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

High‐Entropy Catalysis Accelerating Stepwise Sulfur Redox Reactions for Lithium–Sulfur Batteries DOI Creative Commons
Yunhan Xu,

Wenchuang Yuan,

Chuannan Geng

и другие.

Advanced Science, Год журнала: 2024, Номер 11(31)

Опубликована: Июнь 17, 2024

Abstract Catalysis is crucial to improve redox kinetics in lithium–sulfur (Li–S) batteries. However, conventional catalysts that consist of a single metal element are incapable accelerating stepwise sulfur reactions which involve 16‐electron transfer and multiple Li 2 S n (n = 2–8) intermediate species. To enable fast Li–S batteries, it proposed use high‐entropy alloy (HEA) nanocatalysts, demonstrated effective adsorb lithium polysulfides accelerate their kinetics. The incorporation elements (Co, Ni, Fe, Pd, V) within HEAs greatly enhances the catalytically active sites, not only improves rate capability, but also elevates cycling stability assembled Consequently, HEA‐catalyzed batteries achieve high capacity up 1364 mAh g −1 at 0.1 C experience slight fading 0.054% per cycle over 1000 cycles C, while pouch cell achieves specific 1192 . superior performance demonstrates effectiveness HEA with maximized synergistic effect for conversion reactions, opens way improving electrochemical reactions.

Язык: Английский

Процитировано

27
Atom-Dominated Relay Catalysis of High-Entropy MXene Promotes Cascade Polysulfide Conversion for Lithium-Sulfur Batteries DOI

Mengyao Xu,

Qizhen Zhu, Yanze Li

и другие.

Energy & Environmental Science, Год журнала: 2024, Номер unknown

Опубликована: Янв. 1, 2024

The high-entropy TiVNbMoC 3 MXene, with its atom-dominated relay catalysis effect and resilient lattice configuration, promotes a cascade of sulfur conversions guides uniform Li + deposition, enabling shuttle-free dendrite-free Li–S batteries.

Язык: Английский

Процитировано

19
High Temperature Shock (HTS) Synthesis of Carbon‐Based Nanomaterials for Electrochemical Applications DOI Creative Commons
Wenyu Huang, Xindong Zhu, He Zhu

и другие.

Carbon Neutralization, Год журнала: 2025, Номер 4(1)

Опубликована: Янв. 1, 2025

ABSTRACT Carbon‐based nanomaterials play a significant role in the field of electrochemistry because their outstanding electrical conductivity, chemical and thermal resistance, structural flexibility, so on. In recent years, we have observed rapid rise research interest high‐temperature shock (HTS) method, which is fast, stable, environmentally friendly, versatile. The HTS method offers excellent controllability repeatability while tackling challenges limitations traditional preparation methods, providing new way to prepare optimize carbon‐based for electrochemical applications. During synthesis, reaction driven by high temperature further growth obtained nanoparticles inhibited heating cooling rates. has many advantages, including controlled carbon vacancy that may drive phase transformation, precise engineering carbon, other defects function as active centers, formation preservation metastable owing energy cooling, fine‐tuning interaction between loaded species support optimized performance, facile doping compounding induce synergy different constituents. This article provides comprehensive review various prepared applications during past decade, emphasizing synthesis principles performance. Studies showcasing merits HTS‐derived advancing Lithium‐ion batteries, Lithium‐sulfur Lithium‐air water‐splitting reaction, oxygen reduction CO 2 nitrate electrocatalytic reactions, fuel cells are highlighted. Finally, prospects recommended.

Язык: Английский

Процитировано

3
Catalysis‐Driven Sulfur Conversion: From Electrolyte‐Flooded to Solid‐State Batteries DOI Open Access

Haotian Yang,

Yunhan Xu, Yufei Zhao

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 14, 2025

Abstract Lithium‐sulfur (Li–S) batteries are widely recognized as highly promising energy storage devices owing to their exceptional theoretical density. However, the prevalent use of flooded electrolytes in Li–S significantly restricts To enhance density batteries, transitioning from a flooded‐electrolyte lean‐electrolyte system proves be effective. Additionally, replacing organic liquid electrolyte with solid‐state addresses associated safety concerns. Concurrently, practical application encounters numerous challenges, particularly sluggish electrochemical conversion kinetics and systems. Hence, it is imperative develop suitable catalysts tailored for various battery configurations. This review comprehensively reviews applications development strategies diverse systems, specific focus on outlook explores future direction catalysts, aiming guide rational design facilitate realization high‐energy‐density batteries.

