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Dynamic Control of Cyclic Peptide Assembly to Form Higher-Order Assemblies

Angewandte Chemie 2023年第36期135卷

作者： Dr. Chongyang Wu Hongyue Zhang Nan Kong Bihan Wu Xinhui Lin Prof. Dr. Huaimin Wang Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province Department of Chemistry School of Science Westlake University Institute of Natural Sciences Westlake Institute for Advanced Study No. 600 Dunyu Road Hangzhou 310024 Zhejiang Province China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (equal) Methodology (lead) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Methodology (supporting) Contribution: Formal analysis (supporting) Methodology (supporting) Contribution: Methodology (supporting) Westlake Laboratory of Life Sciences and Biomedicine School of Life Sciences Westlake University Hangzhou 310024 Zhejiang China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Methodology (equal) Project administration (lead) Resources (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

Chirality correction, asymmetry, ring-chain tautomerism and hierarchical assemblies are fundamental phenomena in nature. They are geometrically related and may impact the biological roles of a protein or other supermolecules. It is challenging to study those behaviors within an artificial system due to the complexity of displaying these features. Herein, we design an alternating D,L peptide to recreate and validate the naturally occurring chirality inversion prior to cyclization in water. The resulting asymmetrical cyclic peptide containing a 4-imidazolidinone ring provides an excellent platform to study the ring-chain tautomerism, thermostability and dynamic assembly of the nanostructures. Different from traditional cyclic D,L peptides, the formation of 4-imidazolidinone promotes the formation of intertwined nanostructures. Analysis of the nanostructures confirmed the left-handedness, representing chirality induced self-assembly. This proves that a rationally designed peptide can mimic multiple natural phenomena and could promote the development of functional biomaterials, catalysts, antibiotics, and supermolecules.

关键词： Asymmetrical Backbone Cyclic Peptides Intertwined Nanostructures Ring-Chain Tautomerism Self-Assembly

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Author Correction: Predicting the efficiency of prime editing guide RNAs in human cells

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Nature biotechnology 2024年第3期42卷 529页

作者： Hui Kwon Kim Goosang Yu Jinman Park Seonwoo Min Sungtae Lee Sungroh Yoon Hyongbum Henry Kim Department of Pharmacology Yonsei University College of Medicine Seoul Republic of Korea. Brain Korea 21 Plus Project for Medical Sciences Yonsei University College of Medicine Seoul Republic of Korea. Center for Nanomedicine Institute for Basic Science (IBS) Seoul Republic of Korea. Graduate Program of Nano Biomedical Engineering (NanoBME) Advanced Science Institute Yonsei University Seoul Republic of Korea. Electrical and Computer Engineering Seoul National University Seoul Republic of Korea. Interdisciplinary Program in Bioinformatics Seoul National University Seoul Republic of Korea. Graduate School of Data Science Seoul National University Seoul Republic of Korea. Department of Pharmacology Yonsei University College of Medicine Seoul Republic of Korea. hkim1@yuhs.ac. Brain Korea 21 Plus Project for Medical Sciences Yonsei University College of Medicine Seoul Republic of Korea. hkim1@yuhs.ac. Center for Nanomedicine Institute for Basic Science (IBS) Seoul Republic of Korea. hkim1@yuhs.ac. Graduate Program of Nano Biomedical Engineering (NanoBME) Advanced Science Institute Yonsei University Seoul Republic of Korea. hkim1@yuhs.ac. Severance Biomedical Science Institute Yonsei University College of Medicine Seoul Republic of Korea. hkim1@yuhs.ac. Graduate Program of NanoScience and Technology Yonsei University Seoul Republic of Korea. hkim1@yuhs.ac.

