Constructing a multi-functional polymer network for ultra-stable and safe Li-metal batteries

Gao, Shilun; Li, Zhenxi; Zhang, Zhen; Li, Bingrui; Chen, Xi Chelsea; Yang, Guang; Saito, Tomonori; Tian, Ming; Yang, Huabin; Cao, Peng-Fei

doi:10.1016/j.ensm.2022.11.049

Constructing a multi-functional polymer network for ultra-stable and safe Li-metal batteries

Journal Article · Mon Nov 28 00:00:00 EST 2022 · Energy Storage Materials

DOI:https://doi.org/10.1016/j.ensm.2022.11.049· OSTI ID:1907219

Gao, Shilun ^[1]; Li, Zhenxi ^[1]; Zhang, Zhen ^[2]; Li, Bingrui ^[3]; Chen, Xi Chelsea ^[2]; Yang, Guang ^[2]; Saito, Tomonori ^[2]; Tian, Ming ^[4]; Yang, Huabin ^[1]; ^[4]

Nankai Univ., Tianjin (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Univ. of Tennessee, Knoxville, TN (United States)
Beijing University of Chemical Technology (China)

We report the practical application of lithium (Li) metal electrodes is impeded by Li dendrite growth and unstable solid electrolyte interphase (SEI). Herein, a multi-grafting polymer network, poly(dimethyl siloxane)-g-[poly(poly(ethylene glycol) methyl ether methacrylate)-r-sodium poly(p-styrene sulfonate)] (PPS), is chemically synthesized from reversible addition-fragmentation chain transfer (RAFT) polymerization. With integrated stretchability, ionic conductivity, and mechanical robustness, it serves a dual role to stabilize the Li electrode. As artificial SEI layer, the PPS enables superior electrochemical performance in half cells, symmetric cells, and full cells (PPS@Li/LiFePO₄, capacity retention of >70% after 600 cycles). Utilized as solid polymer electrolyte (SPE), the all-solid-state Li/SPE/LiFePO₄ full cell delivers excellent cycling performance with an unprecedented capacity retention of 90% over 1,700 cycles at 0.5 C and 81% over 1,000 cycles at 1.0 C. With high-voltage LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) as cathode, the Li/SPE/NMC811 cell exhibits an initial discharge capacity of 162.2 mAh g^-1 with a capacity retention of 72% after 200 cycles. The assembled solid-state Li/SPE/LiFePO4 pouch cell with SPE exhibits stable cycling performance over 200 cycles with a capacity retention of 75% and still operates well even after curling, folding, and cutting, demonstrating great potential for achieving ultra-safe and high energy density batteries.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: China Postdoctoral Science Foundation; Fundamental Research Funds for the Central Universities; MOE Innovation Team; Natural Science Foundation of China; Natural Science Foundation of Tianjin; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1907219

Alternate ID(s):: OSTI ID: 1962146

Journal Information:: Energy Storage Materials, Journal Name: Energy Storage Materials Vol. 55; ISSN 2405-8297

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (53)

