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Constructing Donor–Acceptor‑Linked COFs Electrolytes to Regulate Electron Density and Accelerate the Li^(+)Migration in Quasi‑Solid‑State Battery

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Nano-Micro Letters 2025年第1期17卷 456-471页

作者： genfu zhao Hang Ma Conghui Zhang Yongxin Yang Shuyuan Yu Haiye Zhu Yongjiang Sun Hong Guo School of Materials and Energy International Joint Research Center for Advanced Energy Materials of Yunnan ProvinceYunnan UniversityKunming 650091People’s Republic of China Yunnan Yuntianhua Co. LtdR&D CenterKunming 650228People’s Republic of China Southwest United Graduate School Kunming 650091People’s Republic of China

Regulation the electronic density of solid-state electrolyte by donor–acceptor(D–A)system can achieve highly-selective Li^(+)transportation and conduction in solid-state Li metal *** study reports a high-performance solid-state electrolyte thorough D–A-linked covalent organic frameworks(COFs)based on intramolecular charge transfer *** other reported COFbased solid-state electrolyte,the developed concept with D–A-linked COFs not only achieves electronic modulation to promote highly-selective Li^(+)migration and inhibit Li dendrite,but also offers a crucial opportunity to understand the role of electronic density in solid-state Li metal *** introduced strong electronegativity F-based ligand in COF electrolyte results in highlyselective Li^(+)(transference number 0.83),high ionic conductivity(6.7×10^(-4)S cm^(−1)),excellent cyclic ability(1000 h)in Li metal symmetric cell and high-capacity retention in Li/LiFePO_(4)cell(90.8%for 300 cycles at 5C)than substituted C-and N-based *** is ascribed to outstanding D–A interaction between donor porphyrin and acceptor F atoms,which effectively expedites electron transferring from porphyrin to F-based ligand and enhances Li^(+)***,we anticipate that this work creates insight into the strategy for accelerating Li^(+)conduction in high-performance solid-state Li metal batteries through D–A system.

关键词： Electronic modulation engineering Donor-acceptor-linked covalent organic frameworks Quasi-solid-state Li metal battery

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Interfacial engineering of perfluoroalkyl functionalized covalent organic framework achieved ultra-long cycled and dendrite-free lithium anodes

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Nano Research 2023年第7期16卷 9289-9298页

作者： Yongxin Yang Conghui Zhang Zhiyuan Mei Yongjiang Sun Qi An Qi Jing genfu zhao Hong Guo International Joint Research Center for Advanced Energy Materials of Yunnan Province Yunnan Key Laboratory of Carbon Neutrality and Green Low-carbon TechnologiesSchool of Materials and EnergyYunnan UniversityKunming 650091China

The finite lithium-ion utilization,short cycling life,and lower capacity retention caused by irreversible dendrite growth become the maximum dilemma in lithium metal batteries’(LMBs’)***,a perfluoroalkyl-functionalized covalent organic framework(COF-F6)equipped with high stability and supernal proton conduction is introduced as an artificial solid electrolyte interface to stable the lithium metal *** from the strong electron-withdrawing effect of perfluoroalkyl,Li^(+)will be freed more by the competition of electronegative fluorine(F)and bis(trifluoromethanesulphonyl)imide anion(TFSI^(-)).The dissociation of LiTFSI and process of Li^(+)desolvation are easier to *** addition,high electronegative fluorine can also regulate local electron-cloud density to induce the fast immigration of Li^(+).All the above roles contribute to improving the Li^(+)transfer number(0.7)and achieving the goal of inhibiting Li *** a result,the perfluoroalkyl COF-F6 modified LMB presents outstanding cycling *** symmetric batteries accomplish an overlong life-span of more than 5000 h with a lower hysteresis voltage(11 mV)at 5 mA·cm^(-2).Also,no dendrites are observed when using an in-situ optical microscope to learn the process of Li ***,this dendrite-free protection tactic holds broad prospects for the practical application of Li metal anodes.

