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Dynamic Sulfur-Rich polymers from Elemental Sulfur and Epoxides

Chinese Journal of polymer Science 2024年第10期42卷 1479-1487页

作者： Ke-Xiang Chen Chen-Hui Cui Zhen Li Ting Xu Hao-Qing Teng Zhi-Yuan He Yin-Zhou Guo Xiao-Qing Ming Zhi-Shen Ge Yan-Feng Zhang Tie-Jun Wang School of chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education Xi'an Jiaotong University state key lab for Strength and Vibration of Mechanical Structures Department of Engineering Mechanics Xi'an Jiaotong University

Sulfur-containing dynamic polymers had attracted significant attention due to their unique chemical structures with high *** sulfur, an inexpensive industrial waste product, to synthesize dynamic polysulfide polymers through reverse vulcanization has been a notable approach. However, this method required high temperatures and resulted in the release of unpleasant oders. In this study, we presented a robust method for the preparation of sulfur-rich polymers with dynamic polysulfide bonds from elemental sulfur and inexpensive epoxide monomers via a one-pot strategy at the mild room temperature. Different types of polysulfide molecules and polymers were synthesized by reacting various epoxide compounds with sulfur, along with the investigation of their structures and dynamic behaviors. It was noteworthy that the obatined polymers prepared from m-(2,3-epoxypropoxy)-N,N-bis(2,3-epoxypropyl)aniline and elemental sulfur exhibit multiple dynamic behaviors, including polysulfide metathesis and polysulfide-thiol exchange, enabling their rapid stress relaxation, self-healing, reprocessing and degradable properties of the cross-linked polymer. More importantly, the hydroxyl groups at the side chains from epoxide ring opening exhibited potential transesterification. This work provided a facile strategy for designing dynamic sulfur-rich polymers via a mild synthesis route.

关键词： Dynamic covalent bond Dynamic polymer Elemental sulfur Sulfur-containing polymer

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AI for organic and polymer synthesis

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Science China chemistry 2024年第8期67卷 2461-2496页

作者： Xin Hong Qi Yang Kuangbiao Liao Jianfeng Pei Mao Chen Fanyang Mo Hua Lu Wen-Bin Zhang Haisen Zhou Jiaxiao Chen Lebin Su Shuo-Qing Zhang Siyuan Liu Xu Huang Yi-Zhou Sun Yuxiang Wang Zexi Zhang Zhunzhun Yu Sanzhong Luo Xue-Feng Fu Shu-Li You Center of chemistry for Frontier Technologies Department of ChemistryZhejiang UniversityHangzhou 310027China Center of Basic Molecular Science Department of ChemistryTsinghua UniversityBeijing 100084China Guangzhou National laboratory Guangzhou 510005China Center for Quantitative Biology Academy for Advanced Interdisciplinary StudiesPeking UniversityBeijing 100871China state key laboratory of Molecular Engineering of polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China School of Materials Science and Engineering Peking UniversityBeijing 100871China Beijing National laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China AI for Science(AI4S)-Preferred Program Shenzhen Graduate SchoolPeking UniversityShenzhen 518055China state key laboratory of Chemical Biology Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China Department of Chemical Sciences National Natural Science Foundation of ChinaBeijing 100085China state key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Recent years have witnessed the transformative impact from the integration of artificial intelligence with organic and polymer synthesis. This synergy offers innovative and intelligent solutions to a range of classic problems in synthetic chemistry. These exciting advancements include the prediction of molecular property, multi-step retrosynthetic pathway planning, elucidation of the structure-performance relationship of single-step transformation, establishment of the quantitative linkage between polymer structures and their functions, design and optimization of polymerization process, prediction of the structure and sequence of biological macromolecules, as well as automated and intelligent synthesis platforms. Chemists can now explore synthetic chemistry with unprecedented precision and efficiency, creating novel reactions, catalysts, and polymer materials under the datadriven paradigm. Despite these thrilling developments, the field of artificial intelligence(AI) synthetic chemistry is still in its infancy, facing challenges and limitations in terms of data openness, model interpretability, as well as software and hardware support. This review aims to provide an overview of the current progress, key challenges, and future development suggestions in the interdisciplinary field between AI and synthetic chemistry. It is hoped that this overview will offer readers a comprehensive understanding of this emerging field, inspiring and promoting further scientific research and development.

