ACS Publications. Most Trusted. Most Cited. Most Read
Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells

OR SEARCH CITATIONS

My Activity
Publications

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:Chem. Mater. 2018, 30, 3, 685-691
    Article

    Aqueous-Processable Redox-Active Supramolecular Polymer Binders for Advanced Lithium/Sulfur Cells
    Click to copy article linkArticle link copied!

    View Author Information
    † Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, United States
    ‡ Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, United States
    § The Joint Center for Energy Storage Research, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, United States
    ∥ The Molecular Foundry, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720, United States
    *E-mail: [email protected] (B.A.H.).
    *E-mail: [email protected] (E.J.C.)
    Other Access OptionsSupporting Information (1)

    Chemistry of Materials

    Cite this: Chem. Mater. 2018, 30, 3, 685–691
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.7b03870
    Published January 9, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    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.

    Copyright © 2018 American Chemical Society

    Subjects

    what are subjects

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.7b03870.

    • 7Li NMR spectra, SEM, TGA results, Nyquist plots, and electrochemical test results (Figures S1–S8) (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!
    Citation Statements
    Explore this article's citation statements on scite.ai
    powered by  Scite

    This article is cited by 46 publications.

    1. Yuncong Xue, Yu Jin, Yifei Zhang, Fengmin Han, Feng Wang. Stimuli-Triggered Dynamic Transformations in Supramolecular Polymers. Chemistry of Materials 2024, 36 (13) , 6347-6369. https://doi.org/10.1021/acs.chemmater.4c01265
    2. Rui-Yang Wang, Haneol Kang, Moon Jeong Park. High-Capacity, Sustainable Lithium–Sulfur Batteries Based on Multifunctional Polymer Binders. ACS Applied Energy Materials 2021, 4 (3) , 2696-2706. https://doi.org/10.1021/acsaem.0c03244
    3. Feifei Wang, Jing Li, Juan Zhao, Yixiao Yang, Chenliang Su, Yu Lin Zhong, Quan-Hong Yang, Jiong Lu. Single-Atom Electrocatalysts for Lithium Sulfur Batteries: Progress, Opportunities, and Challenges. ACS Materials Letters 2020, 2 (11) , 1450-1463. https://doi.org/10.1021/acsmaterialslett.0c00396
    4. Yoon Hwa, Eongyu Yi, Hao Shen, Younghoon Sung, Jiawei Kou, Kai Chen, Dilworth Y. Parkinson, Marca M. Doeff, Elton J. Cairns. Three-Dimensionally Aligned Sulfur Electrodes by Directional Freeze Tape Casting. Nano Letters 2019, 19 (7) , 4731-4737. https://doi.org/10.1021/acs.nanolett.9b01805
    5. Xi-Yao Li, Meng Zhao, Yun-Wei Song, Chen-Xi Bi, Zheng Li, Zi-Xian Chen, Xue-Qiang Zhang, Bo-Quan Li, Jia-Qi Huang. Polysulfide chemistry in metal–sulfur batteries. Chemical Society Reviews 2025, 54 (10) , 4822-4873. https://doi.org/10.1039/D4CS00318G
    6. Christian Julien, Alain Mauger. Lithium-Sulfur Batteries. 2025, 591-749. https://doi.org/10.1007/978-3-031-67470-9_7
    7. Qiang He, Jiaoyi Ning, Hongming Chen, Zhixiang Jiang, Jianing Wang, Dinghui Chen, Changbin Zhao, Zhenguo Liu, Igor F. Perepichka, Hong Meng, Wei Huang. Achievements, challenges, and perspectives in the design of polymer binders for advanced lithium-ion batteries. Chemical Society Reviews 2024, 53 (13) , 7091-7157. https://doi.org/10.1039/D4CS00366G
