A Dual–Phase Electrolyte for High–Energy Lithium–Sulfur Batteries

Ren, Yuxun; Manthiram, Arumugam

doi:10.1002/aenm.202202566

A Dual–Phase Electrolyte for High–Energy Lithium–Sulfur Batteries

Journal Article · Fri Oct 07 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202566· OSTI ID:2217442

Ren, Yuxun ^[1]; ^[2]

Univ. of Texas, Austin, TX (United States); University of Texas at Austin
Univ. of Texas, Austin, TX (United States)

Dissolution of lithium polysulfides (LiPSs) is essential for fast cathode kinetics, but detrimental for anode stability, especially under lean electrolyte conditions. Here in this work, the phase separation phenomenon between solvents with different polarities (tetramethyl sulfone [TMS] and dibutyl ether [DBE]) is utilized to enable the design of a dual-phase electrolyte. High-polarity, high-density TMS–lithium bis(trifluoromethanesulfonyl)imide–ammonium trifluoroacetate as the cathode electrolyte strongly solvates LiPSs, which propel the sulfur redox reaction. Moreover, the composite of DBE and a polymeric ion conductor serves as the anode electrolyte. The addition of DBE in the anode side effectively prevents the crossover of corrosive species (LiPSs and ammonia trifluoroacetate), enabling a significant improvement in Li-metal anode stability. The electrode-specific dual-phase electrolyte design provides electrochemical performance superior to conventional electrolytes. Without additional electrode engineering, pouch cells assemble with the dual-phase electrolyte cycle under a lean electrolyte (4 µL mg^–1) and low-Li-excess condition (N/P = 3) for 120 cycles.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: EE0007762