关键词： organic synthesis polymer synthesis machine learning prediction chemical database automated synthesis

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A DNA Force Circuit for Exploring Protein-Protein Interactions at the Single-Molecule Level

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Chinese Journal of chemistry 2024年第13期42卷 1456-1464页

作者： Kangkang Ma Luoan Xiong Zhuofei Wang Xin Hu Lihua Qu Xuetong Zhao Yao Li Zhongbo Yu state key laboratory of Medicinal Chemical Biology Frontiers Science Center for Cell Responsesand College of PharmacyNankai University38 Tongyan RoadTianjin 300350China School of physics and key laboratory of Functional polymer Materials of Ministry of Education Nankai Universityand Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300071China

Protein-protein interactions(PPls)play a crucial role in drug discovery and disease ***,the development of effective drugs targeting PPls remains challenging due to limited methodologies for probing their spatiotemporal ***,we propose a single-molecule approach using a unique force circuit to investigate Ppl dynamics and anisotropy under mechanical *** conventional techniques,this approach enables the manipulation and real-time monitoring of individual proteins at specific amino acids with defined geometry,offering insights into molecular mechanisms at the single-molecule *** DNA force circuit was constructed using click chemistry conjugation methods and genetic code expansion techniques,facilitating orthogonal conjugation between proteins and nucleic *** SET domain of the MLL1 protein and the tail of histone H3 were used as a model system to demonstrate the application of the DNA force *** the use of atomic force microscopy and magnetic tweezers,optimized assembly procedures were *** DNA force circuit provides an exceptional platform for studying the anisotropy of PPis and holds promise for advancing drug discovery research targeted at PPIs.

关键词： Single-molecule studies Protein-protein interactions Click chemistry Genetic code expansion Molecular dynamics

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Carbon dots-enhanced pH-responsive lubricating hydrogel based on reversible dynamic covalent bondings

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Chinese Chemical Letters 2024年第5期35卷 232-237页

作者： Jianye Kang Xinyu Yang Xuhao Yang Jiahui Sun Yuhang Liu Shutao Wang Wenlong Song state key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China CAS key laboratory of Bio-inspired Materials and Interfacial Science CAS Center for Excellence in NanoscienceTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Due to the various pH liquid environment in nature,the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface ***,the applied liquid environment will lead to poor mechanical property and weaken the pH-responsive *** this work,a carbon dotsenhanced pH-responsive lubricating hydrogel is developed by combining a pH-responsive section of dynamic PVA-borax network into a PAAm covalent polymer *** formed hydrogel presents a partial gel-sol transition under controlled pH *** low pH environments(<6.0),the formed lubricating layer originated from dynamic disassembly of PVA-borax hydrogel,and brings the lubricating properties on the hydrogel ***,the mechanical strength and lubrication properties are well promoted by introducing the carbon dots into the hydrogel,the blue sol layer can be observed more visually under the fluorescence *** pH-response also exhibits well *** prepared hydrogel broadens the idea for designing pH-responsive soft materials for soft lubricating actuator or robot.

