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Unlocking the multi-electron transfer reaction in NASICON-type cathode materials

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materials Futures 2023年第2期2卷 109-122页

作者： Yuan Liu Xiaohui Rong Fei Xie Yaxiang Lu Junmei Zhao Liquan Chen Yong-Sheng Hu Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190People’s Republic of China College of materials Science and Optoelectronic Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China Yangtze River Delta Physics Research Center Co.Ltd Liyang 213300People’s Republic of China Huairou Division Institute of PhysicsChinese Academy of SciencesBeijing 101400People’s Republic of China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Biochemical EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijingPeople’s Republic of China

The growing concern about scarcity and large-scale applications of lithium resources has attracted efforts to realize cost-effective phosphate-based cathode materials for next-generation Na-ion batteries(NIBs).In previous work,a series of materials(such as Na_(4)Fe_(3)(PO_(4))_(2)(P_(2)O_(7)),Na_(3)VCr(PO_(4))_(3),Na_(4)VMn(PO_(4))3,Na_(3)MnTi(PO_(4))_(3),Na_(3)MnZr(PO_(4))3,etc)with∼120 mAh g^(-1) specific capacity and high operating potential has been proposed.However,the mass ratio of the total transition metal in the above compounds is only∼22 wt%,which means that one-electron transfer for each transition metal shows a limited capacity(the mass ratio of Fe is 35.4 wt%in LiFePO_(4)).Therefore,a multi-electron transfer reaction is necessary to catch up to or go beyond the electrochemical performance of LiFePO_(4).This review summarizes the reported NASICON-type and other phosphate-based cathode materials.On the basis of the aforementioned experimental results,we pinpoint the multi-electron behavior of transition metals and shed light on designing rules for developing high-capacity cathodes in NIBs.

关键词： NASICON Na-ion batteries cathode materials multi-electron transfer reactions

3D anchoring structured for LiFe_(0.5)Mn_(0.5)PO_(4)@cornstalk-C cathode materials

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中国化学快报:英文版 2023年第8期34卷 302-305页

作者： Guangliang Zhang Riran Zang Man Mo Zhijie Fang Yangxian Huang Kunsong Hu Jiali Huang Xinxiang Liu Lingyun Huang Guohui Kang Weijian Li Haiqing Zhan Xianquan Ming Guanhan Huang Guiliang Li Feng Zhan School of Resources Environment and materials Guangxi UniversityNanning 530004China School of Electronics Engineering Guangxi University of Science and TechnologyLiuzhou 545006China State Key Laboratory of Featured Metal materials and Life-cycle Safety for Composite Structures Guangxi UniversityNanning 530004China Guangxi Higher Education Key Laboratory of High Performance Structural materials and Heat Treatment&Surface Processing Guangxi UniversityNanning 53004China South Manganese Group Limited Nanning 530029China

The organic carbon source coating LiFe_(x)Mn_(1-x)PO_(4)suffers from the problem of non-uniform carbon cladding.Too thick carbon cladding layer instead hinders the de-embedding of lithium ions.In this paper,we choose cornstalk as the carbon source,then LiFe_(0.5)Mn_(0.5)PO_(4)@cornstalk-C(LFMP@C-C)with 3D anchoring structure is prepared by the solvothermal method.The results show that the LFMP with cornstalk as the carbon source has better performance compared to the sucrose-coated LFMP material(LFMP@C).The discharge capacity of LFMP@C-C is 116 mAh/g for the first cycle at 1 C and the capacity retention rate is 94.0%after 500 cycles,and the discharge capacity of LFMP@C-C is more than 17.17%higher than that of LFMP@C.

