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Manipulating guest-responsive spin transition to achieve switchable fluorescence in a Hofmann-type framework

Science china chemistry 2024年第10期67卷 3339-3346页

作者： Xue-Ru Wu Shu-Qi Wu Zhi-Kun liu Ming-Xing Chen Jun Tao Osamu Sato Hui-Zhong Kou Engineering Research Center of Advanced Rare Earth Materials(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084China institute for Materials chemistry and Engineering&IRCCS Kyushu University744 MotookaNishi-kuFukuoka 819-0395Japan key laboratory of Cluster Science of Ministry of Education School of Chemistry and Chemical EngineeringLiangxiang CampusBeijing Institute of TechnologyBeijing 102488China Analytical Instrumentation Center College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The change of fluorescence emission manipulated by spin state transition attracts considerable attention owing to its potential applications in magneto-optical switching ***,we report two two-dimensional(2.)Hofmann-type spin crossover(SCO)metal-organic frameworks(MOFs)[Fe^(Ⅱ)(PNI)_(2.{Ag^(Ⅰ)(CN)_(2.}_(2.]·CHCl_(3)(3Ag·CHCl_(3))and[FeⅡ(PNI)_(2.{AuⅠ(CN)_(2.}_(2.]·CHCl_(3)(3Au·CHCl_(3))based on the fluorescent ligand N-(4-pyridylmethyl)-1,8-naphthalimide(PNI).Both complexes exhibit interesting SCO behaviors switched by guest solvent molecules,namely three-step transitions for the solvated complexes and complete onestep hysteretic SCO for the desolvated ones,verified by temperature-dependent magnetic susceptibility measurements,Mossbauer spectra,structural analyses,and differential scanning calorimetry ***,temperature-dependent fluorescence spectra exhibit double peaks(monomer and excimer emission)with both emission peaks change consistent with the change in SCO properties during the solvent molecule *** this study,we integrated guest-responsive SCO behavior into MOFs to manipulate the multistability of spin state and fluorescence switching,providing a rational strategy for the development of stimuli-responsive multifunctional materials.

关键词： spin crossover fluorescence multifunctional materials metal-organic frameworks Hofmann-type

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A molecular-Sieving Interphase Towards Low-Concentrated Aqueous Sodium-Ion Batteries

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Nano-Micro Letters 2024年第8期16卷 51-63页

作者： Tingting liu Han Wu Hao Wang Yiran Jiao Xiaofan Du Jinzhi Wang Guangying Fu Yaojian Zhang Jingwen Zhao Guanglei Cui Qingdao Industrial Energy Storage Research institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia Shandong Energy institute Qingdao 266101People’s Republic of China Qingdao New Energy Shandong laboratory Qingdao 266101People’s Republic of China

Aqueous sodium-ion batteries are known for poor rechargeability because of the competitive water decomposition reactions and the high electrode *** have been reported by saltconcentrated and organic-hybridized electrolyte designs,however,at the expense of cost and ***,we report the prolonged cycling of ASIBs in routine dilute electrolytes by employing artificial electrode coatings consisting of NaX zeolite and NaOH-neutralized perfluorinated sulfonic *** as-formed composite interphase exhibits a {2.sieving effect jointly played by zeolite channels and size-shrunken ionic domains in the polymer matrix,which enables high rejection of hydrated Na^(+)ions while allowing fast dehydrated Na^(+)*** this coating to electrode surfaces expands the electrochemical window of a practically feasible 2.mol kg^(-1) sodium trifluoromethanesulfonate aqueous electrolyte to 2.70 V and affords Na_(2.MnFe(CN)_(6)//NaTi_(2.(PO_(4))_(3) full cells with an unprecedented cycling stability of 94.9%capacity retention after 2.0 cycles at 1 *** with emerging electrolyte modifications,this {2.-sieving interphase brings amplified benefits in long-term operation of ASIBs.

关键词： molecular sieving effect Electrode coatings Aqueous sodium ion batteries Dilute aqueous electrolytes

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Separation of Recombinant Human Erythropoietin by Carboxylmethyl Chitosan-coated Capillary Electrophoresis

Separation of Recombinant Human Erythropoietin by Carboxylme...

