Engineering Triple‐Nanolayer VN/C@TCF Cathode with Synergistic Polysulfide Regulation for High‐Performance Li‐S Batteries DOI Open Access

Jing Lan,

Ruohan Hou,

Guangpei Wang

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 9, 2025

Abstract Lithium‐sulfur batteries face three fundamental challenges: uncontrolled polysulfide shuttling, substantial volumetric fluctuations during cycling, and the inherent electrical insulation of sulfur. To address these limitations, an asymmetric self‐supporting cathode is developed, featuring TiO₂‐decorated carbon nanofibers synergistically integrated with hollow shells encapsulating vanadium nitride catalysts (VN/C@TCF). Distinct from conventional configurations, this hierarchically structured “triple‐nanolayer” system establishes sequential mitigation mechanisms: (I) TiO 2 nanoparticles in inner layer provide chemical immobilization polysulfides; (II) intermediate shell enables physical confinement; (III) outer VN nanosheets offer anchoring capacity. Combined density functional theory calculations experimental analyses reveal that VN/C@TCF architecture simultaneously enhances conductivity, demonstrates superior catalytic activity, accommodates volume variations electrochemical cycling. The optimized delivers exceptional performance metrics, including a high initial discharge capacity 1417.9 mAh g⁻¹ at 0.1 C remarkable rate capability (803.2 5 C). Notably, electrode can maintain impressive areal 6.30 cm⁻ after 80 cycles under stringent operational conditions sulfur loading (8.1 mg ) lean electrolyte (E/S ratio = 4.8 µL mg⁻¹). This strategic design paradigm provides new insights for developing electrocatalytic systems advanced lithium‐sulfur batteries.

Язык: Английский

In Situ Reconstruction of Electrocatalysts for Lithium–Sulfur Batteries: Progress and Prospects DOI
Pan Zeng, Bin Su,

Xiaolian Wang

и другие.

Advanced Functional Materials, Год журнала: 2023, Номер 33(33)

Опубликована: Май 1, 2023

Abstract The current research of Li–S batteries primarily focuses on increasing the catalytic activity electrocatalysts to inhibit polysulfide shuttling and enhance redox kinetics. However, stability is largely neglected, given premise that they are stable over extended cycles. Notably, reconstruction during electrochemical reaction process has recently been proposed. Such in situ inevitably leads varied electrocatalytic behaviors, such as sites, selectivity, activity, amounts sites. Therefore, a crucial prerequisite for design highly effective an in‐depth understanding variation active sites influence factors which not achieved fundamental summary. This review comprehensively summarizes recent advances behaviors different process, mainly including metal nitrides, oxides, selenides, fluorides, metals/alloys, sulfides. Moreover, unexplored issues major challenges chemistry summarized prospected. Based this review, new perspectives offered into true batteries.

Язык: Английский

Процитировано

57

MoC‐MoSe2 Heterostructures as Multifunctional Catalyst Toward Promoting the Stepwise Polysulfide Conversion for Lithium‐Sulfur Batteries DOI

Wenlong Xia,

Yufang Chen, Mingyu Han

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер 34(33)

Опубликована: Апрель 10, 2024

Abstract Catalyzing polysulfides conversion for lithium‐sulfur batteries is an efficient strategy to overcome the sluggish kinetics of as well its serious shuttling effect. Due multistep and complicated phase transformation sulfur species, monofunctional catalyst can hardly promote overall redox process. Herein, a molybdenum‐based heterostructure proposed, that facilitates entire reduction process by tandemly catalyzing liquid‐liquid liquid‐solid conversion. It uncovered MoC physiochemically immobilizes soluble long‐chain polysulfide accelerates between S 8 Li 2 4 through adsorbing extending S─S bond distance. Then, precipitation enhanced facilitating migration from MoSe . This driven internal electric field at heterogeneous interface low diffusion energy barrier on Li2S Moreover, MoC‐MoSe exhibits smallest degree disproportionation throughout Consequently, cell with /C/S cathode delivers initial discharge‐specific capacity 841.1 mAh g −1 long‐term cycling stability attenuation rate 0.08% per cycle 1.0 C. work presents novelty view design rational multifunction sequentially accelerating stepwise polysulfides.