Highly‐Cyclable Room‐Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries Rojaee, Ramin; Cavallo, Salvatore; Mogurampelly, Santosh Advanced Functional Materials, Vol. 30, Issue 32 https://doi.org/10.1002/adfm.201910749	journal	June 2020
A Flexible Solid Electrolyte Interphase Layer for Long-Life Lithium Metal Anodes Li, Nian-Wu; Shi, Yang; Yin, Ya-Xia Angewandte Chemie International Edition, Vol. 57, Issue 6 https://doi.org/10.1002/anie.201710806	journal	January 2018
Temperature-Dependent Nucleation and Growth of Dendrite-Free Lithium Metal Anodes Yan, Kang; Wang, Jiangyan; Zhao, Shuoqing Angewandte Chemie International Edition, Vol. 58, Issue 33 https://doi.org/10.1002/anie.201905251	journal	July 2019
Self‐Healing Polymer Electrolytes Formed via Dual‐Networks: A New Strategy for Flexible Lithium Metal Batteries Zhou, Binghua; Zuo, Cai; Xiao, Zhuliu Chemistry – A European Journal, Vol. 24, Issue 72 https://doi.org/10.1002/chem.201803943	journal	November 2018
Advances in Artificial Layers for Stable Lithium Metal Anodes Qi, Liya; Wu, Zhengwei; Zhao, Binglu Chemistry – A European Journal, Vol. 26, Issue 19 https://doi.org/10.1002/chem.201904631	journal	April 2020
Simultaneous Stabilization of LiNi _0.76 Mn _0.14 Co _0.10 O ₂ Cathode and Lithium Metal Anode by Lithium Bis(oxalato)borate as Additive Zhao, Wengao; Zou, Lianfeng; Zheng, Jianming ChemSusChem, Vol. 11, Issue 13 https://doi.org/10.1002/cssc.201800706	journal	June 2018
Alkali Metal Anodes for Rechargeable Batteries Wang, Hua; Yu, Dandan; Kuang, Chengwei Chem, Vol. 5, Issue 2 https://doi.org/10.1016/j.chempr.2018.11.005	journal	February 2019
Polymer Electrolytes for Lithium-Based Batteries: Advances and Prospects Zhou, Dong; Shanmukaraj, Devaraj; Tkacheva, Anastasia Chem, Vol. 5, Issue 9 https://doi.org/10.1016/j.chempr.2019.05.009	journal	September 2019
Single Ion Conducting Polymer Electrolytes Based On Versatile Polyurethanes Porcarelli, Luca; Manojkumar, Kasina; Sardon, Haritz Electrochimica Acta, Vol. 241 https://doi.org/10.1016/j.electacta.2017.04.132	journal	July 2017
Effect of diethylenetriamine as additive to stabilize the lithium metal anode Chen, Zhihui; Huang, Xianli; Gong, Hao Electrochimica Acta, Vol. 292 https://doi.org/10.1016/j.electacta.2018.09.120	journal	December 2018
Poly (dimethylsiloxane) modified lithium anode for enhanced performance of lithium-sulfur batteries Li, Qian; Zeng, Fang-Lei; Guan, Yue-Peng Energy Storage Materials, Vol. 13 https://doi.org/10.1016/j.ensm.2018.01.002	journal	July 2018
Rational design of robust-flexible protective layer for safe lithium metal battery Li, Siyuan; Fan, Lei; Lu, Yingying Energy Storage Materials, Vol. 18 https://doi.org/10.1016/j.ensm.2018.09.015	journal	March 2019
Stable lithium metal anode enabled by high-dimensional lithium deposition through a functional organic substrate Zhao, Peiyu; Feng, Yangyang; Li, Tongtong Energy Storage Materials, Vol. 33 https://doi.org/10.1016/j.ensm.2020.08.025	journal	December 2020
Solid electrolytes reinforced by infinite coordination polymer nano-network for dendrite-free lithium metal batteries Wu, Xiaoxue; Zheng, Yongjian; Li, Wenbo Energy Storage Materials, Vol. 41 https://doi.org/10.1016/j.ensm.2021.06.009	journal	October 2021
Design of ionic liquid like monomers towards easy-accessible single-ion conducting polymer electrolytes Porcarelli, Luca; Vlasov, Petr S.; Ponkratov, Denis O. European Polymer Journal, Vol. 107 https://doi.org/10.1016/j.eurpolymj.2018.08.014	journal	October 2018
A Dynamic, Electrolyte-Blocking, and Single-Ion-Conductive Network for Stable Lithium-Metal Anodes Yu, Zhiao; Mackanic, David G.; Michaels, Wesley Joule, Vol. 3, Issue 11 https://doi.org/10.1016/j.joule.2019.07.025	journal	November 2019
Superior high-temperature rate performance of LiFePO4 cathode: The stabilizing effect of a multicomponent gel biopolymer binder Ding, Ling; Leones, Rita; Schmeida, Toni Journal of Power Sources, Vol. 521 https://doi.org/10.1016/j.jpowsour.2021.230955	journal	February 2022
Artificial Interphases for Highly Stable Lithium Metal Anode Xu, Rui; Cheng, Xin-Bing; Yan, Chong Matter, Vol. 1, Issue 2 https://doi.org/10.1016/j.matt.2019.05.016	journal	August 2019
