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Covalent Organic Framework with 3D Ordered Channel and Multi-Functional Groups Endows Zn Anode with Superior Stability

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Nano-Micro Letters 2024年第4期16卷 350-363页

作者： Bin Li Pengchao Ruan Xieyu Xu Zhangxing He Xinyan Zhu Liang Pan Ziyu Peng Yangyang Liu Peng Zhou bingan lu Lei Dai Jiang Zhou School of Chemical Engineering North China University of Science and TechnologyTangshan 063009People’s Republic of China School of Materials Science and Engineering Central South UniversityChangsha 410083People’s Republic of China State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China Hunan Provincial Key Defense Laboratory of High Temperature Wear‑Resisting Materials and Preparation Technology Hunan University of Science and TechnologyXiangtan 411201People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction,corrosion,and passivation,etc.Herein,an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups(COF-S-F)is developed on Zn metal(Zn@COF-S-F)as the artificial solid electrolyte interface(SEI).Sulfonic acid group(-SO_(3)H)in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions,and the three-dimensional channel with fluoride group(-F)can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects,endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions.Consequently,Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage(50.5 m V)at the current density of 1.5 m A cm^(-2).Zn@COF-S-F|Mn O_(2)cell delivers the discharge specific capacity of 206.8 m Ah g^(-1)at the current density of 1.2 A g^(-1)after 800 cycles with high-capacity retention(87.9%).Enlightening,building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.

关键词： Aqueous Zn ion batteries Covalent organic framework Interfacial modification Zn ion flux regulation Desolvation effect

Reversible Oxygen-Rich Functional Groups Grafted 3D Honeycomb-Like Carbon Anode for Super-Long Potassium Ion Batteries

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Nano-Micro Letters 2022年第9期14卷 132-146页

作者： Na Cheng Wang Zhou Jilei Liu Zhigang Liu bingan lu School of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082People’s Republic of China School of Materials Science and Engineering Hunan UniversityChangsha 410082People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Studies have found that oxygen-rich-containing functional groups in carbon-based materials can be used as active sites for the storage performance of K^(+),but the basic storage mechanism is still unclear.Herein,we construct and optimize 3D honeycomb-like carbon grafted with plentiful COOH/C=O functional groups(OFGC)as anodes for potassium ion batteries.The OFGC electrode with steady structure and rich functional groups can effectively contribute to the capacity enhancement and the formation of stable solid electrolyte interphase(SEI)film,achieving a high reversible capacity of 230 mAh g^(-1) at 3000 mA g^(-1) after 10,000 cycles(almost no capacity decay)and an ultra-long cycle time over 18 months at 100 mA g^(-1).The study results revealed the reversible storage mechanism between K^(+)and COOH/C=O functional groups by forming C-O-K compounds.Meanwhile,the in situ electrochemical impedance spectroscopy proved the highly reversible and rapid de/intercalation kinetics of K+in the OFGC electrode,and the growth process of SEI films.In particular,the full cells assembled by Prussian blue cathode exhibit a high energy density of 113 Wh kg^(-1) after 800 cycles(calculated by the total mass of anode and cathode),and get the light-emitting diodes lamp and ear thermometer running.

关键词： Honeycomb-like Super-long Carbon anode Potassium-ion batteries

Building ultra-stable K–Te battery by molecular regulation

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Journal of Energy Chemistry 2022年第6期31卷 100-107,I0004页

作者： Jiawan Zhou Dongyang Shen Xinzhi Yu bingan lu School of Physics and Electronics Hunan UniversityChangsha 410082HunanChina College of Science Hunan University of Technology and BusinessChangsha 410205HunanChina

Tellurium (Te) is an ideal electrode for potassium ion batteries (PIBs) owing to its excellent electronic conductivity and high volumetric capacity.However,the Te electrode is prone to capacity fading as the shuttle effect.To address this challenge,we propose molecular regulated Se–Te solid solutions on N-doped porous carbon as the PIBs electrode.After optimizing the Se content in Se–Te solid solutions,the resultant SeTe_(6.8) on N-doped porous carbon (SeTe_(6.8)@C) delivered a capacity of over 400 mAh g^(-1) with a flat plateau of 1.0 V at 500 m A g^(-1).It also achieved a superiorly long cycle life,running for more than 1600 cycles (over 7 months with 0.015%degeneration per cycle) at 100 mA g^(-1) and excellent rate performance (179.9 mAh g^(-1) at 10000 mA g^(-1)).This remarkable electrochemical energy storage of the Te electorde likely arises from suppression of the shuttle effect after doping the Te with strongly electronegative Se atoms (forming K_(s)Te_(3) which is not easily soluble in electrolyte).This study presents a fresh approach for designing and developing ultra-stable Te-based electrodes for PIBs and beyond.

