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In situ thermoresponsive supramolecular assembly for switchable circularly polarized luminescence

Science China Chemistry 2024年第7期67卷 2362-2372页

作者： Menghan Pan Gong Zhang Haotian Ma Xiaoxiao Cheng Jieai Li Wei Zhang State and Local joint engineering laboratory for novel functional polymeric materials Jiangsu Engineering Laboratory of Novel Functional Polymeric MaterialsSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China School of Chemical and Environmental engineering Anhui Polytechnic UniversityWuhu 241000China

The dynamic regulation of circularly polarized luminescence(CPL)holds profound significance in various fields,such as highlevel information storage and *** we developed a chiral amphiphilic molecule,CPSB-GLU-PEG350(CGP),composed of aggregation-induced emission(AIE)chromophores(Z)-4-(1-cyano-2-phenylvinyl)benzoic acid(CPSB),a chiral linker Glutamic acid and polyethylene glycol(PEG)thermoresponsive *** the self-assembled supramolecular system formed by CGP,we have achieved in-situ temperature-responsive chiral structures,facilitating the thermal control switch of the CPL *** dynamics simulations demonstrate the distinct behaviors of AIE and PEG units during the temperature-variable assembly ***,by co-assembling achiral dye molecules with CGP,we have expanded the color range of the temperature-responsive CPL assembly system in situ and confirmed the occurrence of circularly polarizedF?rster resonance energy transfer(C-FRET)phenomenon in this process,which successfully enriched the strategies for in-situ CPL control in aqueous *** addition,the contactless radiative energy transfer of CPL can also be realized in this system,exhibiting more flexible temperature regulation of the CPL *** study provides a convenient and universal strategy for the construction of dynamically smart chiroptical materials.

关键词： circularly polarized luminescence in-situ thermoresponsive supramolecular assembly energy transfer

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Persistent radical anion of perylene dianhydride:an emerging metal-free photocatalyst for near-infrared photocontrolled RAFT polymerization

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Science China Chemistry 2024年第2期67卷 677-686页

作者： Haitao Zhao Guoqing Bian Xiang Xu Weiwei He Lifen Zhang Zhenping Cheng State and Local joint engineering laboratory for novel functional polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China

Developing a new type of photocatalyst(PC) and catalytic mechanism for near-infrared(NIR) photocontrolled reversibledeactivation radical polymerization(RDRP) system is charming but ***,a novel PC of the persistent radical anion(PRA)(possessing the properties of both radical and anion) was developed for NIR photocontrolled reversible additionfragmentation chain transfer(RAFT) polymerization,enabling successful polymerization while gaining a deep insight into the mechanism of photo-induced electron transfer RAFT(PET-RAFT) *** from the conventional and wellaccepted reductive quenching(RQ) pathway,in which the radical anion intermediates of PCs(PCs^(·-)) must be generated in an excited state(ES),here,the PRA(3,4,9,10-perylenetetracarboxylic dianhydride radical anion(PTCDA^(·-))) could generate conveniently in situ in the ground state(GS) and subsequently serve as highly efficient PC in the NIR region(740–850 nm).The successful implementation of this strategy elucidates the peculiar role played by light and the real way of electron transfer *** fact,the transfer of a single electron from PRA to chain transfer agent(CTA) and cleavage of the C–S bonds is a process from ES to GS,rather than always from GS(PCs^(·-)) to GS(CTA) in the RQ pathway as is well known to *** addition,the excellent spatial-temporal control and powerful penetration ability of the NIR light were also confirmed by this PRAcatalyzed polymerization system.

关键词： photocatalyst persistent radical anion(PRA) near-infrared(NIR)light reversible-deactivation radical polymerization(RDRP) photo-induced electron transfer RAFT(PET-RAFT)polymerization

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Polymer Mechanochemistry on Reactive Species Generated from Mechanochemical Reactions

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Chinese Journal of Chemistry 2024年第12期42卷 1418-1432页

作者： Xiaolong Chen Hang Shen Zhengbiao Zhang State and Local joint engineering laboratory for novel functional polymeric materials Suzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China

Comprehensive Summary Polymer mechanochemistry on reactive species has attracted more and more attentions over the past 20 years,as the mechanochemical generation of reactive species has a great potential in developing different polymeric materials for various purposes,such as stress detection,self-healing,self-strengthening,controllable degradation and release of small *** this review,we first discuss the recent progress on polymer mechanochemistry of the reactive species that are generated from the mechanochemical reactions of *** types of reactive species,including radical,zwitterion,ionic,carbene and neutral intermediates,and their applications were reviewed in *** mechanochemical reactions are sensitive to the mechanophore structure and polymer framework,we then discuss how mechanophore isomerism,polymer structure,polymer attachment point,and polymer architecture influence the mechanophore *** last,we provide our perspectives on the polymer mechanochemistry of reactivespecies.

