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Organic-semiconductor-assisted dielectric screening effect for stable and efficient perovskite solar cells

Science Bulletin 2022年第12期67卷 1243-1252,M0004页

作者： Haiyang Chen Qinrong Cheng Heng Liu Shuang Cheng Shuhui Wang Weijie Chen Yunxiu Shen Xinqi Li Haidi Yang Heyi Yang Jiachen Xi Ziyuan Chen Xinhui Lu Hongzhen Lin 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 State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSoochow UniversitySuzhou 215123China i-Lab Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Department of Physics Chinese University of Hong KongHong Kong 999077China Beijing National Laboratory for Molecular Sciences Institute of ChemistryChinese Academy of SciencesBeijing 100190China

Perovskite solar cells(pero-SCs)performance is essentially limited by severe non-radiative losses and ion *** numerous strategies have been proposed,challenges remain in the basic understanding of their ***,we report a dielectric-screening-enhancement effect for perovskite defects by using organic semiconductors with finely tuned molecular structures from the atoms *** method produced various perovskite films with high dielectric constant values,reduced charge capture regions,suppressed ion migration,and it provides an efficient charge transport pathway for suppressing non-radiative recombination beyond the passivation *** resulting pero-SCs showed a promising power conversion efficiency(PCE)of 23.35%with a high open-circuit voltage(1.22 V);and the 1-cm^(2) pero-SCs maintained an excellent PCE(21.93%),showing feasibility for scalable *** robust operational and thermal stabilities revealed that this method paved a new way to understand the degradation mechanism of pero-SCs,promoting the efficiency,stability and scaled fabrication of the pero-SCs.

关键词： Organic semiconductors Dielectric screening effect Reduced non-radiative recombination Operational stability Perovskite solar cells

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Redox-responsive ferrocene-containing poly(ionic liquid)s for antibacterial applications

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Science China Chemistry 2019年第1期62卷 95-104页

作者： Tikai Zhang Jiangna Guo Yingying Ding Hailei Mao Feng Yan Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and EngineeringCollege of Chemistry Chemical Engineering and Materials Science Soochow University Department of Anesthesiology and Critical Care Medicine Zhongshan Hospital Fudan University

Ferrocene(Fc)-containing imidazolium type ionic liquids(ILs) and corresponding poly(ionic liquid)(PIL) membranes with tunable antibacterial activity based on electrochemical redox reaction and host-guest chemistry were developed. The effect of Fc moiety on the antimicrobial activities against both Staphylococcus aureus(S. aureus) and Escherichia coli(E. coli) was studied by minimum inhibitory concentration(MIC). The presence of Fc groups highly enhanced the antibacterial efficiency of Fccontaining ILs because of the generation of reactive oxygen species(ROS). The electrochemical oxidation of Fc to Fc+and the formation of inclusion complexes between Fc and β-CD via host-guest interactions decreased the antibacterial activities of ILs and PIL membranes. The antibacterial activities may be recovered in some extent upon the electrochemical reduction of Fc+to Fc or the exclusion of the Fc out of the cavity of β-CD. Furthermore, all the Fc-containing PIL membranes showed relatively low hemolysis activities and none cytotoxicity toward human cells, indicating clinical feasibility in topical applications.

关键词： antibacterial activities imidazolium cations ferrocene poly(ionic liquid) cytotoxicity

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Tuning the Mechanical Properties of 3D-printed Objects by the RAFT Process: From Chain-Growth to Step-Growth

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Angewandte Chemie 2024年第10期136卷

作者： Xiaofeng Pan Dr. Jiajia Li Zhuang Li Qing Li Dr. Xiangqiang Pan 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

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Facile preparation of pH-responsive PEGylated prodrugs for activated intracellular drug delivery

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Chinese Chemical Letters 2019年第12期30卷 2027-2031页

作者： Yue Song Dian Li Jinlin He Mingzu Zhang Peihong Ni College of Chemistry Chemical Engineering and Materials Science State and Local Joint Engineering Laboratory for Novel Functional Polymeric MaterialsJiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision SynthesisSoochow University