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Organic Zinc-Ion Battery: Planar, π-Conjugated Quinone-Based Polymer Endows Ultrafast Ion Diffusion Kinetics

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Angewandte Chemie 2022年第51期134卷

作者： Dr. Fei Ye Qiang Liu Dr. Hongliang Dong Kailin Guan Zhaoyang Chen Na Ju Prof. Linfeng Hu School of Materials Science and Engineering Southeast University Nanjing 211189 China Contribution: Conceptualization (supporting) Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Software (lead) Center for High Pressure Science and Technology Advanced Research Shanghai 201203 P. R. China Contribution: Investigation (equal) Methodology (equal) Resources (equal) Validation (lead) Contribution: Formal analysis (equal) Investigation (lead) Methodology (equal) Contribution: Investigation (equal) Software (equal) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

A novel poly(phenazine-alt-pyromellitic anhydride) (PPPA) has been successfully designed and synthesized via a condensation polymerization strategy as promising cathode material in organic zinc-ion batteries. Electrochemical quartz crystal microbalance (EQCM), FTIR and XPS characterizations verify a reversible Zn 2+ -coordination mechanism in our PPPA cathode. Intriguingly, an ultrahigh Zn 2+ diffusion coefficient of 1.2×10 −7 cm 2 s −1 was found in this large π-conjugated system, which is the highest one among all organic cathode materials for zinc-ion batteries. Theoretical calculations reveal the extended π-conjugated plane in our PPPA sample results in a significant reduction on energy gap, effectively accelerating intramolecular electron transfer during charge/discharge process. Our finding provides insights to achieve high zinc-ion transport kinetics by a design strategy on planar polymer system.

关键词： Energy Gap Linear Polymer Organic Zinc-Ion Batteries Quinone-Based Polymer Zn2+ Diffusion Coefficient

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Designing metamaterials with quantum annealing and factorization machines

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Physical Review Research 2020年第1期2卷 013319-013319页

作者： Koki Kitai Jiang Guo Shenghong Ju Shu Tanaka Koji Tsuda Junichiro Shiomi Ryo Tamura Graduate School of Frontier Sciences The University of Tokyo Chiba 277-8568 Japan Department of Mechanical Engineering The University of Tokyo Tokyo 113-8654 Japan Research and Services Division of Materials Data and Integrated System National Institute for Materials Science Ibaraki 305-0047 Japan Green Computing Systems Research Organization Waseda University Tokyo 162-0042 Japan JST PRESTO Saitama 332-0012 Japan RIKEN Center for Advanced Intelligence Project Tokyo 103-0027 Japan International Center for Materials Nanoarchitectonics National Institute for Materials Science Ibaraki 305-0044 Japan

Automated materials design with machine learning is increasingly common in recent years. Theoretically, it is characterized as black-box optimization in the space of candidate materials. Since the difficulty of this problem grows exponentially in the number of variables, designing complex materials is often beyond the ability of classical algorithms. We show how quantum annealing can be incorporated into automated materials discovery and conduct a proof-of-principle study on designing complex thermofunctional metamaterials. Our algorithm consists of three parts: regression for a target property by factorization machine, selection of candidate metamaterial based on the regression results, and simulation of the metamaterial property. To accelerate the selection part, we rely on the D-Wave 2000Q quantum annealer. Our method is used to design complex structures of wavelength selective radiators showing much better concordance with the thermal atmospheric transparency window in comparison to existing human-designed alternatives.

关键词： Adiabatic quantum optimization Metamaterials Machine learning

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FLOWGAN:Unbalanced Network Encrypted Traffic Identification Method Based on GAN

FLOWGAN:Unbalanced Network Encrypted Traffic Identification ...

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IEEE International Conference on Big data and Cloud Computing (BdCloud)

作者： ZiXuan Wang Pan Wang Xiaokang Zhou ShuHang Li MoXuan Zhang School of Modern Posts University of Nanjing University of Posts and Telecommunications Nanjing China Faculty of Data Science Shiga University Hikone Japan RIKEN Center for Advanced Intelligence Project Tokyo Japan Schools of International Education Jinling Institute of Technology Nanjing China