    8. Rongnan Guo, Yi Yang, Xiang Long Huang, Chongchong Zhao, Binbin Hu, Feng Huo, Hua Kun Liu, Bowen Sun, Zixu Sun, Shi Xue Dou. Recent Advances in Multifunctional Binders for High Sulfur Loading Lithium‐Sulfur Batteries. Advanced Functional Materials 2024, 34 (1) https://doi.org/10.1002/adfm.202307108
    9. Tianpeng Zhang, Runyue Mao, Wanyuan Jiang, Borui Li, Zihui Song, Siyang Liu, Xigao Jian, Fangyuan Hu. Dynamic cross-linking of zwitterionic polymer binder based on host–guest interactions for Li-S batteries with enhanced safety and electrochemical performance. Nano Energy 2023, 114 , 108603. https://doi.org/10.1016/j.nanoen.2023.108603
    10. Jingwen Li, Chengyun Ma, Xinle Geng, Yongxiao Tuo, Ruoxuan Sun, Huiping Du, Meng-Chang Lin, Mian Cai. A chloric polycation binder enables rapid ionic transport in thick electrodes of high-energy aluminum-ion batteries. Journal of Materials Chemistry A 2023, 11 (27) , 14646-14654. https://doi.org/10.1039/D2TA09259J
    11. Yan-Qi Peng, Meng Zhao, Zi-Xian Chen, Qian Cheng, Yiran Liu, Xi-Yao Li, Yun-Wei Song, Bo-Quan Li, Jia-Qi Huang. Boosting sulfur redox kinetics by a pentacenetetrone redox mediator for high-energy-density lithium-sulfur batteries. Nano Research 2023, 16 (6) , 8253-8259. https://doi.org/10.1007/s12274-022-4584-z
    12. Joseph Nishanth, Dinachandra Singh, Santu Panja, T Mani Chandran, Kumar Brajesh, Shobit Omar, Kanwar S Nalwa. Investigating the influence of PVDF binder crystallinity on the performance of LiFePO4 cathode in Li-ion batteries. Oxford Open Materials Science 2023, 3 (1) https://doi.org/10.1093/oxfmat/itad019
    13. Zhen-Hua Xie, Zi-Xin Huang, Ze-Ping Zhang, Min-Zhi Rong, Ming-Qiu Zhang. Imparting Pulley Effect and Self-healability to Cathode Binder of Li-S Battery for Improvement of the Cycling Stability. Chinese Journal of Polymer Science 2023, 41 (1) , 95-107. https://doi.org/10.1007/s10118-022-2820-3
    14. Tong Wu, Jinting Ye, Tunan Li, Yuong Liu, Liu Jia, Liqun Sun, Jinghai Liu, Haiming Xie. Tetrathiafulvalene as a multifunctional electrolyte additive for simultaneous interface amelioration, electron conduction, and polysulfide redox regulation in lithium-sulfur batteries. Journal of Power Sources 2022, 536 , 231482. https://doi.org/10.1016/j.jpowsour.2022.231482
    15. Qing Zhang, Qihua Huang, Shu‐Meng Hao, Shuyi Deng, Qiming He, Zhiqun Lin, Yingkui Yang. Polymers in Lithium–Sulfur Batteries. Advanced Science 2022, 9 (2) https://doi.org/10.1002/advs.202103798
    16. Futoshi Matsumoto, Takao Gunji. Introduction. 2022, 1-4. https://doi.org/10.1007/978-981-16-8786-0_1
    17. Sue‐Faye Ng, Michelle Yu Ling Lau, Wee‐Jun Ong. Lithium–Sulfur Battery Cathode Design: Tailoring Metal‐Based Nanostructures for Robust Polysulfide Adsorption and Catalytic Conversion. Advanced Materials 2021, 33 (50) https://doi.org/10.1002/adma.202008654
    18. Jia-Jia Yuan, Zheng Huang, You-Zhi Song, Ming-Yang Li, Li-Feng Fang, Bao-Ku Zhu, Han-Ying Li. In-situ crosslinked binder for high-stability S cathodes with greatly enhanced conduction and polysulfides anchoring. Chemical Engineering Journal 2021, 426 , 128705. https://doi.org/10.1016/j.cej.2021.128705
    19. Adrian Saal, Tino Hagemann, Ulrich S. Schubert. Polymers for Battery Applications—Active Materials, Membranes, and Binders. Advanced Energy Materials 2021, 11 (43) https://doi.org/10.1002/aenm.202001984
    20. Yufeng Luo, Yuan Gao, Qianyi Guo, Zijian Zheng. Interfacial design of thick sulfur cathodes to achieve high energy density and stability. Journal of Materials Chemistry A 2021, 9 (32) , 17129-17142. https://doi.org/10.1039/D1TA04059F
