Single‐Atom 3d Transition Metals on SnO2 as Model Cell for Conversion Mechanism: Revealing Thermodynamic Catalytic Effects on Enhanced Na Storage of Heterostructures DOI

Minggang Xie,

Zhe Zhang, Cheng Zheng

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(40)

Published: July 3, 2024

Abstract Since the discovery in 2000, conversion‐type materials have emerged as a promising negative‐electrode candidate for next‐generation batteries with high capacity and tunable voltage, limited by low reversibility severe voltage hysteresis. Heterogeneous construction stands out cost‐effective efficient approach to reducing reaction barriers enhancing energy density. However, second term introduced conventional heterostructure inevitably complicates electrochemical analysis poses great challenges harvesting systematic insights theoretical guidance. A model cell is designed established herein conversion reactions between Na TM SA −SnO 2 , where represents single atom modification of eight different 3d transition elements (V, Cr, Mn, Fe, Co, Ni, Cu or Zn). Such unit fundamentally eliminates interference from phase thus enables independent exploration activation manifestations heterogeneous architecture. For first time, thermodynamically dependent catalytic effect proposed verified through statistical data analysis. The mechanism behind unveiled further elucidated which active d orbitals metals weaken surface covalent bonds lower barriers. This research provides both practical demonstrations advanced electrodes.

Language: Английский

Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries DOI

Xiaotian Guo,

Hengyue Xu,

Yijian Tang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 31, 2024

Abstract Aqueous zinc–iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost‐effectiveness, and scalability. However, the inadequate redox kinetics severe shuttling effect of polyiodide ions impede commercial viability. Herein, several Zn‐MOF‐derived porous carbon materials designed, further preparation iron–doped (Fe–N–C, M9) with varied Fe doping contents is optimized based on a facile self‐assembly/carbonization approach. M9, atomic coordinated nitrogen atoms, employed as an efficient cathode host AZIBs. Functional modifications hosts involving species levels investigated. The adsorption tests, in situ Raman spectroscopy, UV–vis results demonstrate capability charge‐discharge mechanism iodine species. Furthermore, experimental findings theoretical analyses have proven that conversion enhanced through physicochemical confinement effect. This study offers basic principles strategic design single‐atom dispersed high‐performance Flexible soft–pack battery wearable microbattery applications also implications future long‐life aqueous designs.

Language: Английский

Citations

53

Heterojunction Vacancies‐Promoted High Sodium Storage Capacity and Fast Reaction Kinetics of the Anodes for Ultra‐High Performance Sodium‐Ion Batteries DOI
Hui Zheng,

Dakai Ma,

Maojun Pei

et al.

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

Published: Sept. 6, 2024

Abstract Transition metal sulfides as anode materials for sodium‐ion batteries (SIBs) have the advantage of high capacity. However, their cycle‐life and rate performance at ultra‐high current density is still a thorny issue that limit applicability these materials. In this paper, carbon‐embedded heterojunction with sulfur‐vacancies regulated by ultrafine bimetallic (vacancy‐CoS 2 /FeS @C) robust interfacial C‐S‐Co/Fe chemical bonds successfully synthesized explored an material battery. By changing ratio two cations, concentration anion sulfur vacancies can be in‐situ adjusted without additional post‐treatment. The as‐prepared vacancy‐CoS @C offers ultrahigh (285.1 mAh g −1 200 A ), excellent long‐cycle stability (389.2 40 after 10000 cycles), outperforming all reported transition sulfides‐based SIBs. Both ex‐situ characterizations provide strong evidence evolution mechanism phases stable solid‐electrolyte interface (SEI) on surface. functional theory calculations show constructing reasonable significantly increase electronic conductivity. Notably, assembled @C//Na 3 V (PO 4 ) /C full‐cell shows capacity 226.2 400 cycles 2.0 , confirming material's practicability.