ISBN: (数字)9781728143286

ISBN: (纸本)9781728143293

It is crucial to accurately identify the type of traffic and application so that it can enable various policy-driven network management and security monitoring. However, with the increasing adoption of Internet applications use encryption protocols to transmit data, traffic classification is becoming more difficult. Although existing machine learning methods and novel deep learning methods have many advantages, which can solve the drawbacks of port and payload based methods, but there are still some shortcomings, one of which is the imbalanced property of network traffic data. In this paper, we proposed a GAN based method called FlowGAN to tackle with the problem of class imbalance for traffic classification. As an instance of Generative Adversarial Network (GAN), FlowGAN leverages the superiority of GAN's data augmentation to produce synthetic traffic data for classes with few samples. Furthermore, we trained a classical deep learning model, Multilayer perceptron (MLP) based network traffic classifier to evaluate the performance of FlowGAN. Based on the public dataset 'ISCX', our experimental results show that our proposed FlowGAN can outperform an unbalanced dataset and balancing dataset by the oversampling method in terms of data augmentation. Based on the public dataset ISCX, our experimental results show that the recognition performance of FlowGAN on small samples, compared with the unbalanced dataset, Precision, Recall, and F1-score increased by 13.2%, 17.0%, and 15.6% on average, compared with the balanced dataset Precision, Recall, F1-score increased by 2.15%, 2.06%, 2.12% on average.

关键词： Cryptography Gallium nitride Generative adversarial networks Training Generators Deep learning Feature extraction

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H2O2-Responsive NIR-II AIE Nanobomb for Carbon Monoxide Boosting Low-Temperature Photothermal Therapy

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Angewandte Chemie 2022年第36期134卷

作者： Gongcheng Ma Zhongke Liu Chunguang Zhu Prof. Huajie Chen Prof. Ryan T. K. Kwok Prof. Pengfei Zhang Ben Zhong Tang Prof. Lintao Cai Prof. Ping Gong Guangdong Key Laboratory of Nanomedicine Shenzhen Engineering Laboratory of Nanomedicine and Nanoformulations CAS-HK Joint Lab for Biomaterials Research Laboratory for Biomedical Optics and Molecular Imaging Shenzhen Key Laboratory for Molecular Imaging CAS Key Lab for Health Informatics Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China University of Chinese Academy of Sciences Beijing 100049 China Contribution: Data curation (lead) Validation (lead) Writing - original draft (lead) Nano Science and Technology Institute University of Science & Technology of China Suzhou 215123 China Contribution: Data curation (equal) Investigation (equal) Key Laboratory of Environmentally Friendly Chemistry and Application of the Ministry of Education College of Chemistry Xiangtan University Xiangtan 411105 China Contribution: Data curation (supporting) Methodology (supporting) Contribution: Project administration (supporting) Resources (supporting) Supervision (supporting) Writing - review & editing (equal) Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Institute for Advanced Study The Hong Kong University of Science and Technology (HKUST) Clear Water Bay Kowloon Hong Kong China Contribution: Funding acquisition (equal) Supervision (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (lead) Methodology (equal) Project administration (lead) Resources (equal) Supervision (equal) Writing - original draft (equal) Writing - review & editing (lead) School of Science and Engineering Shenzhen Institute of Aggregate Science and Technology The Chinese University of Hong Kong Shenzhen Guangdong 518172 China Contribution: Formal analysis (supporting) Funding acquisition (equal) Writing - review & editing (supporting) Contribution: Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - revi

Low-temperature photothermal therapy (PTT), which circumvents the limitations of conventional PTT (e.g., thermotolerance and adverse effects), is an emerging therapeutic strategy which shows great potential for future clinical applications. The expression of heat shock proteins (HSPs) can dramatically impair the therapeutic efficacy of PTT. Thus, inhibition of HSPs repair and reducing the damage of nearby normal cells is crucial for improving the efficiency of low-temperature PTT. Herein, we developed a nanobomb based on the self-assembly of NIRII AIE polymer PBPTV and carbon monoxide (CO) carrier polymer mPEG(CO). This smart nanobomb can be exploded in a tumor microenvironment in which hydrogen peroxide is overexpressed and release CO into cancer cells to significantly inhibit the expression of HSPs and hence improve the antitumor efficiency of the low-temperature PTT.

