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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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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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Methods of improving the initial Coulombic efficiency and rate performance of both anode and cathode materials for sodium-ion batteries

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Chinese Chemical Letters 2022年第2期33卷 730-742页

作者： Nkongolo Tshamala Aristote Kangyu Zou Andi Di wentao deng Baowei Wang Xinglan deng Hongshuai Hou Guoqiang Zou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Department of Materials and Environmental Chemistry Stockholm UniversityStockholm 10691Sweden

Sodium-ion batteries(SIBs) have gained more scientists’ interest, owing to some facts such as the natural abundance of Na, the similarities of physicochemical characteristics between Li and Na. The irreversible Na+ions consumption during the first cycle of charge/discharge process(due to the formation of the solid electrolyte interface(SEI) on the electrode surface and other irreversible reactions) is the factor that determines high performance SIBs and largely reduces the capacity of the full cell SIBs. Thus, the initial coulombic efficiency(ICE) of SIBs for both anode and cathode materials, is a key parameter for high performance SIBs, and the point is to increase the transport rate of the Na+ions. Therefore, developing SIBs with high ICE and rate performance becomes vital to boost the commercialization of SIBs. Here we provide a review on the methods to improve the ICE and the rate performance, by summarizing some methods of improving the ICE and rate performance of the anode and cathode materials for SIBs, and end by a conclusion with some perspectives and recommendations.

关键词： Initial coulombic efficiency Rate performance Sodium-ion batteries Anode materials Cathode materials

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2D Metal-Organic Frameworks for Electrochemical Energy Storage

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Energy & Environmental Materials 2023年第6期6卷 33-49页

作者： dengyi Xiong Xinglan deng Ziwei Cao Shusheng Tao Zirui Song Xuhuan Xiao wentao deng Hongshuai Hou Guoqiang Zou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China

Metal-organic frameworks(MOFs)have been widely adopted in various fields(catalysis,sensor,energy storage,etc.)during the last decade owing to the trait of abundant surface chemistry,porous structure,easy-to-adjust pore size,and diverse functional ***,the limited active sites and the poor conductivity hinder the relative practical application.2D MOFs can shorten the ion transport path with the merit of layered *** large surface area can increase the number of active sites as well as effectively utilize the sufficient active sites,exhibiting enormous potential in the field of energy storage systems(EESs).In this review,the characteristics of the 2D MOFs have been introduced,and the systematic synthesis methods(top-down and bottom-up)of 2D MOFs are presented,providing fundamental understanding for the construction of 2D ***,the applications of 2D MOFs in energy storage fields such as supercapacitors and batteries are demonstrated in ***,the future development prospects have been proposed,offering guidelines for the rational utilization of 2D MOFs and promoting the understanding of 2D MOFs in EESs.

关键词： batteries electrochemical energy storage supercapacitors 2D metal-organic frameworks

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K_(x)C_(y) phase induced expanded interlayer in ultra-thin carbon toward full potassium-ion capacitors

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Carbon Energy 2022年第6期4卷 1151-1168页

作者： Xinglan deng Ye Tian Kangyu Zou Jun Chen Xuhuan Xiao Shusheng Tao Zirui Song wentao deng Hongshuai Hou Guoqiang Zou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangshaHunanChina College of Materials Science and Engineering Zhengzhou UniversityZhengzhouChina

Carbonaceous materials have been regarded as highly promising anode candidates for potassium storage with their cost-effectiveness and environmental ***,low specific capacity and difficulty in large-scale synthesis largely hinder their further ***,a thermal-induced potassium–carbon alloy phase(K_(x)C_(y))with the expanded interlayer spacing strategy is first put *** in situ high-temperature X-ray diffraction,a K_(2)C_(2) phase is evoked by thermal energy during the in-situ carbonization process of carbon quantum dots intermediate derived from potassium-containing precursors,whereas no lithium or sodium–carbon alloy phase is observed from lithium/sodium-containing *** asobtained ultra-thin carbon nanosheets achieve adjustable layer spacing,preparation in bulk,delivering reversible potassium storage of 403.4 mAh g^(−1) at 100 mA g^(−1) and 161.2 mAh g^(−1) even at 5.0 A g^(−1),which is one of the most impressive K-storage performances reported so far with great potential ***,the assembled potassium-ion hybrid capacitor by combining the impressive CFMs-900 anode with the three-dimensional framework-activated carbon delivers a high energy-power density of 251.7 Wh kg^(−1) at 250Wkg^(−1) with long-term *** study opens a scalable avenue to realize the expanded interlayer spacing,which can be extended to other multicarboxyl potassium salts and can provide approach for the design of high-performance carbon anode materials for potassium storage.

