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A solubility limited pyrene-4,5,9,10-tetraone-based covalent organic framework for high-performance aqueous zinc-organic batteries

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Nano Research 2024年第6期17卷 5095-5103页

作者： Min Cheng Shibing Zheng Tianjiang Sun Diantao Li Weijia Zhang Zhengtai Zha Qiong Sun Jing Tian Kai Zhang zhanliang tao Frontiers Science Center for New Organic Matter State Key Laboratory of Advanced Chemical Power SourcesKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Renewable Energy Conversion and Storage CentreNankai UniversityTianjin 300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Pyrene-4,5,9,10-tetraone(PTO),with a high theoretical capacity of 408 mAh·g^(−1),is a promising candidate for rechargeable aqueous zinc-ion batteries(RAZIBs),but its zincated products during discharge process suffer from high solubility in electrolytes.Herein,aβ-ketoenamine-linked two-dimensional(2D)covalent organic framework(COF)based on a 2,7-diaminopyrene-4,5,9,10-tetraone(4KT-BD)monomer and a 2,4,6-trihydroxy-benzene-1,3,5-tricarbaldehyde(Tp)node(4KT-Tp-COF)is synthesized to address the above issue.The well-designed 4KT-Tp-COF displays low solubility in 3 M Zn(CF3SO3)2 owing to the favorableπ-πstacking as well as extended structure.Besides,the ingenious structural design of the active molecule and the long-range ordered nano-channels alter the intramolecular electron distribution,which facilitates the ionic diffusion.Consequently,the 4KT-Tp-COF cathode exhibits a stable capacity of 181 mAh·g^(−1)at 0.2 A·g^(−1),superior rate capability of 139 mAh·g^(−1)at 20 A·g^(−1),and a long lifetime of 1000 cycles without capacity loss at 30 A·g^(−1).Even at a low temperature of−20°C,the electrode also performs an ultralong cycling life of 9000 cycles with a capacity of 106 mAh·g^(−1)at 5 A·g^(−1).The comprehensive characterizations of ex-situ analyses together with the theoretical calculations validate that the groups of C=O can contribute highly accessible redox-active sites for Zn^(2+)storage.The ultra-stable 4KT-Tp-COF cathode provides important insights for designing robust organic electrodes for sustainable and large-scale electrochemical energy storage.

关键词： pyrene-4,5,9,10-tetraone solubility limited covalent organic framework zinc batteries

Molecular Engineering Design for High-Performance Aqueous Zinc-Organic Battery

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Nano-Micro Letters 2023年第3期15卷 98-111页

作者： Tianjiang Sun Weijia Zhang Qingshun Nian zhanliang tao Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryHaihe Laboratory of Sustainable Chemical TransformationsRenewable Energy Conversion and Storage CenterNankai UniversityTianjin 300071People’s Republic of China CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and EngineeringHefei National Laboratory for Physical Science at the MicroscaleUniversity of Science and Technology of China HefeiHefei 230026AnhuiPeople’s Republic of China

Novel small sulfur heterocyclic quinones(6a,16adihydrobenzo[b]naphtho[2′,3′:5,6][1,4]dithiino[2,3-i]thianthrene-5,7,9,14,16,18-hexaone(4S6Q)and benzo[b]naphtho[2′,3′:5,6][1,4]dithiino[2,3-i]thianthrene-5,9,14,18-tetraone(4S4Q))are developed by molecule structural design method and as cathode for aqueous zincorganic batteries.The conjugated thioether(–S–)bonds as connected units not only improve the conductivity of compounds but also inhibit their dissolution by both extendedπ-conjugated plane and constructed flexible molecular skeleton.Hence,the Zn//4S6Q and Zn//4S4Q batteries exhibit satisfactory electrochemical performance based on 3.5 mol L-1(M)Zn(ClO4)2electrolyte.For instance,the Zn//4S6Q battery obtains 240 and 208.6 mAh g^(-1)of discharge capacity at 150 mA g^(-1)and 30 A g^(-1),respectively.The excellent rate capability is ascribed to the fast reaction kinetics.This system displays a superlong life of 20,000 cycles with no capacity fading at 3 A g^(-1).Additionally,the H+-storage mechanism of the 4S6Q compound is demonstrated by ex situ analyses and density functional theory calculations.Impressively,the battery can normally work at-60℃benefiting from the anti-freezing electrolyte and maintain a high discharge capacity of 201.7 mAh g^(-1),which is 86.2%of discharge capacity at 25℃.The cutting-edge electrochemical performances of these novel compounds make them alternative electrode materials for Zn-organic batteries.