    21. Junheng Li, Yifeng Cai, Haomin Wu, Zhiao Yu, Xuzhou Yan, Qiuhong Zhang, Theodore Z. Gao, Kai Liu, Xudong Jia, Zhenan Bao. Polymers in Lithium‐Ion and Lithium Metal Batteries. Advanced Energy Materials 2021, 11 (15) https://doi.org/10.1002/aenm.202003239
    22. Jia-Jia Yuan, Qing-Ran Kong, Zheng Huang, You-Zhi Song, Ming-Yang Li, Li-Feng Fang, Bao-Ku Zhu, Han-Ying Li. A well-designed polymer as a three-in-one multifunctional binder for high-performance lithium–sulfur batteries. Journal of Materials Chemistry A 2021, 9 (5) , 2970-2979. https://doi.org/10.1039/D0TA09489G
    23. Yihan Xu, Dong Zheng, Weixiao Ji, Nidal Abu-Zahra, Deyang Qu. A molecular dynamics study of the binding effectiveness between undoped conjugated polymer binders and tetra-sulfides in lithium–sulfur batteries. Composites Part B: Engineering 2021, 206 , 108531. https://doi.org/10.1016/j.compositesb.2020.108531
    24. Aleksander Cholewinski, Pengxiang Si, Marianna Uceda, Michael Pope, Boxin Zhao. Polymer Binders: Characterization and Development toward Aqueous Electrode Fabrication for Sustainability. Polymers 2021, 13 (4) , 631. https://doi.org/10.3390/polym13040631
    25. Z.H. Xie, Z.X. Huang, M.Z. Rong, M.Q. Zhang. Imparting high robustness and suppression ability of shuttle effect to sulfur cathode in the Li–S battery via a novel multifunctional binder. Materials Today Energy 2020, 18 , 100555. https://doi.org/10.1016/j.mtener.2020.100555
    26. Yoon Hwa, Elton J. Cairns. Nanostructured Sulfur and Sulfides for Advanced Lithium/Sulfur Cells. ChemElectroChem 2020, 7 (19) , 3927-3942. https://doi.org/10.1002/celc.202000758
    27. Hui Wang, Yu Yang, Peitao Zheng, Yinyan Wang, Sze-Wing Ng, Yukun Chen, Yonghong Deng, Zijian Zheng, Chaoyang Wang. Water-based phytic acid-crosslinked supramolecular binders for lithium-sulfur batteries. Chemical Engineering Journal 2020, 395 , 124981. https://doi.org/10.1016/j.cej.2020.124981
    28. Krzysztof Siczek. The Toxicity of Secondary Lithium-Sulfur Batteries Components. Batteries 2020, 6 (3) , 45. https://doi.org/10.3390/batteries6030045
    29. Meng Zhao, Bo‐Quan Li, Hong‐Jie Peng, Hong Yuan, Jun‐Yu Wei, Jia‐Qi Huang. Lithium‐Schwefel‐Batterien mit Magerelektrolyt: Herausforderungen und Perspektiven. Angewandte Chemie 2020, 132 (31) , 12736-12753. https://doi.org/10.1002/ange.201909339
    30. Meng Zhao, Bo‐Quan Li, Hong‐Jie Peng, Hong Yuan, Jun‐Yu Wei, Jia‐Qi Huang. Lithium–Sulfur Batteries under Lean Electrolyte Conditions: Challenges and Opportunities. Angewandte Chemie International Edition 2020, 59 (31) , 12636-12652. https://doi.org/10.1002/anie.201909339
    31. C.M. Costa, E. Lizundia, S. Lanceros-Méndez. Polymers for advanced lithium-ion batteries: State of the art and future needs on polymers for the different battery components. Progress in Energy and Combustion Science 2020, 79 , 100846. https://doi.org/10.1016/j.pecs.2020.100846
    32. Meng Zhao, Hong‐Jie Peng, Jun‐Yu Wei, Jia‐Qi Huang, Bo‐Quan Li, Hong Yuan, Qiang Zhang. Dictating High‐Capacity Lithium–Sulfur Batteries through Redox‐Mediated Lithium Sulfide Growth. Small Methods 2020, 4 (6) https://doi.org/10.1002/smtd.201900344
    33. Rongnan Guo, Shunlong Zhang, Jianli Wang, Hangjun Ying, Weiqiang Han. One‐Pot Synthesis of a Copolymer Micelle Crosslinked Binder with Multiple Lithium‐Ion Diffusion Pathways for Lithium–Sulfur Batteries. ChemSusChem 2020, 13 (4) , 819-826. https://doi.org/10.1002/cssc.201902772