Elastic vitrimers: Beyond thermoplastic and thermoset elastomers Luo, Jiancheng; Demchuk, Zoriana; Zhao, Xiao Matter, Vol. 5, Issue 5 https://doi.org/10.1016/j.matt.2022.04.007	journal	May 2022
Ionic conductive polymers as artificial solid electrolyte interphase films in Li metal batteries – A review Gao, Shilun; Sun, Feiyuan; Liu, Nian Materials Today, Vol. 40 https://doi.org/10.1016/j.mattod.2020.06.011	journal	November 2020
Rechargeable solid-state lithium metal batteries with vertically aligned ceramic nanoparticle/polymer composite electrolyte Wang, Xue; Zhai, Haowei; Qie, Boyu Nano Energy, Vol. 60 https://doi.org/10.1016/j.nanoen.2019.03.051	journal	June 2019
Lithium Metal Anodes with Nonaqueous Electrolytes Zhang, Ji-Guang; Xu, Wu; Xiao, Jie Chemical Reviews, Vol. 120, Issue 24 https://doi.org/10.1021/acs.chemrev.0c00275	journal	November 2020
A Brief Review on Solid Electrolyte Interphase Composition Characterization Technology for Lithium Metal Batteries: Challenges and Perspectives Shan, Xinyi; Zhong, Yu; Zhang, Lingjie The Journal of Physical Chemistry C, Vol. 125, Issue 35 https://doi.org/10.1021/acs.jpcc.1c06277	journal	August 2021
Stability of Solid Electrolyte Interphase Components on Lithium Metal and Reactive Anode Material Surfaces Leung, Kevin; Soto, Fernando; Hankins, Kie The Journal of Physical Chemistry C, Vol. 120, Issue 12 https://doi.org/10.1021/acs.jpcc.5b11719	journal	March 2016
Diversity of Synthetic Approaches to Functionalized Perfluoropolyalkylether Polymers Bonneaud, Céline; Howell, Jon; Bongiovanni, Roberta Macromolecules, Vol. 54, Issue 2 https://doi.org/10.1021/acs.macromol.0c01599	journal	January 2021
Rational Polymer Design of Stretchable Poly(ionic liquid) Membranes for Dual Applications Li, Bingrui; Zhao, Sheng; Zhu, Jiadeng Macromolecules, Vol. 54, Issue 2 https://doi.org/10.1021/acs.macromol.0c02335	journal	December 2020
Structural Dynamics of Strongly Segregated Block Copolymer Electrolytes Oparaji, Onyekachi; Narayanan, Suresh; Sandy, Alec Macromolecules, Vol. 51, Issue 7 https://doi.org/10.1021/acs.macromol.7b01803	journal	March 2018
Elastic Single-Ion Conducting Polymer Electrolytes: Toward a Versatile Approach for Intrinsically Stretchable Functional Polymers Cao, Peng-Fei; Li, Bingrui; Yang, Guang Macromolecules, Vol. 53, Issue 9 https://doi.org/10.1021/acs.macromol.9b02683	journal	April 2020
Lithiophilic Zn Sites in Porous CuZn Alloy Induced Uniform Li Nucleation and Dendrite-free Li Metal Deposition Chi, Shang-Sen; Wang, Qingrong; Han, Bing Nano Letters, Vol. 20, Issue 4 https://doi.org/10.1021/acs.nanolett.0c00352	journal	March 2020
Nanophase-Separated, Elastic Epoxy Composite Thin Film as an Electrolyte for Stable Lithium Metal Batteries Zeng, Ziqi; Chen, Xin; Sun, Mengjun Nano Letters, Vol. 21, Issue 8 https://doi.org/10.1021/acs.nanolett.1c00583	journal	March 2021
Improved Single-Ion Conductivity of Polymer Electrolyte via Accelerated Segmental Dynamics Zhao, Sheng; Zhang, Yiman; Pham, Hoang ACS Applied Energy Materials, Vol. 3, Issue 12 https://doi.org/10.1021/acsaem.0c02079	journal	December 2020
Adhesive Polymers as Efficient Binders for High-Capacity Silicon Electrodes Pan, Yiyang; Ge, Sirui; Rashid, Zahid ACS Applied Energy Materials, Vol. 3, Issue 4 https://doi.org/10.1021/acsaem.9b02420	journal	March 2020
Self-Healing Solid Polymer Electrolyte for Room-Temperature Solid-State Lithium Metal Batteries Zhang, Lanshuang; Zhang, Panpan; Chang, Caiyun ACS Applied Materials & Interfaces, Vol. 13, Issue 39 https://doi.org/10.1021/acsami.1c14462	journal	September 2021
Employing Ni-Embedded Porous Graphitic Carbon Fibers for High-Efficiency Lithium–Sulfur Batteries Wang, Changhao; Li, Yahao; Cao, Feng ACS Applied Materials & Interfaces, Vol. 14, Issue 8 https://doi.org/10.1021/acsami.1c24755	journal	February 2022
Scalable Manufacturing of Solid Polymer Electrolytes with Superior Room-Temperature Ionic Conductivity Zhou, Zekun; Tao, Zengren; Zhang, Linyun ACS Applied Materials & Interfaces, Vol. 14, Issue 29 https://doi.org/10.1021/acsami.2c01416	journal	July 2022
Constructing Effective Interfaces for Li _1.5 Al _0.5 Ge _1.5 (PO ₄ ) ₃ Pellets To Achieve Room-Temperature Hybrid Solid-State Lithium Metal Batteries Yu, Qipeng; Han, Da; Lu, Qingwen ACS Applied Materials & Interfaces, Vol. 11, Issue 10 https://doi.org/10.1021/acsami.8b20413	journal	February 2019
