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Chinese Chemical Letters 2021年第2期32卷 822-825页

作者： Linsen Yang Pei Liu Congcong Zhu Yuanyuan Zhao Miaomiao Yuan Xiang-Yu Kong Liping Wen Lei Jiang Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China School of Future Technology University of Chinese Academy of ScienceBeijing 100049China The Eighth Affiliated Hospital Sun Yat-sen UniversityShenzhen 518033China

Controlling ions transport across the membrane at different pH environments is essential for the physiological process and artificial systems.Many efforts have been devoted to pH-responsive ion gating,while rarely systems can maintain the rectification in pH-changing environments.Here,a composite nanochannel system is fabricated,which shows unidirectional rectification with high performance in a wide pH range.In the system,block copolymer(BCP) and polyethylene te rephthalate(PET) are employed for the amphoteric nanochannels fabrication.Based on the composite system,a model is built for the theoretical simulation.Thereafter,rectification mapping is conducted on the system,which can provide abundant info rmation about the relations between charge distribution and ions transport prope rties.The proposed rectification mapping can definitely help to design new materials with special ion transport properties,such as high-performance membranes used in the salinity gradient power generation field.

关键词： Nanochannel Unidirectional rectification Composited membrane ion transport Rectification mapping

Correlate phonon modes with ion transport via isotope substitution

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Science China Chemistry 2023年第3期66卷 768-777页

作者： Yirong Gao Jianxing Huang Jun Cheng Shou-Hang Bo University of Michigan–Shanghai Jiao Tong University Joint Institute Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Physical Chemistry of Solid Surface iChEMCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Solid-State Battery Research Center Global Institute of Future TechnologyShanghai Jiao Tong UniversityShanghai 200240China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China

Understanding the correlations between lattice dynamics(phonons) and ion transport is important for improving the ionic conductivity of solid-state electrolytes. This understanding largely hinges on selective tuning or excitation of specific phonon modes without changing the chemical environments of atoms, which is, however, challenging to be achieved. In this work, we used ~6Li isotope substitution to selectively change the phonon properties associated with lithium, without introducing additional defects or disorders which would affect the ion transport properties. The changes in the phonon modes were then related to ion transport properties through impedance measurements and deep potential molecular dynamics simulations. Our results demonstrated that lower lithium vibration frequency leads to higher ionic conductivity and lower activation energy in the garnet solid-state electrolyte of Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12). We furthermore quantified the effect of lithium-related phonons on the migration entropy and attempt frequency, which would be difficult to be achieved otherwise. Our work suggests an effective isotope substitution method to decouple the effect of phonon modes to ion transport from that of other complex structural factors. The obtained insights can contribute to innovative understanding of ion transport in solids and strategies to optimize the ionic conductivity of solid-state electrolytes.

关键词： solid-state electrolytes phonon modes ion transport isotope substitution lattice dynamics

支柱策略增强离子传输和结构稳定性的KVPO4F用于超稳定的钾离子电池正极

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Science Bulletin 2023年第6期68卷 593-602,M0004页

作者：赵敬秦棪阳李龙吴虎贾鑫朱小龙赵洪洋苏亚琼丁书江 School of Chemistry University Engineering Research Center of Shaanxi ProvinceEngineering Research Center of Energy Storage Materials and Devices(Ministry of Education)Xi’an Jiaotong UniversityXi’an 710049China

近年来,由于丰富的钾资源储量和低廉的价格,钾离子电池在大规模储能领域表现出极大的应用前景.开发具有高安全性、高能量密度、低成本、长寿命的正极材料是推动钾离子电池实用化的关键.KVPO4F(KVPF)因其工作电压高、能量密度高、热稳定... 详细信息

近年来,由于丰富的钾资源储量和低廉的价格,钾离子电池在大规模储能领域表现出极大的应用前景.开发具有高安全性、高能量密度、低成本、长寿命的正极材料是推动钾离子电池实用化的关键.KVPO4F(KVPF)因其工作电压高、能量密度高、热稳定性好,被认为是一种很有前途的钾离子电池正极材料.然而,由于大半径的钾离子反复脱出/嵌入导致较慢的动力学和大的体积变化,从而影响材料循环稳定性.本文通过将大半径铯离子引入KVPF结构中的“支柱”策略,可有效提高材料的离子传导特性,并改善充放电过程中材料的结构稳定性,从而实现铯掺杂的KVPF正极优异的储钾性能.同时,高循环稳定性的KVPF//石墨全电池也展示了其在钾离子电池中巨大的实际应用潜力.

