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A Cross-linked Polyethylene with Recyclability and Mechanical Robustness Enabled by Establishment of Multiple hydrogen bonds Network via Reactive Melt Blending

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Chinese Journal of Polymer Science 2023年第7期41卷 1104-1114页

作者： Hong-Da Mao Ting-Ting Zhang Zhen-You Guo Dong-Yu Bai Jie Wang Hao Xiu Qiang Fu College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065China Chongqing University Key Laboratory of Micro/Nano Materials Engineering and Technology Chongqing University of Arts and SciencesChongqing402160China Hubei Huifu Nanomaterial Co. LTD.Yichang443007China

Physical cross-linking by hydrogen-bonds (H-bonds), providing a good combination of application properties of thermosets and processability of thermoplastics, is a potential strategy to resolve the recycling problem of traditional chemically cross-linked polyethylene. However, ureidopyrimidone (UPy), the most widely used H-bonding motif, is unfavorable for large-scale industrial application due to its poor thermal stability. In this work, H-bonds cross-linked polyethylene was successfully prepared by reactive melt blending maleic anhydride grafted polyethylene (PE-g-MAH) with 3-amino-1,2,4-triazole (ATA) to form amide triazole ring-carboxylic acid units. Triazole ring can easily generate multiple H-bonds with carboxylic acid and amide. More importantly, these units are more thermal stable than UPy due to the absence of unstable urea group of UPy. The introduction of H-bonds cross-linking leads to an obvious improvement in mechanical properties and creep resistance and a good maintain in thermal properties and recyclability. Furthermore, the reinforcement effect monotonically improves with increasing the density of H-bonds. The obtained good properties are mainly attributed to largely enhanced interchain interactions induced by H-bonds cross-linking and intrinsic reversibility of H-bonds. This work develops a novel way for the simple fabrication of H-bonds cross-linked PE with high performance through reactive melt blending.

关键词： Cross-linked polyethylene hydrogen bonds Recyclability

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Considerable molecular interactions enable robust electrochemical properties:hydrogen bonds in lithium-ion batteries

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Science China Chemistry 2023年第7期66卷 1905-1923页

作者： Dan Duan Xiaohan Cai Cong Ma Zongxi Lin Yao Wang Jianwei Nai Tiefeng Liu Jianmin Luo Yujing Liu Xinyong Tao College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China

Lithium-ion batteries(LIBs)have been in a dominant position in the new energy industry because of their excellent comprehensive performance.The performance of LIBs highly depends on the microstructures of the materials that constitute LIBs.Particularly,the relatively“weak”molecular interactions instead of the common-discussed strong chemical-bonding always affect the structures and the consequent properties of the components in LIBs.As a typical example,the hydrogen bonds,which widely exist inside LIBs,greatly improved the mechanical strength,lithium ion(Li^(+))transport rate and the intrinsic stabilities towards boosting performance of LIBs.This review starts from the interaction force between molecules,and especially summarizes the correlation between the formation of hydrogen bonds and the properties of the typical components in LIBs(cathode,anode,electrolyte,separator).In addition,how the formation of hydrogen bonds affects the performance of LIBs components is discussed.Finally,the strategies of combining hydrogen bonds with LIBs components in the future are prospected,which provide guidance for the rational design of high-performance LIBs.

关键词： hydrogen bonds lithium-ion batteries electrochemical performance

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Dilute Aqueous-Aprotic Electrolyte Towards Robust Zn-Ion Hybrid Supercapacitor with High Operation Voltage and Long Lifespan

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Nano-Micro Letters 2024年第9期16卷 1-12页

作者： Shuilin Wu Yibing Yang Mingzi Sun Tian Zhang Shaozhuan Huang Daohong Zhang Bolong Huang Pengfei Wang Wenjun Zhang Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education&Hubei Key Laboratory of Catalysis and Materials Science South-Central Minzu UniversityWuhan 430074People’s Republic of China Department of Materials Science and Engineering and Center of Super‑Diamond and Advanced FilmsCity University of Hong Kong83 Tat Chee AvenueKowloon TongHong Kong SARPeople’s Republic of China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijingPeople’s Republic of China

With the merits of the high energy density of batteries and power density of supercapacitors,the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required.However,the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan.It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors.Using'water in salt'electrolytes can effectively broaden their electrochemical windows,but this is at the expense of high cost,low ionic conductivity,and narrow temperature compatibility,compromising the electrochemical performance of the Zn-ion hybrid supercapacitors.Thus,designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary.We developed a dilute water/acetonitrile electrolyte(0.5 m Zn(CF_(3)SO_(3))_(2)+1 m LiTFSI-H_(2)O/AN)for Zn-ion hybrid supercapacitors,which simultaneously exhibited expanded electrochemical window,decent ionic conductivity,and broad temperature compatibility.In this electrolyte,the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI-anions.As a result,a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.

