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Study on Catalytic Behavior of Iron-based Catalyst with IITP as Electron Donor in the polymerization of Butadiene

Chinese Journal of polymer science 2024年第5期42卷 612-619,I0007页

作者： Shi-Liang Xu Ying-Nan Zhao Yao Yu Qi Yang Li-Hua Na Heng Liu Chun-Yu Zhang Xue-Quan Zhang Key Laboratory of Advanced Rubber Material Ministry of EducationSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China Shandong Provincial College Laboratory of Rubber Material and Engineering School of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China Key Lab of Rubber-Plastics Ministry of Education/Shandong Provincial Key Lab of Rubber-plasticsSchool of Polymer Science and EngineeringQingdao University of Science&TechnologyQingdao266042China

In this study,a novel iron-based catalyst system,Fe(acac)3/(isocyanoimino)triptenylphosphorane(IITP)/AlR3,was employed for the synthesis of syndiotactic 1,2-polybutadiene in *** catalyst system exhibits remarkably high catalytic activity,achieving a polymerization activity of 762 kgpolymer·molcatalyst^(-1)·h^(-1)at 50℃with a[BD]/[Fe]molar ratio of ***,living polymerization characteristic were observed during the investigation of the polymerization kinetics of 1,3-butadiene *** characteristics were well demonstrated by a narrow molecular weight distribution(PDI≈2.0)of the resulting polybutadiene and a linear relationship between-ln(1-c)and polymerization time as well as number average molecular weight and polymer *** resultant polymer showed a 1,2-selectivity of approximately 76%and stereoregularity ranging from 62%to 73%(rrrr).Additionally,through kinetic studies on polymerization reaction,an apparent activation energy Ea value of this catalytic system was calculated to be 84.98 kJ·mol^(-1),which suggests that high polymerization temperature favors efficient polymerization.

关键词： Iron catalyst Syndiotactic 1,2-polybutadiene Elastomers Donor Selectivity

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Spontaneous Recovery in Directed Dynamical Networks

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Engineering 2024年第6期37卷 208-214页

作者： Xueming Liu Xian Yan H.Eugene Stanley school of Artificial Intelligence and Automation&The MOE Engineering Research Center of Autonomous Intelligent Unmanned Systems&the Key Laboratory of Image Processing Huazhong University of Science and TechnologyWuhan 430074China Center for polymer studies Department of PhysicsBoston UniversityBostonMA 02215USA

Complex networked systems,which range from biological systems in the natural world to infrastructure systems in the human-made world,can exhibit spontaneous recovery after a failure;for example,a brain may spontaneously return to normal after a seizure,and traffic flow can become smooth again after a *** studies on the spontaneous recovery of dynamical networks have been limited to undirected ***,most real-world networks are *** fill this gap,we build a model in which nodes may alternately fail and recover,and we develop a theoretical tool to analyze the recovery properties of directed dynamical *** find that the tool can accurately predict the final fraction of active nodes,and the prediction accuracy decreases as the fraction of bidirectional links in the network increases,which emphasizes the importance of directionality in network *** to different initial states,directed dynamical networks may show alternative stable states under the same control parameter,exhibiting hysteresis *** addition,for networks with finite sizes,the fraction of active nodes may jump back and forth between high and low states,mimicking repetitive failure-recovery *** findings could help clarify the system recovery mechanism and enable better design of networked systems with high resilience.

关键词： Network resilience Directed dynamical networks Spontaneous recovery

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有向动态网络的自发恢复（英文）

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Engineering 2024年第6期 208-214页

作者：刘雪明闫贤 H.Eugene Stanley school of Artificial Intelligence and Automation & The MOE Engineering Research Center of Autonomous Intelligent Unmanned Systems & the Key Laboratory of Image Processing Huazhong University of Science and Technology Center for polymer studies Department of Physics Boston University

