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Boron kagome-layer induced intrinsic superconductivity in a MnB3 monolayer with a high critical temperature

Physical Review B 2020年第7期102卷 075431-075431页

作者： Ziyang Qu Fanjunjie Han Tong Yu Meiling Xu Yinwei Li Guochun Yang Laboratory of Quantum Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou 221116 China Centre for Advanced Optoelectronic Functional Materials Research and Key Laboratory for UV Light-Emitting Materials and Technology of Ministry of Education Northeast Normal University Changchun 130024 China

The design of two-dimensional superconductors has attracted great research interest owing to their wide application in nanoscale devices. Here, we combine first-principles calculations with structure searching technology to identify a unique stable hexagonal h−MnB3 monolayer, exhibiting a slightly higher energy with respect to the reported tetragonal t−MnB3. Interestingly, h−MnB3 contains two boron kagome layers sandwiched with Mn atoms. It exhibits metallic properties and has a superconducting transition temperature of 24.9 K, which is much higher than 2.9 K in t−MnB3. Its superconductivity mainly originates from the coupling between in-plane vibrational phonons of boron kagome layers and electrons of Mn atoms. h−MnB3 exhibits a tunable superconductivity, and reaches a maximum of 34 K at 2% tensile strain resulting from the softening in-plane modes of boron kagome layers. The Si (111) surface may be an ideal substrate for the growth of superconductive h−MnB3. The unique superconducting mechanism observed here could inspire the searching of more boron kagome based two-dimensional superconductors.

关键词： First-principles calculations Superconductors 2-dimensional systems Kagome lattice Two-dimensional electron system

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Iodonium Initiators: Paving the Air-free Oxidation of Spiro-OMeTAD for Efficient and Stable Perovskite Solar Cells

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Angewandte Chemie 2023年第5期136卷

作者： Heyi Yang Tingting Xu Weijie Chen Yeyong Wu Xianming Guo Yunxiu Shen Chengqiang Ding Xining Chen Haiyang Chen Junyuan Ding Xiaoxiao Wu Prof. Guixiang Zeng Prof. Zhengbiao Zhang Prof. Yaowen Li Prof. 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 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 Kuang Yaming Honors School Nanjing University Nanjing 210008 China State Key Laboratory of Radiation Medicine and Protection Soochow University Suzhou 215123 China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies 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

To date, perovskite solar cells (pero-SCs) with doped 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene (Spiro-OMeTAD) hole transporting layers (HTLs) have shown the highest recorded power conversion efficiencies (PCEs). However, their commercialization is still impeded by poor device stability owing to the hygroscopic lithium bis(trifluoromethanesulfonyl)imide and volatile 4-tert-butylpyridine dopants as well as time-consuming oxidation in air. In this study, we explored a series of single-component iodonium initiators with strong oxidability and different electron delocalization properties to precisely manipulate the oxidation states of Spiro-OMeTAD without air assistance, and the oxidation mechanism was clearly understood. Iodine (III) in the diphenyliodonium cation (IP + ) can accept a single electron from Spiro-OMeTAD and forms Spiro-OMeTAD⋅ + owing to its strong oxidability. Moreover, because of the coordination of the strongly delocalized TFSI − with Spiro-OMeTAD⋅ + in a stable radical complex, the resulting hole mobility was 30 times higher than that of pristine Spiro-OMeTAD. In addition, the IP-TFSI initiator facilitated the growth of a homogeneous and pinhole-free Spiro-OMeTAD film. The pero-SCs based on this oxidizing HTL showed excellent efficiencies of 25.16 % (certified: 24.85 % for 0.062-cm 2 ) and 20.71 % for a 15.03-cm 2 module as well as remarkable overall stability.

关键词： Doping Perovskite Solar Cells Spiro-OMeTAD Stability

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Transfer, Amplification, Storage, and Complete Self-Recovery of Supramolecular Chirality in an Achiral polymer System

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Angewandte Chemie 2021年第34期133卷

作者： Tengfei Miao Xiaoxiao Cheng Haotian Ma Zixiang He Prof. Zhengbiao Zhang Prof. Nianchen Zhou Prof. Wei Zhang Prof. Xiulin Zhu 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

Supramolecular chirality and its complete self-recovery ability are highly mystical in nature and biological systems, which remains a major challenge today. Herein, we demonstrate that partially cross-linked azobenzene (Azo) units can be employed as the potential chiral trigger to fully heal the destroyed helical superstructure in achiral nematic polymer system. Combining the self-assembly of Azo units and terminal hydroxyl groups in polymer side chains allows the vapor-induced chiral nematic phase and covalent fixation of the superstructure via acetal reaction. The induced helical structure of Azo units can be stored by inter-chain cross-linking, even after removal of the chiral source. Most interestingly, the stored chiral information can trigger perfect chiral self-recovery (CSR) behavior after being destroyed by UV light, heat, and solvents. The results pave a new way for producing novel chiroptical materials with reversible chirality from achiral sources.