关键词： pH-responsive Carbon dots Dynamic covalent bonding Lubrication

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Frequency-modulated continuous-wave multiplexed gas sensing based on optical frequency comb calibration

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CHINESE physics B 2024年第9期33卷 152-163页

作者： Jia, Linhua Qu, Xinghua Zhang, Fumin Tianjin Univ State Key Lab Precis Measurement Technol & Instrum Tianjin 300072 Peoples R China

Laser absorption spectroscopy has proven to be an effective approach for gas sensing, which plays an important role in the fields of military, industry, medicine and basic research. This paper presents a multiplexed gas sensing system based on optical frequency comb (OFC) calibrated frequency-modulated continuous-wave (FMCW) tuning nonlinearity. The system can be used for multi-parameter synchronous measurement of gas absorption spectrum and multiplexed optical path. Multi-channel parallel detection is realized by combining wavelength division multiplexing (WDM) and frequency division multiplexing (FDM) techniques. By introducing nonlinear optical crystals, broadband spectrum detection is simultaneously achieved over a bandwidth of hundreds of nanometers. An OFC with ultra-high frequency stability is used as the frequency calibration source, which guarantees the measurement accuracy. The test samples involve H13C14N, C2H2 and Rb vapor cells of varying densities and 5 parallel measurement experiments are designed. The results show that the measurement accuracies of spectral absorption line and the optical path are 150 MHz and 20 mu m, respectively. The scheme offers the advantages of multiplexed, multi-parameter, wide spectrum and high resolution detection, which can realize the identification of multi-gas components and the high-precision inversion of absorption lines under different environments. The proposed sensor demonstrates great potential in the field of high-resolution absorption spectrum measurement for gas sensing applications.

关键词： frequency-modulated continuous-wave (FMCW) technology optical frequency comb multiplexing absorption spectroscopy 42.15.Eq 06.20.-f 42.62.Fi 42.62.-b SPECTROSCOPY CONVERSION LIDAR

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In situ sulfur-doped mesoporous tungsten oxides for gas sensing toward benzene series

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Chinese Chemical Letters 2024年第7期35卷 502-507页

作者： Yu Deng Yan Liu Yonghui Deng Jinsheng Cheng Yidong Zou Wei Luo state key laboratory for Modification of Chemical Fibers and polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China Department of chemistry State Key Laboratory of Molecular Engineering of PolymersShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsiChEMFudan UniversityShanghai 200433China Department of polymeric Materials School of Materials Science and EngineeringTongji UniversityShanghai 201804China Henry-Fork School of Food Sciences Shaoguan UniversityShaoguan 512005China state key lab of Transducer Technology Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China

Benzene series as highly toxic gases have inevitably entered human life and produce great threat to human health and ecological environment,and thus it is distinctly meaningful to monitor benzene series with quickly,real-time and efficient ***,novel sulfur-doped mesoporous WO_(3)materials were synthesized via classical in-situ solvent evaporation induced co-assembly strategy combined with doping engineering,which possessed highly crystallized frameworks,high specific surface area(40.9–63.8 m^(2)/g)and uniform pore size(~18 nm).Benefitting from abundant oxygen vacancy and defects via S-doping,the tailored mesoporous S/m WO_(3)exhibited excellent benzene sensing performance,including high sensitivity(50 ppm vs.48),low detection limit(ca.500 ppb),outstanding selectivity and favorable *** addition,the reduction of band gap resulted from S-doping promotes the carrier migration in the sensing materials and the reaction at the gas–solid sensing *** provides brand-new approach to design sensitive materials with multiple reaction sites.

关键词： Mesoporous materials Benzene series Tungsten oxides Sulfur doping Gas sensor

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不同尺寸橡胶/帘线H型拉拔试验界面参数的归一化处理评价方法

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Acta Mechanica Sinica 2024年第3期40卷 99-108页

作者：王琮文肖驰代玉静王君马寒松郇勇郇彦 state key laboratory of Nonlinear Mechanics(LNM) Institute of MechanicsChinese Academy of SciencesBeijing100190China School of Engineering Science University of Chinese Academy of SciencesBeijing100049China School of Aerospace Engineering Beijing Institute of TechnologyBeijing100081China state key laboratory of polymer physics and chemistry and polymer Composite Engineering laboratory Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China

H型拉拔试验被广泛应用于橡胶/帘线复合材料界面粘结强度的估算.然而,目前的国际标准只要求在橡胶/帘线H型拉拔试验中记录拔出力的大小,并强调从不同尺寸的样品中获得的结果不具有可比性.在本文中,我们研究了不同尺寸橡胶/帘线试验样品... 详细信息

