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Nano-Micro Letters 2020年第11期12卷 39-50页

作者： Ruiting Guo Xiong Liu Bo Wen Fang Liu Jiashen Meng Peijie Wu Jinsong Wu Qi Li Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200People’s Republic of China

Amorphous carbon shows great potential as an anode material for high-performance potassium-ion batteries;however,its abundant defects or micropores generally capture K ions,thus resulting in high irreversible capacity with low initial coulombic efficiency(ICE)and limited practical ***,pore engineering via a facile self-etching strategy is applied to achieve mesoporous carbon(meso-C)nanowires with interconnected *** and evenly distributed mesopores could provide short K^+ pathways for its rapid *** to microporous carbon with highly disordered structure,the meso-C with Zn-catalyzed short-range ordered structure enables more K^+to reversibly intercalate into the graphitic ***,the mesoC shows an increased capacity by ~100 mAh g^-1 at 0.1 A g^-1,and the capacity retention is 70.7% after 1000 cycles at 1 A g^-*** in/ex situ characterizations reveal the reversible structural changes during the charging/discharging ***,benefiting from the mesoporous structure with reduced specific surface area by 31.5 times and less defects,the meso-C generates less irreversible capacity with high ICE up to 76.7%,one of the best reported values so *** work provides a new perspective that mesopores engineering can effectively accelerate K^+ diffusion and enhance K^+ adsorption/intercalation storage.

关键词： Potassium-ion battery Mesopores engineering Storage mechanism initial coulombic efficiency

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

Mg-doped,carbon-coated,and prelithiated SiO_(x) as anode materials with improved initial coulombic efficiency for lithium-ion batteries

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Carbon Energy 2024年第3期6卷 204-214页

作者： Bin Liu Jie Liu Cheng Zhong Wenbin Hu Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education) School of Materials Science and EngineeringTianjin UniversityTianjinChina Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and EngineeringTianjin UniversityTianjinChina Joint School of National University of Singapore and Tianjin University TianjinChina International Campus of Tianjin University Binhai New CityFuzhouChina

Silicon suboxide(SiO_(x),x≈1)is promising in serving as an anode material for lithium-ion batteries with high capacity,but it has a low initial coulombic efficiency(ICE)due to the irreversible formation of lithium silicates during the first *** this work,we modify SiO_(x) by solid-phase Mg doping reaction using low-cost Mg powder as a reducing *** show that Mg reduces SiO_(2) in SiO_(x) to Si and forms MgSiO_(3) or Mg_(2)SiO_(4).The MgSiO_(3) or Mg_(2)SiO_(4) are mainly distributed on the surface of SiO_(x),which suppresses the irreversible lithium-ion loss and enhances the ICE of SiO_(x).However,the formation of MgSiO_(3) or Mg_(2)SiO_(4) also sacrifices the capacity of SiO_(x).Therefore,by controlling the reaction process between Mg and SiO_(x),we can tune the phase composition,proportion,and morphology of the Mg-doped SiO_(x) and manipulate the *** obtain samples with a capacity of 1226 mAh g^(–1) and an ICE of 84.12%,which show significant improvement over carbon-coated SiO_(x) without Mg *** the synergistical modification of both Mg doping and prelithiation,the capacity of SiO_(x) is further increased to 1477 mAh g^(–1) with a minimal compromise in the ICE(83.77%).

关键词： initial coulombic efficiency lithium-ion batteries magnesium doping prelithiation silicon suboxide

Molten-LiCl induced thermochemical prelithiation of SiOx:Regulating the active Si/O ratio for high initial coulombic efficiency

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Nano Research 2022年第1期15卷 230-237页

作者： Yang Li Yong Qian Jie Zhou Ning Lin Yitai Qian Department of Applied Chemistry University of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China