关键词： perfluoroalkyl-functionalized covalent organic framework(COF-F6) artificial solid electrolyte interface strong electronwithdrawing effect dendrite-free lithium metal anode

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Understanding a Single-Li-Ion COF Conductor for Being Dendrite Free in a Li-Organic Battery

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Research 2023年第1期2022卷 209-218页

作者： Yongjiang Sun genfu zhao Yao Fu Yongxin Yang Conghui Zhang Qi An Hong Guo School of Materials and Energy Yunnan UniversityNo.2Green Lake North RoadKunming 650091China

In addition to improving ion conductivity and the transference number,single-Li-ion conductors(SLCs)also enable the elimination of interfacial side reactions and concentration difference ***,the SLCs can achieve high performance in solid-state batteries with Li metal as anode and organic molecule as *** organic frameworks(COFs)are leading candidates for constructing SLCs because of the excellent 1D channels and accurate chemical-modification ***,various contents of lithium-sulfonated covalently anchored COFs(denoted as LiO,S-COF1 and LiO,S-COF2)are controllably synthesized as *** to the directional ion channels,high Li contents,and single-ion frameworks,LiO,SCOF2 shows exceptional Li-ion conductivity of 5.47×10^(-5)***^(-1),high transference number of 0.93,and low activation energy of 0.15eV at room *** preeminent Li-ion-transported properties of LiO_(3)S-F2 permit stable Li+plating/stripping in a symmetric lithium metal battery,effectively impeding the Li dendrite growth in a liquid ***,the designed quasi-solid-state cell(organic anthraquinone(AQ)as cathode,Li metal as anode,and LiO_(3)S-COF2 as electrolyte)shows high-capacity retention and rate ***,LiO_(3)S-COF2 implies a potential value restraining the dissolution of small organic molecules and Li dendrite growth.

关键词： lithium Battery restrain

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COF-based single Li^(+)solid electrolyte accelerates the ion diffusionandrestrains dendritegrowthin quasi-solid-state organic batteries

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Carbon Energy 2023年第2期5卷 171-183页

作者： genfu zhao Zhiyuan Mei Lingyan Duan Qi An Yongxin Yang Conghui Zhang Xiaoping Tan Hong Guo School of Materials and Energy Yunnan UniversityKunmingYunnanChina College of Chemistry and Chemical Engineering Yangtze Normal UniversityFulingChongqingChina

A solid-state electrolyte(SSE),which is a solid ionic conductor and electroninsulating material,is known to play a crucial role in adapting a lithium metal anode to a high-capacity cathode in a solid-state *** the various SSEs,the single Li-ion conductor has advantages in terms of enhancing the ion conductivity,eliminating interfacial side reactions,and broadening the electrochemical *** organic frameworks(COFs)are optimal platforms for achieving single Li-ion conduction behavior because of wellordered one-dimensional channels and precise chemical modification ***,we study in depth three types of Li-carboxylate COFs(denoted LiOOC-COFn,n=1,2,and 3)as single Li-ion conducting *** from well-ordered directional ion channels,the single Li-ion conductor LiOOC-COF3 shows an exceptional ion conductivity of 1.36×10^(-5) S cm^(-1) at room temperature and a high transference number of ***,it shows excellent electrochemical performance with long-term cycling,high-capacity output,and no dendrites in the quasi-solid-state organic battery,with the organic small molecule cyclohexanehexone(C_(6)O_(6))as the cathode and the Li metal as the anode,and enables effectively avoiding dissolution of the organic electrode by the liquid electrolyte.

关键词： covalent organic frameworks quasi-solid-state organic battery single Li-ion conductor solid-state electrolyte

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Understanding Dual-Polar Group Functionalized COFs for Accelerating Li-Ion Transport and Dendrite-Free Deposition in Lithium Metal Anodes

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Energy & Environmental Materials 2023年第2期6卷 293-302页

作者： Qi An Hong-en Wang genfu zhao Shimin Wang Lufu Xu Han Wang Yao Fu Hong Guo School of Materials and Energy Yunnan UniversityNo.2Green Lake North RoadKunming 650091China College of Physics and Electronics Information Yunnan Key Laboratory of Optoelectronic Information TechnologyYunnan Normal UniversityKunming 650500China

Lithium metal batteries(LMBs)have attracted wide attentions because of their high theoretical specific capacity and low electrochemical ***,the growth of lithium dendrites seriously affects the practical application of ***,the lithium-philic carbonyl and carboxy dualgroup-modified covalent organic framework(COF-COOH)is designed to coat the polypropylene(PP)separator(COF-COOH@PP separator),realizing the regulation of ion transport and uniform lithium *** plentiful and negative charge sites in the COF-COOH can suppress the diffusion of the freely movable lithium salt anion by the electrostatic *** functional theory(DFT)calculations demonstrate that the COF-COOH possesses the function of anchoring anion and ***,the Li^(+)transference number(0.7),ion conductivity(0.64 mS cm^(-1)),and desolvating of Li^(+)are obviously improved by using the COF-COOH@PP *** modified Li-Li symmetric battery delivers stable cycle for more than 1000 h and lower voltage hysteresis(0.02 V).This dendrite-free deposition strategy holds great promise for practical application of Li metal anodes.

