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Polyelectrolyte complex-based thermochromic hydrogels containing carbonized polymer dots for smart windows with fast response,excellent solar modulation ability,and high durability

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SmartMat 2024年第2期5卷 124-136页

作者： Yuting Wang Xu Fang Siheng Li Ni An Hongyu Pan Junqi Sun state key laboratory of supramolecular structure and materials Jilin UniversityChangchunChina

Thermochromic smart windows have gained increasing popularity in light modulation and energy management in buildings.However,the fabrication of flexible thermochromic smart windows with high luminous transmittance(Tlum),tailorable critical temperature(τc),strong solar modulation ability(ΔTsol),and long-term durability remains a huge challenge.In this study,hydrogel-based thermochromic smart windows are fabricated by sandwiching thermochromic hydrogels of polyallylamine hydrochloride,polyacrylic acid,and carbonized polymer dots(CPDs)complexes between two pieces of transparent substrates.Benefiting from the incorporation of nanosized CPDs,the thermochromic hydrogel has an ultrahigh Tlum of~98.7%,a desirableτc of~24.2℃,aΔTsol of~89.3%and a rapid transition time of~3 s from opaque state to transparent state.Moreover,the thermochromic hydrogel exhibits excellent anti-freezing ability,tight adhesion toward various substrates,and excellent self-healing capability.The self-healing capability enables the fabrication of large-area smart windows by welding multiple hydrogel pieces.The smart windows retain their original thermochromic properties after being stored under ambient conditions for at least 147 days or undergoing 10,000 uninterrupted heating/cooling cycles.The model houses with smart windows can achieve a temperature reduction of 9.2℃,demonstrating the excellent indoor temperature modulation performance of the smart windows.

关键词： carbonized polymer dots polyelectrolyte complexes smart windows thermochromic hydrogels

Differentiated self-assembly through orthogonal noncovalent interactions towards the synthesis of two-dimensional woven supramolecular polymers

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Chinese Chemical Letters 2024年第5期35卷 179-182页

作者： Zhenzhu Wang Chenglong Liu Yunpeng Ge Wencan Li Chenyang Zhang Bing Yang Shizhong Mao Zeyuan Dong state key laboratory of supramolecular structure and materials College of ChemistryJilin UniversityChangchun 130012China Center for supramolecular Chemical Biology Jilin UniversityChangchun 130012China

Molecular weaving is a powerful approach to make molecularly woven materials that have showed unprecedented characteristics and properties intrinsically distinct to those of non-woven materials.We here report a facile and efficient approach for the synthesis of 2D woven supramolecular polymers by differentiated self-assembly through orthogonal noncovalent interactions.Importantly,the difference in binding strength of two orthogonal noncovalent interactions can be used to control the process of molecular weaving.Consequently,single-layered 2D woven supramolecular polymers were synthesized and fully characterized by various techniques.This study demonstrates a controllable method for molecular weaving,and will significantly hasten the development of molecularly woven materials.

关键词： Differentiated self-assembly Double-stranded helix Molecular weaving supramolecular chemistry Two-dimensional polymer

Chemoselective and Living/Controlled Polymerization of Alkenyl Methacrylates by the Phosphonium Ylide/Organoaluminum Lewis Pairs

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Chinese Journal of Polymer Science 2024年第2期42卷 159-167,I0005页

作者： Zhi-Kang Chen Wu-Chao Zhao Yi-Ling Zhao Cong-Lei Liu Liu-Yin Jiang Yue-Tao Zhang Hong-Ping Zhu state key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China state key laboratory of supramolecular structure and materials College of ChemistryJilin UniversityChangchun130012China

Chemoselective,living/controlled polymerizations of allyl methacrylate(AMA) and vinyl methacrylate(VMA) with/without methyl methacrylate(MMA) by using the phosphonium ylide/organoaluminum based Lewis pairs(LPs) have been realized.The P-ylide-2/AIMe(BHT)_(2)(Pylide-2=Ph_(3)P=CHMe and BHT=2,6-iBu_(2)-4-MeC_(6)H_(2)O) was demonstrated to be superior by which homopolymers PAMAs(M_(n)=27.6-111.5kg/mol and ■=1.14-1.25) and PVMAs(M_(n)=28.4-78.4 kg/mol and ■=1.12-1.18) and block copolymers PMMA-b-PAMA,PAMA-b-PVMA,PAMA-bPMMA,PMMA-b-PAMA-b-PMMA,PAMA-b-PMMA-b-PAMA,and PAMA-b-PVMA-b-PAMA were synthesized.In the polymerizations,all of the monomers were reacted by the conjugated ester vinyl groups leaving intactly the nonconjugated acryloxy groups.The pendant acryloxy groups attached to the main chain enable further to post-functionalization by the AIBN-induced radical "thiol-ene" reaction using PhCH_(2)SH.The thiolether side group-containing polymers PAMA-SCH_(2)Ph and PAMA-SCH_(2)Ph-b-PMMA-b-PAMA-SCH_(2)Ph were thus prepared.