关键词： Stimuli-responsive polymers Polymer mechanochemistry Mechanophore Mechanochemical reaction Reactive species

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Enhancing stability of diradical polycyclic hydrocarbons via P=O-attaching

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Chinese Chemical Letters 2024年第8期35卷 309-313页

作者： Jingyuan Yang Xinyu Tian Liuzhong Yuan Yu Liu 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

Diradical polycyclic hydrocarbons(PHs)have unique open-shell structures and interesting physical ***,owing to high reactivity of unpaired electrons,such open-shell organic diradicaloids are usually less stable than closed-shell systems,limiting their practical *** this study,we report P=O-attaching of diradical PHs as a new strategy to enhance their stability while maintaining diradi-cal *** P=O-attached PHs containing the indeno[1,2-b]fluorene,fluoreno[3,2-b]fluorene and indeno[2,1-b]fluoreneπ-skeletons,respectively,were designed and *** theoretically and ex-perimentally proved,two of them have the relatively large diradical characters and open-shell singlet diradical *** comparison to their all-carbon analogues,the attached electron-withdrawing P=O groups endow them with much lower LUMO/HOMO energy levels but preserved magnetic activities and physical properties,such as thermally accessible triplet species and multi-redox ***,the P=O groups effectively decrease their oxidation activities and thereby lead to their remarkably excellent ambient ***,this P=O-attaching strategy will be applicable to other diradical PH systems and may promote the generation of stable organic diradicaloids for radical chemistry and materials.

关键词： Polycyclic hydrocarbons Open-shell structure Diradical character Stability Oxidation activity

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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,*** 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 ***,although 2 has a largerπ-conjugated skeleton and open-shell electronic state,it exhibits larger bandgap and blue-shifted *** 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 *** 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

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A nanoplatform with oxygen self-supplying and heat-sensitizing capabilities enhances the efficacy of photodynamic therapy in eradicating multidrug-resistant biofilms

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Journal of materials Science & Technology 2024年第2期169卷 209-219页

作者： Haixin Zhang Yi Zou Kunyan Lu Yan Wu Yuancheng Lin Jingjing Cheng Chunxia Liu Hong Chen Yanxia Zhang Qian Yu State and Local joint engineering laboratory for novel functional polymeric materials College of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Department of Cardiovascular Surgery of the First Affiliated Hospital and Institute for Cardiovascular Science Suzhou Medical College of Soochow UniversitySoochow UniversitySuzhou 215007China

Bacterial biofilms,especially those caused by multidrug-resistant bacteria,have emerged as one of the greatest dangers to global public *** acceleration of antimicrobial resistance to conventional an-tibiotics and the severe lack of new drugs necessitates the development of novel agents for biofilm *** therapy(PDT)is a promising non-antibiotic method for treating bacterial ***,its application in biofilm eradication is hampered by the hypoxic microenvironment of biofilms and the physical protection of extracellular polymeric *** this study,we develop a composite nanoplatform with oxygen(O_(2))self-supplying and heat-sensitizing capabilities to improve the PDT efficacy against ***_(2)/ICG@PDA nanoparticles(CIP NPs)are fabricated by combining calcium peroxide(CaO_(2))with the photosensitizer indocyanine green(ICG)via electrostatic interactions,followed by coating with polydopamine(PDA).The CIP NPs can gradually generate O_(2)in response to the acidic microenvironment of the biofilm,thereby alleviating its hypoxic *** near-infrared(NIR)irradiation,the nanoplatform converts O_(2)into a significant amount of singlet oxygen(^(1)O_(2))and heat to eradicate *** generated heat enhances the release of O_(2),accelerates the generation of^(1)O_(2)in PDT,increases cell membrane permeability,and increases bacterial sensitivity to^(1)O_(2).This nanoplatform significantly improves the efficacy of PDT in eradicating biofilm-dwelling bacteria without fostering drug *** on biofilm eradication demonstrate that this nanoplatform can eradicate over 99.9999%of methicillin-resistant Staphylococcus aureus(MRSA)biofilms under 5-min NIR ***,these integrated advantages enable the system to promote the healing of MRSA biofilm-infected wounds with negligible toxicity in vivo,indicating great promise for overcoming the obstacles associated with bacterial biofilm eradication.

