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High‑Entropy Electrode Materials:Synthesis,Properties and Outlook

Nano-Micro Letters 2025年第1期17卷 472-506页

作者： Dongxiao Li Chang Liu Shusheng Tao Jieming Cai Biao Zhong Jie Li Wentao Deng hongshuai hou Guoqiang Zou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083People’s Republic of China School of Chemistry and Chemical Engineering Hunan Institute of EngineeringXiangtan 411104People’s Republic of China

High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two *** definition of high-entropy materials has continuously *** the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode ***,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation ***,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy *** should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy *** this review,the definition and development of high-entropy materials are briefly ***,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis ***,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.

关键词： High-entropy Energy storage Electrode materials

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Carbon Dot-Modified TiO_(2)@SiO_(2) Aerogel as an Anode for Lithium-Ion Batteries

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Nanomanufacturing and Metrology 2023年第2期6卷 1-10页

作者： Zanyu Chen Jiugang Hu Kuixing Ding Jun Tan hongshuai hou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China

Titanium oxides have been considered promising anode materials for lithium-ion batteries(LIBs).However,the poor conductivity and low specific capacity of bulk titanium oxides limit their *** this study,a carbon dot-modified TiO_(2)@SiO_(2)aerogel was successfully fabricated through a facile ambient pressure drying strategy and used as an anode material of *** from the crosslinking of carbon dots and the surface modification of SiO_(2),the as-prepared hierarchical aerogel exhibited a high initial discharge capacity of 974 mAh g^(−1)and maintained a capacity of 299 mAh g^(−1)after 100 cycles at 0.1 A g^(−1).It also retained a discharge capacity of 111 mAh g^(−1)with a CE of 99.9%at 3 A g^(−1).The carbon dot-modified cross-linking skeleton contributes to the structural integrity of the TiO_(2)@SiO_(2)aerogel during repeated insertion/extraction of lithium ions,guaranteeing outstanding cycling and high-rate *** ambient pressure drying strategy provides a facile and feasible way to produce high-performance aerogel anode materials for lithium-ion storage.

关键词： Aerogel Ambient pressure drying Titanium oxide Lithium-ion battery

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Revealing dual capacitive mechanism of carbon cathode toward ultrafast quasi-solid-state lithium ion capacitors

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Journal of Energy Chemistry 2021年第9期30卷 209-221页

作者： Kangyu Zou Peng Cai Xinglan Deng Baowei Wang Cheng Liu Jiayang Li hongshuai hou Guoqiang Zou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China College of Metallurgy and Chemical Engineering Jiangxi University of Science and TechnologyGanzhou 341000China

High-performance lithium ion capacitors(LICs) have been seriously hindered by the very low capacity and unclear capacitive mechanism of carbon ***,after the combination of experimental results and theoretical calculations,it is found that the critical pore size of 0.8 nm for PF_6~-ion adsorption decreases strong interactive repulsion of electrons and largely reduces adsorption energy barrier,which greatly improves the charge accommodation capacity in electrical double-layer *** importantly,the chemical-bond evolution process of C=O group has been firstly revealed by X-ray photoelectron spectroscopy(XPS),indicating that the introduction of C=O group can provide abundant redox active sites for PF_6~-ion adsorption accompanied with enhanced pseudocapacitive *** to the synergistic effect of dual capacitive mechanism,porous carbon sheet(PCS) cathode shows a reversible specific capacity of 53.6 mAh g^(-1) even at a high current density of 50 A g^(-1).Significantly,the quasisolid-state LIC manifests state-of-the-art electrochemical performances with an integrated maximum energy density of 163 Wh kg^(-1) and an outstanding power density of 15,000 W kg^(-1).This elaborate work promotes better fundamental understanding about capacitive mechanism of PF_6~-ion and offers a rational dual-capacitive strategy for the design of advanced carbon cathodes.