关键词： Phosphonium ylide Alkenyl methacrylate Chemoselectivity Living/controlled polymerization Post-functionalization

Living/controlled polymerization of vinylpyridines into sequence-regulated copolymers by Lewis pair

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Science China Chemistry 2024年第8期 2737-2746页

作者： Qiankun Ding Wuchao Zhao Fukuan Li Jianghua He Yuetao Zhang Department of state key laboratory of supramolecular structure and materials College of Chemistry Jilin University

The poly(vinylpyridine)(PVP) based(co)polymers are of particular interest in materials science, due to their multifunctionality and diverse applications. So far, there is no report on the sequence-regulated copolymerization of vinylpyridines(VPs) and methacrylate monomer in one-step manner yet. Here we designed and synthesized a series of guanidine phosphines as Lewis base(LB), which is combined with bulky organoaluminium to construct Lewis pairs(LPs) for polymerization of VPs. The living/controlled polymerization of 4-vinylpyridine(4-VP) or 2-vinylpyridine(2-VP) can be accomplished with remarkable efficiency by such Lewis pair polymerization(LPP), furnishing polymers with high molecular weight(up to 288 kg/mol) and narrow molecular weight distribution(as low as 1.17). Mechanistic studies reveal the interaction of LPs and formation of zwitterionic intermediates, providing solid evidences to support the proposed polymerization mechanism. More importantly, by simply adjusting the LA dosage, this LPP strategy realizes the unprecedented control over the sequence regulation of 2-VP-based copolymers from gradient to block in one-step manner, regardless of the monomer ratio, which greatly expands the versatility of the LPP.

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High-efficiency crystalline white organic lightemitting diodes

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Light(Science & Applications) 2024年第4期13卷 747-759页

作者： Yijun Liu Feng Zhu Yue Wang Donghang Yan state key laboratory of Polymer Physics and Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China. School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China. state key laboratory of supramolecular structure and materials Jilin UniversityChangchun 130012China

Crystalline white organic light-emitting diodes(C-WOLEDs)are promising candidates for lighting and display applications.It is urgently necessary,however,to develop energy-saving and high-efficiency C-WOLEDs that have stable and powerful emission to meet commercial demands.Here,we report a crystalline host matrix(CHM)with embedded nanoaggregates(NA)structure for developing high-performance C-WOLEDs by employing a thermally activated delayed fluorescence(TADF)material and orange phosphorescent dopants(Phos.-D).The CHM-TADFNA-D WOLED exhibit a remarkable EQE of 12.8%,which is the highest performance WOLEDs based on crystalline materials.The device has a quick formation of excitons and a well-designed energy transfer process,and possesses a fast ramping of luminance and current density.Compared to recently reported high-performance WOLEDs based on amorphous material route,the C-WOLED achieves a low series-resistance Joule-heat loss ratio and an enhanced photon output,demonstrating its significant potential in developing the next-generation WOLEDs.

关键词： diodes dopant crystalline

Thienothiophene-centered ladder-type π-systems that feature distinct quinoidal π-extension

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Chinese Chemical Letters 2024年第5期35卷 249-253页

作者： Jiaxiang Guo Zeyi Li Tianyu Zhang Xinyu Tian Yue Wang Chuandong Dou state key laboratory of supramolecular structure and materials College of ChemistryJilin UniversityChangchun 130012China Jiangsu Engineering laboratory of Novel Functional Polymeric materials Soochow UniversitySuzhou 215123China

Quinoidalπ-conjugated structures,a kind of fundamental subunits for organicπ-systems,may produce some intriguing optical,electronic and magnetic properties of polycyclic hydrocarbons(PHs).Herein,we report two thienothiophene-centered ladder-type polycyclic molecules(1 and 2),which possess one quinoidal thienothiophene moiety and two para-quinodimethane(p-QDM)subunits,respectively.As theoretically and experimentally studied,while 1 is a fully closed-shell molecule,2 owns an open-shell structure along with partial contribution of tetraradical state that is induced by the resonance of p-QDM.Moreover,although 2 has a largerπ-conjugated skeleton and open-shell electronic state,it exhibits larger bandgap and blue-shifted absorption.On the other hand,the reversible oxidation activity of 1 enables the preparation of its dication 1^(2+),and the studies on its single-crystal and aromatic structures demonstrate that its two positive charges are delocalized onto the oxygen atoms,thus achieving fullyπ-extended structure and near-infrared absorption.This study not only gains insight into quinoidalπ-subunits,but also provides an important basis for the development of antiaromatic and open-shellπ-electron materials.