OSTI ID:: 2217442

Alternate ID(s):: OSTI ID: 1902545

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 46 Vol. 12; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Addressing Passivation in Lithium-Sulfur Battery Under Lean Electrolyte Condition Pan, Huilin; Han, Kee Sung; Engelhard, Mark H. Advanced Functional Materials, Vol. 28, Issue 38 https://doi.org/10.1002/adfm.201707234	journal	February 2018
Solvent-Mediated Li ₂ S Electrodeposition: A Critical Manipulator in Lithium-Sulfur Batteries Li, Zhejun; Zhou, Yucun; Wang, Yu Advanced Energy Materials, Vol. 9, Issue 1 https://doi.org/10.1002/aenm.201802207	journal	November 2018
Liquid‐Based Janus Electrolyte for Sustainable Redox Mediation in Lithium–Oxygen Batteries Ko, Youngmin; Kim, Hong‐I; Cho, Sung‐Ju Advanced Energy Materials, Vol. 11, Issue 38 https://doi.org/10.1002/aenm.202102096	journal	August 2021
Difluorobenzene‐Based Locally Concentrated Ionic Liquid Electrolyte Enabling Stable Cycling of Lithium Metal Batteries with Nickel‐Rich Cathode Liu, Xu; Mariani, Alessandro; Diemant, Thomas Advanced Energy Materials, Vol. 12, Issue 25 https://doi.org/10.1002/aenm.202200862	journal	May 2022
Hydrophobic Organic‐Electrolyte‐Protected Zinc Anodes for Aqueous Zinc Batteries Cao, Longsheng; Li, Dan; Deng, Tao Angewandte Chemie, Vol. 132, Issue 43 https://doi.org/10.1002/ange.202008634	journal	August 2020
The Formation/Decomposition Equilibrium of LiH and its Contribution on Anode Failure in Practical Lithium Metal Batteries Xu, Gaojie; Li, Jiedong; Wang, Chao Angewandte Chemie, Vol. 133, Issue 14 https://doi.org/10.1002/ange.202013812	journal	February 2021
Anode‐Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules Ren, Yuxun; Bhargav, Amruth; Shin, Woochul Angewandte Chemie, Vol. 134, Issue 35 https://doi.org/10.1002/ange.202207907	journal	July 2022
Amorphous Lithium Sulfide as Lithium‐Sulfur Battery Cathode with Low Activation Barrier Lodovico, Lucas; Milad Hosseini, Seyed; Varzi, Alberto Energy Technology, Vol. 7, Issue 12 https://doi.org/10.1002/ente.201801013	journal	March 2019
Enhanced Li ⁺ Transport in Ionic Liquid‐Based Electrolytes Aided by Fluorinated Ethers for Highly Efficient Lithium Metal Batteries with Improved Rate Capability Liu, Xu; Zarrabeitia, Maider; Mariani, Alessandro Small Methods, Vol. 5, Issue 7 https://doi.org/10.1002/smtd.202100168	journal	June 2021
Localized High-Concentration Sulfone Electrolytes for High-Efficiency Lithium-Metal Batteries Ren, Xiaodi; Chen, Shuru; Lee, Hongkyung Chem, Vol. 4, Issue 8 https://doi.org/10.1016/j.chempr.2018.05.002	journal	August 2018
Li2S-based anode-free full batteries with modified Cu current collector Chen, Jie; Xiang, Jingwei; Chen, Xin Energy Storage Materials, Vol. 30 https://doi.org/10.1016/j.ensm.2020.05.009	journal	September 2020
Effect of organic cations in locally concentrated ionic liquid electrolytes on the electrochemical performance of lithium metal batteries Liu, Xu; Mariani, Alessandro; Zarrabeitia, Maider Energy Storage Materials, Vol. 44 https://doi.org/10.1016/j.ensm.2021.10.034	journal	January 2022
Lithium-Sulfur Batteries: Attaining the Critical Metrics Bhargav, Amruth; He, Jiarui; Gupta, Abhay Joule, Vol. 4, Issue 2 https://doi.org/10.1016/j.joule.2020.01.001	journal	February 2020
A Stirred Self-Stratified Battery for Large-Scale Energy Storage Meng, Jintao; Tang, Qi; Zhou, Liangyi Joule, Vol. 4, Issue 4 https://doi.org/10.1016/j.joule.2020.03.011	journal	April 2020
A self-cleaning Li-S battery enabled by a bifunctional redox mediator Ren, Y. X.; Zhao, T. S.; Liu, M. Journal of Power Sources, Vol. 361 https://doi.org/10.1016/j.jpowsour.2017.06.083	journal	September 2017
Novel gel polymer electrolyte for high-performance lithium–sulfur batteries Liu, Ming; Zhou, Dong; He, Yan-Bing Nano Energy, Vol. 22 https://doi.org/10.1016/j.nanoen.2016.02.008	journal	April 2016
Tailoring Lithium Polysulfide Coordination and Clustering Behavior through Cationic Electrostatic Competition Gupta, Abhay; Bhargav, Amruth; Manthiram, Arumugam Chemistry of Materials, Vol. 33, Issue 9 https://doi.org/10.1021/acs.chemmater.1c00893	journal	April 2021
Influence of Lithium Polysulfide Clustering on the Kinetics of Electrochemical Conversion in Lithium–Sulfur Batteries Gupta, Abhay; Bhargav, Amruth; Jones, John-Paul Chemistry of Materials, Vol. 32, Issue 5 https://doi.org/10.1021/acs.chemmater.9b05164	journal	February 2020
Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium–Sulfur Batteries Pan, Huilin; Han, Kee Sung; Vijayakumar, M. ACS Applied Materials & Interfaces, Vol. 9, Issue 5 https://doi.org/10.1021/acsami.6b04158	journal	July 2016
Evoking High-Donor-Number-Assisted and Organosulfur-Mediated Conversion in Lithium–Sulfur Batteries Gupta, Abhay; Bhargav, Amruth; Manthiram, Arumugam ACS Energy Letters, Vol. 6, Issue 1 https://doi.org/10.1021/acsenergylett.0c02461	journal	December 2020
Nanotechnology for Sulfur Cathodes Li, Matthew; Lu, Jun; Amine, Khalil ACS Nano, Vol. 15, Issue 5 https://doi.org/10.1021/acsnano.1c01999	journal	May 2021
Rechargeable Lithium–Sulfur Batteries Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng Chemical Reviews, Vol. 114, Issue 23 https://doi.org/10.1021/cr500062v	journal	July 2014
Direct observation of lithium polysulfides in lithium–sulfur batteries using operando X-ray diffraction Conder, Joanna; Bouchet, Renaud; Trabesinger, Sigita Nature Energy, Vol. 2, Issue 6 https://doi.org/10.1038/nenergy.2017.69	journal	May 2017
Double-slit photoelectron interference in strong-field ionization of the neon dimer Kunitski, Maksim; Eicke, Nicolas; Huber, Pia Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-07882-8	journal	January 2019
Achieving three-dimensional lithium sulfide growth in lithium-sulfur batteries using high-donor-number anions Chu, Hyunwon; Noh, Hyungjun; Kim, Yun-Jung Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-07975-4	journal	January 2019
A reflection on lithium-ion battery cathode chemistry Manthiram, Arumugam Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15355-0	journal	March 2020
Tuning the electrolyte network structure to invoke quasi-solid state sulfur conversion and suppress lithium dendrite formation in Li–S batteries Pang, Quan; Shyamsunder, Abhinandan; Narayanan, Badri Nature Energy, Vol. 3, Issue 9 https://doi.org/10.1038/s41560-018-0214-0	journal	August 2018
Solid-state polymer electrolytes with in-built fast interfacial transport for secondary lithium batteries Zhao, Qing; Liu, Xiaotun; Stalin, Sanjuna Nature Energy, Vol. 4, Issue 5 https://doi.org/10.1038/s41560-019-0349-7	journal	March 2019
Formulating energy density for designing practical lithium–sulfur batteries Zhou, Guangmin; Chen, Hao; Cui, Yi Nature Energy, Vol. 7, Issue 4 https://doi.org/10.1038/s41560-022-01001-0	journal	April 2022
Toward sustainable batteries Yaghoobnejad Asl, Hooman; Manthiram, Arumugam Nature Sustainability, Vol. 4, Issue 5 https://doi.org/10.1038/s41893-020-00664-5	journal	December 2020
The role of polysulfide dianions and radical anions in the chemical, physical and biological sciences, including sulfur-based batteries Steudel, Ralf; Chivers, Tristram Chemical Society Reviews, Vol. 48, Issue 12 https://doi.org/10.1039/C8CS00826D	journal	January 2019
Monolithic heterojunction quasi-solid-state battery electrolytes based on thermodynamically immiscible dual phases Cho, Sung-Ju; Jung, Gwan Yeong; Kim, Su Hwan Energy & Environmental Science, Vol. 12, Issue 2 https://doi.org/10.1039/C8EE01503A	journal	January 2019
Direct tracking of the polysulfide shuttling and interfacial evolution in all-solid-state lithium–sulfur batteries: a degradation mechanism study Song, Yue-Xian; Shi, Yang; Wan, Jing Energy & Environmental Science, Vol. 12, Issue 8 https://doi.org/10.1039/C9EE00578A	journal	January 2019
Anin situencapsulation approach for polysulfide retention in lithium–sulfur batteries Ren, Y. X.; Jiang, H. R.; Xiong, C. Journal of Materials Chemistry A, Vol. 8, Issue 14 https://doi.org/10.1039/C9TA14003D	journal	January 2020
Implications of in situ chalcogen substitutions in polysulfides for rechargeable batteries Nanda, Sanjay; Bhargav, Amruth; Jiang, Zhou Energy & Environmental Science, Vol. 14, Issue 10 https://doi.org/10.1039/D1EE01113H	journal	January 2021
Elasticity-oriented design of solid-state batteries: challenges and perspectives Ren, Yuxun; Hatzell, Kelsey B. Journal of Materials Chemistry A, Vol. 9, Issue 24 https://doi.org/10.1039/D1TA01545A	journal	January 2021
Unifying the clustering kinetics of lithium polysulfides with the nucleation behavior of Li ₂ S in lithium–sulfur batteries Gupta, Abhay; Manthiram, Arumugam Journal of Materials Chemistry A, Vol. 9, Issue 22 https://doi.org/10.1039/D1TA02779D	journal	January 2021
Upgrading traditional liquid electrolyte via in situ gelation for future lithium metal batteries Liu, Feng-Quan; Wang, Wen-Peng; Yin, Ya-Xia Science Advances, Vol. 4, Issue 10 https://doi.org/10.1126/sciadv.aat5383	journal	October 2018

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