关键词： Capacitive mechanism Carbon cathode Carbonyl group Quasi-solid-state Lithium ion capacitors

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Insights into Enhanced Capacitive Behavior of Carbon Cathode for Lithium Ion Capacitors: The Coupling of Pore Size and Graphitization Engineering

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Nano-Micro Letters 2020年第9期12卷 239-257页

作者： Kangyu Zou Peng Cai Baowei Wang Cheng Liu Jiayang Li Tianyun Qiu Guoqiang Zou hongshuai hou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083People’s Republic of China College of Metallurgy and Chemical Engineering Jiangxi University of Science and Technology86 Hongqi RoadGanzhou 341000People’s Republic of China

The lack of methods to modulate intrinsic textures of carbon cathode has seriously hindered the revelation of in-depth relationship between inherent natures and capacitive behaviors,limiting the advancement of lithium ion capacitors(LICs).Here,an orientateddesigned pore size distribution(range from 0.5 to 200 nm)and graphitization engineering strategy of carbon materials through regulating molar ratios of Zn/Co ions has been proposed,which provides an effective platform to deeply evaluate the capacitive behaviors of carbon ***,after the systematical analysis cooperating with experimental result and density functional theory calculation,it is uncovered that the size of solvated PF6-ion is about 1.5 ***,the capacitive behaviors of carbon cathode could be enhanced attributed to the controlled pore size of 1.5-3 *** with synergistic effect of graphitization and appropriate pore size distribution,optimized carbon cathode(Zn90Co10-APC)displays excellent capacitive performances with a reversible specific capacity of^50 mAh g-1at a current density of 5 A ***,the assembly pre-lithiated graphite(PLG)//Zn90Co10-APC LIC could deliver a large energy density of 108 Wh kg-1 and a high power density of 150,000 W kg-1 as well as excellent long-term ability with 10,000 *** elaborate work might shed light on the intensive understanding of the improved capacitive behavior in LiPF6 electrolyte and provide a feasible principle for elaborate fabrication of carbon cathodes for LIC systems.

关键词： Carbon materials Pore size regulation Graphitization Capacitive behavior Lithium ion capacitor

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N,S-Doped Carbon Dots as Additive for Suppression of Zinc Dendrites in Alkaline Electrolyte

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Chinese Journal of Chemistry 2023年第14期41卷 1697-1704页

作者： Shan Cai Ge Chang Jiugang Hu Jiae Wu Yuqing Luo Guoqiang Zou hongshuai hou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangshaHunan410083 China

The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc-based *** is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the *** this study,N,S-doped carbon dots(TU-CQDs)were synthesized and used as additives to regulate zinc deposition in a typical KOH *** experimental and three-dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the ***,TU-CQDs can not only inhibit the hydrogen evolution reaction,but also achieve uniform zinc *** in-situ synchrotron radiation X-ray imaging elucidated that TU-CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping *** work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte.

关键词： Zinc anode Carbon dots Alkaline electrolyte Dendrite-free Electrode interfacesI Electrolyte additives

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Channel regulation of TFC membrane with hydrophobic carbon dots in forward osmosis

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Chinese Chemical Letters 2021年第9期32卷 2882-2886页

作者： Zongju Zhang Jiugang Hu Shijun Liu Xin Hao Lin Li Guoqiang Zou hongshuai hou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China

Zero-dimensional carbon dots have emerged as important nanofillers for the separation membrane due to their small specific size and rich surface functional *** study proposed a strategy based on hydrophobic carbon dots(HCDs)to regulate water channels for an efficient forward osmosis(FO)***-film composite(TFC)membranes with superior FO performance are fabricated by introducing HCDs as the nanofiller in the polyacrylonitrile support *** introduction of HCDs promotes the formation of the support layer with coherent finger-like hierarchical channels and micro-convex structure and an integrated polyamide active *** to the original membrane,TFC-FO membrane with 10 wt%HCDs exhibits high water flux(15.47 L m^(-2)h^(-1))and low reverse salt flux(2.9 g m^(-2)h^(-1))using 1 mol/L Na Cl as the draw *** improved FO performance is attributed to the lower structural parameters of HCDs-induced water channels and alleviated internal concentration ***,this paper provides a feasible strategy to design the membrane structure and boost FO performance.

