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Volatile Perovskite Precursor Ink Enables Window Printing of Phase-Pure FAPbI3Perovskite Solar Cells and Modules in Ambient Atmosphere

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Angewandte Chemie 2023年第7期136卷

作者： Linhao Yuan Xining Chen Xianming Guo Shihao Huang Xiaoxiao Wu Yunxiu Shen Hao Gu Yujin Chen Guixiang Zeng Hans-Joachim Egelhaaf Christoph J. Brabec Fu Yang Yaowen Li Yongfang Li Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China School of Chemistry and Chemical Engineering Nanjing University Nanjing 210008 China Suzhou Sunflex New Energy Company Limited Suzhou 215100 China Kuang Yaming Honors School Nanjing University Nanjing 210023 China Institute of Materials for Electronics and Energy Technology (i-MEET) Friedrich-Alexander University Erlangen-Nürnberg Martensstrasse 7 91058 Erlangen Germany Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (HI ERN) Immerwahrstrasse 2 91058 Erlangen Germany Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 Jiangsu P. R. China 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 Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

Despite the great success of perovskite photovoltaics in terms of device efficiency and stability using laboratory-scale spin-coating methods, the demand for high-throughput and cost-effective solutions remains unresolved and rarely reported because of the complicated nature of perovskite crystallization. In this work, we propose a stable precursor ink design strategy to control the solvent volatilization and perovskite crystallization to enable the wide speed window printing (0.3 to 18.0 m/min) of phase-pure FAPbI 3 perovskite solar cells (pero-SCs) in ambient atmosphere. The FAPbI 3 perovskite precursor ink uses volatile acetonitrile (ACN) as the main solvent with DMF and DMSO as coordination additives is beneficial to improve the ink stability, inhibit the coffee rings, and the complicated intermediate FAPbI 3 phases, delivering high-quality pin-hole free and phase-pure FAPbI 3 perovskite films with large-scale uniformity. Ultimately, small-area FAPbI 3 pero-SCs (0.062 cm 2 ) and large-area modules (15.64 cm 2 ) achieved remarkable efficiencies of 24.32 % and 21.90 %, respectively, whereas the PCE of the devices can be maintained at 23.76 % when the printing speed increases to 18.0 m/min. Specifically, the unencapsulated device exhibits superior operational stability with T 90 >1350 h. This work represents a step towards the scalable, cost-effective manufacturing of perovskite photovoltaics with both high performance and high throughput.

关键词： Large-Area Printing Perovskite Solar Cells Solar Module Volatile Solvent Wide Speed Window

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Controlling Polymer Molecular Weight Distribution through a Latent Mediator Strategy with Temporal Programming

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Angewandte Chemie 2021年第36期133卷

作者： Miao Chen Dr. Jiajia Li Kaiqi Ma Prof. Guoqin Jin Dr. Xiangqiang Pan Prof. Zhengbiao Zhang Prof. Jian Zhu State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China School of Mechanical and Electric Engineering Soochow University Suzhou 215006 China

Polymer molecular weight distribution (MWD) is a key parameter of polymers. Here we present a robust method for controlling polymer MWD in controlled cationic polymerizations. A latent mediator strategy was designed and combined with temporal programming to regenerate mediators at different times during polymerization. Both the breadths and shapes of MWD curves were tuned easily by adjusting an external light source. Bimodal, trimodal, and tetramodal distributions were obtained, and the breadths could be varied from 1.06 to 2.09. polymers with different MWDs prepared by this method had good chain end fidelity, which was demonstrated with successful chain-extension experiments. In addition, the introduction of temporal programming with a computer-controlled single chip for the light source opened an avenue for the use of artificial intelligence in polymer synthesis.

关键词： latent mediators living cationic polymerization molecular weight distribution temporal programming

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Crystallization-driven Nanoparticle Crystalsomes

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Angewandte Chemie 2023年第15期135卷

作者： Dr. Lingfeng Gao Dr. Shan Mei Qian Qian Shichen Yu Prof. Dr. Bin Zhao Prof. Yingfeng Tu Prof. Dr. Christopher Y. Li Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University China Department of Materials Science and Engineering Drexel University USA Contribution: Data curation (lead) Formal analysis (supporting) Contribution: Formal analysis (supporting) Department of Chemistry University of Tennessee USA Contribution: Formal analysis (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Supervision (lead) Writing - review & editing (lead)

Nanoparticle (NP) assembly has been extensively studied, and a library of NP superstructures has been synthesized. These intricate structures show unique collective optical, electronic, and magnetic properties. In this work, we report a bottom-up approach for fabricating spherical gold nanoparticle (AuNP) assemblies that mimic colloidosomes. Co-crystallization of lipoic acid-end-functionalized poly(ethylene oxide) (PEO) and AuNPs in solution via a self-seeding method led to the formation of hollow spherical NP assemblies named nanoparticle crystalsomes (NPCs). Due to the spherical shape, the translational symmetry of PEO crystals is broken in NPCs, which can be attributed to the competition between NP close packing and polymer crystallization. This was confirmed by tuning the NPC morphology via varying the self-seeding temperature, crystallization temperature, and PEO molecular weight. We envisage that this strategy paves the way to attaining exquisite morphological control of NP assemblies with broken translational symmetry.

关键词： Crystalsomes Nanoparticle Assembly Nanoparticle Vesicles Polymer Crystallization Polymer Single Crystals

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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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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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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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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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Aggregation-Induced Emission-Based Ionic Liquids for Bacterial Killing, Imaging, Cell Labelling and Bacterial Detection in Blood Cells

SSRN

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SSRN 2019年

作者： Shi, Jie Wang, Mengyao Sun, Zhe Liu, Yangyang Guo, Jiangna Mao, Hailei Yan, Feng Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou215123 China Department of Anesthesiology and Critical Care Medicine Zhongshan Hospital Fudan University Shanghai200032 China

A series of aggregation-induced emission (AIE)-based imidazolium type ionic liquids (ILs) were designed and synthesized for bacterial killing and imaging, cell labelling and bacterial detection in blood cells. The AIE-based ILs showed antibacterial activities against both E. coli and S. aureus. The carbon chain length of substitution at the N3 position of the imidazolium cations highly affect the antibacterial properties of ILs. Due to their AIE characteristics, the ILs could selectively fluorescent image dead bacteria while killing the bacteria. The fluorescence intensity varied with the concentration of bacteria, indicating that the AIE-based ILs would be an excellent antibacterial material as well as an efficient probe for bacterial viability assay. In addition, the synthesized AIE-based ILs exhibit relatively low cytotoxicity and hemolysis rate, and therefore potential for cell labelling, as well as bacterial detection in blood cells. © 2019, The Authors. All rights reserved.

关键词： Ionic liquids

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