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第四届海峡两岸分析化学学术会议

作者： liu Hu-wei,Fu Xiao-fang, Huang Ling, Zhai Mao-lin (beijing {2. laboratory for molecular Science, College of chemistry and molecular Engineering, Peking University, beijing 100871)

＜正＞A hydrophilic basic polysaccharide, carboxymethyl chitosan （CMC）, as a derivative of chitosan, was utilized to coat fused silica capillary for the separation of recombinant human erythropoietin （rhEPO） by capillary electrophoresis （CE）. The coating procedure with different concentrations and molecular weights of CMC was also investigated. The CMC coated capillary showed a long life time of more than 100 runs , and good tolerance to some inorganic and organic solutions, 0.1 M HCl, 0.1 M NaOH and 5 M urea. The relative standard deviations （RSDs） of run-to-run, day-to-day and capillary-to-capillary coating were all below 2.0% for the determination of electroosmotic flow （EOF）. Furthermore, several experimental parameters, such as the concentration and pH of the running buffer, temperature, and applied voltage were also optimized for the separation of rhEPO glycoforms. Comparison of uncoated capillary with chitosan-coated and CMC-coated capillaries for the separation of rhEPO glycoforms was also discussed. The results demonstrated that rhEPO glycoforms can be well separated by CMC-coated capillary within 8 min with good reproducibility and resolution under the following conditions: 100 mM HAc-NaAc （pH=4.5）, 2.℃ and applied voltage -30 kV. Volatile background electrolyte HAc-NH4Ac was also employed to separate rhEPO for its further application with CE-mass spectrometry （MS） method, achieving satisfactory result.

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Recent progress in stretchable organic field-effect transistors

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Science china(Technological sciences) 2019年第8期62卷 1255-1276页

作者： liu Kai GUO yunLong liu yunqi beijing national {2. for molecular sciences Organic Solid Laboratory Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Department of chemistry University of Chinese Academy of Sciences Beijing 100049 China

Stretchable organic field-effect transistors (STOFETs) employing organic semiconductors as active layers are highly attractive ongoing from health monitoring to biological research owing to some favorable advantages over their inorganic counterpart, including light weight, low cost, solution processing, high flexibility and simple adjustment of functionalities through molecular design. Although the development of STOFETs with original electrical performances under large mechanical deformation remain rudimentary, major efforts have recently been devoted to the investigation on STOFETs, and remarkable advances in stretchable components and novel fabrication methods have been achieved. A detailed overview of the advantages, challenges and current achievements in STOFETs was given including stretchable electrodes, semiconductors, dielectrics and substrates. Furthermore, conclusions and prospects for the future development of STOFETs with both high stretchability and superb electrical performances fabricated using intrinsically stretchable components are proposed.

关键词： STOFETs organic semiconductor high stretchability high carrier mobility

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A thriving decade: rational design, green synthesis, and cutting-edge applications of isoindigo-based conjugated polymers in organic field-effect transistors

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Science china chemistry 2022年第7期65卷 1225-1264页

作者： Mingliang Zhu yunlong Guo yunqi {2. beijing national {2. for molecular sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of chinese academy of sciences Beijing 100049China

Recent advances in organic electronics of novel materials and optoelectronic devices spark great interest in the design and synthesis of high-performance polymer semiconductors. During the last decade, isoindigo(ⅡD) and its derivatives have sprung up as common electron-deficient building blocks and obtained extensive applications in organic field-effect transistors(OFETs).In this review, we first present the current status, basic principles, and general material design strategies for OFETs. Then,multiple ⅡD-type acceptors, mature synthetic routes to monomers, and typical ⅡDs-based conjugated polymers are *** also introduce side-chain engineering and cutting-edge applications, like stretchable transistors, sensing, active-matrix driving, etc., of the classic copolymer poly(isoindigo-co-bithiophene). Green polymerization approaches towards conjugated polymers incorporating ⅡDs are subsequently discussed for efficient polymerization. Finally, we conclude this review and propose in-depth prospects with respect to material synthesis and device applications. Undoubtedly, ⅡDs-based conjugated polymers would occupy a significant position in the future of organic electronics, due to diverse building blocks, mature synthetic pathways, tunable side chains, and unique optoelectronic properties.

