D-orbital Reconstruction Achieves Low Charge Overpotential in Li-oxygen Batteries

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: April 9, 2025

Language: Английский

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Upcycling Spent Lithium‐Ion Batteries: Constructing Bifunctional Catalysts Featuring Long‐Range Order and Short‐Range Disorder for Lithium‐Oxygen Batteries

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 25, 2025

Abstract Upcycling of high‐value metals (M = Ni, Co, Mn) from spent ternary lithium‐ion batteries to the field lithium‐oxygen is highly appealing, yet remains a huge challenge. In particular, alloying recovered M components with Pt and applied as cathode catalysts have not been reported. Herein, fresh L1 2 ‐type 3 medium‐entropy intermetallic nanoparticle first proposed, confined on N‐doped carbon matrix (L1 ‐Pt (Ni 1/3 Co Mn )@N‐C) based 111 typed LiNi 1‐x‐y x y O cathode. This well‐defined catalyst combines both features long‐range order face‐centered cubic structure short‐range disorder in sites. The former contributes enhancing structural stability, latter further facilitates deeply activating catalytic activity Experiments theoretical results demonstrate that local coordination environment electronic distribution are fundamentally modulated via surrounding disordered atoms, which greatly optimize affinity toward oxygen‐containing intermediates facilitate deposition/decomposition kinetics thin‐film Li discharge products. Specifically, 1/3) @N‐C exhibits an ultra‐low overpotential 0.48 V achieves 220 cycles at 400 mA g −1 under 1000 mAh . work provides important insights for recycling into advanced catalyst‐related applications.

Language: Английский

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Ultra‐tough Dynamic Supramolecular Ion‐conducting Elastomer Induced Uniform Li+ Transport and Stabilizes Interphase Ensures Dendrite‐free Lithium Metal Anodes

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 11, 2024

Abstract Artificial polymer solid electrolyte interphases (SEIs) with microphase‐separated structures provide promising solutions to the inhomogeneity and cracking issues of natural SEIs in lithium metal batteries (LMBs). However, achieving homogeneous ionic conductivity, excellent mechanical properties, superior interfacial stability remains challenging due interference from hard‐phase domains ion transport solid‐solid interface metal. Herein, we present a dynamic supramolecular ion‐conducting poly (urethane‐urea) interphase (DSIPI) that achieves these three properties through modulating constructing composite SEI situ. The soft‐phase polytetrahydrofuran backbone, featuring loose Li + −O coordinating interactions, ensures uniform transport. Concurrently, sextuple hydrogen bonds hard phase dissipate strain energy sequential bond cleavage, thereby imparting exceptional properties. Moreover, enriched bis (trifluoromethanesulfonyl) imide anion (TFSI − ) DSIPI promotes situ formation stable polymer‐inorganic during cycling. Consequently, DSIPI‐protected anode (DSIPI@Li) enables symmetric cells cyclability exceeding 4,000 hours at an ultra‐high current density 20 mA cm −2 , demonstrating cycling stability. Furthermore, DSIPI@Li facilitates operation pouch under constraints high‐loading LiNi 0.8 Co 0.1 Mn O 2 cathode low negative/positive capacity (N/P) ratio. This work presents powerful strategy for designing artificial high‐performance LMBs.

Language: Английский

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Partial‐Oxidation Enabling Homologous Ru/RuO₂ Heterostructures With Proper d‐Dand Center as Efficient and Durable Cathode Catalysts for Ultralong Cycle Life in Li–O₂ Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 22, 2024

Abstract The sluggish cycle kinetics is one of the major obstacles to commercial application Li–O 2 batteries (LOBs), despite their large theoretical energy density. Efficient and long‐term durable cathode catalysts are urgently desired strengthen stability rate performance. Density functional theory calculations reveal that Ru/RuO Mott–Schottky heterostructures can manipulate adsorption capacities intermediates by modulating d‐band center redistribute interfacial charges, enabling efficient redox kinetics, reducing overpotentials, optimizing growth pathway discharge products. Herein, a wet impregnation approach followed partial oxidization Ru nanodots construct homologous as advanced for boosting electrochemical activities LOBs employed. They exhibit superior performance, including high specific capacity (17 120 mAh g −1 at 200 mA ), small overpotential (0.96 V), ultralong lifetime 1209 cycles (>2400 h) 500 . Over 1260‐h stable in air atmosphere demonstrates potential prospects Li‐air batteries. Multiple ex/in situ measurements calculation conducted investigate mechanism performances.

Language: Английский

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Ultra‐tough Dynamic Supramolecular Ion‐conducting Elastomer Induced Uniform Li+ Transport and Stabilizes Interphase Ensures Dendrite‐free Lithium Metal Anodes

Angewandte Chemie, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 11, 2024

Abstract Artificial polymer solid electrolyte interphases (SEIs) with microphase‐separated structures provide promising solutions to the inhomogeneity and cracking issues of natural SEIs in lithium metal batteries (LMBs). However, achieving homogeneous ionic conductivity, excellent mechanical properties, superior interfacial stability remains challenging due interference from hard‐phase domains ion transport solid‐solid interface metal. Herein, we present a dynamic supramolecular ion‐conducting poly (urethane‐urea) interphase (DSIPI) that achieves these three properties through modulating constructing composite SEI situ. The soft‐phase polytetrahydrofuran backbone, featuring loose Li + −O coordinating interactions, ensures uniform transport. Concurrently, sextuple hydrogen bonds hard phase dissipate strain energy sequential bond cleavage, thereby imparting exceptional properties. Moreover, enriched bis (trifluoromethanesulfonyl) imide anion (TFSI − ) DSIPI promotes situ formation stable polymer‐inorganic during cycling. Consequently, DSIPI‐protected anode (DSIPI@Li) enables symmetric cells cyclability exceeding 4,000 hours at an ultra‐high current density 20 mA cm −2 , demonstrating cycling stability. Furthermore, DSIPI@Li facilitates operation pouch under constraints high‐loading LiNi 0.8 Co 0.1 Mn O 2 cathode low negative/positive capacity (N/P) ratio. This work presents powerful strategy for designing artificial high‐performance LMBs.

Language: Английский

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Solid‐State Electrolytes for Lithium‐Air Batteries

Batteries & Supercaps, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 24, 2024

Abstract Li‐air batteries (LABs) have attracted widespread attention due to their extremely high theoretical capacity and energy density. However, the practical application of liquid‐stateLABs is substantially hindered by safety concerns, including flammability, leakage, electrolyte decomposition. In comparison, solid‐state electrolytes (SSEs) possess excellent mechanical strength, safety, good stability, non‐flammable characteristics, offering a feasible strategy for achieving stable LABs. this review, we will focus on development challenges lithium‐air (SSLABs), providing an overview various types SSEs discussing interfacial issues within SSLABs along with potential solutions, finally propose strategies outlooks advanced SSLABs. It expected that review provide systematic understanding framework guide design high‐performance

Language: Английский

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