关键词： Aqueous Zn-organic battery Small sulfur heterocyclic quinones Conjugated thioether skeleton Superlong cycling life H+-involved mechanism -60℃

Hollow tubular conjugated organic polymer for lithium batteries

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Nano Research 2023年第2期16卷 2474-2479页

作者： Weijia Zhang Shibing Zheng tao Ma Tianjiang Sun zhanliang tao Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Renewable Energy Conversion and Storage CentreCollege of ChemistryNankai UniversityHaihe Laboratory of Sustainable Chemical TransformationsTianjin 300071China

Polymerization is a valid strategy to solve the dissolution issue of organic electrode materials in aprotic electrolytes.However,conventional polymers usually with amorphous structures and morphology’s influence on electrochemistry have rarely been studied.Herein,a hollow tubular poly phenyl pyrene-4,5,9,10-tetraone(T-PPh-PTO)organic cathode material was designed and synthesized based on the concentration-gradient of the precursor(PTO-Br2)and asymmetrical internal diffusion during the reaction.The unique hollow structure endowed T-PPh-PTO with a short Li+diffusion path accompanied by a high diffusion Li+coefficient(D≈10−8 cm^(2)·s^(−1)).Thus,T-PPh-PTO presented a capacitance-dominated redox pseudocapacitance action with an outstanding rate performance(173 mAh·g^(−1)at 2 A·g^(−1))and high cycle stability(capacity retention ratio is 91.7%after 2,000 cycles).Our study leads to further developments in designing unique organic structures for energy storage.

关键词： conjugated organic polymer hollow tubular structure lithium batteries ionic migration

Alloxazine as anode material for high-performance aqueous ammonium-ion battery

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Nano Research 2022年第3期15卷 2047-2051页

作者： Yuan Ma Tianjiang Sun Qingshun Nian Shibing Zheng tao Ma Qiaoran Wang Haihui Du zhanliang tao Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Renewable Energy Conversion and Storage CenterCollege of ChemistryNankai UniversityTianjin 300071China Hefei National Laboratory for Physical Science at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Aqueous ammonium-ion battery(AAIB)has attracted much attention due to its low cost,safety,and environmental friendliness,but its electrode materials have many limitations.Here,alloxazine(ALO)is introduced as the anode for the AAIB.With its pseudocapacitive effect and fast diffusion kinetics of NH4+,ALO anode shows excellent rate performance with a specific capacity of 120 mAh/g at 40 C(10 A/g).The full battery is further fabricated by ALO anode and Prussian white analogs cathode.Its specific capacity can reach 110 mAh/g and it can work up to 10,000 cycles with no obvious capacity fading at 20 C(5 A/g).In addition,the system delivers a high energy density of 122.5 Wh/kg and a power density of 5,055 W/kg.This work broadens the application prospect of the AAIB.

关键词： aqueous ammonium-ion battery alloxazine anode material pseudocapacitive effect

Synergistic Effect of Cation and Anion for Low-Temperature Aqueous Zinc-Ion Battery

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Nano-Micro Letters 2021年第12期13卷 301-310页

作者： Tianjiang Sun Shibing Zheng Haihui Du zhanliang tao Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Renewable Energy Conversion and Storage CenterCollege of ChemistryNankai UniversityTianjin 300071People’s Republic of China

Although aqueous zinc-ion batteries have gained great development due to their many merits,the frozen aqueous electrolyte hinders their practical application at low temperature conditions.Here,the synergistic e ect of cation and anion to break the hydrogen-bonds network of original water molecules is demonstrated by multi-perspective characterization.Then,an aqueous-salt hydrates deep eutectic solvent of 3.5 M Mg(ClO_(4))_(2)+1 M Zn(ClO_(4))_(2)is proposed and displays an ultralow freezing point of-121℃.A high ionic conductivity of 1.41 mS cm-1 and low viscosity of 22.9 mPa s at-70℃ imply a fast ions transport behavior of this electrolyte.With the benefits of the low-temperature electrolyte,the fabricated Zn||Pyrene-4,5,9,10-tetraone(PTO)and Zn||Phenazine(PNZ)batteries exhibit satisfactory low-temperature performance.For example,Zn||PTO battery shows a high discharge capacity of 101.5 mAh g^(-1)at 0.5 C(200 mA g^(-1))and 71 mAh g^(-1)at 3C(1.2 A g^(-1))when the temperature drops to-70℃.This work provides an unique view to design anti-freezing aqueous electrolyte.

关键词： Low-temperature aqueous zinc-ion battery 3.5M Mg(ClO_4)_(2)+1M Zn(ClO_4)_(2)electrolyte Synergistic effect Pyrene-4 5 9 10-tetraone Phenazine

Recent progress and strategies toward high performance zinc-organic batteries

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Journal of Energy Chemistry 2021年第12期30卷 87-112,I0003页

作者： Shibing Zheng Qiaoran Wang Yunpeng Hou Lin Li zhanliang tao Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Renewable Energy Conversion and Storage Center.College of ChemistryNankai UniversityTianjin 300071China

Energy sustainable development has stimulated the pursuit of an eco-friendly energy storage system.Carbon peak and neutrality targets oriented energy storage development will guide the way of further studies on batteries system.However,conventional batteries system(lead-acid batteries,lithium-ion batteries)based on ungreen transition metal oxide,flammable electrolytes or hazardous metals cannot keep pace with the development of society sooner or later.Thus,vast explorations on the advanced rechargeable battery systems were conducted.Compared with other battery systems,zinc ion battery systems with inherent safety,low cost were widely investigated.Especially,the zinc organic batteries based on the eco-efficiency organic cathodes were promising alternative advanced batteries for future energy storage systems.Therefore,various organics and different electrochemistry mechanisms were explored in the zinc batteries system.Herein,a timely review on elaborate analysis about functional groups,fundamentals,progress accompanied by the discussion on the four core issues:voltage,capacity,rate performance,cycle life was presented.Specifically,aiming at these issues,three levels of solution strategies:materials design concepts,morphology structure optimization and electrolyte environment were summarized and proposed for the development and innovation of zinc organic batteries.

