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Mn-based cathode materials for rechargeable batteries

Science China Chemistry 2024年第1期67卷 87-105页

作者： Xu Zhang Shiqi Liu boya wang Guoqing wang Haozhe Du Xuanyu wang Haidong Zhang Shu Zhao Lin wang Haijun Yu Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Key Laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China Create Energy&Benefit Future Co.Ltd. Beijing 100176China

The rapid expansion of renewable energies asks for great progress of energy-storage technologies for sustainable energy supplies,which raises the compelling demand of high-performance rechargeable batteries.To satisfy the huge demand from the coming energy-storage market,the resource and cost-effectiveness of rechargeable batteries become more and more important.Manganese(Mn)as a key transition element with advantages including high abundance,low cost,and low toxicity derives various kinds(spinels,layered oxides,polyanions,Prussian blue analogs,etc.)of high-performance Mn-based electrode materials,especially cathodes,for rechargeable batteries ranging from Li-ion batteries,Na-ion batteries,aqueous batteries,to multivalent metal-ion batteries.It is anticipated that Mn-based materials with Mn as the major transition-metal element will constitute a flourishing family of Mn-based rechargeable batteries(Mn RBs)for large-scale and differentiated energy-storage applications.On the other hand,several critical issues including Jahn-Teller effect,Mn dissolution,and O release greatly hinder the pace of Mn RBs,which require extensive material optimizations and battery/system improvements.This review aims to provide an investigation about Mn-based materials and batteries for the coming energy-storage demands,with compelling issues and challenges that must be overcome.

关键词： manganese cathode materials Mn-based rechargeable batteries energy storage

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Symmetry-breaking of LiMn6 hexatomic-ring in grain surface of Li2MnO3

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Journal of Energy Chemistry 2023年第6期81卷 110-117页

作者： Lihang wang Shu Zhao boya wang Haijun Yu Institute of Advanced Battery Materials and Devices Faculty of Materials and Manufacturing Beijing University of Technology Key Laboratory of Advanced Functional Materials Ministry of Education Beijing University of Technology

LiMn6hexatomic-rings act as functional units in Li-rich layered oxides(LLOs), which determine the capacity, voltage, and structural stability of LLOs. However, the symmetry of the LiMn6hexatomic-ring is always broken, especially in the grain surface of LLOs, which will greatly affect its electrochemical performance. Herein, the symmetry-breaking of LiMn6hexatomic-ring in the grain surface of Li2MnO3was studied, and their effect on charge compensation mechanism and structure evolution behavior was thoroughly investigated. The results show that the electrochemical activity of the symmetry-broken LiMn6hexatomic-ring is higher than that of the unbroken LiMn6, and the former is more favorable for spinelization on the grain surface. Furthermore, the exposure proportion of crystallographic planes with different symmetry-broken LiMn6hexatomic-ring has also been discussed, which can be adjusted by changing the partial pressure of oxygen. The in-depth understanding of the symmetry-breaking of LiMn6hexatomic-ring will provide more targeted strategies for designing high-performance LLOs cathodes for lithium-ion batteries.

关键词： Li-rich layered oxides LiMn6 functional unit Symmetry-breaking Surface structure Density functional theory

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Determination of growth kinetics of microorganisms linked with 1,4-dioxane degradation in a consortium based on two improved methods

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Frontiers of Environmental Science & Engineering 2022年第5期16卷 97-107页

作者： Yi Xiong boya wang Chao Zhou Huan Chen Gang Chen Youneng Tang Department of Civil and Environmental Engineering FAMU-FSU College of EngineeringFlorida State UniversityTallahasseeFL 32310USA Geosyntec Consultants Inc. Huntington BeachCA 92648USA National High Magnetic Field Laboratory TallahasseeFL 32310USA

