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Strong Magneto-Chiroptical Effects through Introducing Chiral Transition-Metal Complex Cations to Lead Halide

Angewandte Chemie 2024年第3期137卷

作者： Haolin Lu Fenglian Qi Hebin Wang Tengfei He Bing Sun Prof. Xiaoqing Gao Andrew H. Comstock Sehrish Gull Yunxin Zhang Tianjiao Qiao Tianyin Shao Prof. You-Xuan Zheng Prof. Dali Sun Prof. Yongsheng Chen Prof. Hao-Li Zhang Prof. Zhiyong Tang Prof. Guankui Long Tianjin Key Lab for Rare Earth Materials and Applications Renewable Energy Conversion and Storage Center (RECAST) Smart Sensing Interdisciplinary Science Center School of Materials Science and Engineering National Institute for Advanced Materials Nankai University Tianjin 300350 China Chinese Academy of Science (CAS) Key Laboratory of Nanosystem and Hierarchy Fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Beijing 100190 China The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials Institute of Polymer Chemistry Renewable Energy Conversion and Storage Center (RECAST) College of Chemistry Nankai University Tianjin 300350 China State Key Laboratory of Applied Organic Chemistry (SKLAOC) Key Laboratory of Special Function Materials and Structure Design (MOE) College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 China Wenzhou Institute University of Chinese Academy of Sciences Wenzhou 325000 China Department of Physics North Carolina State University Raleigh NC 27695–8202 USA State Key Laboratory of Coordination Chemistry Collaborative Innovation Center of Advanced Microstructures Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 China

The interplay between chirality with magnetism can break both the space and time inversion symmetry and have wide applications in information storage, photodetectors, multiferroics and spintronics. Herein, we report the chiral transition-metal complex cation-based lead halide, R -CDPB and S -CDPB. In contrast with the traditional chiral metal halides with organic cations, a novel strategy for chirality transfer from the transition-metal complex cation to the lead halide framework is developed. The chiral complex cations directly participate the band structure and introduce the d - d transitions and tunable magneto-chiroptical effects in both the ultraviolet and full visible range into R -CDPB and S -CDPB. Most importantly, the coupling between magnetic moment of the complex cation and chiroptical properties is confirmed by the magneto-chiral dichroism. For the band-edge transition, the unprecedented modulation of +514 % for S -CDPB and −474 % for R -CDPB was achieved at −1.3 Tesla. Our findings demonstrate a novel strategy to combine chirality with magnetic moment, and provide a versatile material platform towards magneto-chiroptical and chiro-spintronic applications.

关键词： chiral lead halide complex ion chiroptical effect magneto-chiral dichroism A-site engineering

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Synthesis of Cyclic Oligo(ethylene adipate)s and Their Melt polymerization to Poly(ethylene adipate)

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Chinese Journal of polymer Science 2017年第9期35卷 1051-1060页

作者： min lu xiang zhu xiao-hong li xiao-ming yang 屠迎锋 Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

We present here the first synthesis of cyclic oligo（ethylene adipate）s （COEAs） via pseudo-high dilution condensation reaction of adipoyl chloride with ethylene glycol, and the synthesis of corresponding poly（ethylene adipate）（PEA） via the melt polymerization of COEAs. The structure of COEAs was characterized and proved by 1H-NMR and MALDI-TOF mass measurements. The effects of organic base, reaction temperature and the ratio of adipoyl chloride to ethylene glycol on the yield of COEAs were studied, and the optimum reaction condition was revealed. PEA, a diacid and diol based semi-crystalline green aliphatic polyester, was synthesized by the melt polymerization of COEAs using Ti（n-C4H90）4 as catalyst and 1,10-decanediol as initiator at 200 ℃, which follows the polycondensation-coupling ring- opening polymerization method. Our strategy should be applicable to the synthesis of versatile aliphatic polyesters based on diacid and diol monomers, which have potential applications as biocompatible and biodegradable materials.

关键词： Cyclic oligoesters Pseudo-high dilution reaction condition Polycondensation-coupling ring-openingpolymerization Aliphatic polyesters

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Recent Advances of CuAAC Click Reaction in Building Cyclic polymer

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Chinese Journal of polymer Science 2017年第3期35卷 317-341页

作者： zhi-hao huang yan-yan zhou zi-mu wang ying li wei zhang nian-chen zhou 张正彪朱秀林 State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

Cyclic polymers have attracted more and more attentions in recent years because of their unique topological structures and characteristic properties in both solution and bulk state. There are relatively few reports on cyclic polymers, partly because of the more demanding synthetic procedures. In recent years, 'click' reaction, especially Cu(I)-catalyzed azide-alkyne cycloaddition(CuAAC), has been widely utilized in the synthesis of cyclic polymer materials because of its high efficiency and low susceptibility to side reactions. In this review, we will focus on three aspects:(1) Constructions of monocyclic polymer using CuAAC 'click' chemistry;(2) Formation of complex cyclic polymer topologies through CuAAC reactions;(3) Using CuAAC 'click' reaction in the precise synthesis of molecularly defined macrocycles. We believe that the CuAAC click reaction is playing an important role in the design and synthesis of functional cyclic polymers.

