Reactive Polymer as Artificial Solid Electrolyte Interface for Stable Lithium Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(26)

Published: April 29, 2023

Lithium (Li) metal anodes have the highest theoretical capacity and lowest electrochemical potential making them ideal for Li batteries (LMBs). However, dendrite formation on anode impedes proper discharge practical cycle life of LMBs, particularly in carbonate electrolytes. Herein, we developed a reactive alternative polymer named P(St-MaI) containing carboxylic acid cyclic ether moieties which would situ form artificial polymeric solid electrolyte interface (SEI) with Li. This SEI can accommodate volume changes maintain good interfacial contact. The presence pendant groups greatly contribute to induction uniform ion deposition. In addition, benzyl rings makes certain mechanical strength plays key role inhibiting growth dendrites. As result, symmetric Li||Li cell P(St-MaI)@Li layer stably over 900 h under 1 mA cm-2 without polarization voltage increasing, while their Li||LiFePO4 full high retention 96 % after 930 cycles at 1C innovative strategy is broadly applicable designing new materials inhibit anodes.

Language: Английский

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Roadmap for rechargeable batteries: present and beyond

Science China Chemistry, Journal Year: 2023, Volume and Issue: 67(1), P. 13 - 42

Published: Dec. 26, 2023

Language: Английский

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Multiple Dynamic Bonds‐Driven Integrated Cathode/Polymer Electrolyte for Stable All‐Solid‐State Lithium Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(35)

Published: July 11, 2023

All-solid-state lithium metal batteries (LMBs) are considered as the promising higher-energy and improved-safety energy-storage systems. Nevertheless, electrolyte-electrodes interfacial issues due to limited solid physical contact lead discontinuous charge transport large resistance, thereby suffering from unsatisfactory electrochemical performance. Herein, we construct an integrated cathode/polymer electrolyte for all-solid-state LMBs under action of polymer chains exchange recombination originating multiple dynamic bonds in our well-designed supramolecular ionic conductive elastomers (DSICE) molecular structure. The DSICE acts electrolytes with excellent performance mechanical properties, achieving ultrathin pure thickness (12 μm). Notably, also functions iron phosphate (LiFePO4 , LFP) cathode binders enhanced adhesive capability. Such well-constructed Li|DSICE|LFP-DSICE cells generate delicate at level, providing continuous Li+ pathways promoting uniform deposition, further delivering superior long-term charge/discharge stability (>600 cycles, Coulombic efficiency, >99.8 %) high capacity retention (80 % after 400 cycles). More practically, pouch show stable performance, flexibility safety abusive tests.

Language: Английский

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Lithiophilic Covalent Organic Framework as Anode Coating for High‐Performance Lithium Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)

Published: Jan. 16, 2024

Abstract The growth of disorganized lithium dendrites and weak solid electrolyte interphase greatly impede the practical application metal batteries. Herein, we designed synthesized a new kind stable polyimide covalent organic frameworks (COFs), which have high density well‐aligned lithiophilic quinoxaline phthalimide units anchored within uniform one‐dimensional channels. COFs can serve as an artificial on anode, effectively guiding deposition ions inhibiting dendrites. unsymmetrical Li||COF−Cu battery exhibits Coulombic efficiency 99 % at current 0.5 mA cm −2 , be well retained up to 400 cycles. Meanwhile, Li‐COF||LFP full cell shows over charge 0.3 C. And its capacity maintained 91 even after 150 Therefore, significant electrochemical cycling stability illustrates feasibility employing in solving disordered

Language: Английский

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Rational Design of F-Modified Polyester Electrolytes for Sustainable All-Solid-State Lithium Metal Batteries

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(9), P. 5940 - 5951

Published: Feb. 22, 2024

Solid polymer electrolytes (SPEs) are one of the most practical candidates for solid-state batteries owing to their high flexibility and low production cost, but application is limited by Li+ conductivity a narrow electrochemical window. To improve performance, it necessary reveal structure–property relationship SPEs. Here, 23 fluorinated linear polyesters were prepared editing coordination units, flexible linkage segments, interface passivating groups. Besides traditionally demonstrated coordinating capability chains, molecular asymmetry resulting interchain aggregation observed critical conductivity. By tailoring ability polyesters, can be raised 10 times. Among these solvent-free poly(pentanediol adipate) delivers highest room-temperature 0.59 × 10–4 S cm–1. The chelating oxalate leads an electron delocalization alkoxy oxygen, enhancing antioxidation lower high-value LiTFSI in SPEs recycled at 90%, regenerated 86%. This work elucidates polyester-based SPEs, displays design principles provides way development sustainable batteries.