关键词： isoindigos green synthesis cutting-edge applications polymer field-effect transistors

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Thiazoloisoindigo-based Polymer Semiconductors: Synthesis,Structure-Property Relationship, Charge Carrier Polarity, and Field-Effect Transistor Performance

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chinese Journal of Polymer Science 2024年第1期42卷 24-31,I0006页

作者： Bo-Wen Li Miao Xiong Mei-Hua liu Zhi-Gao Li Long Sang Zi-Han Xiong Biao Xiao Jian Pei Xiao-Bo Wan key laboratory of Optoelectronic Chemical Materials and Devices Ministry of EducationSchoolofOptoelectronic Materials&TechnologyJianghan UniversityWuhan430056China Bejing national laboratoryfor {2. sciences the Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Developing new polymeric semiconductors with excellent device performance is essential for organic electronics. Herein, we synthesized two new thiazoloisoindigo(Tz II)-based polymers, namely, P(Tz II-d Th-d Th) and P(Tz II-d Th-d Tz), by copolymerizing thiophene-flanked Tz II with bithiophene and bithiazole, respectively. Owing to the more electron-deficient nature of bithiazole than bithiophene, P(Tz II-d Th-d Tz)possesses deeper LUMO/HOMO levels of-3.45/-5.47 e V than P(Tz II-d Th-d Th)(-3.34/-5.32.e V). The organic field-effect transistor(OFET) devices based on P(Tz II-d Th-d Th) exhibited p-type behaviors with an average hole mobility value as high as 1.43 cm^(2.·V^(-1)·s^(-1), while P(Tz II-d Th-d Tz)showed typical ambipolar characteristics with average hole and electron mobilities of 0.38 and 0.56 cm^(2.·V^(-1)·s^(-1). In addition, we compared the performances of both polymers with other Tz II-based polymers reported in our previous work, and showed that the charge carrier polarity can be manipulated by adjusting the number of the thiophene units between the acceptor unit. As the increase of the number of thiophene rings,charge carrier polarity shifts from electron-dominated ambipolar transport to hole-dominated ambipolar transport and then to unipolar hole transport in OFETs, which provides an effective {2. design strategy for further optimization of polymer OFET performance.

关键词： Field-effect transistor Charge carrier polarity Thiazoloisoindigo

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Intrinsically flexible displays: key materials and devices

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national Science Review 2022年第6期9卷 171-188页

作者： Zhiyuan Zhao Kai liu Yanwei liu yunlong Guo yunqi liu key laboratory of {2. solids Beijing National Laboratory for Molecular Sciences Institute of Chemistry Chinese Academy of Sciences School of chemistry and Chemical Engineering University of Chinese Academy of Sciences

Continuous progress in flexible electronics is bringing more convenience and comfort to human lives. In this field, interconnection and novel display applications are acknowledged as important future ***, it is a huge scientific and technical challenge to develop intrinsically flexible displays due to the limited size and shape of the display panel. To address this conundrum, it is crucial to develop intrinsically flexible electrode materials, semiconductor materials and dielectric materials, as well as the relevant flexible transistor drivers and display panels. In this review, we focus on the recent progress in this field from seven aspects: background and concept, intrinsically flexible electrode materials, intrinsically flexible organic semiconductors and dielectric materials for organic thin film transistors(OTFTs), intrinsically flexible organic emissive semiconductors for electroluminescent devices, and OTFT-driven electroluminescent devices for intrinsically flexible displays. Finally, some suggestions and prospects for the future development of intrinsically flexible displays are proposed.

