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Goldilocks Energy Minimum: Peptide-Based Reversible Aggregation and Biosensing (Vol 15, Pg 42293, 2023)

ACS APPLIED materials & INTERFACES 2023年第41期15卷 48838-48838页

作者： Yim, Wonjun Retout, Maurice Chen, Amanda A. Ling, Chuxuan Amer, Lubna Jin, Zhicheng Chang, Yu-Ci Chavez, Saul Barrios, Karen Lam, Benjamin Li, Zhi Zhou, Jiajing Shi, Lingyan Pascal, Tod A. Jokerst, Jesse V. Materials Science and Engineering Program University of California San Diego La Jolla California 92093 United States Department of Nano and Chemical Engineering University of California San Diego La Jolla California 92093 United States Shu Chien-Gene Lay Department of Bioengineering University of California San Diego La Jolla California 92093 United States Department of Radiology University of California San Diego La Jolla California 92093 United States

Colorimetric biosensors based on gold nanoparticle (AuNP) aggregation are often challenged by matrix interference in biofluids, poor specificity, and limited utility with clinical samples. Here, we propose a peptide-driven nanoscale disassembly approach, where AuNP aggregates induced by electrostatic attractions are dissociated in response to proteolytic cleavage. Initially, citrate-coated AuNPs were assembled via a short cationic peptide (RRK) and characterized by experiments and simulations. The dissociation peptides were then used to reversibly dissociate the AuNP aggregates as a function of target protease detection, i.e., main protease (Mpro), a biomarker for severe acute respiratory syndrome coronavirus 2. The dissociation propensity depends on peptide length, hydrophilicity, charge, and ligand architecture. Finally, our dissociation strategy provides a rapid and distinct optical signal through Mpro cleavage with a detection limit of 12.3 nM in saliva. Our dissociation peptide effectively dissociates plasmonic assemblies in diverse matrices including 100% human saliva, urine, plasma, and seawater, as well as other types of plasmonic nanoparticles such as silver. Our peptide-enabled dissociation platform provides a simple, matrix-insensitive, and versatile method for protease sensing.

关键词： colorimetric biosensor DLVO theory reversible aggregation dissociation peptide matrix-insensitive SARS-CoV-19

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Method for the extraction of circulating nucleic acids based on MOF reveals cell-free RNA signatures in liver cancer

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National science Review 2024年第1期11卷 94-106页

作者： Yuqing Sun Haixin Yu Shaoqing Han Ruoxi Ran Ying Yang Yongling Tang Yuhao Wang Wenhao Zhang Heng Tang Boqiao Fu Boshi Fu Xiaocheng Weng Song-Mei Liu Hexiang Deng Shuang Peng Xiang Zhou College of Chemistry and Molecular Sciences Key Laboratory of Biomedical Polymers-Ministry of Education Wuhan University Department of Digestive Surgical Oncology Union Hospital Tongji Medical College Huazhong University of Science and Technology Cancer Center Union HospitalTongji Medical CollegeHuazhong University of Science and Technology Department of Clinical Laboratory Center for Gene Diagnosis and Program of Clinical Laboratory Zhongnan Hospital of Wuhan University College of Chemistry and Materials Science Hubei Engineering University Department of Pharmacology School of Pharmacy China Medical University Taikang Center for Life and Medical Sciences Wuhan University Department of Hematology Zhongnan Hospital of Wuhan University

Cell-free RNA(cf RNA) allows assessment of health, status, and phenotype of a variety of human organs and is a potential biomarker to non-invasively diagnose numerous diseases. Nevertheless, there is a lack of highly efficient and bias-free cf RNA isolation technologies due to the low abundance and instability of cf ***, we developed a reproducible and high-efficiency isolation technology for different types of cell-free nucleic acids(containing cf RNA and viral RNA) in serum/plasma based on the inclusion of nucleic acids by metal-organic framework(MOF) materials, which greatly improved the isolation efficiency and was able to preserve RNA integrity compared with the most widely used research kit method. Importantly, the quality of cf RNA extracted by the MOF method is about 10-fold that of the kit method, and the MOF method isolates more than three times as many different RNA types as the kit method. The whole transcriptome mapping characteristics of cf RNA in serum from patients with liver cancer was described and a cf RNA signature with six cf RNAs was identified to diagnose liver cancer with high diagnostic efficiency(area under curve = 0.905 in the independent validation cohort) using this MOF method. Thus, this new MOF isolation technique will advance the field of liquid biopsy, with the potential to diagnose liver cancer.