关键词： Zn-ion supercapacitors Zn metal anode Electrolyte engineering hydrogen bonds Solvation structures

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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 absorbing.However,the development of controllable HLSs still lacks rational structure design of nanoporous materials matching the molecular sizes of adopted liquids.Besides that,thoroughly understanding the underlying transportation mechanism in the confined nano channels is greatly challenging.In 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 nanopores.Structural characterizations confirm the heterometallic coordination in the Co/Zn-doped frameworks.Water 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 shock-absorber.In addition,cycling tests indicate the reversible structure change of Co/Zn ZIFs encountering pressure-induced water intrusion.In 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 average.After transition to the post-intrusion situation,the associative configuration of water tends to exhibit the tetrahedral structure.Herein,we highlight the roles of pore size and HB in synergically dominating the pressure-induced intrusion–extrusion of liquid water in hydrophobic nanopores.Furthermore,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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Intermolecular hydrogen-bonding as a robust tool toward significantly improving the photothermal conversion efficiency of a NIR-II squaraine dye

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Chinese Chemical Letters 2024年第4期35卷 310-315页

作者： Songtao Cai Liuying Wu Yuan Li Soham Samanta Jinying Wang Bing Liu Feihu Wu Kaitao Lai Yingchao Liu Junle Qu Zhigang Yang Center for Biomedical Photonics&Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China

The photothermal therapy(PTT) has come across as a promising noninvasive therapeutic strategy for tumor treatment. However, low photothermal conversion efficiency(PCE) and hydrophobicity may impede the therapeutic efficacy of organic photothermal agents and an efficient PTT-agent must overcome these two major challenges. In this work, we developed a new strategy to promote higher PCE wherein the intermolecular hydrogen-bonding interaction between the single dye molecule and water facilitated the transformation of the absorbed energy into the heat. A hydrophilic squaraine dye(SCy1) with the second near-infrared region(NIR-II) absorption and extremely low emission were designed to exhibit much higher PCE than that of the analogues of pentamethine-dyes(PCy1, PCy2). The presence of the ‘–O-' at middle of squaric cycle enabled the intermolecular H-bonding formation between the SCy1 and water to promote the energy dissipation channel. Moreover, the introduction of long-chain phenylsulfonate groups helped in to improve the water solubility apart from serving as an additional means of further enhancing PCE through fluorescence quenching. Therefore, SCy1 with a squaraine backbone and long-chain sulfonate moieties revealed outstanding photothermal stability and anti-aggregation activity apart from showing exceptionally high PCE(74%) in water. SCy1 demonstrated excellent therapeutic efficacy when applied in the PTT treatment of tumor-bearing mice under a laser irradiation of 915 nm.

关键词： Squaraine-based cyanine hydrogen bonds High PCE Anti-aggregation Photothermal therapy

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A Disulfide-Based Poly(ether-b-amide)Copolymer with Rapid Self-healing Ability under Moderate

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Chinese Journal of Chemistry 2024年第9期42卷 943-950页

作者： Weijan Lu ping Zhu Ying Zhao Dujin Wang Xia Dong Institute of Chemistry Chinese Academy of SciencesBeijing 100190China Schoolof Chemical Sciences University of Chinese Academy of SciencesBejing 100049China

Comprehensive Summary A disulfide-based poly(ether-b-amide)copolymer with rapid self-healing capability under moderate conditions was synthesized from 4,4’-dithiodibutyric acid(DTDBA),isophorondiamine(IPDA)and poly(tetramethylene oxide)(PTMO)based on a two-step method.The incorporation of IPDA with asymmetric structure and substantial steric hindrance not only effectively decreased the number of regular H-bonds,but also inhibited the crystallization of polyamide segments,imparting the synthesized poly(ether-b-amide)copolymer with an amorphous structural feature.Based on the coordination of segmental diffusion and recombination of disulfide bonds and hydrogen bonds,the scratches and damaged mechanical properties of PEBADS-I611 could be completely self-healed after healing at 40°C for only 11 min and 3 h,respectively.

关键词： Poly(ether-b-amide)copolymer Disulfide bonds hydrogen bonds Polycondensation Smart polymers Self-healing

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Supramolecular Bonding Competition Enabled Nanostructure Evolution and Mechanical Reinforcement

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CCS Chemistry 2024年第1期6卷 157-164页

作者： Yuting Wang Peng Meng Aidan Brock Yanan Xu Hang Meng Zixuan Liu Kan Zhang John McMurtrie Jingsan Xu School of Chemistry and Physics and Centre for Materials Science Queensland University of TechnologyBrisbaneQueensland 4000 Central Analytical Research Facility Institute for Future EnvironmentsQueensland University of TechnologyBrisbaneQueensland 4000 State Key Laboratory of Superhard Materials Department of Materials Science and Key Laboratory of Automobile MaterialsMOEJilin UniversityChangchun 130012

In this work,competition between different supramolecular interactions is investigated based on a fibrous crystal composed of hydrogen-bonded cyanuric acid(CA)and amidinothiourea(ADT).Melamine(M)is found to prevail over ADT and bond to CA due to its stronger triple H-bonding affiliation,forming hollow microtubes assembled by oriented CAM crystalline arrays,as guided by the directionality of peripheral hydrogen bonds.Furthermore,competitive interaction between hydrogen bonding and ionic/covalent bonding is demonstrated by mixing Ag+ions with the CA-ADT fibers,where sulfur atoms are abstracted from ADT molecules to produce Ag_(2)S ligaments.The in situ-formed Ag_(2)S serves as a binding glue to generate CA-ADT/Ag_(2)S composites with significantly enhanced mechanical strength compared to the pristine CA-ADT fiber pellet.