关键词： expanded interlayer K_(x)C_(y)phase potassium-ion capacitors themal-induced ultra-thin carbon

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Ultra-Low-Dose Pre-Metallation Strategy Served for Commercial Metal-Ion Capacitors

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Nano-Micro Letters 2022年第3期14卷 276-291页

作者： Zirui Song Guiyu Zhang Xinglan deng Kangyu Zou Xuhuan Xiao Roya Momen Abouzar Massoudi wentao deng Jiugang Hu Hongshuai Hou Guoqiang Zou Xiaobo Ji College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083People’s Republic of China Department of Semiconductors Materials and Energy Research Center P.O.Box 14155/4777TehranIran College of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China

Sacrificial pre-metallation strategy could compensate for the irreversible consumption of metal ions and reduce the potential of anode,thereby elevating the cycle performance as well as open-circuit voltage for full metal ion capacitors(MICs).However,suffered from massive-dosage abuse,exorbitant decomposition potential,and side effects of decomposition residue,the wide application of sacrificial approach was ***,assisted with density functional theory calculations,strongly coupled interface(M-O-C,M=Li/Na/K)and electron donating group have been put forward to regulate the band gap and highest occupied molecular orbital level of metal oxalate(M_(2)C_(2)O_(4)),reducing polarization phenomenon and Gibbs free energy required for decomposition,which eventually decrease the practical decomposition potential from 4.50 to 3.95 ***,full sodium ion capacitors constituted of commercial materials(activated carbon//hard carbon)could deliver a prominent energy density of 118.2 Wh kg^(−1)as well as excellent cycle stability under an ultra-low dosage pre-sodiation reagent of 15-30 wt%(far less than currently 100 wt%).Noteworthily,decomposition mechanism of sacrificial compound and the relative influence on the system of MICs after pre-metallation were initially revealed by in situ differential electrochemical mass spectrometry,offering in-depth insights for comprehending the function of cathode *** addition,this breakthrough has been successfully utilized in high performance lithium/potassium ion capacitors with Li_(2)C_(2)O_(4)/K_(2)C_(2)O_(4) as pre-metallation reagent,which will convincingly promote the commercialization of MICs.

关键词： Coupled interface Pre-metallation Metal oxalate Decomposition potential

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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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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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Cu-substitution P2-Na_(0.66)Mn_(1-x)Cu_(x)O_(2) sodium-ion cathode with enhanced interlayer stability

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Journal of Energy Chemistry 2022年第12期75卷 478-485,I0012页

作者： Huanqing Liu Xu Gao Jun Chen Jinqiang Gao Haoji Wang Yu Mei Huan Liu wentao deng Guoqiang Zou Hongshuai Hou Xiaobo Ji State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083HunanChina School of Materials Science and Engineering Hunan Provincial Key Lab of Advanced Materials for New Energy Storage and ConversionHunan University of Science and TechnologyXiangtan 411201HunanChina

P2-type Mn-based layered oxides are viewed as promising cathode materials for sodium ion battery by virtue of their high theoretical *** that pure Na_(2/3)MnO_(2)suffers from poor cycling performances,Cu-substitution strategy is proposed to effectively alleviate this ***,the structural evolution mechanism of the Cu-containing samples still remains ***,we propose that CuSubstitution P2-type Na_(0.66)Mn_(1-x)Cu_(x)O_(2)with enlarged lattice parameters are conducive to improving the interlayer structure stability through mitigating TMO_(2)slabs *** by synchrotron XAS spectra and ex/in situ XRD,the expansion/contraction of MnO_6 octahedron is dramatically reduced with the increased Cu content,showing the facilitated Na ion ***,when the ratio of Cu to Mn reaches 1:4,the phase transition from P2 to P'2 type at the end of discharge can be suppressed,resulting in the improved interlayer skeleton *** Cu-containing samples with stable interlayer structure exhibit high capacity retention and outstanding rate performances(a capacity of 79.9 m Ah g^(-1)at 5C).This Cu-substitution strategy provides a promising approach to designing highly stable cathodes.

关键词： Sodium-ion battery Manganese-based cathode Cu-substitution In-plane distortion Jahn-Teller effect

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Mitigating the Jahn-Teller distortion driven by the spin-orbit coupling of lithium manganate cathode

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Journal of Energy Chemistry 2022年第9期31卷 379-387,I0011页

作者： Shu Zhang Hongyi Chen Jun Chen Shouyi Yin Yu Mei Lianshan Ni Andi Di wentao deng Guoqiang Zou Hongshuai Hou Xiaobo Ji State Key Laboratory of Powder Metallurgy College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083HunanChina Department of Materials and Environmental Chemistry Stockholm UniversityStockholm 10691Sweden

Spinel LiMn_(2)O_(4)is recognized as one of the most competitive cathode candidates for lithium-ion batteries ascribed to environmentally benign and rich ***,the wholesale application of LiMn_(2)O_(4)is predominately plagued by its severe capacity degradation,mainly associated with the innate Jahn-Teller ***,single-crystalline LiMn_(2)O_(4)with Eu^(3+) doping is rationally designed to mitigate the detrimental Jahn-Teller distortion by tuning the chemical environment of MnO_(6) octahedra and accommodating localized electron,based on the unique aspheric flexible 4f electron orbit of rare-earth metal ***,the stretching of MnO_(6) octahedron stemmed from the Jahn-Teller effect in Eu-doped LiMn_(2)O_(4)is effectively suppressed,confirmed by theoretical ***,the structural stability of the material has been significantly enhanced due to the robust Mn–O band coherency and weakened phase transition,proved by synchrotron radiation absorption spectrum and operando X-ray *** corresponding active cathode manifests superior long-cycle stability after 300 loops at 2C and displays only a 0.011%capacity drop per cycle even at *** this,this modification tactic sheds new light on achieving superior long-cycle performances by suppressing distortion in various cathode materials.

关键词： Spinel lithium manganate Spin-orbit coupling Jahn-Teller distortion Cathode material

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