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In Situ High-performance Gel Polymer Electrolyte with Dual-reactive Cross-linking for Lithium Metal Batteries

Energy & Environmental Materials 2024年第1期7卷 51-59页

作者： Fuhe Wang Honghao Liu Yaqing Guo Qigao Han Ping Lou Long Li Jianjie Jiang Shijie Cheng Yuancheng Cao School of Materials Science and Engineering Huazhong University Huazhong University of Science and Technology Wuhan 430074China State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic Engineering Huazhong University of Science and TechnologyWuhan 430074China State Grid Huzhou Power Supply Company Huzhou 313000China Huzhou Electric Power Design Institute Company Huzhou 311404China

Lithium metal batteries have been considered as one of the most promising next-generation power-support devices due to their high specific energy and output ***,the uncontrollable side-reaction and lithium dendrite growth lead to the limited serving life and hinder the practical application of lithium metal ***,a tri-monomer copolymerized gel polymer electrolyte(TGPE)with a cross-linked reticulation structure was prepared by introducing a cross-linker(polyurethane group)into the acrylate-based in situ polymerization *** soft segment of polyurethane in TGPE enables the far migration of lithium ions,and the-NH forms hydrogen bonds in the hard segment to build a stable cross-linked *** system hinders anion migration and leads to a high Li^(+)migration number(t_(Li^(+))=0.65),which achieves uniform lithium deposition and effectively inhibits lithium dendrite *** a result,the assembled symmetric cell shows robust reversibility over 5500 h at a current density of 1 mA cm^(-2).The LFP∷TGPE∷Li cell has a capacity retention of 89.8%after cycling 800 times at a rate of *** summary,in situ polymerization of TGPE electrolytes is expected to be a candidate material for high-energy-density lithium metal batteries.

关键词： gel polymer electrolytes hydrogen bonds in situ polymerization lithium metal batteries polyurethane

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Syntheses and Crystal Structures of Two Coordination Polymers with Aromatic Dioxide as Bridge Ligands

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Chinese Journal of Structural Chemistry 2007年第2期26卷 214-218页

作者： SHI Jing-Min XU Hai-Yan ZHANG Feng-Xia WU Chang-Ju LIU Lian-Dong Department of Chemistry Shandong Normal University Jinan 250014 China

Two coordination polymers, namely, two-dimensional complex 1 {[Cu（μ- L）1.5（ClO4）2（H2O）].（H2O）0.5]n （L = pyrazine-1,4-dioxide） and one-dimensional complex 2 [Co（μ-L）Br2（H2O）2]n, have been synthesized with pyrazine-1,4-dioxide as bridging ligands, and their crystal structures were determined by X-ray crystallography. Crystal data for complex 1： monoclinic system, space group C2/c, with a = 23.310（3）, b = 12.2338（17）, c = 10.6075（15） A, β= 110.487（2）°, V = 2833.6（7） A3, Z = 8, C6H9C12CuN3O12.5, Mr = 457.60, Dc = 2.145 g/cm^3, F（000） = 1832 and μ = 1.998 mm^-1; and those for 2： monoclinic system, space group C2/c, with a = 11.012（3）, b = 7.483（2）, c = 11.451（3） A, β = 101.654（4）°, V = 924.2（4） A3, Z = 4, C4HsBr2CoN2O4, Mr = 366.87, Dc = 2.637 g/cm^3, F（000） = 700 and μ = 10.487 mm^-1. 1 shows a two-dimensional sheet structure on the ac plane through the coordination of μ-L bridging ligands with Cu（Ⅱ） ions, while 2 displays a zigzag one-dimensional chain along the c axis via the coordination of μ-L bridging ligand with Co（Ⅱ） ions. hydrogen bonds in 1 and 2 make the sheets （or chains） connect each other to form a three-dimensional structure.