关键词： Organic materials Zinc batteries Optimization strategies

A novel PMA/PEG-based composite polymer electrolyte for all-solid-state sodium ion batteries

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Nano Research 2018年第12期11卷 6244-6251页

作者： Xuejing Zhang Xingchao Wang Shuang Liu zhanliang tao Jun Chen Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Key Laboratory of Energy Materials Chembtry Ministry of EducationKey Laboratory of Advanced Functional MaterialsAutonomous RegionInstitute of Applied ChemistryXinjiang UniversityUrumqi 830046China

In recent years, development of all-solid-state batteries has become a promising approach to improve the safety of batteries. Herein, we report the preparation of a new composite polymer electrolyte (CPE) for use in all-solid-state sodium ion batteries. The CPE comprising of poly(methacrylate) (PMA), poly(ethylene glycol) (PEG), α-Al2O3 with acidic surface sites, and NaClO4 exhibited high ionic conductivity (1.46 × 10-4 S·cm-1 at 70 °C), wide electrochemical stability window (4.5 V vs. Na+/Na), and good mechanical strength. With the introduction of the prepared CPE and Na3V2(PO4)3, the final all-solid-state sodium ion batteries showed good rate and cycle performance, with a high reversible capacity of 85 mAh·g-1 when operated at 0.5 C (1 C = 118 mA·g–1) and 94.1% capacity retention rate after 350 cycles at 70 °C. Our work provides a novel solid electrolyte for the development of all-solid-state sodium ion batteries.

关键词： solid-state composite polymer electrolyte poly(ethylene glycol) α -Al 2 O 3 sodium ion batteries

Understanding electrode materials of rechargeable lithium batteries via DFT calculations

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Progress in Natural Science:Materials International 2013年第3期23卷 256-272页

作者： Tianran Zhang Daixin Li zhanliang tao Jun Chen Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai University

Rechargeable lithium batteries have achieved a rapid advancement and commercialization in the past decade owing to their high capacity and high power density.Different functional materials have been put forward progressively,and each possesses distinguishing structural features and electrochemical properties.In virtue of density functional theory(DFT) calculations,we can start from a specific structure to get a deep comprehension and accurate prediction of material properties and reaction mechanisms.In this paper,we review the main progresses obtained by DFT calculations in the electrode materials of rechargeable lithium batteries,aiming at a better understanding of the common electrode materials and gaining insights into the battery performance.The applications of DFT calculations involve in the following points of crystal structure modeling and stability investigations of delithiated and lithiated phases,average lithium intercalation voltage,prediction of charge distributions and band structures,and kinetic studies of lithium ion diffusion processes,which can provide atomic understanding of the capacity,reaction mechanism,rate capacity,and cycling ability.The results obtained from DFT are valuable to reveal the relationship between the structure and the properties,promoting the design of new electrode materials.

关键词： Lithium ion batteries Density functional method Electrode

Hydrothermal synthesis of spindle-like Li_2FeSiO_4-C composite as cathode materials for lithium-ion batteries

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Journal of Energy Chemistry 2014年第3期23卷 274-281页

作者： Haiyan Gao Zhe Hu Kai Zhang Fangyi Cheng zhanliang tao Jun Chen Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryCollaborative Innovation Center of Chemical Science and EngineeringNankai University

In this paper,we report on the preparation of Li2FeSiO4,sintered Li2FeSiO4,and Li2FeSiO4-C composite with spindle-like morphologies and their application as cathode materials of lithium-ion batteries.Spindle-like Li2FeSi04 was synthesized by a facile hydrothermal method with（NH4）2Fe（SO4）2 as the iron source.The spindle-like Li2FeSiO4 was sintered at 600 ℃ for 6 h in Ar atmosphere.Li2FeSiO4-C composite was obtained by the hydrothermal treatment of spindle-like Li2FeSiO4 in glucose solution at 190 ℃ for 3 h.Electrochemical measurements show that after carbon coating,the electrode performances such as discharge capacity and high-rate capability are greatly enhanced.In particular.Li2FeSiO4-C with carbon content of 7.21 wt%delivers the discharge capacities of 160.9 mAh·g-1 at room temperature and 213 mAh·g-1 at45℃（0.1 C）,revealing the potential application in lithium-ion batteries.

关键词： Li2FeSiO4-C composite spindle like hydrothermal synthesis cathode material lithium-ion battery