关键词： Cu(I)-catalyzed azide-alkyne cycloaddition(CuAAC) 'Click' chemistry Cyclic polymer Reversible deactivation radical polymerization(RDRP) Atom transfer radical polymerization(ATRP) Reversible addition fragmentation chain transfer polymerization(RAFT)

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Effect of Sequence Structure on Wetting Behaviors of Fluorinated Methacrylate polymers Based on Perfluorohexylethyl Methacrylate and Stearyl Acrylate

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Chinese Journal of polymer Science 2017年第9期35卷 1061-1072页

作者： zi-xu gu jun cheng ming-zu zhang jin-lin he 倪沛红 College of Chemistry Chemical Engineering and Materials Science State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis Soochow University Suzhou 215123 China

Due to the non-crystalline properties of short chain perfluoroalkyl groups, using short chain perfluoroalkyl to stabilize low surface free energy polymers has been a challenging task. In this study, we prepare a series of random copolymers poly（perfluorohexylethyl methacrylate）-co-poly（stearyl acrylate）（P13FMA-co-PSA） and block copolymers poly（perfluorohexylethyl methacrylate）-b-poly（stearyl acrylate）（P13FMA-b-PSA）, and systematically investigate the effects of the sequence structure and the content of 13FMA of the fluorinated copolymers on surface free energy and surface reorganization. Static/dynamic contact angle goniometry and water/oil repellency analyses demonstrate that the random polymer P13FMA-co-PSA could not achieve low surface free energy and low surface reorganization at the same time. In contrast, for the block copolymer P13FMA-b-PSA, both low surface free energy and low surface reorganization are acquired simultaneously. The results of X-ray photoelectron spectroscopy （XPS）, dynamic contact angle goniometry and differential scanning calorimetry （DSC） reveal the above-mentioned properties. The consecutive 13FMA segments improve the surface fluorine density, while the consecutive SA chains enhance the crystallinity of the SA segments, and further hinder the surface reorganization of the perfluoroalkyl groups. Therefore, P13FMA-b-PSA exhibits a higher utilization efficiency of fluorine atoms and a better structural stability than P13FMA-co-PSA.

关键词： Surface free energy Surface reorganization Perfluorohexylethyl methacrylate （13FMA） Stearyl acrylate （SA） Water/oil repellency

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Precise Molecular Weight Determination and Structure Characterization of End-functionalized polymers:An NMR Approach via Combination of One-dimensional and Two-dimensional Techniques

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Chinese Journal of polymer Science 2017年第5期35卷 681-692页

作者： dong-xue chen ling-feng gao 李晓虹屠迎锋 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 UniversitySuzhou 215123China

We present here the application of one-dimensional and two-dimensional NMR techniques to characterize the structure of methoxyl end-functionalized polystyrenes （PS）. The peaks in 1H-NMR spectra corresponding to main-chain, side-chain and chain-end groups are assigned by 1H-1H gCOSY, 1H-13C gHSQC and gHMBC spectra. For the first time, the spin-lattice relaxation time （T1） of protons of the chain-ends is revealed to be affected more by polymer molecular weight （MW） than by the protons of the main-chains and the side-chains （almost independent from MW）. As a result, a much higher delay time （dl） for chain-ends （d1〉 20T1） is needed for quantitative NMR measurement when using end-group estimation method to obtain the MW of PS, which is in accordance with the value estimated by GPC. An improved method for the polymer MW determination is established, by combination of different NMR techniques to distinguish the peaks, and a large dl setting to achieve quantitative NMR analysis.

关键词： NMR spectroscopy Molecular weight determination Quantitative NMR analysis 2D NMR

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Polylipopeptide-based multifunctional nanomedicines for targeted cancer delivery

Polylipopeptide-based multifunctional nanomedicines for targ...

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The 3rd International Conference on Nanomedicine of China（ChinaNanomedicine 2018）

作者： Chao Deng Min Qiu Jian Zhang Huanli Sun Fenghua Meng Ru Cheng Zhiyuan Zhong Biomedical Polymers Laboratory and Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationCollege of ChemistryChemical Engineering and Materials ScienceSoochow University

Poly(ethylene glycol)-b-polypeptide copolymers with excellent safety,are one of the most clinically studied materials for anticancer drug delivery[1].For example,paclitaxel(PTX),doxorubicin(Dox),and cisplatin-loaded polypeptidebased nanotherapeutics have proceeded into phase Ⅱ and Ⅲ clinical trials,and achieved enhanced therapeutic efficacy against intractable tumors and reduced side effects in comparison with free *** should be noted,however,that these nanoformulations,mostly based on hydrophilic polypeptides,usually involve multistep synthesis,including protection and deprotection of functional groups and drug *** based on hydrophobic polypeptide often plagued with low drug loading and insufficient in vivo *** this end,we designed and prepared a series of poly(a-aminopalmitic acid)-based nanoplatforms,including micelles and polymersomes for targeted delivery of small anti-cancer drugs,protein,and siRNA[2-3].