关键词： ion transport Structural stability KVPO4F Cs-substitution Stable potassium-ion batteries

Photothermal regulated ion transport in nanofluidics:From fundamental principles to practical applications

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Nano Research 2023年第7期16卷 10061-10071页

作者： Pei Liu Lei Jiang Liping Wen Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450052China Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China

Light regulated ion transport across membranes is central to nature.Based on this,artificial nanofluidics with light driven ion transport behaviors has been developed for both fundamental study and practical applications.Here,we focus on recent progress in photothermal controlled ion transport systems and review the corresponding construction strategies in diverse photothermal nanofluidics with various dimensions and structures.We systematically emphasize the three underlying working principles including temperature gradient,water evaporation induced ion transport blockage,and evaporation gradient.On the basis of these fundamental research,photothermal regulated ion transport has been mainly introduced into ionic devices,desalination,and energy conversion.Furthermore,we provide some perspectives for the current challenges and future developments of this promising research field.We believe that this review could encourage further understanding and open the minds to develop new advances in this fertile research field.

关键词： nanofluidics ion transport photothermal conversion ion pump energy conversion

Fibrous Separator with Surface Modification and Micro-Nano Fibers Lamination Enabling Fast ion transport for Lithium-ion Batteries

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Chinese Journal of Polymer Science 2023年第2期41卷 222-232页

作者： Yi-Ge Zhou Li Fan He-Qin Li Yu-Jia Cui Shu-Fa Yu Zhen-Zhen Wei Yan Zhao College of Textile and Clothing Engineering National Engineering Laboratory for Modern SilkSoochow UniversitySuzhou215123China Jiangsu Yingyang Nonwoven Machinery Co. LTD.Changshu215500China

Appropriate materials collaborated with reasonable structure can significantly increase the separator performance for lithium-ion batteries.In this work,taking the advantages of microfibrous and nanofibrous membranes and compensating for their defects,we developed a composited separator(GOPPH)with excellent overall performance by first wetting-modifying the polyethylene terephthalate microfibers and then laminating a polyvinylidene fluoride-hexafluoropropylene nanofiber layer.Such a combination not only offers the GOPPH separator,from the perspective of structure,with high porosity and hierarchical structure in terms of fiber diameter and pore size,but also provides satisfactory features including wettability,mechanical strength and thermal shutdown function that benefit from the selected materials.Meanwhile,as determined by experimental and theoretical approaches,the obtained GOPPH separator exhibits considerably enhanced lithium ion transport ability with a high lithium ion transference number and transport rate,which thereby endowing the cell with superior cycling stability with a capacity retention of 93%after 200 cycles at 1 C.Therefore,considering battery safety and performance,the GOPPH fibrous membrane could be a promising separator candidate for lithium-ion batteries.

关键词： Fibrous separator Surface modification Micro-nano fiber lamination ion transport Lithium-ion batteries

1D/2D composite subnanometer channels for ion transport:The role of confined water

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Nano Research 2023年第8期16卷 10913-10921页

作者： Yuhao Li Xiaorui Jin Xinhai Yan Xinyu Ai Xin Yang Zi-Jian Zheng Kun Huang Gaofeng Zhao Yongan Yang Meiling Wu Kai-Ge Zhou Institute of Molecular Plus Department of ChemistryTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Ministry of Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer MaterialsHubei UniversityWuhan 430062China School of Chemical Engineering and Analytical Science National Graphene InstituteUniversity of ManchesterManchesterM139PLUK School of Civil Engineering Tianjin UniversityTianjin 300072China