关键词： Bacterial biofilm Multidrug-resistant bacteria Photodynamic therapy Oxygen supplying Photothermal therapy

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Manipulating the Phase Transition Behavior of Dual Temperature-Responsive Block Copolymers by Adjusting Composition and Sequence

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Chinese Journal of Polymer Science 2024年第2期42卷 176-187,I0006页

作者： Zhi Zou Xiang Xu Hai-Tao Zhao Jian-Nan Cheng Wei-Wei He Li-Fen Zhang Zhen-Ping Cheng Suzhou key laboratory of Macromolecular Design and Precision Synthesis Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationState and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou215123China State Key laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of JiangsuSoochow UniversitySuzhou215123China

Temperature-responsive polymers have garnered significant attention due to their ability to respond to external *** this work,dual temperature-responsive block copolymers are synthesized via reversible addition-fragmentation chain transfer polymerization(RAFT)polymerization utilizing zwitterionic monomer methacryloyl ethyl sulfobetaine(SBMA) and N-isopropyl acrylamide(NIPAAm) as *** thermal responsive behaviors can be easily modulated by incorporating additional hydrophobic monomer benzyl acrylate(BN) or hydrophilic monomer acrylic acid(AA),adjusting concentration or pH,or varying the degree of polymerization of the block chain *** cloud points of the copolymers are determined by UV-Vis spectrophotometry,and these copolymers exhibit both controlled upper and lower critical solu bility temperatures(LCST and UCST) in aqueous *** study analyzes and summarizes the influencing factors of dual temperature responsive block copolymers by exploring the effects of various conditions on the phase transition temperature of temperature-sensitive polymers to explore the relationship between their properties and environment and structure to make them more selective in terms of temperature application range and regulation *** is very interesting that the introduction of poly-acrylic acid(PAA) segments in the middle of di-block copolymer PSBMA_(55)-b-PNIPAAm_(80) to form PSBMA_(55)-b-PAA_(x)-b-PNIPAAm_(80) results in a reversal of temperature-responsive behaviors from 'U'(LCST UCST) type,while the copolymer PSBMA_(55)-b-P(NIPAAm_(80)-co-AA_(x)) *** work provides a clue for tuning the phase transition behavior of polymers for manufacture of extreme smart materials.

关键词： Temperature responsive polymers High critical solubility temperature(UCST) Low critical solubility temperature(LCST) Block copolymers

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Near-infrared organic lasers with ultra-broad emission bands by simultaneously harnessing four-level and six-level systems

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Chinese Chemical Letters 2024年第8期35卷 288-293页

作者： Lei Wang Jun-Jie Wu Chang-Cun Yan Wan-Ying Yang Zong-Lu Che Xin-Yu Xia Xue-Dong Wang Liang-Sheng Liao Jiangsu Key laboratory for Carbon-Based functional materials&Devices Institute of Functional Nano&Soft Materials(FUNSOM)Soochow UniversitySuzhou 215123China Jiangsu engineering laboratory of novel functional polymeric materials College of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Macao Institute of materials Science and engineering Macao University of Science and TechnologyMacao SAR 999078China

Organic lasers with broad emission bands in near-infrared(NIR)region are crucial for their applications in laser communication,night-vision as well as bioimaging owing to the abundance of selectable lasing ***,for most organic gain materials,gain regions are limited in a small wavelength range because of the fixed energy level ***,we design a strategy to realize NIR organic lasers with broad emission bands based on tunable energy level systems induced by cascaded excited-state intramolecular proton transfer(ESIPT).A novel gain material named DHNN was developed,which can undergo a cascaded double-ESIPT process supporting four-level and six-level systems *** doping DHNN into polystyrene microspheres,NIR lasers with tunable emission bands can be achieved based on the careful modulation of ***,organic lasers with an ultra-broad emission band ranging from 700 nm to 900 nm was successfully achieved by harnessing four-level and six-level systems simultaneously.

