skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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)
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. https://doi.org/10.1021/acs.chemmater.7b03870
Hwa, Yoon, Frischmann, Peter D., Helms, Brett A., and Cairns, Elton J. 2018. "Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells". United States. https://doi.org/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},
url = {https://www.osti.gov/biblio/1530337}, journal = {Chemistry of Materials},
issn = {0897-4756},
number = 3,
volume = 30,
place = {United States},
year = {Tue Jan 09 00:00:00 EST 2018},
month = {Tue Jan 09 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 33 works
Citation information provided by
Web of Science

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

Save / Share:

Works referenced in this record:

Li–O2 and Li–S batteries with high energy storage
journal, January 2012


Advances in Li–S batteries
journal, January 2010


Nanostructured sulfur cathodes
journal, January 2013


Rechargeable Lithium–Sulfur Batteries
journal, July 2014


Polysulfide Shuttle Study in the Li/S Battery System
journal, January 2004


Electrochemistry of a nonaqueous lithium/sulfur cell
journal, January 1983


Amphiphilic Surface Modification of Hollow Carbon Nanofibers for Improved Cycle Life of Lithium Sulfur Batteries
journal, February 2013


A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries
journal, May 2009


Graphene Oxide as a Sulfur Immobilizer in High Performance Lithium/Sulfur Cells
journal, November 2011


Strong Lithium Polysulfide Chemisorption on Electroactive Sites of Nitrogen-Doped Carbon Composites For High-Performance Lithium-Sulfur Battery Cathodes
journal, February 2015


A Long-Life, High-Rate Lithium/Sulfur Cell: A Multifaceted Approach to Enhancing Cell Performance
journal, November 2013


Cathode Composites for Li–S Batteries via the Use of Oxygenated Porous Architectures
journal, October 2011


Graphene-Based Three-Dimensional Hierarchical Sandwich-type Architecture for High-Performance Li/S Batteries
journal, September 2013


Polysulfide-Blocking Microporous Polymer Membrane Tailored for Hybrid Li-Sulfur Flow Batteries
journal, August 2015


Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer
journal, January 2012


Polysulfide-containing Glyme-based Electrolytes for Lithium Sulfur Battery
journal, June 2015


Recent Advances in Electrolytes for Lithium-Sulfur Batteries
journal, April 2015


Electrochemical performance of lithium/sulfur cells with three different polymer electrolytes
journal, August 2000


Stabilizing lithium metal using ionic liquids for long-lived batteries
journal, June 2016


Challenges Facing Lithium Batteries and Electrical Double-Layer Capacitors
journal, September 2012


Redox-Active Supramolecular Polymer Binders for Lithium–Sulfur Batteries That Adapt Their Transport Properties in Operando
journal, October 2016


Supramolecular Perylene Bisimide-Polysulfide Gel Networks as Nanostructured Redox Mediators in Dissolved Polysulfide Lithium–Sulfur Batteries
journal, September 2015


The Use of Redox Mediators for Enhancing Utilization of Li 2 S Cathodes for Advanced Li–S Battery Systems
journal, February 2014


Review on Li-Sulfur Battery Systems: an Integral Perspective
journal, May 2015


Efficient dispersion of multi-walled carbon nanotubes in aqueous solution by non-covalent interaction with perylene bisimides
journal, January 2013


Self-assembled π-stacks of functional dyes in solution: structural and thermodynamic features
journal, January 2009


Molecular Assemblies of Perylene Bisimide Dyes in Water
journal, May 2012


Works referencing / citing this record:

High-Energy Aqueous Lithium Batteries
journal, June 2018


Dictating High‐Capacity Lithium–Sulfur Batteries through Redox‐Mediated Lithium Sulfide Growth
journal, June 2019


A Review of Functional Binders in Lithium-Sulfur Batteries
journal, October 2018


Housing Sulfur in Polymer Composite Frameworks for Li–S Batteries
journal, February 2019


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