关键词： Polylipopeptide-based multifunctional nanomedicines for targeted cancer delivery

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Biodegradable polymersomes with Structure Inherent Fluorescence and Targeting Capacity for Enhanced Photo-Dynamic Therapy

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Angewandte Chemie 2021年第32期133卷

作者： Dr. Shoupeng Cao Yifeng Xia Dr. Jingxin Shao Beibei Guo Yangyang Dong Dr. Imke A. B. Pijpers Prof. Dr. Zhiyuan Zhong Prof. Dr. Fenghua Meng Dr. Loai K. E. A. Abdelmohsen Dr. David S. Williams Prof. Dr. Jan C. M. van Hest Bio-Organic Chemistry Institute for Complex Molecular Systems Eindhoven University of Technology P.O. Box 513 (STO 3.41) 5600 MB Eindhoven The Netherlands Biomedical Polymers Laboratory and Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 P. R. China School of Cellular and Molecular Medicine University of Bristol Bristol UK

Biodegradable nanostructures displaying aggregation-induced emission (AIE) are desirable from a biomedical point of view, due to the advantageous features of loading capacity, emission brightness, and fluorescence stability. Herein, biodegradable polymers comprising poly (ethylene glycol)-block-poly(caprolactone-gradient-trimethylene carbonate) (PEG-P(CLgTMC)), with tetraphenylethylene pyridinium-TMC (PAIE) side chains have been developed, which self-assembled into well-defined polymersomes. The resultant AIEgenic polymersomes are intrinsically fluorescent delivery vehicles. The presence of the pyridinium moiety endows the polymersomes with mitochondrial targeting ability, which improves the efficiency of co-encapsulated photosensitizers and improves therapeutic index against cancer cells both in vitro and in vivo. This contribution showcases the ability to engineer AIEgenic polymersomes with structure inherent fluorescence and targeting capacity for enhanced photodynamic therapy.

关键词： aggregation-induced emission biodegradable polymersomes mitochondria targeting photo-dynamic therapy polycarbonates

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Preparation of optical active single-handed helical barium titanate nanotubes and characterization of dielectric properties

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Chinese Chemical Letters 2017年第5期28卷 1111-1113页

作者： Shu-Wei Lin Wen-Hu Qian Hong-Jing Huo Bao-Zong Li Yi Li Yong-Gang Yang Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and EngineeringState and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

Left and right-handed helical barium titanate nanotubes are prepared with the impregnation of Ba（OH）2 into single-handed helical titania *** angle X-ray diffraction pattern and transmission electron microscopy image indicate that they are constructed by nanoparticles with a partially crystalline *** diffuse reflertance circular dichroism spectra indicate that they exhibit optical activity which was proposed to originate from chiral defects on the inner surfaces of the *** the dielectric constant and tanδ decrease with increasing the *** 10 and 100 Hz,one dielectric constant peak at 9.6℃ and one tanδ peak at 5.0℃ are observed at -120℃ to 180℃.

关键词： Dielectrics Barium titanate Optical materials and properties Templating approach Nanoparticles

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Characterization of a Chiral Low Molecular Weight Gelator in Gel State Using Various Circular Dichroism Methods

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Chemical Research in Chinese Universities 2017年第1期33卷 119-121页

作者： SUN Huayan QIN Jiaming LI Yi LI Baozong YANG Yonggang Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 P. R. China

Circular dichroism（CD） is usually used to study supramolecular chirality. With the development of CD methods, diffuse transmission CD（DTCD） and diffuse reflectance CD（DRCD） have been developed. However, the relationship among CD, DTCD and DRCD has not been well-studied. A chiral low molecular weight gelator was synthesized, which can result in a transparent physical gel in deionized water. The field-emission electron microscopy images show that the gel is able to self-assemble into left-handed helical fibers. The CD and DTCD spectra are al- most identical, but they partially differ from the DRCD spectrum. Based on the TD-DFT calculated CD spectrum, the DRCD spectrum is shown to be more accurate.

关键词： Optical activity Circular dichroism Self-assembly

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Preface: The Fourth Symposium on Innovative polymers for Controlled Delivery, September 23-26, 2016, Suzhou, China

Preface: The Fourth Symposium on Innovative Polymers for Con...

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作者： Zhong, Zhiyuan Feijen, Jan Biomedical Polymers Laboratory Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University China

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