关键词： LiFe_(0.5)Mn_(0.5)PO_(4) Cornstalk Solvothermal method 3D anchoring structure cathode materials

Cascading V_(2)O_(3)/N-doped carbon hybrid nanosheets as high-performance cathode materials for aqueous zinc-ion batteries

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Chinese Chemical Letters 2022年第3期33卷 1430-1434页

作者： Yue Niu Denghui Wang Yingjie Ma Linjie Zhi CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China University of Chinese Academy of Sciences Beijing 100039China

In recent years, especially when there is increasing concern about the safety issue of lithium-ion batteries (LIBs), aqueous Zn-ion batteries (ZIBs) have been getting a lot of attention because of their cost-effectiveness, materials abundance, high safety, and ecological friendliness. Their working voltage and specific capacity are mainly determined by their cathode materials. Vanadium oxides are promising cathode materials for aqueous ZIBs owing to their low cost, abundant resources, and multivalence. However, vanadium oxide cathodes still suffer from unsatisfactory capacity, poor stability, and low electrical conductivity. In this work, cascading V_(2)O_(3)/nitrogen doped carbon (V_(2)O_(3)/NC) hybrid nanosheets are prepared for high-performance aqueous ZIBs by pyrolyzing pentyl viologen dibromide (PV) intercalated V_(2)O5 nanosheets. The unique structure features of V_(2)O_(3)/NC nanosheets, including thin sheet-like morphology, small crystalline V_(2)O_(3) nanoparticles, and conductive NC layers, endow V_(2)O_(3)/NC with superior performance compared to most of the reported vanadium oxide cathode materials for aqueous ZIBs. The V_(2)O_(3)/NC cathode exhibits the discharge capacity of 405 mAh/g at 0.5 A/g, excellent rate capability (159 mAh/g at 20 A/g), and outstanding cycling stability with 90% capacity retention over 4000 cycles at 20 A/g.

关键词： Aqueous zinc ion batteries cathode materials Vanadium oxides Nitrogen doped carbon 2D nanosheets High performance

Bismuth chloride@mesocellular carbon foam nanocomposite cathode materials for rechargeable chloride ion batteries

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Chinese Chemical Letters 2022年第4期33卷 2200-2204页

作者： Chang Zhang Shijiao Sun Meifen Wu Xiangyu Zhao College of materials Science and Engineering Nanjing Tech UniversityNanjing 211816China CAS Key Laboratory of materials for Energy Conversion Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China Jiangsu Collaborative Innovation Center for Advanced Inorganic Functional Composites Nanjing Tech UniversityNanjing 211816China

Chloride ion batteries(CIB) are considered to be one of the most promising energy storage devices. As cathode materials for CIBs, metal chlorides have many advantages, such as high theoretical energy density, abundant elemental resources and ideal discharge voltage plateau. However, the dissolution and huge volume change of metal chlorides during cycling lead to considerable short lifespan, which limits their potential application for CIBs. Herein, the bismuth chloride nanocrystal is confined in mesocellular carbon foam matrix by a new vacuum impregnation approach. The mesocellular carbon foam with large interconnected pores(15.7 or 23.2 nm) may buffer the large volume variation of bismuth chloride during charge and discharge, giving rise to significantly enhanced electrochemical performance. The as-prepared bismuth chloride@mesocellular carbon foam cathode delivered an initial discharge capacity of 298 m Ah/g and a reversible capacity of 91 m Ah/g after 60 cycles. In contrast, the pure bismuth chloride cathode almost cannot discharge after 30 cycles. This is the first report that the metal chloride cathode can achieve a prolonged cycling in CIBs.