PEGylated prodrug,covalent attaching polyethylene glycol(PEG) polymer chains to therapeutic drugs,is one of the most promising techniques to improve the water-solubility,stability,and therapeutic effect of *** this study,three PEGylated acid-sensitive prodrugs DOX-PEG-DOX with different molecular weights,were prepared via Schiff-base reaction between aldehyde-modified PEG and the amino groups of doxorubicin(DOX).This kind of amphiphilic polymeric prodrug could be self-assemble into nanoparticles in aqueous *** average particle size and morphologies of the prodrug nanoparticles under different pH conditions were observed by dynamic light scattering(DLS) and transmission electron microscopy(TEM),re s *** turned out that the nanoparticles could be kept stable in the physiological environment,but degraded in acidic ***,we also investigated in vitro drug release behavior and found that the prodrug had acid-sensitive *** cytotoxicity and intracellular uptake assays revealed that the prodrugs could rapidly internalized by HeLa or HepG2 cells to release DOX and effectively inhibited the proliferation of the tumor cells,which have the potential for use in cancer therapy.

关键词： Polyethylene glycol Doxorubicin Prodrug Schiff-base reaction pH-Responsiveness

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Thin Film of Polyimide/Mof Nanocomposite Membrane with Substantially Improved Stability for Co2/Ch4 Separation

SSRN

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SSRN 2022年

作者： Jin, Jian Zhu, Shouwen Wang, Zhenggong Bi, Xiangyu Shi, Yapeng Shi, Yanshu Zhang, Yatao College of Chemistry Chemical Engineering and Materials Science Collaborative Innovation Center of Suzhou Nano Science and Technology Innovation Center for Chemical Science Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Soochow University Suzhou215123 China School of Chemical Engineering and Energy Zhengzhou University Zhengzhou450001 China

The development of thin-film nanocomposite (TFN) membranes is necessary due to the demand of high gas permeance for industrial applications. Nevertheless, it is a great challenge to achieve TFN membranes with stable separation performance owing to the high chain mobility in thin films. In this work, we report an efficient and less destructive coordination crosslinking strategy to improve the TFN membrane stability for CO2/CH4 separation. The selective layer of TFN membranes is made of carboxylated polyimide as matrix and UiO-66 nanoparticles as fillers. By immersing these TFN membranes in methanol solution containing Cu(NO3)2, coordination bonds are successfully constructed between Cu2+ and carboxyl groups (-COOH). The crosslinked TFN membranes exhibit high CO2/CH4 selectivity up to 29~35 with CO2 permeance of 110~350 GPU, outperforming most of previously reported TFN membranes. Moreover, the plasticization pressure of the crosslinked membranes improves from 0.3-0.9 MPa to 0.9-1.5 MPa. In the CO2/CH4 (50 v:50 v) mixed gas permeation tests, the crosslinked membranes remain constant CO2/CH4 selectivity at 23.9~25.2 with increasing feed gas pressure. The crosslinked membranes also demonstrate stable CO2/CH4 selectivity in the range of 27.2~31.2 within 100 hours testing time under 1.0 MPa CO2 partial pressure. © 2022, The Authors. All rights reserved.

关键词： Separation

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Second-order topological magneto-optical effects in noncoplanar antiferromagnets

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Physical Review B 2022年第17期106卷 174427-174427页

作者： Ping Yang Wanxiang Feng Xiaodong Zhou Xiuxian Yang Yugui Yao Centre for Quantum Physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (MOE) School of Physics Beijing Institute of Technology Beijing 100081 China Beijing Key Lab of Nanophotonics & Ultrafine Optoelectronic Systems School of Physics Beijing Institute of Technology Beijing 100081 China Laboratory of Quantum Functional Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou 221116 China

The second-order magneto-optical effects, represented by Voigt and Schäfer-Hubert effects, are effective methods to detect the spin textures in antiferromagnets, whereas the previous studies are usually limited to collinear antiferromagnets. In noncollinear antiferromagnets, the spin textures characterized by spin chirality have been revealed to play a critical role in many exciting physics. In particular, the first-order topological magneto-optical effects originated from scalar spin chirality have been discovered recently. In this work, using the first-principles calculations and group-theory analysis, we generalize the first-order topological magneto-optical effects to the second-order cases, that is, topological Voigt and Schäfer-Hubert effects, by taking the noncoplanar 3Q spin state of γ−FexMn1−x alloy as an example. The conventional Voigt and Schäfer-Hubert effects are comparatively studied in the collinear 1Q and 2Q spin states of γ−FexMn1−x alloy. In addition, the natural linear birefringence due to crystal anisotropy is discussed in the strained 1Q, 2Q, and 3Q states, and a unique fingerprint for experimentally distinguishing the second-order topological magneto-optical effects and natural linear birefringence is identified. Our work brings a topological insight into the second-order magneto-optical effects in noncoplanar antiferromagnets and also provides γ−FexMn1−x as an attractive material platform for future experimental exploration.