关键词： Thienothiophene Quinoidal conjugation Open-shell structure Aromaticity Photophysical properties

A highly reduced Mo_(74) polyoxometalate featuring high proton conductivity accessed by building block strategy

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Science China Chemistry 2024年第3期67卷 862-868页

作者： Shi-Yi Liu Xue-Xin Li Wei-Chao Chen Kui-Zhan Shao Xin-Long Wang Chao Qin Zhong-Min Su key laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China state key laboratory of supramolecular structure and materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Highly reduced polyoxometalates(POMs) are predicted to be used as rather high energy density materials;however,it still suffers from the limited cluster species and reduction ratio.Here we demonstrate that it is possible to employ the building block strategy to generate a highly reduced polyoxomolybdate(C_(2)H_(8)N)_(14)(NH_(4))_(4)H_(14)[Mo_(48)-ⅤMo_(26)ⅥO_(202)(OH)_(12)(SO_(4))_(6)]·46H_(2)O(Mo_(74)).The fundamental Mo-based{Mo_x}(x=4,5,and 6) building blocks,which are templated by tetra-coordinated anions{MoO_(4)}or{SO_(4)},not only lay foundation for the formation of Mo_(74) featuring an unprecedented reduction ratio of 65%,but also give rise to SBBs-mediated(secondary building blocks) supramolecular dense packing interactions among the isolated Mo_(74) clusters that are favorable for proton conduction.Remarkably,high proton conductivity(2.04×10^(-2)S cm^(-1)) had been realized at 50℃ and 90% relative humidity,revealing one of the well-known POMs-based crystalline proton conducting materials.This result highlights that this building block approach possesses great potential in producing highly reduced POM systems that can achieve controllable reduced ratio and desirable properties.

关键词： polyoxometalate building block molybdenum highly reduced state proton conduction

A scalable one-pot strategy for the development of polymer electrolytes adaptable to room-temperature high-voltage lithium batteries

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Chinese Chemical Letters 2024年第3期35卷 461-467页

作者： Yue Guo Xinxin Qu Zhen Li Ruiyuan Tian Xiaokong Liu state key laboratory of supramolecular structure and materials College of ChemistryJilin UniversityChangchun 130012China key laboratory of Physics and Technology for Advanced Batteries(Ministry of Education) College of PhysicsJilin UniversityChangchun 130012China

Poly(ethylene oxide)(PEO)polymer electrolytes(PEs)have been commercially applied in LiFePO_(4)||Li solid-state lithium batteries(SSLBs).However,it remains challenging to develop PEO-based PEs applicable to the high-voltage SSLBs with higher energy density,owing to the poor electrochemical stability of PEO.Herein,we report a scalable strategy for fabricating PEO-based PEs with high-voltage compatibility,by exploiting a new mechanism to stabilize the cathode-electrolyte interface in the highvoltage SSLBs.The protocol only involves a one-pot synthesis procedure to covalently crosslink the PEO chains,in the presence of high-content lithium bis(trifluoromethylsulphonyl)imide(LiTFSI)salts and N,N-dimethylformamide(DMF).LiTFSI-DMF supramolecular aggregates are formed and firmly embedded in the polymer network,endowing the PE with high room-temperature ionic conductivity.The dissociated and highly concentrated TFSI^-anions can enter the Helmholtz layer close to the high-voltage cathode,leading to the formation of a thin and homogeneous cathode electrolyte interface(CEI),mainly composed of LiF,on the cathode.The CEI with high electrochemical stability can effectively stabilize the cathode-electrolyte interface,enabling long-term stable cycling of the high-voltage LiCoO_(2)||Li and nickelrich NCM_(622)||Li batteries at room temperature.The simplicity and scalability of the strategy makes the reported PEO-based PE potentially applicable in high-voltage SSLBs in practice.

关键词： Lithium batteries Polymer electrolytes Poly(ethylene oxide) Energy density High-voltage cathodes

In situ preparation of Nanoparticles/polymer composites

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Science China(Technological Sciences) 2008年第11期51卷 1886-1901页

作者： SUN HaiZhu & YANG Bai state key lab of supramolecular structure and materials, College of Chemistry, Jilin University, Changchun 130012, China College of Chemistry, Northeast Normal University, Changchun 130024, China state key lab of supramolecular structure and materials College of Chemistry Jilin University Changchun China College of Chemistry Northeast Normal University Changchun China

Nanoparticle (NP) is the matter between molecule and bulk material. It has attracted much attention in catalysis, optoelectronics and biology due to its unique physical and chemical properties. Incorporation of these NPs into the polymer matrix is one of the best methods to display their special functions, which not only stabilize the NPs but also realize the functional assembly of NPs and polymers. However, reali- zation of this idea depends largely on the compatibility of NPs and polymers as well as the interaction between them. Therefore, many methods have been developed to prepare the composites of NPs and polymers in order to obtain the function ex- pected. In this review, we mainly focus on the combination of in situ method with other methods to synthesize different functional one-dimension, two-dimension as well as bulk composites, which has been recently developed by our group. The most striking character of our method is the excellent compatibility between NPs and polymers which ensures a homogeneous distribution of NPs in the polymer matrix. The existence of the polymer network makes the NPs more stable, and is significant for displaying their functions.

关键词： in situ nanoparticle polymer composite function