Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes

Li, Longjun; Pascal, Tod A.; Connell, Justin G.; Fan, Frank Y.; Meckler, Stephen M.; Ma, Lin; Chiang, Yet-Ming; Prendergast, David; Helms, Brett A.

doi:10.1038/s41467-017-02410-6

Title: Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes

Journal Article · Fri Dec 22 00:00:00 EST 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-02410-6· OSTI ID:1417620

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^[3]; Fan, Frank Y. ^[4]; Meckler, Stephen M. ^[5]; Ma, Lin ^[1]; Chiang, Yet-Ming ^[4];

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Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research, Molecular Foundry

Polymer binders in battery electrodes may be either active or passive. This distinction depends on whether the polymer influences charge or mass transport in the electrode. Although it is desirable to understand how to tailor the macromolecular design of a polymer to play a passive or active role, design rules are still lacking, as is a framework to assess the divergence in such behaviors. Here, we reveal the molecular-level underpinnings that distinguish an active polyelectrolyte binder designed for lithium–sulfur batteries from a passive alternative. The binder, a cationic polyelectrolyte, is shown to both facilitate lithium-ion transport through its reconfigurable network of mobile anions and restrict polysulfide diffusion from mesoporous carbon hosts by anion metathesis, which we show is selective for higher oligomers. Furthermore, these attributes allow cells to be operated for >100 cycles with excellent rate capability using cathodes with areal sulfur loadings up to 8.1mgcm^–2.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: SC-22.2 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Office of Basic Energy Sciences (BES) (SC-22). Joint Center for Energy Storage Research (JCESR); USDOE Office of Science (SC), National Energy Research Scientific Computing Center (NERSC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1417620

Alternate ID(s):: OSTI ID: 1489228

Journal Information:: Nature Communications, Vol. 8, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 117 works

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Metal Coated Polypropylene Separator with Enhanced Surface Wettability for High Capacity Lithium Metal Batteries Din, Mir Mehraj Ud; Murugan, Ramaswamy Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-019-53257-4	journal	November 2019
Stabilization of Li–S batteries with a lean electrolyte via ion-exchange trapping of lithium polysulfides using a cationic, polybenzimidazolium binder Pham, Chuyen Van; Liu, Lili; Britton, Benjamin Sustainable Energy & Fuels, Vol. 4, Issue 3 https://doi.org/10.1039/c9se01092k	journal	January 2020
Free-Standing Sulfur and Graphitic Porous Carbon Nanofibers Composite Cathode for High Electrochemical Performance of Lithium–Sulfur Batteries Zhang, Yaoxuan; Wang, Panpan; Tan, Hua Journal of The Electrochemical Society, Vol. 165, Issue 5 https://doi.org/10.1149/2.0201805jes	journal	January 2018
Bioinspired Binders Actively Controlling Ion Migration and Accommodating Volume Change in High Sulfur Loading Lithium–Sulfur Batteries Jin, Biyu; Yang, Lifeng; Zhang, Jiawen Advanced Energy Materials, Vol. 9, Issue 48 https://doi.org/10.1002/aenm.201902938	journal	November 2019
An adaptive and stable bio-electrolyte for rechargeable Zn-ion batteries Zhang, Silan; Yu, Nengsheng; Zeng, Sha Journal of Materials Chemistry A, Vol. 6, Issue 26 https://doi.org/10.1039/c8ta04298e	journal	January 2018
Housing Sulfur in Polymer Composite Frameworks for Li–S Batteries Hencz, Luke; Chen, Hao; Ling, Han Yeu Nano-Micro Letters, Vol. 11, Issue 1 https://doi.org/10.1007/s40820-019-0249-1	journal	February 2019
PIM-1-based carbon–sulfur composites for sodium–sulfur batteries that operate without the shuttle effect Jeon, Jun Woo; Kim, Dong-Min; Lee, Jinyoung Journal of Materials Chemistry A, Vol. 8, Issue 7 https://doi.org/10.1039/c9ta10939k	journal	January 2020
Interfacial active fluorine site-induced electron transfer on TiO ₂ (001) facets to enhance polysulfide redox reactions for better liquid Li ₂ S ₆ -Based lithium–sulfur batteries Zha, Chenyang; Gu, Xiuquan; Wu, Donghai Journal of Materials Chemistry A, Vol. 7, Issue 11 https://doi.org/10.1039/c8ta11732b	journal	January 2019
Structural Design of Lithium–Sulfur Batteries: From Fundamental Research to Practical Application Yang, Xiaofei; Li, Xia; Adair, Keegan Electrochemical Energy Reviews, Vol. 1, Issue 3 https://doi.org/10.1007/s41918-018-0010-3	journal	June 2018
Porphyrin-Derived Graphene-Based Nanosheets Enabling Strong Polysulfide Chemisorption and Rapid Kinetics in Lithium-Sulfur Batteries Kong, Long; Li, Bo-Quan; Peng, Hong-Jie Advanced Energy Materials, Vol. 8, Issue 20 https://doi.org/10.1002/aenm.201800849	journal	April 2018
High Stable Sulfur Cathode with Self‐Healable and Physical Confining Polydimethylsiloxane Interlayer Cui, Ximing; Pan, Qinmin ChemElectroChem, Vol. 6, Issue 22 https://doi.org/10.1002/celc.201901625	journal	October 2019
Recent Advances in Applying Vulcanization/Inverse Vulcanization Methods to Achieve High-Performance Sulfur-Containing Polymer Cathode Materials for Li-S Batteries Zhao, Fulai; Li, Yu; Feng, Wei Small Methods, Vol. 2, Issue 11 https://doi.org/10.1002/smtd.201800156	journal	August 2018
Natural Vermiculite Enables High‐Performance in Lithium–Sulfur Batteries via Electrical Double Layer Effects Wu, Feixiang; Lv, Haifeng; Chen, Shuangqiang Advanced Functional Materials https://doi.org/10.1002/adfm.201902820	journal	May 2019
Research Progress of the Solid State Lithium-Sulfur Batteries Wang, HangChao; Cao, Xin; Liu, Wen Frontiers in Energy Research, Vol. 7 https://doi.org/10.3389/fenrg.2019.00112	journal	October 2019