关键词： Magneto-optical effect Antiferromagnets Chiral magnets First-principles calculations

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Crystal Thermal Transport in Altermagnetic RuO2

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Physical Review Letters 2024年第5期132卷 056701-056701页

作者： Xiaodong Zhou Wanxiang Feng Run-Wu Zhang Libor Šmejkal Jairo Sinova Yuriy Mokrousov Yugui Yao Centre for Quantum Physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (MOE) School of Physics Beijing Institute of Technology Beijing 100081 China Beijing Key Lab of Nanophotonics and Ultrafine Optoelectronic Systems School of Physics Beijing Institute of Technology Beijing 100081 China Laboratory of Quantum Functional Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou 221116 China Institute of Physics Johannes Gutenberg University Mainz 55099 Mainz Germany Institute of Physics Czech Academy of Sciences Cukrovarnická 10 162 00 Praha 6 Czech Republic Peter Grünberg Institut and Institute for Advanced Simulation Forschungszentrum Jülich and JARA 52425 Jülich Germany

We demonstrate the emergence of a pronounced thermal transport in the recently discovered class of magnetic materials—altermagnets. From symmetry arguments and first-principles calculations performed for the showcase altermagnet, RuO2, we uncover that crystal Nernst and crystal thermal Hall effects in this material are very large and strongly anisotropic with respect to the Néel vector. We find the large crystal thermal transport to originate from three sources of Berry’s curvature in momentum space: the Weyl fermions due to crossings between well-separated bands, the strong spin-flip pseudonodal surfaces, and the weak spin-flip ladder transitions, defined by transitions among very weakly spin-split states of similar dispersion crossing the Fermi surface. Moreover, we reveal that the anomalous thermal and electrical transport coefficients in RuO2 are linked by an extended Wiedemann-Franz law in a temperature range much wider than expected for conventional magnets. Our results suggest that altermagnets may assume a leading role in realizing concepts in spin caloritronics not achievable with ferromagnets or antiferromagnets.

关键词： Magnetism Nernst effect Thermal Hall effect Topological materials First-principles calculations

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Ultra-Fast Selenol-Yne Click (SYC) Reaction Enables Poly(selenoacetal) Covalent Adaptable Network Formation

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Angewandte Chemie 2024年第40期136卷

作者： Mengyao Zhang Sisi Chen Guichuan Xu Weihong Lu Jiajia Li Jiandong Zhang Zhengbiao Zhang Jian Zhu Xiangqiang Pan State and Local Joint Engineering Laboratory for Novel Functional Department 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

The emergence of covalent adaptable networks (CANs) based on dynamic covalent bonds (DCBs) presents a promising avenue for achieving resource recovery and utilization. In this study, we discovered a dynamic covalent bond called selenacetal, which is obtained through a double click reaction between selenol and activated alkynes. Density functional theory (DFT) calculations demonstrated that the ΔG for the formation of selenoacetals ranges from 12 to 18 kJ mol −1 , suggesting its potential for dynamic reversibility. Dynamic exchange experiments involving small molecules and polymers provide substantial evidence supporting the dynamic exchange properties of selenoacetals. By utilizing this highly efficient click reaction, we successfully synthesized dynamic materials based on selenoacetal with remarkable reprocessing capabilities without any catalysts. These materials exhibit chemical recycling under alkaline conditions, wherein selenoacetal (SA) can decompose into active enone selenide (ES) and diselenides. Reintroducing selenol initiates a renewed reaction with the enone selenide, facilitating material recycling and yielding a newly developed dynamic material exhibiting both photo- and thermal responsiveness. The results underscore the potential of selenoacetal polymers in terms of recyclability and selective degradation, making them a valuable addition to conventional covalent adaptable networks.