关键词： chiral induction chiral self-recovery chiral storage supramolecular chirality

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Molecular Self-Assembly Regulated Dopant-Free Hole Transport Materials for Efficient and Stablen-i-pPerovskite Solar Cells and Scalable Modules

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Angewandte Chemie 2022年第42期134卷

作者： Qinrong Cheng Haiyang Chen Fu Yang Ziyuan Chen Weijie Chen Heyi Yang Yunxiu Shen Xue-Mei Ou Yeyong Wu Prof. Yaowen Li Prof. 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 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 Jiangsu Key Laboratory of Advanced Negative Carbon Technologies 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

Dopant-free organic hole transport materials (HTMs) remain highly desirable for stable and efficient n - i - p perovskite solar cells (pero-SCs) but rarely succeed. Here, we propose a molecular assembly strategy to overcome the limited optoelectronic properties of organic HTMs by precisely designing a linear organic small molecule BDT-DPA-F from the atomic to the molecular levels. BDT-DPA-F can assemble into a fibril network, showing an obviously improved hole mobility and decreased energy disorder. The resultant pero-SCs showed a promising efficiency of 23.12 % (certified 22.48 %), which is the highest certified value of pero-SCs with dopant-free HTMs, to date. These devices also showed a weak-dependence of efficiency on size, enabling a state-of-the-art efficiency of 22.50 % for 1-cm 2 device and 20.17 % for 15.64-cm 2 module. For the first time, the pero-SCs based on dopant-free HTMs realized ultralong stabilities with T 80 lifetimes over 1200 h under operation or thermal aging at 85 °C.

关键词： Dopant-Free Hole Transport Materials Intermolecular Interactions Operational and Thermal Stabilities Perovskite Solar Cells Self-Assembly

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Self-promoted Controlled Ring-opening polymerization via Side Chain-mediated Proton Transfer for the Synthesis of Tertiary Amine-pendant Polypeptoids

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Angewandte Chemie 2024年第6期137卷

作者： Mingzhen Liao Yao Yao Kunyu Gan Xianghua Su Ning Zhao Ronald N. Zuckermann Sunting Xuan Zhengbiao Zhang State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Materials Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Suzhou GenePharma Co. Ltd. Suzhou 215123 China College of Pharmaceutical Sciences Soochow University Suzhou 215123 China. The Molecular Foundry Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley California 94720 United States State Key Laboratory of Radiation Medicine and Protection Soochow University Suzhou 215123 China

Proton transfer is essential in virtually all biochemical processes, with enzymes facilitating this transfer by optimizing the proximity and orientation of reactants through site-specific hydrogen bonds. Proton transfer is also crucial in the rate-determining step for the ring-opening polymerization of N -carboxyanhydrides (NCAs), widely used to prepare various peptidomimetic materials. This study utilizes side chain-assisted strategy to accelerate the rate of chain propagation by using NCAs with tertiary amine pendants. This moiety enables hydrogen bond formation between the incoming NCA and the polymer amino growing end. The tertiary amine side chain of the NCA forms a proton shuttle, via a less constrained transition state, to facilitate the proton transfer process. Moreover, the tertiary amine side chains enable the precipitation of NCA monomers through in situ protonation during the monomer synthesis. This greatly facilitates the synthesis of these unreported monomers, allowing the direct controlled synthesis of tertiary amine-pendant polypeptoids. This side chain-promoted polymerization has rarely been reported. Additionally, the tertiary amine side chains, as widely used functional groups, endow the polymers with unique properties including pH- and thermo-responsiveness, tunable p K a s, and siRNA transfection capability. The self-promoted synthesis, facile monomer preparation, and attractive properties make tertiary amine-pendant polypeptoids promising materials for various applications.

关键词： Self-promoted Side chain-promoted Proton transfer Tertiary amine-pendant Polypeptoids Controlled ring-opening polymerization

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

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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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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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