Language: Английский

Citations

34

Enabling Efficient Anchoring‐Conversion Interface by Fabricating Double‐Layer Functionalized Separator for Suppressing Shuttle Effect DOI
Junan Feng,

Chaoyue Zhang,

Wendong Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(41)

Published: July 15, 2024

Abstract Lithium‐sulfur batteries (LiSBs) with high energy density still face challenges on sluggish conversion kinetics, severe shuttle effects of lithium polysulfides (LiPSs), and low blocking feature ordinary separators to LiPSs. To tackle these, a novel double‐layer strategy functionalize is proposed, which consists Co atomically dispersed CoN 4 decorated Ketjen black (Co/CoN @KB) layer an ultrathin 2D Ti 3 C 2 T x MXene layer. The theoretical calculations experimental results jointly demonstrate metallic sites provide efficient adsorption catalytic capability for long‐chain LiPSs, while active facilitate the absorption short‐chain LiPSs promote Li S. stacking serves as microscopic barrier further physically block chemically anchor leaked from pores gaps Co/CoN @KB layer, thus preserving within anchoring‐conversion reaction interfaces balance accumulation “dead S” Consequently, ultralight loading @KB‐MXene, LiSBs exhibit amazing electrochemical performance even under sulfur lean electrolyte, outperforming lithium‐selenium (LiSeBs) can also be achieved. This work exploits universal effective functionalized separator regulate equilibrium adsorption‐catalytic interface, enabling high‐energy long‐cycle LiSBs/LiSeBs.

Language: Английский

Citations

28

Physical Field Effects to Suppress Polysulfide Shuttling in Lithium–Sulfur Battery DOI
Junan Feng, Chuan Shi, Xiaoxian Zhao

et al.

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

Published: Oct. 14, 2024

Lithium-sulfur batteries (LSB) with high theoretical energy density are plagued by the infamous shuttle effect of lithium polysulfide (LPS) and sluggish sulfur reduction/evolution reaction. Extensive research is conducted on how to suppress effects, including physical structure confinement engineering, chemical adsorption strategy, design redox catalysts. Recently, rational mitigate effects enhance reaction kinetics based field has been widely studied, providing a more fundamental understanding interactions species. Herein, focused their methods mechanisms interaction summarized systematically LPS. Overall, working principle LSB system, origin effect, kinetic trouble in briefly described. Then, mechanism application materials concepts external field-assisted elaborated, electrostatic force, built-in electric field, spin state regulation, strain magnetic photoassisted other strategies pivotally elaborated discussed. Finally, potential directions enhancing performance weakening high-energy anticipated.

Language: Английский

Citations

20

Ideal Bi-Based Hybrid Anode Material for Ultrafast Charging of Sodium-Ion Batteries at Extremely Low Temperatures DOI Creative Commons
Jie Bai,

Jian Hui Jia,

Yu Wang

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Nov. 13, 2024

Abstract Sodium-ion batteries have emerged as competitive substitutes for low-temperature applications due to severe capacity loss and safety concerns of lithium-ion at − 20 °C or lower. However, the key capability ultrafast charging ultralow temperature SIBs is rarely reported. Herein, a hybrid Bi nanoparticles embedded in carbon nanorods demonstrated an ideal material address this issue, which synthesized via high shock method. Such shows unprecedented rate performance (237.9 mAh g −1 2 A ) 60 °C, outperforming all reported SIB anode materials. Coupled with Na 3 V (PO 4 cathode, energy density full cell can reach 181.9 Wh kg 40 °C. Based on work, novel strategy high-rate activation proposed enhance performances Bi-based materials cryogenic conditions by creating new active sites interfacial reaction under large current.

Language: Английский

Citations

11

Heteroatom Immobilization Engineering toward High-Performance Metal Anodes DOI
Jianan Gu, Yongzheng Zhang, Yu Shi

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 11, 2024

Heteroatom immobilization engineering (HAIE) is becoming a forefront approach in materials science and engineering, focusing on the precise control manipulation of atomic-level interactions within heterogeneous systems. HAIE has emerged as an efficient strategy to fabricate single-atom sites for enhancing performance metal-based batteries. Despite significant progress achieved through metal anodes batteries, several critical challenges such dendrites, side reactions, sluggish reaction kinetics are still present. In this review, we delve into fundamental principles underlying heteroatom anodes, aiming elucidate its role electrochemical We systematically investigate how facilitates uniform nucleation inhibits reactions at anode-electrolyte interface, promoting desolvation ions accelerating Finally, discuss various strategies implementing electrode materials, high-temperature pyrolysis, vacancy reduction, molten-salt etching anchoring. These include selecting appropriate heteroatoms, optimizing methods, constructing material architectures. They can be utilized further refine enhance capabilities facilitate widespread application next-generation battery technologies.