Polyoxyethylene (PEO)\|PEO–Perovskite\|PEO Composite Electrolyte for All-Solid-State Lithium Metal Batteries Liu, Ke; Zhang, Ruihan; Sun, Jing ACS Applied Materials & Interfaces, Vol. 11, Issue 50 https://doi.org/10.1021/acsami.9b16936	journal	November 2019
Improving Lithium Metal Composite Anodes with Seeding and Pillaring Effects of Silicon Nanoparticles Wang, Hansen; Cao, Xia; Gu, Hanke ACS Nano, Vol. 14, Issue 4 https://doi.org/10.1021/acsnano.0c00184	journal	April 2020
Dynamic Regulation of Lithium Dendrite Growth with Electromechanical Coupling Effect of Soft BaTiO ₃ Ceramic Nanofiber Films Xia, Shuhui; Zhao, Yun; Yan, Jianhua ACS Nano, Vol. 15, Issue 2 https://doi.org/10.1021/acsnano.0c09745	journal	January 2021
Surface Fluorination of Reactive Battery Anode Materials for Enhanced Stability Zhao, Jie; Liao, Lei; Shi, Feifei Journal of the American Chemical Society, Vol. 139, Issue 33 https://doi.org/10.1021/jacs.7b05251	journal	August 2017
High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes Lee, Yong-Gun; Fujiki, Satoshi; Jung, Changhoon Nature Energy, Vol. 5, Issue 4 https://doi.org/10.1038/s41560-020-0575-z	journal	March 2020
Understanding and applying coulombic efficiency in lithium metal batteries Xiao, Jie; Li, Qiuyan; Bi, Yujing Nature Energy, Vol. 5, Issue 8 https://doi.org/10.1038/s41560-020-0648-z	journal	June 2020
Designing solid-state electrolytes for safe, energy-dense batteries Zhao, Qing; Stalin, Sanjuna; Zhao, Chen-Zi Nature Reviews Materials, Vol. 5, Issue 3 https://doi.org/10.1038/s41578-019-0165-5	journal	February 2020
Interface layer formation in solid polymer electrolyte lithium batteries: an XPS study Xu, Chao; Sun, Bing; Gustafsson, Torbjörn J. Mater. Chem. A, Vol. 2, Issue 20 https://doi.org/10.1039/C4TA00214H	journal	January 2014
A dual-functional polymer coating on a lithium anode for suppressing dendrite growth and polysulfide shuttling in Li–S batteries Luo, Jing; Lee, Rung-Chuan; Jin, Jian-Ting Chemical Communications, Vol. 53, Issue 5 https://doi.org/10.1039/C6CC09248A	journal	January 2017
A composite solid polymer electrolyte incorporating MnO ₂ nanosheets with reinforced mechanical properties and electrochemical stability for lithium metal batteries Li, Yuhan; Sun, Zongjie; Liu, Dongyu Journal of Materials Chemistry A, Vol. 8, Issue 4 https://doi.org/10.1039/C9TA11542K	journal	January 2020
Recent progress on pristine metal/covalent-organic frameworks and their composites for lithium–sulfur batteries Zheng, Zi-Jian; Ye, Huan; Guo, Zai-Ping Energy & Environmental Science, Vol. 14, Issue 4 https://doi.org/10.1039/D0EE03181J	journal	January 2021
Hexagonal boron nitride induces anion trapping in a polyethylene oxide based solid polymer electrolyte for lithium dendrite inhibition Li, Yuhan; Zhang, Libo; Sun, Zongjie Journal of Materials Chemistry A, Vol. 8, Issue 19 https://doi.org/10.1039/D0TA03677C	journal	January 2020
Aligned artificial solid electrolyte interphase layers as versatile interfacial stabilizers on lithium metal anodes Li, Zihao; Ding, Xuesong; Feng, Wei Journal of Materials Chemistry A, Vol. 10, Issue 19 https://doi.org/10.1039/D2TA00119E	journal	January 2022
An anion-immobilized composite electrolyte for dendrite-free lithium metal anodes Zhao, Chen-Zi; Zhang, Xue-Qiang; Cheng, Xin-Bing Proceedings of the National Academy of Sciences, Vol. 114, Issue 42 https://doi.org/10.1073/pnas.1708489114	journal	October 2017
Elastic and Li-ion–percolating hybrid membrane stabilizes Li metal plating Pang, Quan; Zhou, Laidong; Nazar, Linda F. Proceedings of the National Academy of Sciences, Vol. 115, Issue 49 https://doi.org/10.1073/pnas.1809187115	journal	November 2018
Poly(dimethyl siloxane) (PDMS) XPS Reference Core Level and Energy Loss Spectra Louette, Pierre; Bodino, Frederic; Pireaux, Jean-Jacques Surface Science Spectra, Vol. 12, Issue 1 https://doi.org/10.1116/11.20050908	journal	December 2005
Electrochemical Kinetics of Lithium Plating and Stripping in Solid Polymer Electrolytes: Pulsed Voltammetry Berliner, Marc D.; McGill, Brandon C.; Majeed, Muneeb Journal of The Electrochemical Society, Vol. 166, Issue 2 https://doi.org/10.1149/2.0851902jes	journal	January 2019

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