关键词： Chloride ion batteries cathode materials Bismuth chloride Mesocellular carbon foam Electrochemistry

Sulfur-containing polymer cathode materials: From energy storage mechanism to energy density

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InfoMat 2022年第8期4卷 1-24页

作者： Rong Zou Wenwu Liu Fen Ran State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals School of Material Science and EngineeringLanzhou University of TechnologyLanzhouP.R.China

Besides lithium-ion batteries, it is imperative to develop new battery energystorage system with high energy density. In conjunction with the developmentof Li-S batteries, emerging sulfur-containing polymers with tunable sulfur-chain length and organic groups gradually attract much attention as cathodematerials. This can avoid the problems that are impeding the development ofthe typical Li-S batteries, such as volume expansion, active material dissolu-tion, shuttle effect, and so on. This review aims to generalize the type ofsulfur-containing polymers and the working principles in Li-S batteries. Thesulfur-containing polymers (R-Sn-R) with different sulfur-chain length (n > 6,n ≤ 2, and 3 ≤ n ≤ 6) are summarized. It also discusses several organic groupssuch as phenyl rings, N-heterocycles, and unique structure with cross-linkednetworks and multi-micropores skeleton. This review also explores other strat-egies of sulfur-containing polymers in the rest of Li-S batteries, providing asummary of the advantages of sulfur-containing polymers, recent develop-ment, in-depth discussion of the mechanism in Li-S batteries, and organicgroup-structure-performance relationship. This review would have guidelinesfor future development of sulfur-containing polymers in Li-S batteries.

关键词： cathode materials energy density energy storage mechanism Li-S batteries sulfur-containing polymer

The discovery of cathode materials for lithium-ion batteries from the view of interdisciplinarity

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Interdisciplinary materials 2022年第3期1卷 323-329页

作者： Yunhui Huang State Key Laboratory of Material Processing and Die&Mold Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanHubeiChina

In honor of Professor John B.Goodenough for his 100th birthday,this article tries to find the relationship between the discovery of cathode materials for lithium-ion batteries and the interdisciplinary research in his career.The original ideas of lithium cobalt oxide,lithium manganese oxide,and LiFePO4 came from his early research in solid state physics and from his strong knowledge of chemical structure and bonding.Some examples are given to demonstrate the importance of interdisciplinary interactions among materials,chemistry,and physics.With the rapid development of rechargeable batteries,such interdisciplinarity is further extended to engineering,information,and even artificial intelligence.Although there are still many challenges like energy density and safety in the batteries,we are confident that a better solution will be soon found.

关键词： cathode materials interdisciplinarity John B.Goodenough

Application of deep learning for informatics aided design of electrode materials in metal-ion batteries

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Green Energy & Environment 2024年第5期9卷 877-889页

作者： Bin Ma Lisheng Zhang Wentao Wang Hanqing Yu Xianbin Yang Siyan Chen Huizhi Wang Xinhua Liu School of Transportation Science and Engineering Beihang UniversityBeijing102206China College of Automotive Engineering Jilin UniversityChangchun130022China Department of Mechanical Engineering Imperial College LondonLondonSW72BXUK

To develop emerging electrode materials and improve the performances of batteries,the machine learning techniques can provide insights to discover,design and develop battery new materials in high-throughput way.In this paper,two deep learning models are developed and trained with two feature groups extracted from the materials Project datasets to predict the battery electrochemical performances including average voltage,speciﬁc capacity and speciﬁc energy.The deep learning models are trained with the multilayer perceptron as the core.The Bayesian optimization and Monte Carlo methods are applied to improve the prediction accuracy of models.Based on 10 types of ion batteries,the correlation coefﬁcients are maintained above 0.9 compared to DFT calculation results and the mean absolute error of the prediction results for voltages of two models can reach 0.41 V and 0.20 V,respectively.The electrochemical performance prediction times for the two trained models on thousands of batteries are only 72.9 ms and 75.7 ms.Besides,the two deep learning models are applied to approach the screening of emerging electrode materials for sodium-ion and potassium-ion batteries.This work can contribute to a high-throughput computational method to accelerate the rational and fast materials discovery and design.