The conventional method for determining growth kinetics of microbial consortia relies on the total biomass concentration.This may be inaccurate for substrates that are uncommon in nature and can only be degraded by a small portion of the microbial community.1,4-dioxane,an emerging contaminant,is an example of such substrates.In this work,we evaluated an improved method for determining the growth kinetics of a 1,4-dioxane-degrading microbial consortium.In the improved method,we considered only bacterial taxa whose concentration increase correlated to 1,4-dioxane concentration decrease in duplicate microcosm tests.Using PEST(Parameter Estimation),a modelindependent parameter estimator,the kinetic constants were estimated by fitting the Monod kineticsbased simulation results to the experimental data that consisted of the concentrations of 1,4-dioxane and the considered bacterial taxa.The estimated kinetic constants were evaluated by comparing the simulation results with experimental results from another set of microcosm tests.The evaluation was quantified by the sum of squared relative residual,which was four orders of magnitude lower for the improved method than the conventional method.By further dividing the considered bacterial taxa into oligotrophs and copiotrophs,the sum of squared relative residual further decreased.

关键词： Biodegradation 1,4-Dioxane Kinetics Microbial consortium 16S rRNA

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V-substituted pyrochlore-type polyantimonic acid for highly enhanced lithium-ion storage

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Chinese Chemical Letters 2023年第5期34卷 539-547页

作者： Haoyu Fang Kai Yong boya wang Kaipeng Wu Yun Zhang Hao Wu College of Materials Science and Engineering Sichuan UniversityChengdu 610064China

Pyrochlore-structured polyantimonic acid(PAA)is a potential high-capacity electrode material,but its innately poor electroconductivity(~10^(-10)S/cm)seriously impairs its electrochemical reversibility for lithium-ion storage.Herein,we report design and synthesis of a novel V-substituted PAA(PAA-V),where V^(5+)are introduced to partially replace Sb^(5+).Owing to identical valence and close ionic radius relative to Sb^(5+),the V^(5+)cation can constitute the covalent VO_6octahedra framework without changing the pyrochlore crystal structure of PAA.As a result,the V^(5+)-substitution is capable to modulate the electronic structure of PAA with significantly improved electrical conductivity(~10^(-6)S/cm for PAA-V)and meanwhile decreases the size of crystals with reduced diffusion length for Li^(+)-ions.With varying the ratio of V^(5+)-substitution,the PAA-V with optimized substitution molar ratio(18%)exhibits the best lithium-ion storage performance,delivering a long cycling life with high reversible capacity(731 m Ah/g after 1200cycles at 1 A/g)and outstanding rate capability(279 mAh/g at 15 A/g).More importantly,by pairing the PAA-V as anode and commercial LiFePO_(4)as cathode,the full cell with a limited negative/positive capacity ratio of 1.2 exhibits decent cycling stability at 1 C after 150 cycles with 85.5%capacity retention.

关键词： Lithium-ion batteries Anode materials Polyantimonic acid Element substitution Electrochemical reaction mechanism

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First‑principles computational insights into lithium battery cathode materials

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Electrochemical Energy Reviews 2022年第1期5卷 1-31页

作者： Shu Zhao boya wang Zihe Zhang Xu Zhang Shiman He Haijun Yu Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Key Laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China

Lithium-ion batteries(LIBs)are considered to be indispensable in modern society.Major advances in LIBs depend on the development of new high-performance electrode materials,which requires a fundamental understanding of their properties.First-principles calculations have become a powerful technique in developing new electrode materials for high-energy–den-sity LIBs in terms of predicting and interpreting the characteristics and behaviors of electrode materials,understanding the charge/discharge mechanisms at the atomic scale,delivering rational design strategies for electrode materials,etc.In this review,we present an overview of first-principles calculation methods and highlight their valuable role in contemporary research on LIB cathode materials.This overview focuses on three LIB cathode scenarios,which are divided by their cati-onic/anionic redox mechanisms.Then,representative examples of rational cathode design based on theoretical predictions are presented.Finally,we present a personal perspective on the current challenges and future directions of first-principles calculations in LIBs.