关键词： MOF circulating cell-free RNA biomarker liver cancer diagnosis

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End-to-End Reaction Field Energy Modeling via Deep Learning based Voxel-to-voxel Transform

arXiv

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arXiv 2024年

作者： Wu, Yongxian Zhu, Qiang Luo, Ray Department of Chemical and Biomolecular Engineering Molecular Biology and Biochemistry Materials Science and Engineering and Biomedical Engineering University of California Irvine IrvineCA92697 United States

In computational biochemistry and biophysics, understanding the role of electrostatic interactions is crucial for elucidating the structure, dynamics, and function of biomolecules. The Poisson-Boltzmann (PB) equation is a foundational tool for modeling these interactions by describing the electrostatic potential in and around charged molecules. However, solving the PB equation presents significant computational challenges due to the complexity of biomolecular surfaces and the need to account for mobile ions. While traditional numerical methods for solving the PB equation are accurate, they are computationally expensive and scale poorly with increasing system size. To address these challenges, we introduce PBNeF, a novel machine learning approach inspired by recent advancements in neural network-based partial differential equation solvers. Our method formulates the input and boundary electrostatic conditions of the PB equation into a learnable voxel representation, enabling the use of a neural field transformer to predict the PB solution and, subsequently, the reaction field potential energy. Extensive experiments demonstrate that PBNeF achieves over a 100-fold speedup compared to traditional PB solvers, while maintaining accuracy comparable to the Generalized Born (GB) model. Copyright © 2024, The Authors. All rights reserved.

关键词： Boltzmann equation

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High-Performance Unipolar n-Type Conjugated Polymers Enabled by Highly Electron-Deficient Building Blocks Containing F and CN Groups (vol 55, pg 4429, 2022)

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MACROMOLECULES 2022年第14期55卷 6295-6295页

作者： Zhang, Chan Tan, Wen Liang Liu, Zhongwei He, Qiao Li, Yanru Ma, Jianeng Chesman, Anthony S. R. Han, Yang McNeill, Christopher R. Heeney, Martin Fei, Zhuping Institute of Molecular Plus Department of Chemistry Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin University Tianjin 300072 China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192 China Department of Materials Science and Engineering Monash University Clayton Victoria 3800 Australia Department of Chemistry and Centre for Plastic Electronics White City Campus Imperial College London London W120BZ U.K. CSIRO Manufacturing Ian Wark Laboratories Clayton Victoria 3168 Australia School of Materials Science and Engineering and Tianjin Key Laboratory of Molecular Optoelectronic Science Tianjin University Tianjin 300072 China

A highly electron-deficient building block, (E)-2,2′-(ethene-1,2-diyl)bis(4-chlorothiophene-3-carbonitrile) (2F2CNTVT), was designed and synthesized by the introduction of fluorine and cyano groups simultaneously onto the β position of thiophene units in (E)-1,2-di(thiophen-2-yl)ethene (TVT). A series of conjugated copolymers with different alkyl side chains were successfully synthesized via direct arylation polymerization (DArP) of 2F2CNTVT with thiophene-flanked diketopyrrolopyrrole (DPP) or isoindigo (IID) monomers. The resulting polymers exhibited improved planarity due to intramolecular or intermolecular F···S or F···H weak interactions and low-lying energy levels to realize stable and unipolar electron transport in organic thin film transistors (OTFTs). The microstructure and electrical performance of the polymers were confirmed to be dependent on the length of the side chains. Containing the longest side chains, P2F2CNTVT–DPP-3 and P2F2CNTVT–IID-3 displayed relatively higher μe of 2.03 and 2.92 cm2 V–1 s–1 with on/off ratios of up to 105–106, respectively, which was related to the favorable alignment of polymer chains for lower paracrystallinity and more ordered transport channels. Furthermore, the high-mobility OTFTs showed good air stability after a 1 month exposure to an ambient atmosphere due to their sufficiently low-lying LUMO levels. Our strategy of combining both F and CN groups in the same unit demonstrated its potential for high-performance n-type OTFT materials and can be extended to the design of new electron-deficient building blocks.