Language: Английский

Citations

9

Tailoring a High Loading Atomic Zinc with Weak Binding to Sodium Toward High‐Energy Sodium Metal Batteries DOI Open Access
S. Zhao, Xudong Chen, David Patrun

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 10, 2025

Abstract Single‐atom materials provide a platform to precisely regulate the electrochemical redox behavior of electrode with atomic level. Here, multifield‐regulated sintering route is reported rapidly prepare single‐atom zinc very high loading mass 24.7 wt.% by significantly improved diffusion kinetics and stronger charge transfer between nitrogen atoms. X‐ray absorption near edge structure (XANES) spectra for Zn K‐edges during discharge process verify stable reversible slight reduction oxidation sites, which much different from previous report alloying reaction process. This result suggests acts as an active sites through weak binding sodium Na ion fluxes. Finally, Cu foil coated ≈2 µm layer such material exhibits Coulombic efficiency ≈99.99% up 1700 cycles at 1 mA h cm −2 . An ultra‐low overpotential 3 mV unprecedented life span over 3200 in symmetrical cell achieved. Due thin coating layer, anode‐free battery fabricated V 2 (PO 4 ) cathode displays prominent energy density 320 Wh Kg −1 , demonstrating strong potential practical application.

Language: Английский

Citations

1

MXenes-based separators with nanoconfined two-dimensional channels for high-performance lithium–sulfur battery DOI
Yüe Zhao, Shuai Li,

Yu-Lu Huo

et al.

Rare Metals, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 17, 2025

Language: Английский

Citations

1

Promoting Robust and Rapid Na‐Ion Storage of Molybdenum‐Based Sulfide via Rational Hetero and Hollow Structure Design DOI Open Access
Wei Liu,

Ren Huang,

Caiyan Yu

et al.

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

Published: March 3, 2025

Abstract Molybdenum disulfide (MoS 2 ), characterized by its two‐dimensional structure and high theoretical specific capacity, is considered a prospective anode of Na‐ion battery. However, the cycling rate capabilities are hampered sluggish charge transfer kinetics poor structural stability. To overcome issues, most efforts have been focused on optimizing MoS . Nevertheless, rationally designing that can present rapid durable storage while ensuring large remains challenges. Herein, /MnS heterostructure featuring sphere‐like hollow morphology designed according to Ostwald ripening process Kirkendall effect. This construction effectively establish an interfacial built‐in electric field activated MnS , which exhibit P‐type N‐type semiconductor characteristics, respectively, thereby promoting electrochemical kinetics. Moreover, excellent stability after repeated (de)sodiation processes remarkably achieved thanks robust design, significantly achieving outstanding tolerance changes. Consequently, delivers capacity (594.8 mAh g −1 at 0.1 A superior performance (up 100 ultrastable capability (30 000 cycles with ≈81.4% retention). The work affords effective optimization tactic develop high‐performance conversion‐type electrodes for alkali‐ion batteries.

Language: Английский

Citations

1

Origin of the High Catalytic Activity of MoS2 in Na–S Batteries: Electrochemically Reconstructed Mo Single Atoms DOI

Xue Zhong,

Yujie Huang,

Jieming Cai

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(46), P. 32124 - 32134

Published: Nov. 8, 2024

Room-temperature sodium–sulfur (RT Na–S) batteries with high energy density and low cost are considered promising next-generation electrochemical storage systems. However, their practical feasibility is seriously impeded by the shuttle effect of sodium polysulfide (NaPSs) resulting from sluggish reaction kinetics. Introducing a suitable catalyst to accelerate conversion NaPSs most used strategy inhibit effect. Traditional catalytic approaches often want avoid irreversible phase transition at deep discharge. On contrary, here, we leverage intrinsic structural tunability MoS2 in opposite direction innovatively propose voltage modulation for situ generation trace Mo single atoms (MoSAC) during first charge–discharge process, leading formation highly active phases (MoS2/MoSAC) through self-reconstruction. Theoretical calculations reveal that incorporation MoSAC modulates electronic structure d-band center, which not only effectively promotes d–p orbital hybridization but also accelerates intermediate desorption bonding transition, dynamic single-atom synergistic mechanism enhances adsorption response between metal site NaPSs, significantly improves sulfur redox (SRR), initial capacity MoS2/MoSAC/CF@S cell 0.2 A g–1 increased 46.58% compared MoS2/CF@S cell. The discovery MoS2/MoSAC/CF provides new insights into adjusting function disulfide catalysts atomic scale, offering hope development high-specific-energy RT Na–S batteries.

Language: Английский

Citations

5