关键词： Forward osmosis Thin-film nanocomposite Hydrophobic carbon dots Channel regulation Nanofillers

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High-yield red phosphorus sponge mediated robust lithium-sulfur battery

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Nano Research 2023年第6期16卷 8329-8337页

作者： Zheng Luo Shusheng Tao Ye Tian Hanyu Tu Laiqiang Xu Wentao Deng Guoqiang Zou hongshuai hou Xiaobo Ji State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083China

Although lithium-sulfur(Li-S)batteries with high specific energy exhibit great potential for next-generation energy-storage systems,their practical applications are limited by the growth of Li dendrites and lithium polysulfides(LiPSs)***,a highly porous red phosphorus sponge(HPPS)with well distributed pore structure was efficiently prepared via a facile and largescale hydrothermal process for polysulfides adsorption and dendrite *** experimental demonstrated,the porous red phosphorus modified separator with increased active site greatly promotes the chemisorption of LiPSs to efficiently immobilize the active sulfur within the cathode section,while Li metal anode activated by Li_(3)P interlayer with abundant ionically conductive channels significantly eliminates the barrier for uniform Li^(+)permeation across the interlayer,contributing to the enhanced stability for both S cathode and Li *** by the HPPS,long-term stability of 1,200 h with minor voltage hysteresis is achieved in symmetric cells with Li_(3)P@Li electrode while Li-S half-cell based on HPPS modified separator delivers an outperformed reversibility of 783.0 mAh·g^(−1)after 300 cycles as well as high-rate performance of 694.5 mAh·g^(−1)at 3 C,which further boosts the HPPS tuned full cells in practical S loading(3 mg·cm^(−2))and thin Li3P@Li electrode(100μm)with a capacity retention of 71.8%after 200 cycles at 0.5 *** work provides a cost-effective and metal free mediator for simultaneously alleviating the fundamental issues of both S cathode and Li anode towards high energy density and long cycle life Li-S full batteries.

关键词： lithium-sulfur battery red phosphorus sponge separator chemical adsorption Li dendrite

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Graphitic Carbon Quantum Dots Modified Nickel Cobalt Sulfide as Cathode Materials for Alkaline Aqueous Batteries

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Nano-Micro Letters 2020年第2期12卷 1-18页

作者： Yirong Zhu Jingying Li Xiaoru Yun Ganggang Zhao Peng Ge Guoqiang Zou Yong Liu hongshuai hou Xiaobo Ji College of Metallurgy and Material Engineering Hunan University of TechnologyZhuzhou 412007People’s Republic of China College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083People’s Republic of China State Key Lab of Powder Metallurgy Central South UniversityChangsha 410083People’s Republic of China

Carbon quantum dots(CQDs)as a new class of emerging materials have gradually drawn researchers’concern in recent *** this work,the graphitic CQDs are prepared through a scalable approach,achieving a high yield with more than 50%.The obtained CQDs are further used as structure-directing and conductive agents to synthesize novel N,S-CQDs/NiCo2S4 composite cathode materials,manifesting the enhanced electrochemical properties resulted from the synergistic effect of highly conductive N,S-codoped CQDs offering fast electronic transport and unique micro-/nanostructured NiCo2S4 microspheres with Faradaic redox characteristic contributing large ***,the nitrogen-doped reduced graphene oxide(N-rGO)/Fe2O3 composite anode materials exhibit ultrahigh specific capacity as well as significantly improved rate property and cycle performance originating from the high-capacity prism-like Fe2O3 hexahedrons tightly wrapped by highly conductive N-rGO.A novel alkaline aqueous battery assembled by these materials displays a specific energy(50.2 Wh kg^−1),ultrahigh specific power(9.7 kW kg^−1)and excellent cycling performance with 91.5%of capacity retention at 3 A g^−1 for 5000 *** present research offers a valuable guidance for the exploitation of advanced energy storage devices by the rational design and selection of battery/capacitive composite materials.