H型拉拔试验被广泛应用于橡胶/帘线复合材料界面粘结强度的估算.然而,目前的国际标准只要求在橡胶/帘线H型拉拔试验中记录拔出力的大小,并强调从不同尺寸的样品中获得的结果不具有可比性.在本文中,我们研究了不同尺寸橡胶/帘线试验样品的H拔出结果的可比性,并提出了一种归一化的评价方法来处理这些结果.分别对尺寸为5 mm、6.4 mm、10 mm的试验样品进行橡胶/帘线H拉拔试验(尺寸为7.5 mm、8.5 mm的试件结果作为支撑性试验).在试验结果的基础上,采用有限元法内聚单元模型对界面粘结强度进行了分析,所得出的内聚力参数比国际标准中所规定的拔出力更能准确地反映界面粘结性能.因此,采用内聚单元法能够更合理地比较不同橡胶/帘线试样的界面粘结强度.我们首先基于6.4 mm尺寸样品的试验结果建立有限元模型,并确定满足条件的内聚单元参数,然后将其应用于其他尺寸的样品模型.尽管试验样品的尺寸大小在变化,但在保持内聚单元参数不变的前提下,模拟结果与试验结果仍然保持良好的一致性,这表明内聚参数不受样本尺寸的影响.在此基础上,我们提出了一种归一化方法,使不同尺寸样品的橡胶/帘线H拉拔试验的结果具有了可比性.本文提出的归一化方法是对现有国际、国内标准实验方法的扩展.

关键词： Rubber Composites Finite element method Cohesive elements H pull-out test

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A Dielectric Ink Combining Acrylate and Cyanate Moieties for Inkjet 3D Printing with Good Thermal Stability

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Chinese Journal of polymer Science 2024年第6期42卷 766-774页

作者： Yi-Xuan Li Liang-Ying Wu Yan Yang Yao-Zhong Lu Zhong-Ying Ji Yu-Xiong Guo Xiao-Long Wang Qiao-Sheng Pu state key laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China state key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsLanzhou730000China Lanzhou Traditional Chinese Medicine Hospital of Orthopedics and Traumatology Lanzhou730000China Shandong laboratory of Advanced Materials and Green Manufacturing at Yantai Yantai Zhongke Research Institute of Advanced Materials and Green Chemical EngineeringYantai264006China

Inkjet 3D printing has potential in the additive manufacturing of electronic circuits and ***,inks that can be used for printing layers with T5%>300℃ or hardness>200 MPa have been rarely *** ester(CE)polymers have excellent thermal stability,high strength,and low shrinkage compared to other common dielectric inks for inkjet 3D printing,but cannot be quickly shaped by ultraviolet(UV)irradiation or thermal *** CEs with UV-curable monomers may be a possible way to accelerate crosslinking,but there are challenges from the adverse effects of the dilution of both *** this study,dielectric inks with acrylate and cyanate moieties were *** low viscosity and surface tension of the CE precursor(Bisphenol E cyanate ester)were combined with photocurable acrylate diluent monomers and cross-linker to realize an ink suitable for inkjet 3D *** internal dual three-dimensional cross-linked network structure resin was prepared by a combination of photocuring and thermal curing with T5%up to 326.69℃,hardness up to 431.84 MPa,dielectric constant of 2.70 at 8 GHz,and shrinkage of 1.64%.The developed dielectric inks can be applied to the 3D printing of printed circuit boards and other electronic devices that require dielectric properties.