Language: Английский

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Build a High‐Performance All‐Solid‐State Lithium Battery through Introducing Competitive Coordination Induction Effect in Polymer‐Based Electrolyte

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 22, 2024

Abstract Polymer‐inorganic composite electrolytes (PICE) have attracted tremendous attention in all‐solid‐state lithium batteries (ASSLBs) due to facile processability. However, the poor Li + conductivity at room temperature (RT) and interfacial instability severely hamper practical application. Herein, we propose a concept of competitive coordination induction effects (CCIE) reveal essential correlation between local structure chemistry PEO‐based PICE. CCIE introduction greatly enhances ionic electrochemical performances ASSLBs 30 °C. Owing (Cs … TFSI − , Cs C−O−C 2,4,6‐TFA ) from cation CsPF 6 molecule (2,4,6‐TFA: 2,4,6‐trifluoroaniline), multimodal weak environment is constructed enabling high efficient migration °C (Li conductivity: 6.25×10 −4 S cm −1 ; t =0.61). Since tends be enriched interface, PF situ form LiF‐Li 3 N‐Li 2 O‐Li solid electrolyte interface with electrostatic shielding effects. The assembled without adding wetting agent exhibit outstanding rate capability (LiFePO 4: 147.44 mAh g @1 C 107.41mAhg @2 C) cycling stability 4 :94.65 %@[email protected] C; LiNi 0.5 Co 0.2 Mn 0.3 O : 94.31 %@200 [email protected] C). This work proposes reveals its mechanism designing PICE as well compatibility near RT for high‐performance ASSLBs.

Language: Английский

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Computational approach inspired advancements of solid-state electrolytes for lithium secondary batteries: from first-principles to machine learning

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(6), P. 3134 - 3166

Published: Jan. 1, 2024

The utilization of computational approaches at various scales, including first-principles calculations, MD simulations, multi-physics modeling, and machine learning techniques, has been instrumental in expediting the advancement SSEs.

Language: Английский

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Revealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Aug. 8, 2024

Understanding the Li-ions conduction network and transport dynamics in polymer electrolyte is crucial for developing reliable all-solid-state batteries. In this work, advanced nano- X-ray computed tomography combined with Raman spectroscopy solid state nuclear magnetic resonance are used to multi-scale qualitatively quantitatively reveal ion of poly(ethylene) oxide (PEO)-based (from atomic, nano macroscopic level). With clear mapping microstructural heterogeneities segments, aluminium-oxo molecular clusters (AlOC) reconstruct a high-efficient conducting high available (76.7%) continuous amorphous domains via strong supramolecular interactions. Such superionic PEO conductor (PEO-LiTFSI-AlOC) exhibites molten-like Li-ion behaviour among whole temperature range delivers an ionic conductivity 1.87 × 10

Language: Английский

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A comprehensive review on peptide-bearing biomaterials: From ex situ to in situ self-assembly

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 502, P. 215600 - 215600

Published: Dec. 14, 2023

Language: Английский

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Surface Li₂CO₃ Mediated Phosphorization Enables Compatible Interfaces of Composite Polymer Electrolyte for Solid‐State Lithium Batteries

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(35)

Published: May 10, 2023

Abstract Composite polymer electrolytes (CPEs) are subject to interface incompatibilities due the space charge layer of ceramic and phases. The intensive dehydrofluorination poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) incorporating Li 7 La 3 Zr 2 O 12 (LLZO) significantly compromises electro‐chemo‐mechanical properties compatibilities with electrodes. Herein, this study addresses challenges by precisely phosphatizing LLZO surfaces through a surface CO mediated chemical reaction. designed neutral environment ensures high air stability effective suppression PVDF‐HFP dehydrofluorination. This greatly facilitates uniform distribution phases, fast interfacial + exchange, establishing high‐throughput ion percolation pathways distinctly enhancing ionic conductivity transference number. Moreover, dramatically reduced formation products an in situ formed interphase between phosphatized metal anode stabilize Li/CPE cathode/CPE interfaces, which provide symmetric Li/Li cell solid‐state Li/LiFePO 4 Li/LiNi 0.8 Co 0.1 Mn cells exceptional cycling performance at room temperature. emphasizes vital importance achieving for CPEs provides new waste wealth route.

Language: Английский

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