关键词： Energy storage Alkaline aqueous batteries Carbon quantum dot Nickel cobalt sulfide

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Interfacial/bulk synergetic effects accelerating charge transferring for advanced lithium-ion capacitors

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Chinese Chemical Letters 2024年第6期35卷 168-175页

作者： Chang Liu Zirui Song Xinglan Deng Shihong Xu Renji Zheng Wentao Deng hongshuai hou Guoqiang Zou Xiaobo Ji School of Chemistry and Chemical Engineering Hunan Institute of EngineeringXiangtan 411104China College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Key Laboratory of Hunan Province for Clean and Efficient Utilization of Strategic Calcium-Containing Mineral Resources School of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083China

The exploration of advanced materials through rational structure/phase design is the key to develop highperformance lithium-ion capacitors(LICs).However,high complexity of material preparation and difficulty in quantity production largely hinder the further ***,Cu_(5)FeS_(4-x)/C(CFS@C)heterojunction with rich sulfur vacancies has successfully achieved from natural bornite,presenting low costeffective and bulk-production *** functional theory(DFT)calculations indicate that rich vacancies in bulk phase can decrease band gap of bornite and thus improve its intrinsic electron conductivity,as well as the heterojunction spontaneously evokes a built-in electric field between its interfacial region,largely reducing the migration barrier from 1.27 e V to 0.75 e *** from these merits,the CFS@C electrodes deliver outperformed lithium storage performance,e.g.,high reversible capacity(822.4m Ah/g at 0.1 A/g),excellent cycling stability(up to 820 cycles at 2 A/g and 540 cycles at 5 A/g with respective capacity retention of over or nearly 100%).With CFS@C as anode and porous carbon nanosheets(PCS)as cathode,the assembled CFS@C//PCS LIC full cells exhibit high energy/power density characteristics of 139.2 Wh/kg at 2500 W/*** work is expected to offer significant insights into structure modifications/devising toward natural minerals for advanced energy-storage systems.

关键词： Bulk/interfacial modification Heterostructure Sulfur vacancies Lithium ion capacitors Capacitors

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Natural Stibnite for Lithium‑/Sodium‑Ion Batteries:Carbon Dots Evoked High Initial Coulombic Efficiency

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Nano-Micro Letters 2022年第8期14卷 208-228页

作者： Yinger Xiang Laiqiang Xu Li Yang Yu Ye Zhaofei Ge Jiae Wu Wentao Deng Guoqiang Zou hongshuai hou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083People’s Republic of China College of Science Hunan University of Technology and BusinessChangsha 410205People’s Republic of China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China

The application of Sb_(2)S_(3)with marvelous theoretical capacity for alkali metal-ion batteries is seriously limited by its poor electrical conductivity and low initial coulombic efficiency(ICE).In this work,natural stibnite modified by carbon dots(Sb_(2)S_(3)@xCDs)is elaborately designed with high ***,chemical processes of local oxidation–partial reduction–deep coupling for stibnite reduction of CDs are clearly demonstrated,confirmed with in situ high-temperature X-ray *** impressively,the ICE for lithium-ion batteries(LIBs)is enhanced to 85%,through the effect of oxygen-rich carbon matrix on C–S bonds which inhibit the conversion of sulfur to sulfite,well supported by X-ray photoelectron spectroscopy characterization of solid electrolyte interphase layers helped with density functional theory *** than less,it is found that Sb–O–C bonds existed in the interface effectively promote the electronic conductivity and expedite ion transmission by reducing the bandgap and restraining the slip of the *** a result,the optimal sample delivers a tremendous reversible capacity of 660 mAh g^(−1)in LIBs at a high current rate of 5 A g^(−1).This work provides a new methodology for enhancing the electrochemical energy storage performance of metal sulfides,especially for improving the ICE.

关键词： Carbon dots Sb_(2)S_(3) Initial Coulombic efficiency Interfacial bond Anode

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