关键词： cathode materials Material design Electrochemical performance prediction Deep learning Metal-ion batteries

Reversible Mn^(2+)/Mn^(4+)double-electron redox in P3-type layer-structured sodium-ion cathode

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Journal of Energy Chemistry 2024年第2期89卷 79-88,I0004页

作者： Jie Zeng Jian Bao Ya Zhang Xun-Lu Li Cui Ma Rui-Jie Luo Chong-Yu Du Xuan Xu Zhe Mei Zhe Qian Yong-Ning Zhou Department of materials Science Fudan UniversityShanghai 200433China Shanghai Xuanyi New Energy Development Co. LtdShanghai 201800China Global Institute of Future Technology Shanghai Jiao Tong UniversityShanghai 200240China

The balance between cationic redox and oxygen redox in layer-structured cathode materials is an important issue for sodium batteries to obtain high energy density and considerable cycle stability.Oxygen redox can contribute extra capacity to increase energy density,but results in lattice instability and capacity fading caused by lattice oxygen gliding and oxygen release.In this work,reversible Mn^(2+)/Mn^(4+)redox is realized in a P3-Na_(0.65)Li_(0.2)Co_(0.05)Mn_(0.75)O_(2)cathode material with high specific capacity and structure stability via Co substitution.The contribution of oxygen redox is suppressed significantly by reversible Mn^(2+)/Mn^(4+)redox without sacrificing capacity,thus reducing lattice oxygen release and improving the structure stability.Synchrotron X-ray techniques reveal that P3 phase is well maintained in a wide voltage window of 1.5-4.5 V vs.Na^(+)/Na even at 10 C and after long-term cycling.It is disclosed that charge compensation from Co/Mn-ions contributes to the voltage region below 4.2 V and O-ions contribute to the whole voltage range.The synergistic contributions of Mn^(2+)/Mn^(4+),Co^(2+)/Co^(3+),and O^(2-)/(O_n)^(2-)redox in P3-Na_(0.65)Li_(0.2)Co_(0.05)Mn_(0.75)O_(2)lead to a high reversible capacity of 215.0 m A h g^(-1)at 0.1 C with considerable cycle stability.The strategy opens up new opportunities for the design of high capacity cathode materials for rechargeable batteries.

关键词： Sodium batteries cathode materials Layered structure Co substitution

Revealing the role of calcium ion intercalation of hydrated vanadium oxides for aqueous zinc-ion batteries

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Journal of Energy Chemistry 2024年第8期95卷 9-19页

作者： Tao Zhou Xuan Du Guo Gao Key Laboratory for Thin Film and Micro Fabrication of the Ministry of Education School of Sensing Science and Engineering School of Electronic Information and Electrical Engineering Shanghai Jiao Tong University

Exploring suitable high-capacity V2O5-based cathode materials is essential for the rapid advancement of aqueous zinc ion batteries（ZIBs）.However,the typical problem of slow Zn2+diffusion kinetics has severely limited the feasibility of such materials.In this work,unique hydrated vanadates（CaVO,BaVO） were obtained by intercalation of Ca2+or Ba2+into hydrated vanadium pentoxide.In the CaVO//Zn and BaVO//Zn batteries systems,the former delivered up to a 489.8 mAh g-1discharge specific capacity at 0.1 A g-1.Moreover,the remarkable energy density of 370.07 Wh kg-1and favorable cycling stability yard outperform BaVO,pure V2O5,and many reported cathodes of similar ionic intercalation compounds.In addition,pseudocapacitance analysis,galvanostatic intermittent titration（GITT） tests,and Trasatti analysis revealed the high capacitance contribution and Zn2+diffusion coefficient of CaVO,while an in-depth investigation based on EIS elucidated the reasons for the better electrochemical performance of CaVO.Notably,ex-situ XRD,XPS,and TEM tests further demonstrated the Zn2+insertion/extraction and Zn-storage mechanism that occurred during the cycle in the CaVO//Zn battery system.This work provides new insights into the intercalation of similar divalent cations in vanadium oxides and offers new solutions for designing cathodes for high-capacity aqueous ZIBs.

关键词： Aqueous zinc ion batteries cathode materials Energy storage mechanism Ion pre-intercalation Vanadium oxides