention after 250 cycles at 1.5 C are reported for the prelithiated, supramolecular binder compared to control samples. These improvements are attributed to the self-assembly of lithiated perylene bisimide binders in water to yield nanowire web morphologies that increase interfacial area between electrode components and exhibit enhanced electrode-current collector adhesion.

Authors:
 [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1530337
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 3; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Hwa, Yoon, Frischmann, Peter D., Helms, Brett A., and Cairns, Elton J. Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.7b03870.
Hwa, Yoon, Frischmann, Peter D., Helms, Brett A., & Cairns, Elton J. Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells. United States. doi:10.1021/acs.chemmater.7b03870.
Hwa, Yoon, Frischmann, Peter D., Helms, Brett A., and Cairns, Elton J. Tue . "Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells". United States. doi:10.1021/acs.chemmater.7b03870. https://www.osti.gov/servlets/purl/1530337.
@article{osti_1530337,
title = {Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells},
author = {Hwa, Yoon and Frischmann, Peter D. and Helms, Brett A. and Cairns, Elton J.},
abstractNote = {Lithium/Sulfur (Li/S) cells are a promising chemistry with potential to deliver a step-change in energy density compared to state-of-the-art Li-ion batteries. To minimize the environmental impact of the Li/S cell manufacturing and to compete with Li-ion cells in both performance and cost, electrodes cast using an aqueous process are highly desirable. Here we describe the discovery and application of a lithiated redox-mediating supramolecular binder based on the well-known n-type semiconductor, perylene bisimide, that forms high-fidelity sulfur electrodes from water-processed slurries. A 1.4-fold improvement in sulfur utilization at 3.0 C and 58% increase in capacity retention after 250 cycles at 1.5 C are reported for the prelithiated, supramolecular binder compared to control samples. These improvements are attributed to the self-assembly of lithiated perylene bisimide binders in water to yield nanowire web morphologies that increase interfacial area between electrode components and exhibit enhanced electrode-current collector adhesion.},
doi = {10.1021/acs.chemmater.7b03870},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 3,
volume = 30,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 10 works
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Figures / Tables:

Figure 1 Figure 1: (a) Structure of supramolecular binder PBI 1, deprotonation to yield water soluble Li41, and operando reduction of Li41 to Li61. S electrodes with PBI binder were processed from water with either 1 or Li41 in this study. During Li/S cell cycling the electroactive PBI core undergoes reversible redoxmore » chemistry between Li41 and Li61 at 2.5 V vs. Li/Li+. (b) Aqueous solubility screens of PBI binders 1 and Li41. (c) Self-assembly of Li41 into lithiated supramolecular polymers via π-π stacking and intermolecular ion pairing.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.