关键词： Alkyls Charge transport Conjugated polymers Polymer films Polymers

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engineering H2O2 Self-Supplying Platform for Xdynamic Therapies via Ru-Cu Peroxide Nanocarrier: Tumor Microenvironment-Mediated Synergistic Therapy

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ACS Applied materials and Interfaces 2024年第19期16卷 24172-24190页

作者： Dirersa, Worku Batu Kan, Tzu-Chun Chang, Jungshan Getachew, Girum Ochirbat, Sonjid Kizhepat, Shamsa Wibrianto, Aswandi Rasal, Akash Chen, Hung-An Ghule, Anil Vithal Chou, Tzung-Han Chang, Jia-Yaw Department of Chemical Engineering National Taiwan University of Science and Technology Taipei106335 Taiwan Graduate Institute of Medical Sciences College of Medicine Taipei Medical University Taipei11031 Taiwan International Master/Ph.D. Program in Medicine College of Medicine Taipei Medical University Taipei11031 Taiwan International Ph.D. Program for Cell Therapy and Regeneration Medicine College of Medicine Taipei Medical University Taipei11031 Taiwan Green Nanotechnology Laboratory Department of Chemistry Shivaji University Kolhapur416004 India Department of Chemical and Materials Engineering National Yunlin University of Science and Technology Yunlin64002 Taiwan

Of the most common, hypoxia, overexpressed glutathione (GSH), and insufficient H2O2 concentration in the tumor microenvironment (TME) are the main barriers to the advancment of reactive oxygen species (ROS) mediated Xdynamic therapies (X = photo, chemodynamic, chemo). Maximizing Fenton catalytic efficiency is crucial in chemodynamic therapy (CDT), yet endogenous H2O2 levels are not sufficient to attain better anticancer efficacy. Specifically, there is a need to amplify Fenton reactivity within tumors, leveraging the unique attributes of the TME. Herein, for the first time, we design RuxCu1-xO2-Ce6/CPT (RCpCCPT) anticancer nanoagent for TME-mediated synergistic therapy based on heterogeneous Ru-Cu peroxide nanodots (RuxCu1-xO2 NDs) and chlorine e6 (Ce6), loaded with ROS-responsive thioketal (TK) linked-camptothecin (CPT). The Ru-Cu peroxide NDs (RCp NDs, x = 0.50) possess the highest oxygen vacancy (OV) density, which grants them the potential to form massive Lewis’s acid sites for peroxide adsorption, while the dispersibility and targetability of the NDs were improved via surface modification using hyaluronic acid (HA). In TME, RCpCCPT degrades, releasing H2O2, Ru2+/3+, and Cu+/2+ ions, which cooperatively facilitate hydroxyl radical (•OH) formation and deactivate antioxidant GSH enzymes through a cocatalytic loop, resulting in excellent tumor therapeutic efficacy. Furthermore, when combined with laser treatment, RCpCCPT produces singlet oxygen (1O2) for PDT, which induces cell apoptosis at tumor sites. Following ROS generation, the TK linkage is disrupted, releasing up to 92% of the CPT within 48 h. In vitro investigations showed that laser-treated RCpCCPT caused 81.5% cell death from PDT/CDT and chemotherapy (CT). RCpCCPT in cancer cells produces red-blue emission in images of cells taking them in, which allows for fluorescence image-guided Xdynamic treatment. The overall results show that RCp NDs and RCpCCPT are more biocompatible and have excellent Xdynamic the