关键词： Aromatic Dioxide coordination polymers hydrogen bonds

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Interplay between hydrogen Bond Network and Entangled Network in Polymers During Stretching Based on Molecular Simulations

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Chinese Journal of Polymer Science 2024年第12期42卷 2069-2080,I0014页

作者： Jian-Long Wen Yong-Qiang Ming Ao-Fei Zhang Jiang-Long Li Xiao-Yu Du Lang Shuai Yi-Jing Nie Institute of Polymer Materials School of Materials Science and EngineeringJiangsu UniversityZhenjiang212013China

Mechanical properties of polymers can be regulated by changing the numbers of hydrogen bonds and entanglement ***,the interplay between hydrogen bond network and entangled network during stretching has not been fully *** performed molecular dynamics simulations to investigate the changes of hydrogen bonds and entanglements during *** stretching causes the orientation of local segments,leading to the entanglement sliding and disentanglements at different strain ***,the number of entanglement points keeps constant at first and then decreases with increasing ***,the orientation of local segments can cause the change of chain conformation,which leads to the breakage of hydrogen ***,the number of hydrogen bonds decreases with the increase of *** results also demonstrated that the number of hydrogen bonds decreases faster during stretching in systems containing more *** systems with different hydrogen bond site contents,the initial number of entanglement nodes and its decline range during stretching increase firstly and then decrease with the increase of hydrogen bond site content.

关键词： Moleculardynamics simulations hydrogen bonds Entanglements

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Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO_(2)adsorbents

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Chinese Journal of Chemical Engineering 2023年第4期56卷 233-241页

作者： Chao Yang Zhelin Su Yeshuang Wang Huiling Fan Meisheng Liang Zhaohui Chen College of Environmental Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China State Key Laboratory of Multi-phase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

A series of ZnO/SiO_(2) adsorbents were prepared by a sol-gel method using tetraethyl orthosilicate,ethylene glycol(EG)and nitrates as *** effect of gel drying temperature on the structure and desulfurization performance of the adsorbents were investigated in *** is found that the low drying temperature led to a weak interaction among EG,Si AOH/H_(2)O and the nitrates in the gel system,which caused the oxidation of EG by NO3-and formed zinc glyoxylate complex during the gel calcination process,whereas this oxidation process also occurred at a high drying temperature during the gel drying *** formed zinc glyoxylate complex promoted the generation of monodentate carbonate on the surface of Zn O,which resulted in the inferior desulfurization performance of adsorbents despite they have smaller Zn O *** gel dried at 120°C formed the hydrogen bonds between EG and Si AOH/H_(2)O and a strong interaction between zinc oxo-clusters and NO3-was also found in the gel system,which avoided the oxidation of EG by NO3-during the preparation process and the Zn O nanoparticles with sizes of 6 nm were formed by a combustion *** adsorbent affords a highest sulfur capacity of 104.9 mg·g^(-1) in this *** addition,the gel drying temperature has a significant influence on the textural properties of the adsorbents except their surface area.

关键词： Sol-gel method Drying temperature H_(2)S removal Zinc-silica composites hydrogen bonds

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hydrogen-Bonding Crosslinked Supramolecular Polymer Materials:From Design Evolution of Side-Chain hydrogen-Bonding to Applications

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Chinese Journal of Polymer Science 2024年第11期42卷 1619-1641,I0006页

作者： Qian Zhang Zi-Yang Xu Wen-Guang Liu School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional MaterialsTianjin UniversityTianjin300350China

hydrogen bonds(H-bonds)are the most essential non-covalent interactions in nature,playing a crucial role in stabilizing the secondary structures of *** inspiration from nature,researchers have developed several multiple H-bonds crosslinked supramolecular polymer materials through the incorporation of H-bond side-chain units into the polymer chains.N-acryloyl glycinamide(NAGA)is a monomer with dual amides in the side group,which facilitates the formation of multiple dense intermolecular H-bonds within poly(N-acryloyl glycinamide)(PNAGA),thereby exhibiting diverse properties dependent on concentration and meeting various requirements across different ***,numerous attempts have been undertaken to synthesize diverse NAGA-derived units through meticulous chemical structure regulation and fabricate corresponding H-bonding crosslinked supramolecular polymer *** this,the systematic clarification of the impact of chemical structures of side moieties on intermolecular associations and material performances remains *** present review will focus on the design principle for synthesizing NAGA-derived H-bond side-chain units and provide an overview of the recent advancements in multiple H-bonds crosslinked PNAGA-derived supramolecular polymer materials,which can be categorized into three groups based on the chemical structure of H-bonds units:(1)monomers with solely cooperative H-bonds;(2)monomers with synergistic H-bonds and other physical interactions;and(3)diol chain extenders with cooperative *** significance of subtle structural variations in these NAGA-derived units,enabling the fabrication of hydrogen-bonded supramolecular polymer materials with significantly diverse performances,will be ***,the extensive applications of multiple H-bonds crosslinked supramolecular polymer materials will be elucidated.