关键词： covalent organic frameworks dendrite-free functionalized separator lithiophilicity groups

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Oxygen vacancies with localized electrons direct a functionalized separator toward dendrite-free and high loading LiFePO_(4)for lithium metal batteries

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Journal of Energy Chemistry 2022年第12期75卷 38-45,I0002页

作者： Qi An Qing Liu Shimin Wang Lixiang Liu Han Wang Yongjiang Sun Lingyan Duan genfu zhao Hong Guo School of Materials and Energy Yunnan UniversityNo.2Green Lake North RoadKunming 650091YunnanChina Institute for Integrative Nanosciences Leibniz IFW DresdenHelmholtzstraße 2001069 DresdenGermany

The pursuit of high energy density has promoted the development of high-performance lithium metal batteries(LMBs).However,the underestimated but non-negligible dendrites of Li anode have been observed to shorten battery ***,a composite separator(TiO_(2-x)@PP),in which TiO_(2)with electron-localized oxygen vacancies(TiO_(2-x))is coated on a commercial PP separator,is fabricated to homogenize lithium ion transport and stabilize the lithium anode *** the utilization of TiO_(2-x)@PP separators,the symmetric lithium metal battery displays enhanced cycle stability over 800 h under a high current density of 8 m A cm^(-2).Moreover,the LMBs assembled with high-loading LiFePO_(4)(9.24 mg cm^(-2))deliver a stable cycling performance over 900 cycles at a rate of 0.5 *** theoretical studies based on density functional theory(DFT)further unveil the *** favorable TiO_(2-x)is beneficial for facilitating fast Li+migration and impeding anions *** addressing the Li dendrite issues,the use of TiO_(2-x)@PP separator potentially provides a facile and attractive strategy for designing well-performing LMBs,which are expected to meet the application requirements of rechargeable batteries.

关键词： Oxygen vacancy Ionic transport regulation Dendrite-free Localized electrons High loading

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Recycling valuable cobalt from spent lithium ion batteries for controllably designing a novel sea-urchin-like cobalt nitride-graphene hybrid catalyst: Towards efficient overall water splitting

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Journal of Energy Chemistry 2021年第11期30卷 440-450,I0010页

作者： Tingting Liu Sheng Cai genfu zhao Zhihui Gao Shuming Liu Huani Li Lijuan Chen Mian Li Xiaofei Yang Hong Guo School of Materials Science and Engineering Green Energy Key Laboratory of All–Solid Ion Battery in Yunnan Province UniversityYunnan UniversityKunming 650091YunnanChina National and Local Joint Engineering Laboratory for Lithium–ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093YunnanChina Department of Mechanical and Materials Engineering Western University1151 Richmond StLondonOntario N6A 3K7Canada

Along with the continuous consumption in lithium-ion batteries (LIBs), the price of cobalt is inevitably going up in recent years. Therefore, recycling valuable Co element from spent devices, and boosting its service efficiency are becoming two indispensable approaches to promote the utilization of Co in various energy conversion/storage devices. Herein, we realize the recovery of Co from spent LIBs and synthesize a three–dimensional (3D) sea-urchin-like cobalt nitride composite material (labeled as CoN-Gr-2), which is used as a bi-functional catalyst for water splitting. Benefiting from the intrinsic high conductivity, larger surface area and unique 3D sea–urchin–like architecture, CoN-Gr-2 shows an excellent electron transfer efficiency, highly exposed active sites as well as the superior mass transport capacity. The CoN-Gr-2 catalyst exhibits low overpotentials of 128.9 mV and 280 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which are comparable to the commercial 20 wt% Pt/C and RuO_(2) catalysts. Moreover, when adopting CoN-Gr-2 as both anode and cathode materials for overall water splitting (in 1.0 M KOH electrolyte), the assembled cell achieves a current density of 10 mA cm^(−2) at 1.61 V, which almost close to that of Pt/C||RuO_(2) benchmark (1.60 V), demonstrating its superior water-splitting efficiency. Meanwhile, the CoN catalysts exhibit strong chemical interaction with the Gr support, suppressing the aggregation of CoN catalysts and maintains their high activity during HER and OER reactions. So, the cell exhibits a high current retention of 97.3% after 40 h. This work successfully develops an industrial chain from recycling Co wastes in spent energy devices to controllably designing 3D sea-urchin-like CoN-Gr with high water splitting efficiency. Therefore, it could further promote the efficient utilization of valuable Co element in various energy devices.