关键词： Oxidation

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Two-dimensional MXenes:New frontier of wearable and flexible electronics

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InfoMat 2022年第4期4卷 1-28页

作者： Abbas Ahmed Sudeep Sharma Bapan Adak Md Milon Hossain Anna Marie LaChance Samrat Mukhopadhyay Luyi Sun Polymer Program Institute of Materials ScienceUniversity of ConnecticutStorrsConnecticutUSA Advanced Sensor and Energy Research(ASER)Lab Department of Electronic EngineeringKwangwoon UniversitySeoulSouth Korea Department of Textile and Fiber Engineering Indian Institute of TechnologyNew DelhiIndia Department of Textile Engineering Chemistry and ScienceNorth Carolina State UniversityRaleighNorth CarolinaUSA Department of Textile Engineering Khulna University of Engineering&TechnologyKhulnaBangladesh Department of Chemical and Biomolecular Engineering University of ConnecticutStorrsConnecticutUSA

Wearable electronics offer incredible benefits in mobile healthcare monitoring,sensing,portable energy harvesting and storage,human-machine interactions,etc.,due to the evolution of rigid electronics structure to flexible and stretchable ***,transition metal carbides and nitrides(MXenes)are highly regarded as a group of thriving two-dimensional nanomaterials and extraordinary building blocks for emerging flexible electronics platforms because of their excellent electrical conductivity,enriched surface functionalities,and large surface *** article reviews the most recent developments in MXene-enabled flexible electronics for wearable *** MXeneenabled electronic devices designed on a nanometric scale are highlighted by drawing attention to widely developed nonstructural attributes,including 3D configured devices,textile and planer substrates,bioinspired structures,and printed ***,the unique progress of these nanodevices is highlighted by representative applications in healthcare,energy,electromagnetic interference(EMI)shielding,and humanoid control of *** emerging prospects of MXene nanomaterials as a key frontier in nextgeneration wearable electronics are envisioned and the design challenges of these electronic systems are also discussed,followed by proposed solutions.

关键词： flexible electronics MXene nanostructures wearable electronics

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Alkyl-thiophene-alkyl linkers to construct double-cable conjugated polymers for single-component organic solar cells

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Chinese chemical Letters 2024年第1期35卷 542-546页

作者： Wenbin Lai Safakath Karuthedath Chengyi Xiao Lei Meng Frédéric Laquai Weiwei Li Yongfang Li Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Beijing Advanced Innovation Center for Soft Matter Science and Engineering&State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China King Abdullah University of Science and Technology(KAUST) KAUST Solar Center(KSC)Physical Sciences and Engineering Division(PSE)Material Science and Engineering Program(MSE)Thuwal 23955-6900Kingdom of Saudi Arabia University of Chinese Academy of Sciences Beijing 100049China Institute of Materials Research Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

In this work,semirigid linkers of the alkyl-thiophene-alkyl structure are developed to construct double-cable *** alkyl units,propyl(C3H6),hexyl(C6H12),and dodecyl(C12H24),are applied as semirigid linkers,yielding three double-cable polymers:PBC6-T,PBC12-T,and PBC24-T,***12-T which uses C6H12-thiophene-C6H12 linkers is found to exhibit the best device efficiency of 5.56%,while PBC6-T and PBC24-T with shorter or longer linkers yield device efficiencies of only 2.65%and 1.09%in single-component organic solar cells(SCOSCs).Further studies reveal that PBC12-T exhibits higher crystallinity and improved charge transport,resulting in better *** work provides an approach to construct double-cable conjugated polymers with long alkyl linkers,and it shows the importance of the linker length for the photovoltaic performance of SCOSCs.