关键词： Aggregation Induced Emission Gas Therapy Heat Shock Protein NIR-II Photothermal Therapy

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Configuration-Induced Multichromism of Phenanthridine Derivatives: A Type of Versatile Fluorescent Probe for Microenvironmental Monitoring

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Angewandte Chemie 2023年第9期135卷

作者： Wei Huang Dr. Shiyu Feng Jie Liu Baoshuai Liang Ya Zhou Mengya Yu Jiayuan Liang Prof. Jiaguo Huang Prof. Xujie Lü Prof. Weiguo Huang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 155 Yangqiao West Road Fuzhou Fujian 350002 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Validation (lead) Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 P. R. China University of Chinese Academy of Sciences 19 A Yuquan Road Beijing 100049 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Software (equal) Validation (equal) Visualization (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) School of Pharmaceutical Sciences Sun Yat-sen University Guangzhou 510006 P. R. China Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Center for High Pressure Science and Technology Advanced Research (HPSTAR) Shanghai 201203 P. R. China Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead)

Fluorescent probes are attractive in diagnosis and sensing. However, most reported fluorophores can only detect one or few analytes/parameters, notably limiting their applications. Here we have designed three phenanthridine-based fluorophores (i.e., B1 , F1 , and T1 with 1D, 2D, and 3D molecular configuration, respectively) capable of monitoring various microenvironments. In rigidifying media, all fluorophores show bathochromic emissions but with different wavelength and intensity changes. Under compression, F1 shows a bathochromic emission of over 163 nm, which results in organic fluorophore-based full-color piezochromism. Moreover, both B1 and F1 exhibit an aggregation-caused quenching (ACQ) behavior, while T1 is an aggregation-induced emission (AIE) fluorophore. Further, F1 and T1 selectively concentrate in cell nucleus, whereas B1 mainly stains the cytoplasm in live cell imaging. This work provides a general design strategy of versatile fluorophores for microenvironmental monitoring.

关键词： Bioimaging Configuration-Induced Multichromism Microenvironmental Monitoring Optical Sensing Phenanthridine Derivatives

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Favoring CO Intermediate Stabilization and Protonation by Crown Ether for CO2Electromethanation in Acidic Media

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Angewandte Chemie 2023年第50期135卷

作者： Keqiang Xu Jinhan Li Fangming Liu Xijie Chen Tete Zhao Fangyi Cheng Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Engineering Research Center on High-Efficiency Energy Storage (Ministry of Education) Renewable Energy Conversion and Storage Center College of Chemistry Nankai University Tianjin 300071 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Visualization (lead) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (equal) Investigation (supporting) Methodology (equal) Software (equal) Validation (equal) Frontiers Science Center for New Organic Matter Nankai University Tianjin 300071 China Contribution: Formal analysis (equal) Funding acquisition (supporting) Methodology (equal) Project administration (lead) Validation (supporting) Writing - review & editing (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Visualization (supporting) Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192 China Contribution: Conceptualization (lead) Formal analysis (equal) Methodology (equal) Resources (lead) Supervision (lead) Writing - review & editing (equal)

The large-scale deployment of CO 2 electroreduction is hampered by deficient carbon utilization in neutral and alkaline electrolytes due to CO 2 loss into (bi)carbonates. Switching to acidic media mitigates carbonation, but suffers from low product selectivity because of hydrogen evolution. Here we report a crown ether decoration strategy on a Cu catalyst to enhance carbon utilization and selectivity of CO 2 methanation under acidic conditions. Macrocyclic 18-Crown-6 is found to enrich potassium cations near the Cu electrode surface, simultaneously enhancing the interfacial electric field to stabilize the *CO intermediate and accelerate water dissociation to boost *CO protonation. Remarkably, the mixture of 18-Crown-6 and Cu nanoparticles affords a CH 4 Faradaic efficiency of 51.2 % and a single pass carbon efficiency of 43.0 % toward CO 2 electroreduction in electrolyte with pH=2. This study provides a facile strategy to promote CH 4 selectivity and carbon utilization by modifying Cu catalysts with supramolecules.