关键词： supramolecular interaction hydrogen bonds chemical bond competition hollow crystal array organic-inorganic composite

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Syntheses and Crystal Structures of Two 3D Zinc(II) Compounds Involving Coordination and hydrogen bonds

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Chinese Journal of Structural Chemistry 2006年第5期25卷 527-532页

作者： CHEN Bai-Quan HAN Lei WU Ben-Lai WU Ming-Yan HUANG You-Gui HONG Mao-Chun State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter The Chinese Academy of Sciences Fuzhou Fujian 350002 China Graduate School of the Chinese Academy of Sciences Beijing 100039 China

Two zinc（Ⅱ） compounds, [Zn（L）（H2O）2]n 1 and [Zn（4,4＇-bpy）（H2O）4]（L） 2 （H2L = trans,trans-1,3 butadiene 1,4-dicarboxylic acid）, were synthesized by hydrothermal methods and characterized by single-crystal X-ray diffraction analyses. Compound 1 crystallizes in monoclinic, space group C2/c with a=15.4970（16）, b = 5.4976（6）, c = 10.7113（12） A, β=96.298（6）°, C6H8O6Zn, Mr = 241.50, V = 907.06（17） A^3, Z = 4, D, = 1.768 g/cm^3, F（000） = 488,μ = 2.703 mm^-1, S = 1.060, the final R = 0.0256 and wR = 0.0660 for 968 observed reflections with Ⅰ 〉 2σ（Ⅰ）. Compound 2 crystallizes in triclinic, space group P1^- with a = 6.915（2）, b = 7.166（2）, c = 10.363（3） A, α = 73.250（4）, β = 84.429（4）, γ = 61.605（3）°, C16H2ON2O8Zn, Mr = 433.70, V = 432.1 （2） A^3, Z = 1, D, = 1.667 g/cm^3, F（000） = 224 and μ= 1.471 mm^-1, S = 1.118, the final R = 0.0486 and wR = 0.1077 for 1352 observed reflections with Ⅰ〉 2σ（Ⅰ）. Upon using the assembly strategy of combination of coordination polymer chains with intermolecular hydrogen bonds, three-dimensional frameworks of complexes 1 and 2 were formed.

关键词： Zn（Ⅱ） coordination polymer hydrogen bonds crystal structure

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Ab initio path-integral molecular dynamics and the quantum nature of hydrogen bonds

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Chinese Physics B 2016年第1期25卷 230-237页

作者：冯页新陈基李新征王恩哥 International Center for Quantum Materials and School of Physics Peking UniversityBeijing 100871China School of Physics Peking UniversityBeijing 100871China Collaborative Innovation Center of Quantum Matter Beijing 100871China

The hydrogen bond （HB） is an important type of intermolecular interaction, which is generally weak, ubiquitous, and essential to life on earth. The small mass of hydrogen means that many properties of HBs are quantum mechanical in nature. In recent years, because of the development of computer simulation methods and computational power, the influence of nuclear quantum effects （NQEs） on the structural and energetic properties of some hydrogen bonded systems has been intensively studied. Here, we present a review of these studies by focussing on the explanation of the principles underlying the simulation methods, i.e., the ab initio path-integral molecular dynamics. Its extension in combination with the thermodynamic integration method for the calculation of free energies will also be introduced. We use two examples to show how this influence of NQEs in realistic systems is simulated in practice.

关键词： ab initio calculations isotope molecular dynamics hydrogen bonds

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New Supramolecular Complex Assembled through hydrogen bonds. Crystal Structure of Co(PMBP-tsc)_2 ·2DMF·2H_2O

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Chinese Journal of Chemistry 2002年第3期20卷 286-291页

作者：刘浪贾殿赠乔永民郁开北 Institute of Applied Chemistry Xinjiang University Urumqi Xinjiang 830046 China Chengdu Institute of Organic Chemistry Chinese Academy of Sciences Chengdu Sichuan 610012 China

The structure of the complex [Co(PMBP-tsc)_2·2DMF·2H_2O] (PMBP-tsc =1-phenyl-3-methyl-4-benzoylpyrazol-5-one-thiosemicarbazone) has been determined by X-raycrystallography. It crystallizes in the orthorhombic system, space group Pna2_1, with latticeparameters a = 2.1170(3) nm, b = 1.2780(10) nm, c = 1.8956(2) nm, V = 4.5258(9) nm^3 and Z = 4. Thestructure shows that Co^(2+) in the complex is hexa-coordinated with a distorted octahedralcoordination sphere. The water molecules bridge the adjacent stacks through hydrogen bonds and leadto supramolecular formation with three-dimensional network structure.

关键词： cobalt(Ⅱ) compound crystal structure supramolecule hydrogen bonds

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