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synthesis of a Highly Crystalline Amide-Linked Covalent Organic Framework

Chinese Journal of Chemistry 2023年第4期41卷 405-410页

作者： Yuyao Li Zhipeng Zhou Yuexian Hong Xin Dong Yonghang Yang Zihao Liang Junliang Sun Xudong Chen Wei Liu Zhikun Zheng Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education School of Chemistryand State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhouGuangdong510275 China College of Chemistry and Molecular engineering Beijing National Laboratory for Molecular SciencesPeking UniversityBeijing100871 China School of Chemical engineering and Light Industry Guangdong University of TechnologyGuangzhouGuangdong510006 China Jieyang Branch of Chemistry and Chemical engineering Guangdong Laboratory JieyangGuangdong515200 China Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong Province Key Laboratory for Polymeric Composite and Functional Materials of Ministry of EducationSchool of Materials Science and Engineeringand State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-sen UniversityGuangzhouGuangdong510275 China

The dilemma for the synthesis of covalent organic frameworks(COFs)is crystallinity and stability.Herein,we present the synthesis of a single-crystalline amide-linked COF,and demonstrate its excellent chemical as well as thermal stabilities.This study will inspire the synthesis of a wide spectrum of highly crystalline and stable COFs,promote their structure-property investigations and boost their applications in selective gas adsorption,storage and separation.

关键词： Covalent organic frameworks polymers Amides Organic crystals Microporous materials

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De novo synthesis of bifunctional conjugated microporous polymers for synergistic coordination mediated uranium entrapment

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Nano research 2021年第3期14卷 788-796页

作者： Boxuan Yu Lei Zhang Gang Ye Qingzhi Liu Jiongli Li Xudong Wang Jing Chen Shengming Xu Shengqian Ma Collaborative Innovation center of Advanced Nuclear Energy Technology Institute of Nuclear and New Energy TechnologyTsinghua UniversityBeijing100084China beijing Institute of Graphene Technology Beijing100094China beijing Institute of Aeronautical Materials Beijing100085China Department of Chemistry University of South Florida4202 E.Fowler AvenueTampaFL33620USA beijing Key Lab of Radioactive Waste Treatment Tsinghua UniversityBeijing100084China College of Chemistry and Pharmaceutical Sciences Qingdao Agricultural UniversityQingdao266109China

This work reports a de novo synthesis of novel bifunctional conjugated microporous polymers(CMPs)exhibiting a synergistic-effect involved coordination behavior to uranium.It is highlighted that the synthetic strategy enables the engineering of the coordination environment within amidoxime functionalized CMP frameworks by specifically introducing ortho-substituted amino functionalities,enhancing the affinity to uranyl ions via forming synergistic complexes.The CMPs exhibit high Brunauer-Emmett-Teller(BET)surface area,well-developed three-dimensional(3D)networks with hierarchical porosity,and favorable chemical and thermal stability because of the covalently cross-linked structure.Compared with the amino-free counterparts,the adsorption capacity of bifunctional CMPs was increased by almost 70%,from 105 to 174 mg/g,indicating evidently enhanced binding ability to uranium.Moreover,new insights into coordination mechanism were obtained by in-depth X-ray photoelectron spectroscopy(XPS)analysis and density functional theory(DFT)calculation,suggesting a dominant role of the oxime ligands forming a 1:1 metal ions/ligands(M/L)coordination model with uranyl ions while demonstrating the synergistic engagement of the amino functionalities via direct binding to uranium center and hydrogen-bonding involved secondary-sphere interaction.This work sheds light on the underlying principles of ortho-substituted functionalities directed synergistic effect to promote the coordination of amidoxime with uranyl ions.And the synthetic strategy established here would enable the task-specific development of more novel CMP-based functional materials for broadened applications.