关键词： hydrogen bonds High strength Side chain Supramolecular polymer materials

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Synergistic effects of multiple rotors and hydrogen-bond interactions lead to sensitive near-infrared viscosity probes for live-cell microscopy

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Science China Chemistry 2023年第8期66卷 2329-2338页

作者： Dongyang Li Tianruo Shen Xiaoqi Xue Weijie Chen Wenjun Tao Weijie Chi Sheng Hua Liu Ying Tan Xiaogang Liu Jun Yin National Key Laboratory of Green Pesticide International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan430079China Science Mathematics and Technology ClusterSingapore University of Technology and DesignSingapore487372Singapore State Key Laboratory of Chemical Oncogenomics Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen518055China Department of Chemistry School of ScienceHainan UniversityHaikou570228China

Changes in cellular viscosity are associated with various physiological processes and pathological *** study these cellular processes and functions,highly sensitive fluorescent probes that detect subtle changes in viscosity are urgently needed but remain *** this study,we present a series of viscosity-responsive near-infrared(NIR)fluorescent probes based on styrene-coated boron dipyrromethene(BODIPY).The probe modified with dimethylaminostyrene and piperazine at the two terminals of the BODIPY scaffold showed extremely high viscosity sensitivity values(x,around 1.54),with excellent performance for detecting viscosity below 20 c *** outstanding property is attributed to the synergistic effects of multiple rotatable bonds and hydrogen-bond ***,this probe has been successfully deployed to monitor viscosity changes in various cellular compartments(i.e.,cytoplasm)and processes(such as during autophagy).This work provides a rational molecular design strategy to construct fluorescent probes with high viscosity sensitivity for exploring cell functions.

关键词： fluorescent probe high viscosity sensitivity multiple rotors hydrogen bonds bioimaging

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Elucidating and manipulating pressure-induced water intrusion–extrusion in tunable hydrophobic Co/Zn bimetallic ZIFs:Roles of pore size and hydrogen bond

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Nano Research 2024年第1期17卷 344-353页

作者： Diyi Fang Chuanlei Liu Yu Chen Qilong Peng Kongguo Wu Yuxiang Chen Hao Jiang Yuan Wu Benxian Shen Qiumin Wu Di Wu Hui Sun International Joint Research Center of Green Energy Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China Alexandra Navrotsky Institute for Experimental Thermodynamics The Gene and Linda Voiland School of Chemical Engineering and BioengineeringMaterials Science and Engineeringand Department of ChemistryWashington State UniversityWashington 99163USA

Porous heterogeneous lyophobic systems(HLSs)find potential applications in energy restoring,dissipating,and ***,the development of controllable HLSs still lacks rational structure design of nanoporous materials matching the molecular sizes of adopted *** that,thoroughly understanding the underlying transportation mechanism in the confined nano channels is greatly *** this work,a series of Co/Zn bimetallic zeolitic imidazolate frameworks(ZIFs)with tunable structures were synthesized via regulating the Co to Zn ratios and employed to investigate the intrusion–extrusion of liquid water in confined *** characterizations confirm the heterometallic coordination in the Co/Zn-doped *** intrusion–extrusion experiments unlock the relationship between the intrusion pressure and the nanopore size and realize the evolution of the HLSs between molecular spring and *** addition,cycling tests indicate the reversible structure change of Co/Zn ZIFs encountering pressure-induced water *** combination with molecular dynamics simulations,we present that the water multimers intrude into nanopores of ZIFs in chain-like forms along with dissociation of hydrogen bonds(HBs).Water molecules in the pre-intrusion state exhibit reduced HBs in response to the increase of pressure and linear structure with 1.6–3.0 HBs on *** transition to the post-intrusion situation,the associative configuration of water tends to exhibit the tetrahedral ***,we highlight the roles of pore size and HB in synergically dominating the pressure-induced intrusion–extrusion of liquid water in hydrophobic ***,the present work can also guide the development of functional guest–host systems based on porous architectures.