Язык: Английский

Процитировано

40

Electronegativity Matching of Asymmetrically Coordinated Single‐Atom Catalysts for High‐Performance Lithium–Sulfur Batteries DOI

Fengliang Cao,

Xinke Zhang,

Zhihan Jin

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер 14(19)

Опубликована: Март 13, 2024

Abstract Asymmetrically coordinated single‐atom catalysts are attractive for the implementation of high‐performance lithium–sulfur (Li─S) batteries. However, design principle asymmetric coordination that can efficiently promote bidirectional conversion polysulfides has not been fully realized. Herein, a series Co─N 3 X 1 ( refers to F, O, Cl, S, or P) configurations established, and theoretically unravel relative electronegativity value (REV) be used as an index parameter characterizing catalytic activity. By virtue enhanced chemical affinity with sulfur species lowered Li 2 S decomposition, chlorine‐atom‐constructed optimal REV exhibit stronger effect inhibit shuttling. Such REV‐related is termed effect. Following this principle, novel catalyst dominated Cl configuration successfully synthesized through inside‐out thermal reaction strategy modified layer on cathode‐side separator. Interestingly, assembled Li─S batteries quite high rate capacity (804.3 mAh g −1 at 5.0 C), durable cyclability (0.023% decay per cycle), competitive areal (7.0 cm −2 under 7.5 mg loading lean electrolyte). The guideline provided in work gives impetus pursuit highly efficient practical

Язык: Английский

Процитировано

27

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity DOI
Rong Zhou,

Yongqiang Ren,

Weixin Li

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)

Опубликована: Май 18, 2024

Lithium-sulfur (Li-S) batteries have many advantages but still face problems such as retarded polysulfides redox kinetics and Li dendrite growth. Most reported single atom catalysts (SACs) for Li-S are based on d-band transition metals whose d orbital constitutes active valence band, which is inclined to occur catalyst passivation. SACs 4f inner of rare earth challenging their great difficulty be activated. In this work, we design synthesize the first metal Sm has electron-rich promote catalytic conversion uniform deposition Li. enhance catalysis by activated through an f-d-p hybridization. Using Sm-N

Язык: Английский

Процитировано

19

Progresses and Prospects of Asymmetrically Coordinated Single Atom Catalysts for Lithium−Sulfur Batteries DOI Creative Commons
Rong Zhou, Shaonan Gu, Meng Guo

и другие.

Energy & environment materials, Год журнала: 2024, Номер 7(4)

Опубликована: Фев. 11, 2024

Lithium–sulfur batteries (LSBs) are widely regarded as promising next‐generation due to their high theoretical specific capacity and low material cost. However, the practical applications of LSBs limited by shuttle effect lithium polysulfides (LiPSs), electronic insulation charge discharge products, slow LiPSs conversion reaction kinetics. Accordingly, introduction catalysts into is one effective strategy solve issues sluggished LiPS conversion. Because nearly 100% atom utilization electrocatalytic activity, single‐atom (SACs) have been used mediators for LSBs' reactions. Excitingly, SACs with asymmetric coordination structures exhibited intriguing superior catalytic activities when compared traditional M–N 4 active sites. In this review, we systematically describe recent advancements in installation asymmetrically coordinated structure reactions LSBs, including nitrogen SACs, heteroatom support bimetallic SACs. Particularly noteworthy discussion mechanism spanning Finally, a perspective on future developments LSB provided.

Язык: Английский

Процитировано

17

Tuning Redox Behavior of Sulfur Cathodes Via Ternary‐Coordinated Single Fe Atom in Lithium‐Sulfur Batteries DOI

Guiqiang Cao,

Xifei Li, Liping Chen

и другие.