The low initial coulombic efficiency(ICE)of SiOx anode caused by the irreversible generation of LiySiOz and Li20 during lithiation process limits its application for high energy-density lithium-ion ***,we report a molten-salt-induced *** strategy for regulating the electrochemically active Si/O ratio of SiOx and thus enhancing ICE through thermal treatment of pre-synthesized LiNH2-coated SiOx in molten LiCl at 700℃.Bulk SiOx micro-particle was transformed into pomegranatelike prelithiated micro-cluster composite(M-Li-SiOx)with SiOx core and outer nano-sized agglomerates consisting of Li2Si20s,SiO2,and *** the analysis of the reaction intermediates,molten-UC!could initiate reactions and promote mass transfer by the continuous extraction of oxygen component from SiOx particle inner in the form of inert Li2Si20s and SiO2 nanotubes to realize *** degree of prelithiation can be regulated by adjusting the coating amount of LiNH2 layer,and the resulted M-Li-SiOx displays a prominent improvement of ICE from 58.73%to 88.2%.The graphite/M-Li-SiOx(8:2)composite electrode delivers *** capacity of 497.29 mAh·g^(-1) with an ICE of 91.79%.By pairing graphite/M-Li-SiOx anode and LiFeP04 cathode in a full-cell an enhancement of energy density of 37.25%is realized compared with the full-cell containing graphite/SiOx ***,,ex-situ X-ray photoelectron spectroscopy(XPS)/Raman/X-ray diffraction(XRD)and related electrochemical measurements reveal the SiOx core and Si of M-Li-SiOx participate in the lithiation,and pre-generated Li2Si20s with u+diffusivity and *** reduces the reaction resistance and interface impedance of the solid electrolyte interphase(SEI)film.

关键词： initial coulombic efficiency thermochemical prelithiation liquid coating molten-salt mass transfer

Boosting high initial coulombic efficiency of hard carbon by in-situ electrochemical presodiation

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Journal of Energy Chemistry 2023年第2期77卷 310-316,I0008页

作者： Nannan Qin Yanyan Sun Chao Hu Sainan Liu Zhigao Luo Xinxin Cao Shuquan Liang Guozhao Fang School of Materials Science and Engineering Central South UniversityChangsha 410083HunanChina School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083HunanChina College of Chemistry Xiangtan UniversityXiangtan 411105HunanChina Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South UniversityChangsha 410083HunanChina

Hard carbon(HC)is a promising anode material for sodium ion batteries(SIBs),whereas inferior initial coulombic efficiency(ICE)severely limits its practical *** the present work,we propose an in situ electrochemical presodiation approach to improve ICE by mixing sodium biphenyl(Na-Bp)dimethoxyethane(DME)solution with DME-based ether electrolyte.A solid electrolyte interface(SEI)could be formed beforehand on the HC electrode and Na^(+)was absorbed to nanopores and graphene stacks,compensating for the sodium loss and preventing electrolyte decomposition during the initial charge and discharge *** this way,the ICE of half-cells was increased to nearly 100%and that of full-cells from 45%to 96%with energy density from 132.9 to 230.5 W h kg^(-1).Our work provides an efficient and facile method for improving ICE,which can potentially promote the practical application of HCbased materials.

关键词： Hard carbon In situ presodiation initial coulombic efficiency Solid electrolyte interface Sodium-ion batteries

Improving the initial coulombic efficiency of Carbonaceous Materials for Li/Na‑Ion Batteries:Origins,Solutions,and Perspectives

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Electrochemical Energy Reviews 2023年第1期6卷 651-679页

作者： Zheng Tang Siyu Zhou Yuancheng Huang Hong Wang Rui Zhang Qi Wang Dan Sun Yougen Tang Haiyan Wang Hunan Provincial Key Laboratory of Chemical Power Sources College of Chemistry and Chemical EngineeringCentral South UniversityChangsha 410083HunanChina

Carbonaceous materials for lithium(Li)/sodium(Na)-ion batteries have attracted significant attention because of their widespread availability,renewable nature,and low *** the past decades,although great efforts have been devoted to developing high-performance carbonaceous materials with high capacity,long life span,and excellent rate capability,the low initial coulombic efficiency(ICE)of high-capacity carbonaceous materials seriously limits their practical *** methods have been successfully exploited,and a revolutionary impact has been achieved through the utilization of different *** carbonaceous materials possess different ion storage mechanisms,which means that the initial capacity loss may ***,there has rarely been a special review about the origins of and progress in the ICE for carbonaceous materials from the angle of the crystal ***,in this review,the structural differences between and ion storage mechanisms of various carbonaceous materials are first ***,we deduce the correlative factors of low ICE and thereafter summarize the proposed strategies to address these ***,some challenges,perspectives,and future directions on the ICE of carbonaceous materials are *** review will provide deep insights into the challenges of improving the ICE of carbonaceous anodes for high-energy Li/Na-ion batteries,which will greatly contribute to their commercialization process.

