High Spin‐State Modulation of Catalytic Centers by Weak Ligand Field for Promoting Sulfur Redox Reaction in Lithium‐Sulfur Batteries DOI
Qing Li, Zhipeng Ma, Ming Liu

и другие.

Angewandte Chemie, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 8, 2024

Abstract The spin state of transition‐metal compounds in lithium‐sulfur batteries (LSBs) significantly impacts the electronic properties and kinetics sulfur redox reactions (SRR). However, accurately designing remains challenging, which is crucial for understanding structure‐performance relationship developing high‐performance electrocatalysts. Herein, CoF 2 , specifically Co 2+ with 3 d 7 electrons a high‐spin distribution (t 2g 5 e g ), were tailored predictably first time through weak coordination field effect F element. Both DFT calculations experimental results confirm that transitions from low‐ to configurations strongly interacts species Co−S Li−F bonds during SRR process. This interaction weakens S−S bond, promoting its facile cleavage both ends while also facilitating rapid uniform nucleation Li S /Li S, thus resulting LSBs capacity 447.7 mAh −1 at 10 C rates stable cycling 1000 cycles, an acceptable practical 585 high loading mass mg cm −2 . work achieves rational control active electron enriches application accelerate LSBs.

Язык: Английский

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

и другие.

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 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.

Язык: Английский

Процитировано

22

Cu‐Driven Active Cu2Se@MXene Heterointerface Reconstruction and Co Electron Reservoir Toward Superior Sodium Storage DOI Open Access

Chengxing Lu,

Boyu Li, Mengjie Shi

и другие.

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Heterostructure engineering and active component reconstruction are effective strategies for efficient rapid charge storage in advanced sodium‐ion batteries (SIBs). Herein, sandwich‐type CoSe 2 @MXene composites used as a model to reconstruct new Cu Se@MXene heterostructures by situ electrochemical driving. The MXene core provides interconnected pathways electron ion conduction, while also buffering volumetric expansion stabilize the structure. This reconstructed heterointerface features abundant sodium sites, enhanced Na + adsorption, diffusion kinetics, thus increasing capacity. Moreover, elevated Co valence state during discharge process allows it act an reservoir provide additional supply Se conversion accelerate kinetics. When employed anode SIBs, electrode exhibits high capacity (694 mAh g −1 at 0.1 A ), excellent rate performance (425 20 exceptional durability (437 after 10 000 cycles 5 with 0.0014% decay per cycle). mechanism of is further revealed through ex characterization theoretical calculations. work approach designing conversion‐type anodes SIBs.

Язык: Английский

Процитировано

3

Twin S‐Scheme Heterojunction ZnO/UiO‐66‐NH2@ZnIn2S4 Rhombic Octahedra for Efficient Photocatalytic H2 Evolution DOI Open Access

Xiangping Xiao,

Shuangjun Li,

Lu-Yang Zuo

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 3, 2025

Abstract Amid increasing fossil energy scarcity, a key solution is using solar to split water into hydrogen (H 2 ). However, single photocatalysts face limitations of low utilization rate and rapid carrier recombination, so constructing novel composite promising solution. Here, ZnO/UiO‐66‐NH @ZnIn S 4 (ZUN@ZIS) catalyst with twin S‐scheme heterojunction constructed for the first time, in which ZnIn (ZIS) nanosheets are grown situ on surface (ZUN) rhombic octahedra. Under irradiation visible light without help any co‐catalyst, H evolution prepared ZUN@ZIS‐20 5.05 mmol g −1 h , 3.7, 2.1 46 times higher than that ZIS, UiO‐66‐NH /ZIS (UN/ZIS) ZUN, respectively. Moreover, synergistic effect resulting ZUN@ZIS facilitates provision efficient channels carrier/mass transfer ensures structural stability. Various experimental characterizations theoretical calculations confirm by ZUN ZIS can facilitate easy separation photogenerated carriers. This study has developed new idea multi‐heterojunction photocatalysts, provided valuable reference development photocatalysis technology.

Язык: Английский

Процитировано

3

Electron‐Spin Regulation Driving Heterointerface Electron Distribution and Phase Transition toward Ultrafast and Durable Sodium Storage DOI
Yuhang Li, Wenying Li, Meng Zhang

и другие.

Small, Год журнала: 2024, Номер unknown

Опубликована: Сен. 16, 2024

Abstract Phase engineering is an effective strategy for modulating the electronic structure and electron transfer mobility of cobalt selenide (CoSe 2 ) with remarkable sodium storage. Nevertheless, it remains challenging to improve fast‐charging cycling performance. Herein, a heterointerface coupling induces phase transformation from cubic CoSe orthorhombic accompanied by formation MoSe construct /MoSe heterostructure decorated N‐doped carbon layer on 3D graphene foam @NC/GF). The incorporated Mo cations in bridged o‐CoSe not only act donor regulate charge‐spin configurations more active states but also trigger upshift d/p band centers decreased ∆ d‐p center gap, which greatly enhances ion adsorption capability lowers diffusion barrier. As expected, @NC/GF anode demonstrates high‐rate 447 mAh g −1 at A excellent cyclability 298 1 over 1000 cycles. work deepens understanding elaborate construction heterostructured electrodes high‐performance SIBs.

Язык: Английский

Процитировано

7

Curvature-Induced Electron Delocalization Activates the Bifunctional Catalytic Activity of COF/MXene for High-Performance Lithium–Sulfur Batteries DOI Creative Commons
Yanhui Zhuang, Hao Yang, Yuhang Li

и другие.