关键词： CO2 Electroreduction Copper Catalyst Crown Ether Methanation Protonation

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Self-Assembly of Peapod-like Micrometer Tubes from a Planet-Satellite-type Supramolecular Megamer

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Angewandte Chemie 2022年第46期134卷

作者： Dr. Fugui Xu Dr. Ke Li Dr. Shanlong Li Chen Li Dr. Chunyang Yu Dr. Yuling Wang Dr. Wenfeng Jiang Prof. Shaoliang Lin Prof. Yiyong Mai Prof. Yongfeng Zhou School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative Molecules State Key Laboratory of Metal Matrix Composites Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing Shanghai Jiao Tong University 800 Dongchuan Road Shanghai 200240 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Writing - original draft (equal) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Software (lead) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Methodology (supporting) Software (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Formal analysis (supporting) Software (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Project administration (supporting) Contribution: Formal analysis (supporting) Methodology (supporting) Project administration (supporting) Shanghai Key Laboratory of Advanced Polymeric Materials Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China Contribution: Conceptualization (equal) Methodology (supporting) Project administration (equal) Supervision (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Methodology (equal) Project

This study presents interesting self-assembly of peapod-like micrometer tubes from a planet-satellite-type supramolecular megamer, which was constructed through the specific host–guest molecular recognition between azobenzene (AZO)-functionalized hyperbranched poly(ethyl-3-oxetanemethanol)- star -poly(ethylene oxide) (HSP-AZO) and β -cyclodextrin(CD)-based hydrophilic hyperbranched polyglycerol (CD- g -HPG). A peapod-like structure with micrometer-sized tube as the pod and vesicles encapsulated inside as the peas was formed through sequential vesicle entosis, linear association, and fusion processes. Dissipative particle dynamics (DPD) simulations support the structural possibility of the supramolecular peapod formation and its mechanism. UV light irradiation could lead to the disassembly of the peapod-like structure. This study expands the family of supramolecular polymers and opens a new avenue to develop bioinspired complex hierarchical nanoarchitectures at the microscopic level.

关键词： Host–Guest Interaction Hyperbranched Polymers Self-Assembly Supramolecular Polymers Vesicles

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Fluorine-Containing Passivation Layer via Surface Chelation for Inorganic Perovskite Solar Cells

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Angewandte Chemie 2022年第6期135卷

作者： Hao Zhang Prof. Wanchun Xiang Xuejiao Zuo Xiaojing Gu Shiang Zhang Yachao Du Zhiteng Wang Yali Liu Haifeng Wu Peijun Wang Qingyue Cui Hang Su Prof. Qingwen Tian Prof. Shengzhong (Frank) Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University No. 620 West Chang'an Avenue Xi'an 710119 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Writing - original draft (lead) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (equal) Investigation (equal) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) State Key Laboratory of Organic-Inorganic Composites Key Lab of Biomedical Materials of Natural Macromolecules Ministry of Education Beijing Laboratory of Biomedical Materials Beijing University of Chemical Technology No. 15 East Road North Third Ring Chaoyang District Beijing 100029 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Validation (lead) Visualization (lead) Writing - review & editing (lead) Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences No. 457 Zhongshan Road Dalian Liaoning 116023 P. R. China Contribution: Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (equal)

Minimizing surface defect is vital to further improve power conversion efficiency (PCE) and stability of inorganic perovskite solar cells (PSCs). Herein, we designed a passivator trifluoroacetamidine (TFA) to suppress CsPbI 3− x Br x film defects. The amidine group of TFA can strongly chelate onto the perovskite surface to suppress the iodide vacancy, strengthened by additional hydrogen bonds. Moreover, three fluorine atoms allow strong intermolecular connection via intermolecular hydrogen bonds, thus constructing a robust shield against moisture. The TFA-treated PSCs exhibit remarkably suppressed recombination, yielding the record PCEs of 21.35 % and 17.21 % for 0.09 cm 2 and 1.0 cm 2 device areas, both of which are the highest for all-inorganic PSCs so far. The device also achieves a PCE of 39.78 % under indoor illumination, the highest for all-inorganic indoor photovoltaic devices. Furthermore, TFA greatly improves device ambient stability by preserving 93 % of the initial PCE after 960 h.

关键词： Chelation Defect Passivation Inorganic Perovskite Solar Cells

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