关键词： Covalent Adaptable Networks Dynamic Covalent Chemistry Click Reaction Selenoacetal

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Effective and biocompatible antibacterial surfaces via facile synthesis and surface modification of peptide polymers

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Bioactive Materials 2021年第12期6卷 4531-4541页

作者： Ziyi Lu Yueming Wu Zihao Cong Yuxin Qian Xue Wu Ning Shao Zhongqian Qiao Haodong Zhang Yunrui She Kang Chen Hengxue Xiang Bin Sun Qian Yu Yuan Yuan Haodong Lin Meifang Zhu Runhui Liu State Key Laboratory of Bioreactor Engineering College of ChemistryChemical Engineering and Materials ScienceEast China University of Science and TechnologyShanghai200237China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China Jiangsu Key Laboratory of Advanced Functional Polymers Design and Application Soochow UniversitySuzhou215123China Department of Orthopedic Surgery Shanghai General HospitalShanghai Jiao Tong University School of MedicineShanghai200080China Key Laboratory for Ultrafine Materials of Ministry of Education Frontiers Science Center for Materiobiology and Dynamic ChemistryResearch Center for Biomedical Materials of Ministry of EducationSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai200237China

It is an urgent need to tackle drug-resistance microbial infections that are associated with implantable biomedical *** defense peptide-mimicking polymers have been actively explored in recent years to fight against drug-resistant *** recent report on lithium hexamethyldisilazide-initiated superfast polymerization on amino acid N-carboxyanhydrides enables the quick synthesis of host defense peptide-mimicking peptide *** we reported a facile and cost-effective thermoplastic polyurethane(TPU)surface modification of peptide polymer(DLL:BLG=90:10)using plasma surface activation and substitution reaction between thiol and bromide *** peptide polymer-modified TPU surfaces exhibited board-spectrum antibacterial property as well as effective contact-killing ability in ***,the peptide polymer-modified TPU surfaces showed excellent biocompatibility,displaying no hemolysis and *** vivo study using methicillin-resistant Staphylococcus aureus(MRSA)for subcutaneous implantation infectious model showed that peptide polymer-modified TPU surfaces revealed obvious suppression of infection and great histocompatibility,compared to bare TPU *** further explored the antimicrobial mechanism of the peptide polymer-modified TPU surfaces,which revealed a surface contact-killing mechanism by disrupting the bacterial *** results demonstrated great potential of the peptide-modified TPU surfaces for practical application to combat bacterial infections that are associated with implantable materials and devices.

关键词： Peptide polymer Host defense peptide Antimicrobial surface MRSA Subcutaneous infection

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Efficient and targeted drug/siRNA co-delivery mediated by reversibly crosslinked polymersomes toward anti-inflammatory treatment of ulcerative colitis (UC)

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Nano Research 2019年第3期12卷 659-667页

作者： Xin Xu Weijing Yang Qiujun Liang Yanan Shi Wenxin Zhang Xiao Wang Fenghua Meng Zhiyuan Zhong Lichen Yin Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano and Soft Materials (FUNSOM) the Collaborative Innovation Center of Suzhou Nano Science and Technology Soochow University Suzhou 215123 China 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 China

Co-delivery of anti-inflammatory siRNA and hydrophilic drug provides a promising approach for the treatment of ulcerative colitis (UC). However, lack of a suitable and efficient co-delivery carrier poses critical challenge against their utilization. We herein developed macrophage-targeting, reversibly crossli nked polymersomes (TKPR-RCP) based on the TKPR-modified, poly(ethyle ne glycol)-b-poly(trimethylene carbonate-codithiolane trimethylene carbonate)-b-polyethylenimine (PEG-P(TMC-DTC)-PEI) triblock copolymer, which could efficiently encapsulate TNF-α siRNA and dexamethasone sodium phosphate (DSP) in their hydrophilic core. The cationic PEI segments provided additional electrostatic interactions with cargo molecules to promote the encapsulatiion, and disulfide crosslinking of the polymersome membrane endowed the TKPR-RCP with high colloidal stability. Because the cationic PEI was embedded in the hydrophilic core, the polymersomes displayed neutral surface charge and thus possessed high serum stability. The TKPR-RCP co-encapsulating TNF-α siRNA and DSP could be efficiently internalized by macrophages (~98%) and undergo redox-responsive membrane de-crosslinking to accelerate cargo release in the cytoplasm, thus inducing efficient gene silencing and anti-inflammatory effect .Intravenous injectio n of the co-delivery TKPR-RCP mediated pote nt and cooperative anti-inflammatory effect in inflamed colons of UC mice, and significantly prevented animals from colonic injury. This study therefore provides a promising approach for the co-delivery of hydrophilic drug/siRNA toward the treatment of inflammatory bowel diseases.

关键词： ulcerative colitis (UC) anti-inflammatory therapy polymersomes reversible crosslinking siRNA/drug co-delivery macrophage targeting

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