As a mass transport media,water is an alternative of organic solvent applied in rechargeable batteries,due to its unique properties,including fast ionic migration,easy-processibility,economic/environmental friendliness,and flame retardancy.However,due to the high activity of water molecules in aqueous electrolytes,the corrosion of metal anode,side reactions,and inferior metal electrodeposition behavior leads to unstable cycling performance,poor Coulombic efficiency(CE),and early-staged failure of batteries.Despite several attempts to regulate the activity of water,migration of ions is sacrificed,due to the limited methods to control the water states.Herein,we developed a subnanoscale confinement strategy based on a nacre-like structure to modulate the activity of water in the solid electrolytes.By tuning the ratio between the two-dimensional(2D)vermiculite and one-dimensional(1D)cellulose nanofibers(CNFs),the capillary size in the 1D/2D structure is altered to achieve a fast Zn^(2+)transport.Our dielectric relaxation and molecular dynamics studies indicate that the enhanced Zn^(2+)conductivity is attributed to the fast water relaxation in the precisely defined 1D/2D capillary.Taking advantage of the regulated activity of the confined water in 2D capillary,the composite vermiculite membrane can suppress the corrosion and side reactions between Zn electrode and water molecular,endowing a reversible Zn^(2+)stripping/plating behavior and a stable cycling performance for 900 h.Based on our confinement strategy to control the water states by 1D/2D structures,this work will open an avenue toward aqueous energy storage devices with excellent reversibility,high safety,and long-term stability.

关键词： ion transport subnanometer channels confined water aqueous electrolyte limited side reactions

Full-chain enhanced ion transport toward stable lithium metal anodes

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Journal of Energy Chemistry 2023年第4期79卷 390-397页

作者： Yuliang Gao Fahong Qiao Nan Li Jingyuan You Yong Yang Jun Wang Chao Shen Ting Jin Xi Li Keyu Xie State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi’an 710072ShaanxiChina School of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina Department of Applied Physics The Hong Kong Polytechnic UniversityHong Kong 999077China Shanghai Key Lab of Advanced High-temperature Materials and Precision Forming Shanghai Jiao Tong UniversityShanghai 200240China

The dendrite growth that results from the slow electrode process kinetics prevents the lithium(Li) metal anode from being used in practical applications. Here, full-chain enhanced ion transport for stabilizing Li metal anodes is proposed. Experimental and theoretical studies confirm that full-chain enhanced ion transport(electrocrystallization, mass transport in the electrolyte and diffusion in solid electrolyte interphase) under magnetoelectrochemistry contributes to a homogeneous, dense, and dendrite-free morphology. Specifically, the enhanced electrocrystallization behavior promotes the Li nucleation;the enhanced mass transport in the electrolyte alleviates the ion concentration gradient at the electrode surface, which helps to inhibit dendrite growth;and the enhanced diffusion in the solid electrolyte interphase further homogenizes the Li deposition behavior, obtaining regular and uniform Li particles.Consequently, the Li metal anode has exceptional cycling stability in both symmetric and full cells,and the pouch cell performs long cycles(170 cycles) in practice evaluation. This work advances fundamental knowledge of the magneto-dendrite effect and offers a new perspective on stabilizing metal anodes.

关键词： Lithium metal anodes ion transport Pouch cell Lithium dendrites Magnetic field

Light-driven directional ion transport for enhanced osmotic energy harvesting

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National Science Review 2021年第8期8卷 178-185页

作者： Kai Xiao Paolo Giusto Fengxiang Chen Ruotian Chen Tobias Heil Shaowen Cao Lu Chen Fengtao Fan Lei Jiang Max Planck Institute of Colloids and Interfaces Department of Colloid Chemistry Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education School of ChemistryBeihang University State Key Laboratory of New Textile Materials and Advanced Processing Technologies Wuhan Textile University State Key Laboratory of Catalysis 2011-iChEMDalian National Laboratory for Clean Energy (DNL)Dalian Institute of Chemical Physics(DICP)Chinese Academy of Sciences State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology

Light-driven ion(proton) transport is a crucial process both for photosynthesis of green plants and solar energy harvesting of some archaea. Here, we describe use of a TiO2/C3N4semiconductor heterojunction nanotube membrane to realize similar light-driven directional ion transport performance to that of biological systems. This heterojunction system can be fabricated by two simple deposition steps. Under unilateral illumination, the TiO2/C3N4heterojunction nanotube membrane can generate a photocurrent of about 9 μA/cm~2, corresponding to a pumping stream of ～5500 ions per second per nanotube. By changing the position of TiO2and C3N4, a reverse equivalent ionic current can also be realized. Directional transport of photogenerated electrons and holes results in a transmembrane potential, which is the basis of the light-driven ion transport phenomenon. As a proof of concept, we also show that this system can be used for enhanced osmotic energy generation. The artificial light-driven ion transport system proposed here offers a further step forward on the roadmap for development of ionic photoelectric conversion and integration into other applications, for example water desalination.

