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Engineering Functionalized 2D Metal-Organic Frameworks Nanosheets with Fast Li+ Conduction for Advanced Solid Li Batteries

Journal Article · · Advanced Materials
 [1];  [2];  [2];  [2];  [3];  [2];  [3];  [2];  [2];  [3];  [1];  [3];  [2]
  1. Central South University, Changsha (China); Central South University of Forestry and Technology, Changsha (China)
  2. Central South University, Changsha (China)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States)
+ Show Author Affiliations
Solid-state batteries can ensure high energy density and safety in lithium metal batteries, while polymer electrolytes are plagued by slow ion kinetics and low selective transport of Li+. Metal-organic frameworks (MOFs) are proposed as emerging fillers for solid-state poly(ethylene oxide)(PEO) electrolytes, however, developing functionalized MOFs and understanding their roles on ion transfer has proven challenging. Herein, combining computational and experimental results, the functional group regulation in MOFs can effectively change surficial charge distribution and limit anion movement is revealed, providing a potential solution to these issues. Specifically, functionalized 2D MOF sheets are designed through molecular engineering to construct high-performance composite electrolytes, where the electron-donating effect of substituents in 2D-MOFs effectively limits the movement of ClO4- and promotes mechanical properties and ion migration numbers (0.36 up to 0.64) of PEO. As a result, Li/Li cells with composite electrolyte exhibit superior cyclability for 1000 h at a current density of 0.2 mA cm-2. Meanwhile, the solid LiFePO4/Li battery delivers highly reversible capacities of 148.8 mAh g-1 after 200 cycles. In conclusion, these findings highlight a new approach for anion confinement through the use of functional group electronic effects, leading to enhanced ionic conductivity, and a feasible direction for high-performance solid-state batteries.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
Hunan Provincial Natural Science Foundation; National Natural Science Foundation of China (NSFC); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2371816
Alternate ID(s):
OSTI ID: 1995918
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 38 Vol. 35; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

References (42)

Shape‐Assisted 2D MOF/Graphene Derived Hybrids as Exceptional Lithium‐Ion Battery Electrodes journal July 2019
Amine‐Functionalized Boron Nitride Nanosheets: A New Functional Additive for Robust, Flexible Ion Gel Electrolyte with High Lithium‐Ion Transference Number journal February 2020
Asymmetric Polymer Electrolyte Constructed by Metal–Organic Framework for Solid‐State, Dendrite‐Free Lithium Metal Battery journal October 2020
Intermolecular Chemistry in Solid Polymer Electrolytes for High‐Energy‐Density Lithium Batteries journal July 2019
A Single‐Ion Conducting Borate Network Polymer as a Viable Quasi‐Solid Electrolyte for Lithium Metal Batteries journal January 2020
Long‐Life Regenerated LiFePO4 from Spent Cathode by Elevating the d‐Band Center of Fe journal December 2022
Differentiated Lithium Salt Design for Multilayered PEO Electrolyte Enables a High‐Voltage Solid‐State Lithium Metal Battery journal September 2019
Stable Seamless Interfaces and Rapid Ionic Conductivity of Ca–CeO 2 /LiTFSI/PEO Composite Electrolyte for High‐Rate and High‐Voltage All‐Solid‐State Battery journal April 2020
On the Beneficial Impact of Li 2 CO 3 as Electrolyte Additive in NCM523 ∥ Graphite Lithium Ion Cells Under High‐Voltage Conditions journal January 2021
Li 2 S 6 ‐Integrated PEO‐Based Polymer Electrolytes for All‐Solid‐State Lithium‐Metal Batteries journal June 2021
2D MOF with Compact Catalytic Sites for the One‐pot Synthesis of 2,5‐Dimethylfuran from Saccharides via Tandem Catalysis journal July 2022
A 3D Nanostructured Hydrogel-Framework-Derived High-Performance Composite Polymer Lithium-Ion Electrolyte journal January 2018
A Metal–Organic Framework with Tetrahedral Aluminate Sites as a Single‐Ion Li + Solid Electrolyte journal December 2018
Flexible Films of Covalent Organic Frameworks with Ultralow Dielectric Constants under High Humidity journal November 2018
2D Metal–Organic Frameworks for Electrochemical Energy Storage journal February 2023
Carbon Dots Evoked Li Ion Dynamics for Solid State Battery journal August 2021
An All‐Solid‐State Battery Based on Sulfide and PEO Composite Electrolyte journal June 2022
Controllable design of high-efficiency triboelectric materials by functionalized metal—organic frameworks with a large electron-withdrawing functional group journal July 2022
PEO-based composite polymer electrolytes journal July 1998
2D MOFs and their derivatives for electrocatalytic applications: Recent advances and new challenges journal December 2022
High ionic conductivity PEO-based electrolyte with 3D framework for Dendrite-free solid-state lithium metal batteries at ambient temperature journal March 2022
Engineered networking in a family of solvent-free single-ion conducting borate network polymer electrolytes for Li-metal battery applications journal December 2022
Cathode supported solid lithium batteries enabling high energy density and stable cyclability journal March 2021
Few-layer bismuthene enabled solid-state Li batteries journal November 2022
Slurry-like hybrid electrolyte with high lithium-ion transference number for dendrite-free lithium metal anode journal September 2020
Adsorptive removal of aromatic diamines from water using metal-organic frameworks functionalized with a nitro group journal February 2023
High Electrical Conductivity in a 2D MOF with Intrinsic Superprotonic Conduction and Interfacial Pseudo-capacitance journal March 2020
Ultrathin two-dimensional nanosheet metal-organic frameworks with high-density ligand active sites for advanced lithium-ion capacitors journal December 2022
Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review journal July 2017
Highly Conductive PEO-like Polymer Electrolytes journal September 1997
From Hydrated Ni3(OH)2(C8H4O4)2(H2O)4 to Anhydrous Ni2(OH)2(C8H4O4): Impact of Structural Transformations on Magnetic Properties journal January 2014
Molecular Structure and Dynamics of LiClO4-Polyethylene Oxide-400 (Dimethyl Ether and Diglycol Systems) at 25 .degree.C journal August 1994
Metal–Organic Frameworks as Surface Enhanced Raman Scattering Substrates with High Tailorability journal December 2018
Membrane adsorbers with ultrahigh metal-organic framework loading for high flux separations journal September 2019
Pathways for practical high-energy long-cycling lithium metal batteries journal February 2019
Understanding and applying coulombic efficiency in lithium metal batteries journal June 2020
Ultrathin, flexible, solid polymer composite electrolyte enabled with aligned nanoporous host for lithium batteries journal May 2019
Quantifying inactive lithium in lithium metal batteries journal August 2019
MOF-derived nanoporous multifunctional fillers enhancing the performances of polymer electrolytes for solid-state lithium batteries journal January 2019
Determining the limiting factor of the electrochemical stability window for PEO-based solid polymer electrolytes: main chain or terminal –OH group? journal January 2020
Prospects and limitations of single-crystal cathode materials to overcome cross-talk phenomena in high-voltage lithium ion cells journal January 2021
3D nanoprinting of semiconductor quantum dots by photoexcitation-induced chemical bonding journal September 2022

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Related Subjects

25 ENERGY STORAGE
Li+ transport
MOFs
anion confinement
polymer electrolyte
solid-state batteries