关键词： Se–Te solid solutions Ultra-long cycle life Potassium tellurium battery Molecular regulation

Trimming the Degrees of Freedom via a K^(+) Flux Rectifier for Safe and Long‑Life Potassium‑Ion Batteries

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纳微快报:英文版 2023年第11期15卷 157-171页

作者： Xianhui Yi Apparao MRao Jiang Zhou bingan lu School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China Department of Physics and Astronomy Clemson Nanomaterials InstituteClemson UniversityClemsonSC 29634USA School of Materials Science and Engineering Central South UniversityChangsha 410083People’s Republic of China State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body Hunan UniversityChangsha 410082People’s Republic of China

High degrees of freedom(DOF)for K^(+)movement in the electrolytes is desirable,because the resulting high ionic conductivity helps improve potassium-ion batteries,yet requiring support from highly free and flammable organic solvent molecules,seriously affecting battery safety.Here,we develop a K^(+)flux rectifier to trim K ion’s DOF to 1 and improve electrochemical properties.Although the ionic conductivity is compromised in the K^(+)flux rectifier,the overall electrochemical performance of PIBs was improved.An oxidation stability improvement from 4.0 to 5.9 V was realized,and the formation of dendrites and the dissolution of organic cathodes were inhibited.Consequently,the K||K cells continuously cycled over 3,700 h;K||Cu cells operated stably over 800 cycles with the Coulombic efficiency exceeding 99%;and K||graphite cells exhibited high-capacity retention over 74.7%after 1,500 cycles.Moreover,the 3,4,9,10-perylenetetracarboxylic diimide organic cathodes operated for more than 2,100 cycles and reached year-scale-cycling time.We fabricated a 2.18 Ah pouch cell with no significant capacity fading observed after 100 cycles.

关键词： Electrolytes Degrees of freedom Safe Coulombic efficiency Potassium-ion batteries

Interfacial Engineering Strategy for High-Performance Zn Metal Anodes

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Nano-Micro Letters 2022年第1期14卷 121-151页

作者： Bin Li Xiaotan Zhang Tingting Wang Zhangxing He bingan lu Shuquan Liang Jiang Zhou School of Chemical Engineering North China University of Science and TechnologyTangshan 063009People’s Republic of China School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South UniversityChangsha 410083People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Due to their high safety and low cost,rechargeable aqueous Zn-ion batteries(RAZIBs)have been receiving increased attention and are expected to be the next generation of energy storage systems.However,metal Zn anodes exhibit a limited-service life and inferior reversibility owing to the issues of Zn dendrites and side reactions,which severely hinder the further development of RAZIBs.Researchers have attempted to design high-performance Zn anodes by interfacial engineering,including surface modification and the addition of electrolyte additives,to stabilize Zn anodes.The purpose is to achieve uniform Zn nucleation and flat Zn deposition by regulating the deposition behavior of Zn ions,which effectively improves the cycling stability of the Zn anode.This review comprehensively summarizes the reaction mechanisms of interfacial modification for inhibiting the growth of Zn dendrites and the occurrence of side reactions.In addition,the research progress of interfacial engineering strategies for RAZIBs is summarized and classified.Finally,prospects and suggestions are provided for the design of highly reversible Zn anodes.

关键词： Interfacial engineering Zn anode Dendrites Side reactions Aqueous zinc-ion batteries

Tailored ZnF_(2)/ZnS-rich interphase for reversible aqueous Zn batteries

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Nano Research 2023年第4期16卷 4996-5005页

作者： Junmin Ge Yaoyang Zhang Zhengkun Xie Huabin Xie Weihua Chen bingan lu College of Chemistry&Green Catalysis Center Zhengzhou UniversityZhengzhou 450001China School of Physics and Electronics Hunan UniversityChangsha 410082China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

The urgent need for highly safe and sustainable large-scale energy storage systems for residential buildings has led to research into aqueous zinc ion batteries.However,when zinc is used in aqueous zinc ion batteries,it suffers from severe irreversibility due to its low Coulombic efficiency,dendrite growth,and side reactions.To address these challenges,we take advantage of organic cation to induce trifluoromethanesulfonate decomposition to build zinc fluoride/zinc sulfide-rich solid electrolyte interphase(SEI)that not only can adapt to a high areal capacity of deposition/stripping disturbance but also adjust zinc ion deposition path to eliminate dendrite.As a result,the unique interface can promote the Zn battery to achieve excellent electrochemical performance:high levels of plating/stripping Coulombic efficiency(99.8%),stability life(6,600 h),and cumulative capacity(66,000 mAh·cm^(−2))at 68%zinc utilization(20 mAh·cm^(−2)).More importantly,the SEI significantly enhances the cyclability of full battery under limited Zn,lean electrolyte,and high areal capacity cathode conditions.