    34. Luke Hencz, Hao Chen, Han Yeu Ling, Yazhou Wang, Chao Lai, Huijun Zhao, Shanqing Zhang. Housing Sulfur in Polymer Composite Frameworks for Li–S Batteries. Nano-Micro Letters 2019, 11 (1) https://doi.org/10.1007/s40820-019-0249-1
    35. Qi Qi, Xiaohui Lv, Wei Lv, Quan-Hong Yang. Multifunctional binder designs for lithium-sulfur batteries. Journal of Energy Chemistry 2019, 39 , 88-100. https://doi.org/10.1016/j.jechem.2019.02.001
    36. Huan Yi, Tu Lan, Yu Yang, Hongbo Zeng, Tian Zhang, Tian Tang, Chaoyang Wang, Yonghong Deng. A robust aqueous-processable polymer binder for long-life, high-performance lithium sulfur battery. Energy Storage Materials 2019, 21 , 61-68. https://doi.org/10.1016/j.ensm.2018.12.009
    37. Guomin Zhao, Runwen Zhang, Guangji Xu, Shuang Jin. Poly(amic acid) Lithium Salt as a Multi-Functional Binder for High Performance Lithium/Sulfur Battery Cathodes. International Journal of Electrochemical Science 2019, 14 (9) , 8772-8780. https://doi.org/10.20964/2019.09.11
    38. Seong‐Jun Kim, Kookhan Kim, Jungjin Park, Yung‐Eun Sung. Role and Potential of Metal Sulfide Catalysts in Lithium‐Sulfur Battery Applications. ChemCatChem 2019, 11 (10) , 2373-2387. https://doi.org/10.1002/cctc.201900184
    39. Jiadeng Zhu, Pei Zhu, Chaoyi Yan, Xia Dong, Xiangwu Zhang. Recent progress in polymer materials for advanced lithium-sulfur batteries. Progress in Polymer Science 2019, 90 , 118-163. https://doi.org/10.1016/j.progpolymsci.2018.12.002
    40. Krzysztof Jan Siczek. Binders. 2019, 73-78. https://doi.org/10.1016/B978-0-12-816392-4.00006-2
    41. Yoon Hwa, Eongyu Yi, Hao Shen, Younghoon Sung, Jiawei Kou, Kai Chen, Dilworth Y. Parkinson, Marca M. Doeff, Elton Cairns. Three-Dimensionally Aligned Sulfur Electrodes by Directional Freeze Tape Casting. SSRN Electronic Journal 2019, 11 https://doi.org/10.2139/ssrn.3378009
    42. Hong Yuan, Jia‐Qi Huang, Hong‐Jie Peng, Maria‐Magdalena Titirici, Rong Xiang, Renjie Chen, Quanbing Liu, Qiang Zhang. A Review of Functional Binders in Lithium–Sulfur Batteries. Advanced Energy Materials 2018, 8 (31) https://doi.org/10.1002/aenm.201802107
    43. Fulai Zhao, Yu Li, Wei Feng. Recent Advances in Applying Vulcanization/Inverse Vulcanization Methods to Achieve High‐Performance Sulfur‐Containing Polymer Cathode Materials for Li–S Batteries. Small Methods 2018, 2 (11) https://doi.org/10.1002/smtd.201800156
    44. Fumihiro Nomura, Yubin Liu, Toyokazu Tanabe, Takao Gunji, Takashi Tsuda, Shinsaku Ugawa, Hojin Lee, Takeo Ohsaka, Futoshi Matsumoto. Elucidation of key factors of water-resistance of Li-rich solid-solution layered oxide cathode materials applicable to a water-based cathode preparation process for Li-ion battery. Electrochimica Acta 2018, 283 , 478-487. https://doi.org/10.1016/j.electacta.2018.06.183
    45. Ali Eftekhari. High‐Energy Aqueous Lithium Batteries. Advanced Energy Materials 2018, 8 (24) https://doi.org/10.1002/aenm.201801156
    46. Yoon Hwa, Elton J. Cairns. Polymeric binders for the sulfur electrode compatible with ionic liquid containing electrolytes. Electrochimica Acta 2018, 271 , 103-109. https://doi.org/10.1016/j.electacta.2018.03.040
    Download PDF
    Go to Chemistry of Materials
    Get e-Alerts
    Get e-Alerts

    Chemistry of Materials

    Cite this: Chem. Mater. 2018, 30, 3, 685–691
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.7b03870
    Published January 9, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

    Article Views

    2456

    Altmetric

    -

    Citations

    46
    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.