关键词： Lithium/sodium-ion batteries initial coulombic efficiency Carbonaceous materials Energy storage

Sn Alloy and Graphite Addition to Enhance initial coulombic efficiency and Cycling Stability of SiO Anodes for Li-Ion Batteries

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Energy & Environmental Materials 2022年第1期5卷 353-359页

作者： Xingyang Du Hanying Zhang Xuexia Lan Bin Yuan Renzong Hu School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640China

Silicon monoxide(SiO)has aroused increased attention as one of the most promising anodes for high-energy density Li-ion *** enhance the initial coulombic efficiencies(ICE)and cycle stability of SiO-based anodes,a new facile composition and electrode design strategy have been adapted to fabricate a SiO-Sn-Co/graphite(G)*** achieves a unique structure where tiny milled SiO-Sn-Co particles are dispersed among two graphite *** this hybrid electrode,Sn-Co alloys promoted Li;extraction kinetics,and the holistic reversibility of SiO and graphite enhanced the electrical *** SiO-Sn-Co/G electrode delivered an average ICE of 77.6%and a reversible capacity of 640 mAh g^(-1)at 800 mA g^(-1),and the capacity retention was above 98%after 100 cycles,which was much higher than that of the SiO with an ICE of 55.3%and a capacity retention of 50%.These results indicated that this was reliable method to improve the reversibility and cycle ability of the SiO ***,based on its easy and feasible fabrication process,it may provide a suitable choice to combine other alloy anodes with the graphite anode.

关键词： ball milling cycle performance initial coulombic efficiency silicon monoxide tin-cobalt alloy

Surface engineering based on in situ electro-polymerization to boost the initial coulombic efficiency of hard carbon anode for sodium-ion battery

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Rare Metals 2022年第5期41卷 1616-1625页

作者： Cheng-Xin Yu Yu Li Zhao-Hua Wang Xin-Ran Wang Ying Bai Chuan Wu Beijing Key Laboratory of Environmental Science and Engineering School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China Yangtze Delta Region Academy of Beijing Institute of Technology Jiaxing 314019China

Hard carbon(HC) is considered as a commercial candidate for anode materials of sodium-ion batteries due to its low cost and excellent capacity. However, the problem of low initial coulombic efficiency is still urgently needed to be solved to promote the industrialization of *** this paper, 2,2-dimethylvinyl boric acid(DEBA) is used to modify the surface of HC to prepare HC-DEBA materials. During the cycling, the C = C bonds of DEBA molecules will be in situ electro-polymerized to form a polymer network, which can act as the passive protecting layer to inhibit irreversible decomposition of electrolyte,and induce a thinner solid electrolyte interface with lower interface impedance. Therefore, HC-DEBA has higher initial coulombic efficiency and better cycling stability. In ester-based electrolyte, the initial coulombic efficiency of the optimized HC-DEBA-3% increases from 65.2% to77.2%. After 2000 cycles at 1 A·g^(-1), the capacity retention rate is 90.92%. Moreover, it can provide a high reversible capacity of 294.7 m Ah·g^(-1) at 50 mA·g^(-1). This simple surface modification method is ingenious and versatile,which can be extended to other energy storage materials.

关键词： Sodium-ion battery Hard carbon initial coulombic efficiency Solid electrolyte interface Surface modification Ester electrolyte

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

Low-temperature-pyrolysis preparation of nanostructured graphite towards rapid potassium storage with high initial coulombic efficiency

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Nano Research 2024年第6期17卷 5138-5147页

作者： Jingke Ren Boyu Xing Wen Luo Binyang Luo Xinfei Wu Xin Yan Wencong Feng Feiyue Wang Chaojie Cheng Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Physics School of ScienceWuhan University of TechnologyWuhan 430070China

Industrially prepared artificial graphite(AG)is attractive for potassium-ion batteries(PIBs),but its rate performance is poor and the production process is energy intensive,so developing an efficient strategy to produce novel graphite with low energy consumption and high performance is economically ***,a nanostructured graphite composed of multi-walled carbon nanotubes(MWCNTs)and graphite shells was prepared by one-pot method through low-temperature pyrolysis of iron-based metal-organic framework(MOF)and carbon *** high graphitization degree of nanostructured graphite makes the initial coulombic efficiency(ICE)exceed 80%,and the three-dimensional(3D)conductive network ensures a specific capacity of 234 mAh·g^(−1)after 1000 cycles at a high current density of 500 mA·g^(−1).In addition,the typical graphite potassium storage mechanism is also demonstrated by in situ X-ray diffraction(XRD)and in situ Raman spectroscopy,and its practicality is also proved by the voltage of the full *** work provides a feasible way to optimize the practical production process of AG and expand its application in energy storage.

关键词： graphite anode potassium-ion batteries high graphitization degree low-temperature pyrolysis initial coulombic efficiency