关键词： aqueous zinc batteries ZnF_(2)/ZnS-rich interphase reversibility metal anode utilization interfacial chemistry

All-Solid-State Thin-Film Lithium-Sulfur Batteries

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Nano-Micro Letters 2023年第5期15卷 326-338页

作者： Renming Deng Bingyuan Ke Yonghui Xie Shoulin Cheng Congcong Zhang Hong Zhang bingan lu Xinghui Wang College of Physics and Information Engineering Institute of Micro-Nano Devices and Solar CellsFuzhou UniversityFuzhou 350108People’s Republic of China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108FujianPeople’s Republic of China Jiangsu Collaborative Innovation Center of Photovoltaic Science and Engineering Changzhou 213000People’s Republic of China School of Physics and Electronics Hunan UniversityChangsha 410082People’s Republic of China

Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Things microdevice.However,the volatility in high vacuum and intrinsic sluggish kinetics of S hinder researchers from empirically integrating it into allsolid-state thin-film batteries,leading to inexperience in fabricating all-solid-state thin-film Li-S batteries(TFLSBs).Herein,for the first time,TFLSBs have been successfully constructed by stacking vertical graphene nanosheets-Li2S(VGsLi2S)composite thin-film cathode,lithium-phosphorous-oxynitride(LiPON)thin-film solid electrolyte,and Li metal anode.Fundamentally eliminating Lipolysulfide shuttle effect and maintaining a stable VGs-Li2S/LiPON interface upon prolonged cycles have been well identified by employing the solid-state Li-S system with an“unlimited Li”reservoir,which exhibits excellent longterm cycling stability with a capacity retention of 81%for 3,000 cycles,and an exceptional high temperature tolerance up to 60℃.More impressively,VGs-Li2S-based TFLSBs with evaporated-Li thin-film anode also demonstrate outstanding cycling performance over 500 cycles with a high Coulombic efficiency of 99.71%.Collectively,this study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries.

关键词： All-solid-state thin-film batteries Li-S batteries Vertical graphene nanosheets Lithium phosphorous oxynitride Li2S

Integrated ‘all-in-one’ strategy to stabilize zinc anodes for high-performance zinc-ion batteries

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National Science Review 2022年第3期9卷 63-71页

作者： Canpeng Li Xuesong Xie Hui Liu Pinji Wang Canbin Deng bingan lu Jiang Zhou Shuquan Liang School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan ProvinceCentral South University School of Physics and Electronics Hunan University

Many optimization strategies have been employed to stabilize zinc anodes of zinc-ion batteries(ZIBs).Although these commonly used strategies can improve anode performance, they simultaneously induce specific issues. In this study, through the combination of structural design, interface modification, and electrolyte optimization, an ’all-in-one’(AIO) electrode was developed. Compared to the three-dimensional(3D) anode in routine liquid electrolytes, the new AIO electrode can greatly suppress gas evolution and the occurrence of side reactions induced by active water molecules, while retaining the merits of a 3D anode. Moreover, the integrated AIO strategy achieves a sufficient electrode/electrolyte interface contact area, so that the electrode can promote electron/ion transfer, and ensure a fast and complete redox reaction. As a result, it achieves excellent shelving-restoring ability(60 hours, four times)and 1200 cycles of long-term stability without apparent polarization. When paired with two common cathode materials used in ZIBs(α-MnO2and NH4V4O10), full batteries with the AIO electrode demonstrate high capacity and good stability. The strategy of the ’all-in-one’ architectural design is enlightened to solve the issues of zinc anodes in advanced Zn-based batteries.

关键词： all-in-one electrode hydrogen-free electrode/electrolyte interface Zn-based batteries

Biocompatible zinc battery with programmable electro-cross-linked electrolyte

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National Science Review 2023年第3期10卷 203-211页

作者： Xuesong Xie Jingjing Li Zhengyue Xing bingan lu Shuquan Liang Jiang Zhou School of Materials Science and Engineering Central South University Department of Plastic Surgery Xiangya Hospital of Central South University School of Physics and Electronics Hunan University

Aqueous zinc batteries(ZBs) attract increasing attention for potential applications in modern wearable and implantable devices due to their safety and stability.However,challenges associated with biosafety designs and the intrinsic electrochemistry of ZBs emerge when moving to practice,especially for biomedical devices.Here,we propose a green and programmable electro-cross-linking strategy to in situ prepare a multi-layer hierarchical Zn-alginate polymer electrolyte(Zn-Alg) via the superionic binds between the carboxylate groups and Zn2+.Consequently,the Zn-Alg electrolyte provides high reversibility of 99.6 5 %Coulombic efficiency(CE),>500 h of long-time stability and high bio compatibility(no damage to gastric and duodenal mucosa) in the body.A wire-shaped Zn/Zn-Alg/α-MnO2full battery affords 95% capacity retention after 100 cycles at 1 A g-1and good flexibility.The new strategy has three prominent advantages over the conventional methods:(ⅰ) the cross-linking process for the synthesis of electrolytes avoids the introduction of any chemical reagents or initiators;(ⅱ) a highly reversible Zn battery is easily provided from a micrometer to large scales through automatic programmable functions;and(ⅲ) high biocompatibility is capable of implanted and bio-integrated devices to ensure body safety.

关键词： polymer electrolyte green and programmable electro-cross-linking biocompatible zinc battery