关键词： ion pump ion transport nanofluidic porous membrane carbon nitride

Light-Driven ion transport in Nanofluidic Devices:Photochemical,Photoelectric,and Photothermal Effects

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CCS Chemistry 2022年第1期4卷 54-65页

作者： Kai Xiao Oliver G.Schmidt Department of Biomedical Engineering Southern University of Science and Technology(SUSTech)Shenzhen 518055 Center for Materials Architectures and Integration of Nanomembranes(MAIN)Chemnitz University of TechnologyChemnitz 09126 Institute for Integrative Nanosciences Leibniz IFW DresdenDresden 01069

Light-driven ion transport in nanofluidic devices is a phenomenon where ions move unidirectionally by consuming optical energy,either from low concentration to high concentration or vice versa.The light-driven unidirectional ion transport offers intriguing application potential in desalination and ion separation,osmosis energy harvesting,and ionic machines benefiting from the remote noncontact light stimulus.Here,we review recent progress in nanofluidic-based light-driven ion transport systems and emphasize similarities and differences in the three underlying working principles based on photochemical,photoelectric,and photothermal effects.The current challenges and future developments of light-driven ion transport in nanofluidic devices are discussed.We believed that this article encourages further innovation in this exciting and emerging research field.

关键词： nanofluidic artificial ion pump nanochannel ion transport photoelectric effect

内源性电场调控抗菌离子传输以提高植入材料抗菌性能

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Science China Materials 2020年第9期63卷 1831-1841页

作者：翟锦霞周亚红王珍高范磊肖才榕王晓岚李扬帆周正难罗义安黎昌昊戚穗坚谭帼馨周蕾于鹏宁成云 School of Materials Science and Engineering South China University of TechnologyGuangzhou 510640China School of Biomedical Sciences and Engineering National Engineering Research Center for Tissue Restoration and ReconstructionKey Laboratory of Biomedical Engineering of Guangdong ProvinceKey Laboratory of Biomedical Materials and Engineering of the Ministry of EducationInnovation Center for Tissue Restoration and Reconstruction.South China University of TechnologyGuangzhou 510006China CAS Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China School of Food Science and Engineering South China University of TechnologyGuangzhou 510640China

组织植入材料相关感染是临床治疗的一大顽疾,基于抗菌离子释放系统的抗菌植入材料是经济高效的抗生素治疗替代手段.但过量释放的抗菌离子在杀灭细菌的同时也可能引起生物毒性.因此,如何提高释放离子的抗菌效率是急需解决的根本问题.本... 详细信息

组织植入材料相关感染是临床治疗的一大顽疾,基于抗菌离子释放系统的抗菌植入材料是经济高效的抗生素治疗替代手段.但过量释放的抗菌离子在杀灭细菌的同时也可能引起生物毒性.因此,如何提高释放离子的抗菌效率是急需解决的根本问题.本研究设计了一种负载低剂量抗菌离子的铁电植入材料,该植入材料表面电势可在不改变自身成份的前提下通过外源电场极化进行调控.研究发现上述铁电植入材料释放的抗菌离子将在植入材料自身与带电细菌之间形成的内源性电场作用下定向输运到达细菌.研究结果表明在12 h内,高表面电势植入材料向细菌输运的离子量达到低表面电势植入材料输运量的2.4倍,从而使抗菌效率从65%提高到100%,并展现出较低的细胞毒性.本研究表明植入材料与生命体间的内源性电场在介导物质传输中发挥重要作用,为设计高性能抗菌生物材料提供了一个新的视角.

关键词： bacterial infection endogenous electric field ion transport ferroelectric implant