关键词： First-principles calculations Cathode materials Lithium-ion batteries Anionic redox Cationic redox

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Symmetry-breaking of LiMn_(6) hexatomic-ring in grain surface of Li_(2)MnO_(3)

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Journal of Energy Chemistry 2023年第6期 110-117,I0004页

作者： Lihang wang Shu Zhao boya wang Haijun Yu Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Key Laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China

LiMn_(6) hexatomic-rings act as functional units in Li-rich layered oxides(LLOs),which determine the capacity,voltage,and structural stability of LLOs.However,the symmetry of the LiMn_(6) hexatomic-ring is always broken,especially in the grain surface of LLOs,which will greatly affect its electrochemical performance.Herein,the symmetry-breaking of LiMn_(6) hexatomic-ring in the grain surface of Li_(2)MnO_(3) was studied,and their effect on charge compensation mechanism and structure evolution behavior was thoroughly investigated.The results show that the electrochemical activity of the symmetry-broken LiMn_(6) hexatomic-ring is higher than that of the unbroken LiMn_(6),and the former is more favorable for spinelization on the grain surface.Furthermore,the exposure proportion of crystallographic planes with different symmetry-broken LiMn_(6) hexatomic-ring has also been discussed,which can be adjusted by changing the partial pressure of oxygen.The in-depth understanding of the symmetry-breaking of LiMn_(6) hexatomic-ring will provide more targeted strategies for designing high-performance LLOs cathodes for lithium-ion batteries.

关键词： Li-rich layered oxides LiMn_(6)functional unit Symmetry-breaking Surface structure Density functional theory

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Construction of Electrocatalytic and Heat-Resistant Self-Supporting Electrodes for High-Performance Lithium–Sulfur Batteries

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Nano-Micro Letters 2019年第4期11卷 386-402页

作者： Xuemei Zhang Yunhong Wei boya wang Mei wang Yun Zhang Qian wang Hao Wu College of Materials Science and Engineering Sichuan UniversityChengdu 610064People’s Republic of China Department of Advanced Energy Materials Sichuan UniversityChengdu 610064People’s Republic of China

Boosting the utilization efficiency of sulfur electrodes and suppressing the“shuttle effect”of intermediate polysulfides remain the critical challenge for high-performance lithium-sulfur batteries(LSBs).However,most of reported sulfur electrodes are not competent to realize the fast conversion of polysulfides into insoluble lithium sulfides when applied with high sulfur loading,as well as to mitigate the more serious shuttle effect of polysulfides,especially when worked at an elevated temperature.Herein,we reported a unique structural engineering strategy of crafting a unique hierarchical multifunctional electrode architecture constructed by rooting MOF-derived CoS2/carbon nanoleaf arrays(CoS2-CNA)into a nitrogen-rich 3D conductive scaffold(CTNF@CoS2-CNA)for LSBs.An accelerated electrocatalytic effect and improved polysulfide redox kinetics arising from CoS2-CNA were investigated.Besides,the strong capillarity effect and chemisorption of CTNF@CoS2-CNA to polysulfides enable high loading and efficient utilization of sulfur,thus leading to high-performance LIBs performed not only at room temperature but also up to an elevated temperature(55°C).Even with the ultrahigh sulfur loading of 7.19 mg cm?2,the CTNF@CoS2-CNA/S cathode still exhibits high rate capacity at 55°C.

关键词： Metal organic framework Lithium-sulfur batteries Cobalt sulfide Heat-resistant N-doped carbon foam

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Impacts of plant secondary metabolites from conifer litter on the decomposition of Populus purdomii litter

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Journal of Forestry Research 2019年第6期30卷 2237-2245页

作者： Xiaoxi Zhang boya wang Zengwen Liu College of Life Sciences Yan’an UniversityYan’an 716000People’s Republic of China Institute of Soil and Water Conservation Northwest A&F UniversityYangling 712100People’s Republic of China College of Natural Resources and Environment Northwest A&F UniversityYangling 712100People’s Republic of China Key Laboratory of Plant Nutrition and the Agri-environment in Northwest China Ministry of AgricultureNorthwest A&F UniversityYangling 712100People’s Republic of China

A decomposition experiment of Populus purdomii litter,a commonly used afforestation species in the Qinling Mountains,China,was conducted.Water extracts of five conifer litters were used to treat P.purdomii litter and its soil.The P.purdomii litter was incubated at room temperature(20–25℃)and constant soil moisture for 6 months.During the decomposition period,the dynamics of litter mass and nutrient contents were detected to investigate the impacts of plant secondary metabolites.The results indicate that litter extracts of Pinus tabuliformis,Platycladus orientalis,Pinus armandii and Larix principisrupprechtii significantly inhibited the overall nutrient release of P.purdomii litter,while the last three types of litter extracts simultaneously inhibited its decomposition.Conversely,the litter extracts of Picea asperata significantly accelerated the overall nutrient release of P.purdomii.Generally,most of the conifer species,whose litter released terpenoids,phenolics,steroids,and aliphatic acids,will inhibit the decomposition and/or nutrient release from P.purdomii litter.Their negative effects on the decomposers and soil enzymatic activities indicates that planting diversity should be lower when mixed planted with P.purdomii.