关键词： intrinsically flexible display intrinsically flexible electrode organic semiconductor transistor driver electroluminescent device

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Innovations in spider silk-inspired artificial gel fibers:Methods,properties,strengthening,functionality,and challenges

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SusMat 2024年第3期4卷 104-163页

作者： Abdul Qadeer Khan Wenjin Guo Sitong Li yutian Zhu Jie Bai Zunfeng liu Weiqiang Zhao Xiang Zhou State key laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer MaterialsTianjin Key Laboratory of Functional Polymer MaterialsSmart Sensing Interdisciplinary Science CenterCollege of ChemistryNankai UniversityTianjinChina Department of Science China Pharmaceutical UniversityNanjingChina College of Material Chemistry and Chemical EngineeringHangzhou Normal UniversityHangzhouChina Chemical Engineering College Inner Mongolia University of TechnologyHohhotChina

Spider silk,possessing exceptional combination properties,is classified as a biogel ***,it serves as a valuable origin of inspiration for the advancement of various artificial gel fiber materials with distinct *** fibers exhibit promising potential for utilization in diverse fields,including smart textiles,artificial muscle,tissue engineering,and strain ***,there are still numerous challenges in improving the performance and functionalizing applications of spider silk-inspired artificial gel ***,to gain a penetrating insight into bioinspired artificial gel fibers,this review provided a comprehensive overview encompassing three key aspects:the fundamental design concepts and implementing strategies of gel fibers,the properties and strengthening strategies of gel fibers,and the functionalities and application prospects of gel *** particular,multiple strengthening and toughening mechanisms were introduced at micro,nano,and molecular-level structures of gel ***,the existing challenges of gel fibers are *** review aims to offer significant {2.dance for the development and application of artificial gel fibers and inspire further research in the field of high-performance gel fibers.

关键词： artificial gel fibers biomimetic functionality spider silk strengthening

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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 {2. Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China School of Materials Science and Engineering Peking UniversityBeijing 100871China beijing national {2. 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 {2. 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 {2. 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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Polymer Fiber Rigid Network with High Glass Transition Temperature Reinforces Stability of organic Photovoltaics

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Nano-Micro Letters 2024年第11期16卷 56-69页

作者： Qiao Zhou Cenqi Yan Hongxiang Li Zhendong Zhu yujie Gao Jie Xiong Hua Tang Can Zhu Hailin yu Sandra P.Gonzalez Lopez Jiayu Wang Meng Qin Jianshu Li Longbo Luo Xiangyang liu Jiaqiang Qin Shirong Lu Lei Meng Frédéric Laquai Yongfang Li Pei Cheng College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065People’s Republic of China KAUST Solar Center Physical Science and Engineering DivisionKing Abdullah University of Science and Technology(KAUST)ThuwalKingdom of Saudi Arabia beijing national {2. for molecular sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190People’s Republic of China Department of Material Science and Technology Taizhou UniversityTaizhou 318000People’s Republic of China

organic photovoltaics(OPVs)need to overcome limitations such as insufficient thermal stability to be *** reported approaches to improve stability either rely on the development of new materials or on tailoring the donor/acceptor morphology,however,exhibiting limited ***,it is timely to develop an easy method to enhance thermal stability without having to develop new donor/acceptor materials or donor–acceptor compatibilizers,or by introducing another third ***,a unique approach is presented,based on constructing a polymer fiber rigid network with a high glass transition temperature(T_(g))to impede the movement of acceptor and donor molecules,to immobilize the active layer morphology,and thereby to improve thermal stability.A high-T_(g) one-dimensional aramid nanofiber(ANF)is utilized for network *** OPVs with ANF network yield superior thermal stability compared to the ANF-free *** ANF network-incorporated active layer demonstrates significantly more stable morphology than the ANF-free counterpart,thereby leaving fundamental processes such as charge separation,transport,and collection,determining the device efficiency,largely *** strategy is also successfully applied to other photovoltaic *** strategy of incorporating a polymer fiber rigid network with high T_(g) offers a distinct perspective addressing the challenge of thermal instability with simplicity and universality.

关键词： Inverted organic photovoltaics Thermal stability Aramid nanofibers Morphology control Charge carrier dynamics

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