Hydrogen-Bonded Organic Framework as Superior Separator with High Lithium Affinity C═N Bond for Low N/P Ratio Lithium Metal Batteries.

Lithium dendrite and side reactions are two major challenges for lithium metal anode. Here, the highly lithophilic triazine ring in the hydrogen-bonded organic framework is recommended to accelerate the desolvation process of lithium ions. Among them, the formation of Li-N bonds between lithium ions and the triazine ring in CAM reduces the diffusion energy barrier of Li+ crossing the SEI interface and the desolvation energy barrier of Li+ exiting from the solvent sheath so that the rapid and homogeneous deposition of lithium-ion can be achieved. Meanwhile, the lithium-ion migration coefficient can be as high as 0.70. CAM separator is used to assemble lithium metal batteries with nickel-rich cathodes (NCM 622). When N/P = 8 and 5, the capacity retention rates of Li-NCM 622 full cell are 78.2% and 80.5% after 200 and 110 cycles, respectively, and the Coulomb efficiency can be maintained at 99.5%, showing excellent cycle stability.

[1]  Xiangming He,et al.  Significance of Antisolvents on Solvation Structures Enhancing Interfacial Chemistry in Localized High-Concentration Electrolytes , 2022, ACS central science.

[2]  Haoshen Zhou,et al.  A stable quasi-solid electrolyte improves the safe operation of highly efficient lithium-metal pouch cells in harsh environments , 2022, Nature communications.

[3]  Lin Li,et al.  Graphene-Supported Naphthalene-Based Polyimide Composite as a High-Performance Sodium Storage Cathode. , 2022, ACS applied materials & interfaces.

[4]  Min Zhu,et al.  A Self-Supporting Covalent Organic Framework Separator with Desolvation Effect for High Energy Density Lithium Metal Batteries , 2022, ACS Energy Letters.

[5]  Zonghai Chen,et al.  Suppressing electrolyte-lithium metal reactivity via Li+-desolvation in uniform nano-porous separator , 2022, Nature communications.

[6]  M. Winter,et al.  Understanding the Role of Commercial Separators and Their Reactivity toward LiPF6 on the Failure Mechanism of High‐Voltage NCM523 || Graphite Lithium Ion Cells , 2021, Advanced Energy Materials.

[7]  W. He,et al.  Scalable Synthesis of Li2GeO3/Expanded Graphite as a High-Performance Anode for Li-ion Batteries , 2021, Journal of Alloys and Compounds.

[8]  Chaoqun Niu,et al.  High-Voltage Tolerant Covalent Organic Framework Electrolyte with Holistically Oriented Channels for Solid-State Lithium Metal Batteries with Nickel-Rich Cathodes. , 2021, Angewandte Chemie.

[9]  P. He,et al.  Sustainable lithium-metal battery achieved by a safe electrolyte based on recyclable and low-cost molecular sieve. , 2021, Angewandte Chemie.

[10]  Wangda Li,et al.  Long-Term Cyclability of NCM-811 at High Voltages in Lithium-Ion Batteries: an In-Depth Diagnostic Study , 2020 .

[11]  P. He,et al.  A Liquid Electrolyte with De-Solvated Lithium Ions for Lithium-Metal Battery , 2020 .

[12]  M. Winter,et al.  Toward Green Battery Cells: Perspective on Materials and Technologies , 2020 .

[13]  Tianfu Liu,et al.  Record Complexity in the Polycatenation of Three Porous Hydrogen-bonded Organic Frameworks with Stepwise Adsorption Behaviors. , 2020, Journal of the American Chemical Society.

[14]  John C. McMurtrie,et al.  Crystal transformation from the incorporation of coordinate bonds into a hydrogen-bonded network yields robust free-standing supramolecular membranes. , 2019, Journal of the American Chemical Society.

[15]  M. Xiao,et al.  In Situ Preparation of Thin and Rigid COF Film on Li Anode as Artificial Solid Electrolyte Interphase Layer Resisting Li Dendrite Puncture , 2019, Advanced Functional Materials.

[16]  Yulong Sun,et al.  Facile Generation of Polymer-Alloy Hybrid Layer towards Dendrite-free Lithium Metal Anode with Improved Moisture Stability. , 2019, Angewandte Chemie.

[17]  Weishan Li,et al.  Overlooked electrolyte destabilization by manganese (II) in lithium-ion batteries , 2019, Nature Communications.

[18]  Hongkyung Lee,et al.  High-energy lithium metal pouch cells with limited anode swelling and long stable cycles , 2019, Nature Energy.

[19]  Jun Lu,et al.  Commercialization of Lithium Battery Technologies for Electric Vehicles , 2019, Advanced Energy Materials.

[20]  Yayuan Liu,et al.  An Autotransferable g‐C3N4 Li+‐Modulating Layer toward Stable Lithium Anodes , 2019, Advanced materials.

[21]  Venkat R. Subramanian,et al.  Pathways for practical high-energy long-cycling lithium metal batteries , 2019, Nature Energy.

[22]  M. Winter,et al.  Before Li Ion Batteries. , 2018, Chemical reviews.

[23]  Xingcheng Xiao,et al.  A Bottom-Up Formation Mechanism of Solid Electrolyte Interphase Revealed by Isotope-Assisted Time-of-Flight Secondary Ion Mass Spectrometry. , 2018, The journal of physical chemistry letters.

[24]  J. Nan,et al.  Quinone Electrode Materials for Rechargeable Lithium/Sodium Ion Batteries , 2017 .

[25]  Rui Zhang,et al.  Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review. , 2017, Chemical reviews.

[26]  Wangda Li,et al.  Formation and Inhibition of Metallic Lithium Microstructures in Lithium Batteries Driven by Chemical Crossover. , 2017, ACS nano.

[27]  Y. Qi,et al.  Computational Exploration of the Li-Electrode|Electrolyte Interface in the Presence of a Nanometer Thick Solid-Electrolyte Interphase Layer. , 2016, Accounts of chemical research.

[28]  Narendra Kumar,et al.  Lithium-Ion Model Behavior in an Ethylene Carbonate Electrolyte Using Molecular Dynamics , 2016 .

[29]  Yuki Yamada,et al.  Superconcentrated electrolytes for a high-voltage lithium-ion battery , 2016, Nature Communications.

[30]  O. Borodin,et al.  High rate and stable cycling of lithium metal anode , 2015, Nature Communications.