Complex networked systems, which range from biological systems in the natural world to infrastructure systems in the human-made world, can exhibit spontaneous recovery after a failure; for example, a brain may spontaneously return to normal after a seizure, and traffic flow can become smooth again after a jam. Previous studies on the spontaneous recovery of dynamical networks have been limited to undirected networks. However, most real-world networks are directed. To fill this gap, we build a model in which nodes may alternately fail and recover, and we develop a theoretical tool to analyze the recovery properties of directed dynamical networks. We find that the tool can accurately predict the final fraction of active nodes, and the prediction accuracy decreases as the fraction of bidirectional links in the network increases, which emphasizes the importance of directionality in network dynamics. Due to different initial states, directed dynamical networks may show alternative stable states under the same control parameter, exhibiting hysteresis behavior. In addition, for networks with finite sizes, the fraction of active nodes may jump back and forth between high and low states, mimicking repetitive failure-recovery processes. These findings could help clarify the system recovery mechanism and enable better design of networked systems with high resilience.

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Rheo-NMR: A versatile hyphenated technique for capturing molecular dynamics and structure under flow

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Magnetic Resonance Letters 2024年第1期4卷 50-60页

作者： Yuqi Xiong Zishuo Wu Lei Wu Chengyan Li Wei Chen National Synchrotron Radiation Laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer FilmCAS Key Laboratory of Soft Matter ChemistryUniversity of Science and Technology of ChinaHefei230026China Department of Accelerator science and Engineering Physics School of Nuclear Science and TechnologyUniversity of Science and Technology of ChinaHefei230026China

The general development of Rheo-NMR during the last four decades as well as selective hyphenated apparatuses is *** on different magnet types,the current review is divided into two categories,namely low-field and high-field NMR,while the timedomain NMR is normally applied in the former case and the frequency-domain NMR is adopted in the latter *** on different rheometer cells,it can be further divided into tensile and shear mode *** combination of various rheometer cells and NMR facility guarantees our acquisition of molecular level structure and dynamics information under flow conditions,which is crucial for our understanding of the molecular origin of complex fluids.A personal perspective is also presented at last to highlight possible development in this direction.

关键词： Rheo-NMR polymer deformation mechanism polymer rheology Viscoelastic property

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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-textiles Qingdao University Key Laboratory for Physical Electronics and Devices of the Ministry of Education & Shaanxi Key Lab of Photonic Technique for InformationSchool of Electronics Science & Engineering Faculty of Electronic and Information Engineering Xi'an Jiaotong University Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of Sciences Laboratory of Solar Energy Shandong Energy Institute Department of Physics and Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum Studies Beijing Normal University College of polymer science and Engineering State Key Laboratory of Polymer Materials Engineering Sichuan University

Significant nonradiative energy loss and short exciton diffusion length in organic solar cells(OSCs) are two major obstacles to achieving state-of-the-art efficiencies. It is crucial to conduct a study on the intensive mechanism and improvement strategies for future breakthroughs in the efficiency of OSCs. In 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 loss. Moreover, 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 capacity. As 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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Highly efficient solution-processed organic photovoltaics enabled by improving packing behavior of organic semiconductors

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science China Chemistry 2024年第3期67卷 890-897页

作者： Xinyue Cui Hongxiang Li Hao Lu Yuqiang Liu Guangliu Ran Rui Liu Huarui Zhang Xueqing Ma Dawei Li Yi Lin Jifa Yu Wenkai Zhang Lei Cai Yahui Liu Pei Cheng Andong Zhang Zaifei Ma Guanghao Lu Zhishan Bo College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao 266071China State Key Laboratory of polymer Materials Engineering College of Polymer Science and EngineeringSichuan UniversityChengdu 610065China Department of Physics and Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum StudiesBeijing Normal UniversityBeijing 100875China Shandong Province Key Laboratory of Medical Physics and Image Processing Technology School of Physics and ElectronicsShandong Normal UniversityJinan 250014China Beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China Center for Advanced Low-Dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai 201620China Frontier Institute of science and Technology Xi'an Jiaotong UniversityXi'an 710054China