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Март 11, 2025

Covalent organic frameworks (COFs) have shown promise as bifunctional catalysts to simultaneously mitigate shuttle effects and Li dendrite issues of lithium–sulfur (Li–S) batteries. However, the inherent low conductivity COFs has significantly limited their catalytic activity stability. Herein, durability COF/MXene heterostructure are activated by tuning surface curvatures interfaced with MXene. The increased curvature could induce enhanced electron delocalization alter geometry, which in turn strengthens lithium polysulfide adsorption, lowers energy barriers, stabilizes sites promote sulfur redox reactions. Concurrently, hierarchical structure improves electrolyte penetration wettability, facilitates rapid ion transport, homogenizes Li-ion flux distribution, thus achieving uniform deposition. Consequently, 1D-COF/MXene Li–S batteries demonstrate a high-rate capacity 926 mA h g–1 at 4C, stable cycling performance reversible 589 3C after 500 cycles, high 604 cm–2 loading 3.5 mg under electrolyte-to-sulfur ratio 10 μL mg–1. This work offers an efficacious approach regulate stability catalysts.

Язык: Английский

Процитировано

1

Activating Transition-Metal Oxides through In Situ Regulation of Lower Hubbard Band for Catalytic Conversion of Lithium Polysulfides DOI
Pan Zeng, Yong‐Sheng Hu, Bin Su

и другие.

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Апрель 30, 2025

Catalytic conversion of lithium polysulfides (LiPSs) is regarded as an effective avenue to tackle the shuttle effect lithium-sulfur (Li-S) batteries, especially based upon transition-metal oxides (TMOs). However, activity origin and corresponding mechanistic insights into such catalytic systems remain elusive. Herein, activated state associated with lower Hubbard band (LHB) transition proposed elucidate TMOs by taking Mn3O4 a model electrocatalyst. Specifically, broadening LHB width, upshift position, orbital rearrangement LHB, triggered in situ substitution O atoms S LiPSs under working conditions, synergistically enable fast electron transfer modulate adsorption capability moderate level. Benefiting from these advantages, electrocatalyst converted torpid for expediting LiPS conversion. Eventually, Li-S batteries assembled deliver excellent rate performance over 6 C outstanding cycling stability 1000 cycles. Moreover, Ah-scale pouch cell constructed delivers notable energy density 388.1 W h kg-1. Our work offers promising pathway on regulation designing high-performance electrocatalysts beyond.

Язык: Английский

Процитировано

1

Activating Inert Palmeirite Through Co Local‐Environment Modulation and Spin Electrons Rearrangement for Superior Oxygen Evolution DOI Open Access

Jia‐xin Wen,

Yi‐Ru Hao,

Jiawen Sun

и другие.

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 5, 2025

Abstract Mo‐based palmeirite oxide A 2 Mo 3 O 8 is an emerging electrocatalyst, exhibiting a bipartite honeycomb lattice consisting of tetrahedral and octahedral sites with good conductivity. However, as promising catalyst in electrocatalytic remains rarely touched. The rational design clarification the correlation between geometrical configuration modulation properties are challenging. Herein, innovative strategy reported to anchor thiospinel Co S 4 nanoparticles onto surface nanosheet, which can trigger spin electrons rearrangement, thus activating inert sites. According X‐ray absorption spectroscopy, 2+ ─O─Co 3+ bimetallic bridging asymmetric bond polarization constructed interface, triggers favorable transition from low intermediate spin. Interestingly, /Co exhibits remarkable oxygen evolution reaction performance overpotential 227 mV at 10 mA cm −2 . At industrial process temperature, it takes only 2.37 V for overall water splitting obtain large current density 1 theoretical calculation results confirm that distortion‐related optimizes energy, enhancing adsorption * OOH. This work highlights potential achieving seawater by rearrangement.

Язык: Английский

Процитировано

0

Island-like FeS2@TiO2 heterojunction modified separator for enhanced polysulfide management in lithium-sulfur batteries DOI
Jing Song,

Luchao Yue,

Y Dou

и другие.

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 161934 - 161934

Опубликована: Март 1, 2025

Язык: Английский

Процитировано

0

Review on MXenes-Based Electrocatalysts for High-Energy-Density Lithium–Sulfur Batteries DOI Creative Commons

Xintao Zuo,

Yanhui Qiu,

Mengmeng Zhen

и другие.

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Апрель 10, 2025

Abstract Lithium–sulfur batteries (LSBs) hold significant promise as advanced energy storage systems due to their high density, low cost, and environmental advantages. However, despite recent advancements, practical density still falls short of the levels required for commercial viability. The is critically dependent on both sulfur loading amount electrolyte used. High-sulfur coupled with lean conditions presents several challenges, including insulating nature Li 2 S, insufficient absorption, degradation cathode structure, severe lithium polysulfide shuttling, slow redox reaction kinetics, instability metal anode. MXenes-based materials, metallic conductivity, large polar surfaces, abundant active sites, have been identified promising electrocatalysts improve reactions in LSBs. This review focuses significance challenges associated high-sulfur electrolytes LSBs, highlighting advancements aimed at optimizing cathodes anodes. It provides a comprehensive discussion MXenes materials substrates goal enhancing understanding regulatory mechanisms that govern conversion plating/stripping behavior. Finally, explores future opportunities electrocatalysts, paving way application

Язык: Английский

Процитировано

0

A bifunctional NiS2@MXene (Ti3C2Tx) composite separator for high-performance lithium–sulfur batteries with enhanced polysulfide inhibition and uniform lithium-ion transport DOI
Bo Zhang,

Jiyuan You,

Peng Liu

и другие.

Journal of Materials Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Capacity degradation from uncontrolled polysulfide diffusion and dendrite growth at the anode are key challenges in lithium–sulfur batteries.

Язык: Английский

Процитировано

0