关键词： heterometallic zeolitic imidazolate frameworks nanopore intrusion hydrogen bonds

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hydrogen Bond-Assisted Ultra-Stable and Fast Aqueous NH_(4)^(+)Storage

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Nano-Micro Letters 2021年第9期13卷 193-208页

作者： Xikun Zhang Maoting Xia Haoxiang Yu Junwei Zhang Zhengwei Yang Liyuan Zhang Jie Shu School of Materials Science and Chemical Engineering Ningbo UniversityNingboZhejiang 315211People’s Republic of China

Aqueous ammonium ion batteries are regarded as eco-friendly and sustainable energy storage *** applicable host for NH_(4)^(+)in aqueous solution is always in the process of *** the basis of density functional theory calcula-tions,the excellent performance of NH_(4)^(+)insertion in Prussian blue analogues(PBAs)is proposed,especially for copper hexacyanoferrate(CuHCF).In this work,we prove the outstanding cycling and rate performance of CuHCF via electrochemical analyses,delivering no capacity fading during ultra-long cycles of 3000 times and high capacity retention of 93.6%at 50 *** of main contributions to superior performance from highly reversible redox reaction and structural change is verified during the ammoniation/de-ammoniation *** importantly,we propose the NH_(4)^(+)diffusion mechanism in CuHCF based on con-tinuous formation and fracture of hydrogen bonds from a joint theoretical and experimental study,which is another essential reason for rapid charge transfer and superior NH_(4)^(+)***,a full cell by coupling CuHCF cathode and polyaniline anode is constructed to explore the practical application of *** brief,the outstanding aqueous NH_(4)^(+)storage in cubic PBAs creates a blueprint for fast and sustainable energy storage.

关键词： Aqueous ammonium ion batteries Copper hexacyanoferrate Ultra-long cycling performance Excellent rate performance hydrogen bonds

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Characterization of PolyA and PolyC mismatches by Raman spectroscopy

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Chinese Optics Letters 2008年第1期6卷 61-63页

作者：廖昱博孟耀勇雷浩东王英 Photonic Chinese Medicine Lab South China Normal University Guangzhou Institute of Geochemistry Chinese Academy of Sciences

A.C mismatches are studied by Raman spectral characterization of PolyA, PolyC, and their equimolar complex in solution of 0.14 mol/L Na^＋, pH7.0. Experimental results show that A.C mismatches occur to be A/B （mainly A） conformers, and unlike Watson-Crick base pairing, this kind of mismatches is stabilized by only one hydrogen bond involving cytosine N4H2 and adenine N7. The formation of A.C complex makes the base stacking interactions much stronger, and conformation of the backbone more ordered, which leads to obvious Raman hypochromic effect with some shifts in corresponding bands.

关键词： hydrogen bonds

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Synthesis, Crystal Structure and Photoluminescent Property of a 3D hydrogen-bonded Supramolecular Compound with Large Channels

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Chinese Journal of Structural Chemistry 2008年第4期27卷 467-470页

作者：岳呈阳江飞龙袁大强陈莲吴明燕洪茂椿 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter The Chinese Academy of Sciences

The title compound, [Pd（2,2′-bipy）2]（Haadip）2·4H2O, was synthesized via the hydrothermal reaction of PdCl2 with 5-aminodiacetic isophthalic acid （H4adip） in an acetic acid water solution. It was characterized by elemental analysis and infrared spectrum. Crystal data for C44H44N6O20Pd： monoclinic, space group P21/n, a = 11.0674（2）, b = 9.9716（2）, c= 20.5770（3）A, β = 92.7300（3）°, V = 2268.29（7）A^3, Z = 2, Mr = 1083.25, Dc = 1.586 g/cm^3, F（000） = 1112,μ = 0.499 mm^-1, 2（MoKa） = 0.71073 A, T = 293（2） K, 2θmax = 51.38°, GOOF = 1.067, R = 0.0268 and wR = 0.0710 for 3770 reflections with 1 〉 2σ（I）. X-ray diffraction studies reveal that the title compound has an interesting 3D microporous architecture via hydrogen bonds with the cations located inside the channel.

关键词： 5-aminodiacetic isophthalic acid channel hydrogen bonds palladium

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