Solution processability is a unique property of organic semiconductors. The compact and regular π-π stacking between molecules is paramount in the performance of organic optoelectronic devices. However, it is still a challenge to improve their stacking quality without sacrificing the solution-processability from the aspect of materials design. Here, delicately engineered additives are presented to promote the formation of ordered aggregation of conjugated molecules by regulating their nucleation and growth dynamics. Intriguingly, the long-chain BTP-eC9-4F molecules can realize ordered aggregation comparable to short-chain ones without sacrificing processability. The domain size of BTP-eC9-4F aggregation is enlarged from 24.2 to 32.2 nm in blend *** exciton diffusion and charge transport become faster, contributing to the suppression of recombination losses. As a result, a power conversion efficiency of 19.2% is achieved in D18:BTP-eC9-4F based organic photovoltaics. Our findings demonstrate a facile strategy to improve the packing quality of solution-processed organic semiconductors for high-efficiency photovoltaics and beyond photovoltaics.

关键词： organic semiconductor organic photovoltaic charge transport solution processability

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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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Estimation of secondary nucleation kinetics of benzoic acid in batch crystallizer

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Particuology 2024年第4期87卷 232-239页

作者： Yan Zhao Weiyuan Zhang Jinbo Ouyang Guangyang Hou Vamsi Krishna Kamaraju Brian Glennon school of Chemical Engineering Hebei Normal University of Science and TechnologyQinhuangdao066004China Synthesis and Solid State Pharmaceutical Centre School of Chemical and Bioprocess EngineeringUniversity College DublinDublin 4Ireland Jiangxi Province Key Laboratory of polymer Micro/Nano Manufacturing and Devices East China University of TechnologyNanchang330013China APC Ltd Dublin 4Ireland

The nucleation and growth kinetics of benzoic acid were determined in a population balance model,describing the seeded batch antisolvent crystallization *** process analytical technologies(PATs)were utilized to record the evolution of chord length distributions(CLDs)in solid phase together with the concentration decay in liquid phase,which provided essential experimental information for parameter *** model was solved using standard method of moments based on the moments calculated from CLDs and solute concentration.A developed model,incorporating the nucleation and crystal growth as functions of both supersaturation and solvent composition,has been constructed by fitting the zeroth moment of particles and concentration *** determined kinetic parameters were consequently validated against a new experiment with a different flow rate,indicating that the developed model predicted crystallization process reasonably *** work illustrates the strategy in construct a population balance model for further simulation,model-based optimization and control studies of benzoic acid in antisolvent crystallization.

关键词： Benzoic acid Antisolvent crystallization Population balance equation Nucleation Growth

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提高分子结晶度和分子间相互作用以实现有机太阳能电池效率和稳定性的同步提升（英文）

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science China Materials 2024年

作者：赵江通杨欣荣邵一鸣孙瑞闵杰 The Institute for Advanced studies Wuhan University Institute of polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and Devices South China University of Technology Key Laboratory of Advanced Electrode Materials for Novel Solar Cells for Petroleum and Chemical Industry of China School of Chemistry and Life SciencesSuzhou University of Science and Technology

通过分子设计精准控制体异质结(BHJ)形貌是开发高性能有机太阳能电池(OSCs)面临的长期挑战之一.本工作中,我们设计并合成了三种具有不同侧链(分别在苯并三唑单元上引入甲基、2-乙基己基和2-癸基十四烷基)的小分子受体(SMAs),即R-M、R-EH...

通过分子设计精准控制体异质结(BHJ)形貌是开发高性能有机太阳能电池(OSCs)面临的长期挑战之一.本工作中,我们设计并合成了三种具有不同侧链(分别在苯并三唑单元上引入甲基、2-乙基己基和2-癸基十四烷基)的小分子受体(SMAs),即R-M、R-EH和R-DTD.这种侧链调控可以有效调节受体/受体(A/A)和给体/受体(D/A)分子之间的相互作用,从而实现BHJ活性层结构的微调.与R-M和R-DTD相比, R-EH与给体PM6表现出更强的A/A和D/A相互作用,形成更紧密的分子排列,改善了BHJ网络结构,增强了电荷传输和提取性能.因此,在三个体系中, PM6:R-EH不仅表现出超过18%的器件效率,还表现出优异的稳定性.本研究深化了A/A和D/A相互作用对BHJ形貌的协同调节作用,为实现高效且稳定的工业化OSCs提供了新的思路.

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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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