关键词： conjugated microporous polymers uranium adsorption synergistic coordination density functional theory

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General synthesis of high-performing magneto-conjugated polymer core-shell nanoparticles for multifunctional theranostics

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Nano research 2017年第2期10卷 704-717页

作者： Hao Yan Lingyun Zhao Wenting Shang Zhongqun Liu Wensheng Xie Cai Qiang Zhiyuan Xiong Ranran Zhang Baohua Li Xiaodan Sun Feiyu Kang State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Key Laboratory of Advanced Materials of Ministry of Education of China Tsinghua University Beijing 100084 China engineering Laboratory for Functionalized Carbon Materials Graduate School at Shenzhen Tsinghua University Shenzhen 518055 China Key Laboratory of Molecular Imaging Institute of Automation Chinese Academy of Sciences Beijing 100190 China

Recently, increasing attention has been paid to magneto-conjugated polymer core-shell nanoparticles （NPs） as theranostic platforms. However, the utilization of surfactants and extra oxidizing agents with potential toxicity in synthesis, the lack of general methods for the controlled synthesis of various kinds of magnetic NP （MNP）@conjugated polymer NPs, and the difficulty of obtaining balanced magneto-optical properties have greatly limited the applications of magneto-conjugated polymers in theranostics. We developed an in situ surface polymerization method free of extra surfactants and oxidizing agents to synthesize MNP@polypyrrole （PPy） NPs with balanced, prominent magneto-optical properties. MNP@PPy NPs with an adjustable size, different shapes, and a controlled shell thickness were obtained using this method. The method was extended to synthesize other MNP-conjugated polymer core-shell NPs, such as MNP@polyaniline and MNP@poly（3,4-ethylenedioxythiophene）：poly（4- styrenesulfonate）（PEDOT：PSS）. We discuss the formation mechanism of the proposed method according to our experimental results. Finally, using the optical and magnetic properties of the obtained MNP@PEDOT：PSS NPs, in vivo multimodal imaging-guided hyperthermia was induced in mice, achieving an excellent tumor-ablation therapeutic effect. Our work is beneficial for extending the application of MNP-conjugated polymer core-shell NPs in the biomedical field.

关键词： iron oxide,polypyrrole,photothermal,magnetic,hyperthermal,poly（3,4-ethylenedioxythiophene）：poly（4-styrenesulfonate）（PEDOT：PSS）

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聚合物共混薄膜的铁电特性调控及其柔性储能应用

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Science China Materials 2021年第7期64卷 1642-1652页

作者：张鑫江彦达高若棋李昕蕙沈忠慧李宝文张清风张树君南策文 State Key Laboratory of Advanced Technology for Materials synthesis and Processing Center of Smart Materials and DevicesWuhan University of TechnologyWuhan 430070China International School of Materials Science and engineering Wuhan University of TechnologyWuhan 430070China Hubei Key Lab of Ferro&Piezoelectric Materials and Devices School of Materials Science&EngineeringHubei UniversityWuhan 430062China Institute for Superconducting and Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongNorth WollongongNSW 2500Australia School of Materials Science and engineering State Key Lab of New Ceramics and Fine ProcessingTsinghua UniversityBeijing 100084China

铁电聚合物在先进柔性电子器件中通常扮演重要角色,如何调控铁电聚合物薄膜的性能来满足其多样化应用是一个挑战.本文中,我们通过两步法制备了聚偏氟乙烯-三氟乙烯(P(VDFTrFE))与聚甲基丙烯酸甲酯(PMMA)的聚合物共混薄膜并对共混薄膜的... 详细信息

铁电聚合物在先进柔性电子器件中通常扮演重要角色,如何调控铁电聚合物薄膜的性能来满足其多样化应用是一个挑战.本文中,我们通过两步法制备了聚偏氟乙烯-三氟乙烯(P(VDFTrFE))与聚甲基丙烯酸甲酯(PMMA)的聚合物共混薄膜并对共混薄膜的铁电特性进行了调控.不同于常规P(VDF-TrFE)薄膜中铁电晶相的连续有序分布,两步法工艺可以实现聚合物共混薄膜中P(VDF-TrFE)晶相的随机分布,进而打破常规铁电聚合物薄膜中相邻晶相铁电畴间的耦合作用;在此基础上,共混薄膜非晶区内的低极性PMMA组分可以通过降低去极化电场来调节偶极子的翻转行为,使共混薄膜由铁电特性转变为类反铁电特性;此外,铁电聚合物共混薄膜优异的力学与电学性能可以显著提升其击穿强度,最终获得明显优于纯P(VDF-TrFE)薄膜和商业双轴拉伸聚丙烯薄膜的超高储能密度.本论文提出了一种调控聚合物材料铁电特性的有效策略,为高储能密度铁电聚合物薄膜材料的发展带来巨大潜力.

关键词：聚合物共混聚偏氟乙烯击穿强度铁电特性非晶区铁电畴共混薄膜打破常规

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