关键词： Recycling valuable Co element Three-dimensional(3D)sea-urchin-like CoN-Gr Highly exposed active sites Water splitting

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高速三维边界层稳定性问题的数值方法

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空气动力学学报 1999年第3期17卷 262-270页

作者：袁湘江赵耕夫天津大学力学系天津300072

本文把四阶精度紧致差分格式用于求解超声速、高超声速三维边界层稳定性问题。提出了适用于求解高速边界层特征值问题的Ｃｈｅｂｙｓｈｅｖ多项式配置点方法，并将各种数值方法进行了比较。数值结果表明上述两种方法是求解高速三维边... 详细信息

本文把四阶精度紧致差分格式用于求解超声速、高超声速三维边界层稳定性问题。提出了适用于求解高速边界层特征值问题的Ｃｈｅｂｙｓｈｅｖ多项式配置点方法，并将各种数值方法进行了比较。数值结果表明上述两种方法是求解高速三维边界层稳定性问题的有效数值方法。

关键词：可压缩边界层稳定性数值方法高速三维

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二维sp^(2)碳连接共价有机框架作为无枝晶锂金属电池的人工SEI膜

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Science China Materials 2023年第7期66卷 2591-2600页

作者：张从辉杨永欣孙勇疆段玲艳梅至远安琪荆淇赵根福郭洪 International Joint Research Center for Advanced Energy Materials of Yunnan Province Yunnan Key Laboratory of Carbon Neutrality and Green Low-carbon TechnologiesSchool of Materials and EnergyYunnan UniversityKunming 650091China

锂金属负极(LMA)具有前所未有的理论比容量和超低的氧化还原电位,因此锂金属电池(LMBs)得到了广泛的研究.然而,不可控的锂枝晶生长和易碎的固体电解质界面相(SEI)严重阻碍了LMBs的实际商业应用.本文制备了二维sp^(2)碳连接的共价有机框... 详细信息

锂金属负极(LMA)具有前所未有的理论比容量和超低的氧化还原电位,因此锂金属电池(LMBs)得到了广泛的研究.然而,不可控的锂枝晶生长和易碎的固体电解质界面相(SEI)严重阻碍了LMBs的实际商业应用.本文制备了二维sp^(2)碳连接的共价有机框架sp^(2)c-COF,并在LMA表面构建了人工SEI膜,以抑制锂枝晶的形成,并调节界面稳定性.sp^(2)c-COF被设计成沿x和y方向全π共轭的高导电性的结构,从而起到降低界面阻抗、促进Li^(+)通量均匀分布的作用.因此,sp^(2)c-COF改性的对称电池Li^(+)迁移数高达0.85,并且在5mA cm^(-2)电流密度下具有较长的循环寿命(4000 h)和极低的过电位(10 mV).此外还利用原位光学显微镜研究了锂沉积行为,结果表明sp^(2)c-COF能显著提高LMA的界面稳定性.该策略对抑制锂枝晶的形成具有重要的应用价值,可促进COF人工SEI膜的发展.

关键词： covalent organic frameworks Li metal anode artificial SEI film lithium dendrites

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Superconductivity in LaPd2Bi2 with CaBe2Ge2-type structure

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Science China(Physics,Mechanics & Astronomy) 2018年第12期61卷 63-66页

作者： QingGe Mu BoJin Pan BinBin Ruan Tong Liu Kang zhao Lei Shan genfu Chen ZhiAn Ren Institute of Physics and Beijing National Laboratory for Condensed Matter Physics Chinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Collaborative Innovation Center of Quantum Matter Beijing 100190China

Since the discovery of superconductivity in LaFeAsO1-xFx, the high-Tc iron-based superconductors have been extensively studied from both experimental and theoretical viewpoints [1-8].However,the mechanism of the unconventional superconductivity is still to be *** address such issues,numerous 3d,4d,5d transition metal pnietide,silicide,germanide,chalcogenide materials crystalizing in the similar crystal structure with iron pnictide/ selenide suoerconductors were studied [9-24].

关键词： Superconductivity LaPd2Bi2 CaBe2Ge2-type structure

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