Язык: Английский

Процитировано

2
Machine Learning Assisted Design of High‐Entropy Alloy Interphase Layer for Lithium Metal Batteries DOI Open Access
Chenxi Xu, Teng Zhao,

Ke Wang

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 16, 2025

Abstract Lithium dendrite growth and the resulting safety concerns hinder application of lithium metal. Compared with single metal or medium entropy alloys, high‐entropy alloys (HEAs) are a promising solution to solve challenges anodes due their unique properties. However, designing HEA layer appropriate elements proportion has become obstacles. Herein, machine learning (ML), density functional theories (DFT) calculation data analysis reveal contribution Zn in lithiophilicity, Al hardness Fe, Co, Ni providing magnetism. The magnetron sputtering is used construct interphase layer, three parameters (sputtering power, time, substrate rotation speed) optimized via particle swarm optimization (PSO) based on logarithm average coulombic efficiency (CE) Li||Cu half cells. While high strength, compactness, flatness constructed, Li||Li symmetric cell assembled by HEA@Li at 1 mA cm −2 , mAh can cycle stably for 2400 h, discharge capacity retention rate Li||LFP >90% after 300 cycles C CE 99.67%. Design assisted ML provides path potential batteries.

Язык: Английский

Процитировано

1
High-Entropy Alloys in Catalysis: Progress, Challenges, and Prospects DOI Creative Commons
Liang Sun, Kaihua Wen, Guanjie Li

и другие.

ACS Materials Au, Год журнала: 2024, Номер 4(6), С. 547 - 556

Опубликована: Сен. 29, 2024

High-entropy alloys (HEAs) have become pivotal materials in the field of catalysis, offering unique advantages due to their diverse elemental compositions and complex atomic structures. Recent advances computational techniques, particularly density functional theory (DFT) machine learning (ML), significantly enhanced our understanding design HEAs for use catalysis. These innovative atomistic simulations shed light on properties HEAs, enabling discovery optimization catalysis solid-solution This Perspective discusses recent studies that illustrate progress It offers an overview properties, constraints, prospects emphasizing roles enhance catalytic activity selectivity. The discussion underscores capabilities as multifunctional catalysts with stable presented insights aim inspire future experimental efforts address challenges fine-tuning improved performance.

Язык: Английский

Процитировано

7
Rapid Closed Pore Regulation of Biomass‐derived Hard Carbons Based on Flash Joule Heating for Enhanced Sodium Ion Storage DOI Open Access

Yuqian Qiu,

Yanxia Su,

Xiaohan Jing

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 4, 2025

Abstract Closed pores are essential for enhancing the low‐potential (<0.1 V) plateau capacity and initial Coulombic efficiency of hard carbon (HC) anode materials energy‐dense sodium‐ion batteries. However, lack simple effective closed‐pore construction strategies has severely hindered their future commercialization. Herein, a rapid regulation strategy biomass‐derived HCs is proposed through pre‐heat treatment followed by flash Joule heating (FJH). The critical transforming vulnerable biomass into high‐carbonizability frameworks that resistant to over‐graphitization. FJH helps generate enriched closed surrounded resulting walls with expanded interlayer spacing as accessible Na + channels. This shows remarkable universality applicability feedstocks, enabling conversion various carbonization‐vulnerable precursors high‐yield (e.g. HC600‐J‐1500 compared HC25‐J‐1500, ≈14‐fold yield increase) HCs. optimized sample demonstrates an outstanding reversible 377 mAh g −1 superior 93.3%, which stands in record value prepared even competitive via conventional carbonization. Comprehensive tests reveal efficient storage originates from pore‐filling mechanism nanopores. work suggests facile universal approach rational design high‐performance

Язык: Английский

Процитировано

1
Order within disorder: Unveiling the potential of high entropy materials in energy storage and electrocatalysis DOI
Vaibhav C. Lokhande, Dhanaji B. Malavekar, Chihoon Kim

и другие.

Energy storage materials, Год журнала: 2024, Номер 72, С. 103718 - 103718

Опубликована: Авг. 15, 2024

Язык: Английский

Процитировано

6
Unveiling the potential of high-entropy materials toward high-energy metal batteries based on conversion reactions: synthesis, structure, properties, and beyond DOI
Ma Lian,

Weiqian Gong,

Shaofei Guo

и другие.

Energy storage materials, Год журнала: 2025, Номер unknown, С. 104054 - 104054

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

0
D‐Band Center Modulation of Metallic Co‐Incorporated Co7Fe3 Alloy Heterostructure for Regulating Polysulfides in Highly Efficient Lithium‐Sulfur Batteries DOI
Lin Sun, Hongnan Xu, Jie Xie

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 4, 2024

Abstract Lithium‐sulfur (Li‐S) batteries, with their high theoretical energy density and cost‐effectiveness, have become one of the most promising next‐generation storage devices. However, they still face challenges such as “shuttle effect” caused by dissolution polysulfide intermediates slow sulfur conversion kinetics. In this study, based on Co 7 Fe 3 alloy catalyst, additional metal is introduced to form a catalyst heterostructure through simple heat treatment process. This incorporated into Ketjenblack (KB) sulfur‐infused cathode material (designated S/KB/Co Co). Li‐S batteries using demonstrate outstanding electrochemical performance, maintaining reversible specific capacity over 500 mAh g −1 after 1000 cycles at current 1 C, decay rate 0.046% per cycle. DFT calculations experimental results both reveal that introduction effectively regulates d‐band center material, enhancing adsorption promoting bidirectional catalytic conversion. work highlights importance construction heterostructured materials role in improving performance batteries.

Язык: Английский

Процитировано

3