关键词： Mixed afforestation Inhibited litter decomposition Terpenoids Phenolics Steroids Aliphatic acids

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Activating sulfur oxidation reaction via six-electron redox mesocrystal NiS2 for sulfur-based aqueous batteries

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National Science Review 2023年第6期10卷 64-74页

作者： Zhoudong Yang boya wang Yongjin Chen Wanhai Zhou Hongpeng Li Ruizheng Zhao Xinran Li Tengsheng Zhang Fanxing Bu Zaiwang Zhao Wei Li Dongliang Chao Dongyuan Zhao Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials College of Chemistry and Materials Fudan University Center for High Pressure Science and Technology Advanced Research

Sulfur-based aqueous batteries(SABs) are deemed promising candidates for safe,low-cost,and high-capacity energy storage.However,despite their high theoretical capacity,achieving high reversible value remains a great challenge due to the thermodynamic and kinetics problems of elemental sulfur.Here,the reversible six-electron redox electrochemistry is constructed by activating the sulfur oxidation reaction(SOR) process of the elaborate mesocrystal NiS2(M-NiS2).Through the unique 6e-solid-to-solid conversion mechanism,SOR efficiency can reach an unprecedented degree of ca.96.0%.The SOR efficiency is further reve aled to be closely associated with the kinetics feasibility and thermodynamic stability of the M-NiS2intermedium in the formation of elemental sulfur.Benefiting from the boosted SOR,compared with the bulk electrode, the M-NiS2electrode exhibits a high reversible capacity(1258 mAh g-1),ultrafast reaction kinetics(932 mAh g-1at 12 A g-1),and long-term cyclability(2000 cycles at 20 A g-1).As a proof of concept,a new M-NiS2‖ Zn hybrid aqueous battery exhibits an output voltage of 1.60 V and an energy density of 722.4 Wh kgcath-1,which opens a new opportunity for the development of high-energy aqueous batteries.

关键词： sulfur-based aqueous battery mesocrystal material sulfur oxidation reaction high-energy aqueous battery six-electron redox

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Conversion electrochemistry of copper selenides for robust and energetic aqueous batteries

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Carbon Energy 2023年第2期5卷 85-93页

作者： Yichun wang boya wang Jinshu Zhang Dongliang Chao Jiangfeng Ni Liang Li Jiangsu Key Laboratory of Thin Films School of Physical Science and TechnologyCenter for Energy Conversion Materials and Physics(CECMP)Soochow UniversitySuzhouJiangsuChina Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsState Key Laboratory of Molecular Engineering of PolymersSchool of Chemistry and MaterialsFudan UniversityShanghaiChina

The development of highly safe and low-cost aqueous batteries is of great significance in the background of carbon neutrality.However,the practical deployment of aqueous batteries has been plagued due to their relatively low capacity and poor cycling stability.Herein,we propose unique conversion electrochemistry of copper selenides for robust and energetic aqueous charge storage.In situ X-ray diffraction and operando Raman techniques reveal a reversible transformation from CuSe to Cu_(2)Se through the intermediates of Cu_(3)Se_(2) and Cu_(1.8)Se.Such a conversion process activates the redox carrier of Cu^(2+)ion and delivers a remarkable rate capability of 285 mAh g^(-1) at 20 A g^(-1) and electrochemical durability up to 30,000 cycles.Furthermore,Cu^(2+)and H+coinsertion chemistry is proposed to facilitate the conversion process.As a proof-of-concept,a hybrid aqueous pouch cell coupling CuSe//Zn is capable of affording maximum energy and power densities of 190 Wh kg^(-1) and 1366W kg^(-1),respectively.

关键词： aqueous battery conversion electrochemistry Cu-ion battery Se-based electrode

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