关键词： Double-cable conjugated polymer Single-component organic solar cell Crystallinity Semirigid linkers Alkyl-thiophene-alkyl

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Graphene-functionalized textile composites for wearable Joule heating applications

Advanced Nanocomposites

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Advanced Nanocomposites 2025年 2卷 108-123页

作者： Omar Faruk Abbas Ahmed Ashfaqul Hoque Khadem Lu Jia Luyi Sun Department of Materials Science and Engineering Binghamton University State University of New York at Binghamton NY 13902 USA Polymer Program Institute of Materials Science and Department of Chemical & Biomolecular Engineering University of Connecticut Storrs CT 06269 USA Department Mechanical Engineering College of Engineering Computing and Applied Science Clemson University Clemson SC 29634 USA College of Textile Engineering Taiyuan University of Technology Jinzhong Shanxi 030600 China

Thermal comfort is essential for maintaining physiological well-being, with textile materials traditionally serving as the primary medium for regulating heat exchange between the body and its environment. However, conventional textiles often fall short of maintaining optimal thermal balance. So, there is an increasing demand for advanced thermoregulation systems that can effectively reduce heat loss and enhance warmth, ensuring consistent comfort. Recent research has highlighted the promise of advanced functional materials, especially graphene and its composites, for modifying textiles to improve thermal properties. This article comprehensively reviews recent advancements in graphene-functionalized textile composites, focusing on their applications in wearable Joule heaters designed for personalized thermal comfort or thermal therapy. Various graphene-functionalized textile composites are reviewed from the perspectives of material properties, processing strategies and device fabrication methods. Key challenges and future opportunities are summarized for graphene-functionalized textile-based Joule heaters as innovative solutions in wearable thermal regulation.

关键词： Graphene Textile Composite Wearable electronics Joule heater

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A smart DNA hydrogel for isolation of bacterial outer membrane vesicles and localized cancer immunotherapy

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science China materials 2024年第12期67卷 3872-3884页

作者： Rui Zhang Lele Chang Jing Wang Mengxue Huang Zhen Cui Siqi Li Jingwen Zhao Chi Yao Dayong Yang Department of Chemistry State Key Laboratory of Molecular Engineering of PolymersShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsCollege of Chemistry and MaterialsFudan UniversityShanghai 200438China Frontiers Science Center for Synthetic Biology Key Laboratory of Systems Bioengineering(MOE)School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Department of Gastroenterology and Hepatology Tianjin Medical University General HospitalTianjin 300350China

Bacterial outer membrane vesicles(OMVs)have shown great potential in cancer *** isolation of OMVs from complex media with high purity and high bioactivity is the prerequisite of therapeutic applications,which remains highly ***,we report a smart DNA hydrogel for the efficient isolation of OMVs from bacterial culture medium,which is further applied for localized cancer *** DNA hydrogel is constructed through the cross-linking of two ultralong DNA chains generated via rolling circle amplification(RCA).One chain contains polyvalent GN6 aptamer for the specific capture of OMVs,and the other contains polyvalent programmed death-1(PD-1)aptamer for the blocking of PD-1 immune checkpoint on the surface of T *** OMVs capsulated by DNA hydrogel maintain high immunostimulatory *** the mouse model of melanoma,this OMVs-containing DNA hydrogel shows a remarkable tumor inhibition rate of∼95%.This smart DNA hydrogel represents a promising biomedical platform for the efficient isolation of bacterial-derived OMVs,and provides a powerful strategy for cancer immunotherapy.

关键词： DNA nanotechnology DNA hydrogel bacterial outer membrane vesicles cancer immunotherapy

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Using 4D-STEM to Map 3D Morphologies of 2D materials

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Microscopy and microanalysis : the official journal of Microscopy Society of America, Microbeam Analysis Society, Microscopical Society of Canada 2023年第1期29卷 262-263页

作者： Mireles, Adan Shi, Chuqiao Park, Jeongwon Shin, Bongki Sung, Suk Hyun Ophus, Colin Hovden, Robert Kang, Kibum Han, Yimo Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston TX United States Department of Materials Science and NanoEngineering Rice University Houston TX United States Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology (KAIST) Daejeon South Korea Department of Materials Science and Engineering University of Michigan Ann Arbor MI United States National Center for Electron Microscopy Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA United States

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