关键词： Inkjet printing Cyanate ester resin 3D doubly cross-linked network Good thermal stability

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Simultaneously optimizing exciton diffusion length and nonradiative energy loss in organic solar cells via ternary strategy

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Science China chemistry 2024年第9期67卷 3004-3011页

作者： Huanxiang Jiang Hao Lu Zezhou Liang Yonghai Li Guangliu Ran Chenyu Han Yuqiang Liu Hongxiang Li Xichang Bao Zhishan Bo College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao 266071China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China key laboratory for Physical Electronics and Devices of the Ministry of Education&Shaanxi Key Lab of Photonic Technique for InformationSchool of Electronics Science&EngineeringFaculty of Electronic and Information EngineeringXi’an Jiaotong UniversityXi’an 710049China Department of physics and Applied Optics Beijing Area Major laboratory Center for Advanced Quantum StudiesBeijing Normal UniversityBeijing 100875China College of polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China laboratory of Solar Energy Shandong Energy InstituteQingdao 266101China

Significant nonradiative energy loss and short exciton diffusion length in organic solar cells(OSCs)are two major obstacles to achieving state-of-the-art *** is crucial to conduct a study on the intensive mechanism and improvement strategies for future breakthroughs in the efficiency of *** this work,nonradiative energy loss and exciton diffusion length are optimized simultaneously by incorporating a guest acceptor(LA15)to construct ternary OSC(D18:L8-BO:LA15).Firstly,LA15 exhibits excellent compatibility with the host acceptor L8-BO,and effectively improves the fluorescence quantum efficiency(FLQY),resulting in suppressed non-radiative energy ***,LA15 effectively prolongs the fluorescent lifetime of the acceptor phase from 0.85 to 1.12 ns,leading to larger exciton diffusion length,which is beneficial for reducing geminate ***,the addition of LA15 optimizes the crystallinity of the active layer with amplified charge transport *** a result,the optimized D18:L8-BO:LA15 device achieves ultralow nonradiative energy loss of 0.18 e V and improved fill factor(FF)with high efficiency up to 19.13%.These results highlight the crucial roles of regulating FLQYand exciton lifetime in achieving highefficiency OSCs.

关键词： organic solar cells nonradiative energy loss exciton lifetime exciton diffusion length

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Negative enthalpy alloys and local chemical ordering:a concept and route leading to synergy of strength and ductility

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National Science Review 2024年第4期11卷 172-184页

作者： Zibing An Tao Yang Caijuan Shi Shengcheng Mao Lihua Wang Ang Li Wei Li Xianmeng Xue Ming Sun Yifan Bai Yapeng He Fuzeng Ren Zhouguang Lu Ming Yan Yang Ren Chain-Tsuan Liu Ze Zhang Xiaodong Han Beijing key lab of Microstructure and Property of Advanced Materials College of Materials Science &Engineering Beijing University of Technology Department of Materials Science and Engineering City University of Hong Kong key laboratory of Partial Acceleration physics& Technology Institute of High Energy PhysicsChinese Academy of Sciences Department of Materials Science &Engineering Southern University of Science and Technology Department of physics City University of Hong Kong state key laboratory of Silicon Materials Department of Materials Science and Engineering Zhejiang University

Solid solutions are ubiquitous in metals and alloys. Local chemical ordering(LCO) is a fundamental sub-nano/nanoscale process that occurs in many solid solutions and can be used as a microstructure to optimize strength and ductility. However, the formation of LCO has not been fully elucidated, let alone how to provide efficient routes for designing LCO to achieve synergistic effects on both superb strength and ductility. Herein, we propose the formation and control of LCO in negative enthalpy alloys. With engineering negative enthalpy in solid solutions, genetic LCO components are formed in negative enthalpy refractory high-entropy alloys(RHEAs). In contrast to conventional ‘trial-and-error' approaches, the control of LCO by using engineering negative enthalpy in RHEAs is instructive and results in superior strength(1160 MPa) and uniform ductility(24.5%) under tension at ambient temperature, which are among the best reported so far. LCO can promote dislocation cross-slip, enhancing the interaction between dislocations and their accumulation at large tensile strains; sustainable strain hardening can thereby be attained to ensure high ductility of the alloy. This work paves the way for new research fields on negative enthalpy solid solutions and alloys for the synergy of strength and ductility as well as new functions.

关键词： negative enthalpy alloys local chemical ordering strength ductility dislocation

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