Small, Год журнала: 2024, Номер 20(24)

Опубликована: Янв. 4, 2024

Abstract Modulating the coordination configuration of single Fe atom has been an efficient strategy to strengthen redox dynamics for lithium‐sulfur batteries (LSBs) but remains challenging. Herein, is functioned with nitrogen and carbon atoms in first shell, simultaneously, oxidized sulfur (─SOx) second which presents a lower antibonding state well address activity cathodes. In ternary‐coordinated catalyst (FeN 2 C –SOx–NC), binary structure FeN provides Fe–S bonding strength d – p orbital hybridization, obviously optimizes adsorption desorption behavior species during reduction oxidation reaction processes. Simultaneously, ─SOx redistributes electron density coordinating atoms, possesses high electron‐withdrawing ability develops electrocatalytic activity. As result, cathodes –SOx–NC present excellent high‐rate cyclic performance, accompanied by capacity decay rate 0.08% per cycle 500 cycles at 4.0 . This study new insights optimizing LSBs atomic level.

Язык: Английский

Процитировано

16

Precise compressive strain regulation to activate the electrocatalytic activity of FeOOH enabling ultrastable lithium-sulfur batteries DOI
Bo Jiang, Chenghao Zhao,

Xiaoju Yin

и другие.

Energy storage materials, Год журнала: 2024, Номер 66, С. 103237 - 103237

Опубликована: Фев. 1, 2024

Язык: Английский

Процитировано

14

Electronic State‐Modulated Ni4N/Zn3N2 Heterogeneous Nanosheet Arrays Toward Dendrite‐Free and Kinetic‐Enhanced Li‐S Full Batteries DOI Creative Commons
Qiwen Ran, Jintao Liu, Lei Li

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер 34(38)

Опубликована: Апрель 26, 2024

Abstract The applications of lithium (Li)–sulfur (S) batteries are simultaneously hampered by the unlimited dendritic Li growth and sluggish redox kinetics polysulfides (LiPSs). In this work, an electronic state‐modulated Ni 4 N/Zn 3 N 2 heterogeneous nanosheet arrays is painstakingly fabricated on surface carbon cloth (CC@Ni ) as efficient bi‐service host to promote uniform deposition boost LiPSs catalysis. It found that structure heterostructure modulated realize a rational transition metal d‐band center, its built‐in electric field (BIEF) within heterointerfaces facilitates interfacial charge transfer, resulting in low deposition/migration energy barrier adsorption/catalytic conversion kinetics. As result, as‐prepared CC@Ni ‐Li anode can enable Li||Li symmetrical cells possess long‐term lifespan over 500 h even at 10 mA cm −2 /20 mAh , as‐assembled LiNi 0.8 Co 0.1 Mn O ||CC@Ni full cell also shows excellent cycling performance (95.8% capacity retention after 100 cycles). When used for both S loading, ‐S||CC@Ni exhibits outstanding stability (744 g −1 1000 cycles 2C). This work highlights great potential heterostructures fabricating ideal bi‐serve hosts electrodes.

Язык: Английский

Процитировано

13

A unique three-dimensional network double-core–shell structure S@MnO2@MXene suppresses the shuttle effect in high-sulfur-content high-performance lithium-sulfur batteries DOI
Qing Li,

Minhao Fu,

Xiujuan Qin

и другие.

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 674, С. 805 - 812

Опубликована: Июнь 27, 2024

Язык: Английский

Процитировано

10

Rational Design of Janus Metal Atomic‐Site Catalysts for Efficient Polysulfide Conversion and Alkali Metal Deposition: Advances and Prospects DOI

Guangfu Dai,

Shou‐Zhe Li,

Menglin Shi

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер 34(25)

Опубликована: Фев. 1, 2024

Abstract Although metal–sulfur batteries (M–S batteries, M = Li, Na, K) are promising next‐generation energy‐storage devices because of ultrahigh theoretical energy density, low cost, and environmentally friendliness, their practical applications significantly hindered by the shuttle effect polysulfides growth alkali metal dendrites. These issues can be mitigated using Janus atomic‐site catalysts, which possess maximum atom utilization efficiency (≈100%), adjustable electronic structures, tailorable catalytic sites, thereby effectively improving electrochemical performance M–S batteries. In this review, recent progress development atomic‐sites on properties, synthesis, characterizations reviewed. Then, advances in catalysts intended for accelerating polysulfide conversion regulating deposition, briefly introducing working principles systematically summarized. Furthermore, a high emphasis is placed effective regulation strategies rational design Finally, current challenges future research directions also presented to develop high‐efficiency high‐energy

Язык: Английский

Процитировано

9