关键词： Excited-state intramolecular proton transfer Organic solid-state laser Wide gain interval Near-infrared emission Molecular design

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Enhanced charge collection of AgNWs-based top electrode to realize high-performance,all-solution processed organic solar cells

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Science China Chemistry 2024年第10期67卷 3347-3356页

作者： Juanyong Wan Yang Chen Weijie Chen Jinfeng Xia Guang Zeng Jianlei Cao Chuang Jin Yunxiu Shen Xiaoxiao Wu Haiyang Chen Junyuan Ding Xue-mei Ou Yaowen Li Yongfang Li laboratory of Advanced Optoelectronic materials Suzhou Key Laboratory of Novel Semiconductor-Optoelectronics Materials and DevicesCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Jiangsu Key laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China State and Local joint engineering laboratory for novel functional polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Beijing National laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Jiangsu Sidike New materials Science and Technology Co. Ltd.Suqian 215400China

All-solution processed organic solar cells are the ultimate aim of printable photovoltaics,but their electrical losses arising from poor contact of top electrodes greatly limit efficiency *** solve the problem,a solution-processed hybrid top electrode was constructed using silver nanowires(AgNWs)as the skeleton and ZnO nanoparticles(ZnO-NPs)as the *** constructing the skeleton,a spin-rinsing treatment was first used to reduce the amount of the residual insulating polyvinylpyrrolidone wrapped around the AgNWs to promote intimate contact among the AgNWs in the ***,the ZnO-NPs matrix was deposited onto the AgNWs skeleton,bridging the AgNWs skeleton with the underlayer ZnO-NPs electron transporting layer(ETL).The underlayer ZnO-NPs ETL can also induce the growth of the ZnO-NPs matrix to minimize lattice mismatch,which creates additional transport channels from the ETL to the AgNWs skeleton for charge *** a result,the obtained electrode significantly enhances the electrical contact in the device,thus delivering record power conversion efficiencies of 16.04%and 14.54%for rigid and flexible all-solution processed OSCs,respectively.

关键词： solution-processed top electrode organic solar cells AgNWs electrical contact

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Piperazine-Assisted Construction of 2D/3D Wide-Bandgap Perovskite for Realizing High-Efficiency Perovskite/Organic Tandem Solar Cells

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Chinese Journal of Chemistry 2024年第16期42卷 1819-1827页

作者： Ziyue Wang Shuaiqing Kang Xia Zhou Haiyang Chen Xingxing Jiang Zhichao Zhang Jialei Zheng Ruopeng Zhang Weijie Chen Jiandong Zhang Yaowen Li laboratory of Advanced Optoelectronic materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and DevicesCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China Jiangsu Key laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhouJiangsu 215123China State and Local joint engineering laboratory for novel functional polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China College of Physics and Electronics engineering Hengyang Normal UniversityHengyangHunan 421002China

Monolithic perovskite/organic tandem solar cells(TsCs)have gained significant attention due to their easy device integration and the potential to surpass the Shockley-Queisser limit of single-junction solar ***,the surfaces of wide-bandgap perovskite films are densely populated with defects,leading to severe non-radiative recombination and energy *** a consequence,the power conversion efficiency(PCE)of perovskite/organic TSCs lags behind that of other TSC *** address these issues,we designed a functional ammonium salt,4-(2-hydroxyethyl)piperazin-1-ium iodide(Pzol),comprising a piperazine iodide and a terminated hydroxyl group,which was applied for post-treating the perovskite *** findings reveal that Pzol reacts with and consumes residual PbX_(2)(X:I or Br)to form a 2D perovskite component,thereby eliminating Pb^(0)defects,while the terminated hydroxyl group in PZOI can also passivate uncoordinated Pb^(2+).Consequently,the shallow/deep-level defect densities of the 2D/3D perovskite film were significantly reduced,leading to an enhanced PCE of single-junction 2D/3D wide-bandgap perovskite solar cells to 18.18% with a reduced energy loss of 40 ***,the corresponding perovskite/organic TSCs achieved a remarkable PCE of 24.05% with enhanced operational stability(T_(90)~500h).

关键词： Perovskite/organic tandem solar cell Defect states Piperazine ion salt Energy conversion Low-dimensional materials Perovskitesolar cells 2D/3D perovskites Efficiency

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