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Photoresponsive Materials: Photoprogrammable Mesogenic Soft Helical Architectures: A Promising Avenue toward Future Chiro‐Optics (Adv. Mater. 41/2020)

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Advanced Materials 2020年第41期32卷

作者： Zhi‐Gang Zheng Yan‐Qing Lu Quan Li Department of Physics East China University of Science and Technology Shanghai 200237 China National Laboratory of Solid State Microstructures Key Laboratory of Intelligent Optical Sensing and Manipulation Collaborative Innovation Center of Advanced Microstructures and College of Engineering and Applied Sciences Nanjing University Nanjing 210093 China Advanced Materials and Liquid Crystal Institute and Chemical Physics Interdisciplinary Program Kent State University Kent OH 44242 USA

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Overcoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure

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Nature communications 2024年第1期15卷 707页

作者： Mohamed Hammad Elsayed Mohamed Abdellah Ahmed Zaki Alhakemy Islam M A Mekhemer Ahmed Esmail A Aboubakr Bo-Han Chen Amr Sabbah Kun-Han Lin Wen-Sheng Chiu Sheng-Jie Lin Che-Yi Chu Chih-Hsuan Lu Shang-Da Yang Mohamed Gamal Mohamed Shiao-Wei Kuo Chen-Hsiung Hung Li-Chyong Chen Kuei-Hsien Chen Ho-Hsiu Chou Department of Chemistry Faculty of Science Al-Azhar University Nasr City 11884 Cairo Egypt. Institute of Atomic and Molecular Sciences Academia Sinica Taipei 10617 Taiwan. Center for Condensed Matter Sciences National Taiwan University Taipei 10617 Taiwan. Department of Chemical Engineering National Tsing Hua University Hsinchu 300044 Taiwan. Department of Chemistry United Arab Emirates University Al Ain P.O. Box 15551 United Arab Emirates. Department of Chemistry Qena Faculty of Science South Valley University 83523 Qena Egypt. Chemical Physics and NanoLund Lund University 22100 Lund Sweden. Chemistry Department Faculty of Science Al-Azhar University Assiut 71542 Egypt. Sustainable Chemical Science and Technology Taiwan International Graduate Program Taipei Taiwan. Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 30010 Taiwan. Institute of Chemistry Academia Sinica 128 Sec 2 Academia Rd. Nankang Taipei 11529 Taiwan. Institute of Photonics Technologies National Tsing Hua University Hsinchu 300044 Taiwan. Center of Atomic Initiative for New Materials National Taiwan University Taipei 10617 Taiwan. Department of Chemical Engineering National Chung Hsing University Taichung 40227 Taiwan. Department of Materials and Optoelectronic Science Center for Functional Polymers and Supramolecular Materials National Sun Yat-Sen University Kaohsiung 804 Kaohsiung Taiwan. Department of Physics National Taiwan University Taipei 10617 Taiwan. Department of Chemical Engineering National Tsing Hua University Hsinchu 300044 Taiwan. hhchou@mx.nthu.edu.tw.

Designing an organic polymer photocatalyst for efficient hydrogen evolution with visible and near-infrared (NIR) light activity is still a major challenge. Unlike the common behavior of gradually increasing the charge recombination while shrinking the bandgap, we present here a series of polymer nanoparticles (Pdots) based on ITIC and BTIC units with different π-linkers between the acceptor-donor-acceptor (A-D-A) repeated moieties of the polymer. These polymers act as an efficient single polymer photocatalyst for H2 evolution under both visible and NIR light, without combining or hybridizing with other materials. Importantly, the difluorothiophene (ThF) π-linker facilitates the charge transfer between acceptors of different repeated moieties (A-D-A-(π-Linker)-A-D-A), leading to the enhancement of charge separation between D and A. As a result, the PITIC-ThF Pdots exhibit superior hydrogen evolution rates of 279 µmol/h and 20.5 µmol/h with visible (>420 nm) and NIR (>780 nm) light irradiation, respectively. Furthermore, PITIC-ThF Pdots exhibit a promising apparent quantum yield (AQY) at 700 nm (4.76%).

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OpenMM 8: Molecular Dynamics Simulation with Machine Learning Potentials

arXiv

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arXiv 2023年

作者： Eastman, Peter Galvelis, Raimondas Peláez, Raúl P. Abreu, Charlles R.A. Farr, Stephen E. Gallicchio, Emilio Gorenko, Anton Henry, Michael M. Hu, Frank Huang, Jing Krämer, Andreas Michel, Julien Mitchell, Joshua A. Pande, Vijay S. Rodrigues, João P.G.L.M. Rodriguez-Guerra, Jaime Simmonett, Andrew C. Singh, Sukrit Swails, Jason Turner, Philip Wang, Yuanqing Zhang, Ivy Chodera, John D. De Fabritiis, Gianni Markland, Thomas E. Department of Chemistry Stanford University StanfordCA94305 United States Acellera Labs C Dr Trueta 183 Barcelona08005 Spain C Dr. Aiguader 88 Barcelona08003 Spain Chemical Engineering Department School of Chemistry Federal University of Rio de Janeiro Rio de Janeiro68542 Brazil Redesign Science Inc. 180 Varick St. New YorkNY10014 United States EaStCHEM School of Chemistry University of Edinburgh EH9 3FJ United Kingdom Department of Chemistry and Biochemistry Brooklyn College The City University of New York NY United States Ph.D. Program in Chemistry Ph.D. Program in Biochemistry The Graduate Center of the City University of New York New YorkNY United States Stream HPC Koningin Wilhelminaplein 1 - 40601 Amsterdam1062 HG Netherlands Computational and Systems Biology Program Sloan Kettering Institute Memorial Sloan Kettering Cancer Center New YorkNY10065 United States Key Laboratory of Structural Biology of Zhejiang Province School of Life Sciences Westlake University 18 Shilongshan Road Zhejiang Hangzhou310024 China Department of Mathematics and Computer Science Freie Universität Berlin Arnimallee 12 Berlin14195 Germany The Open Force Field Initiative Open Molecular Software Foundation DavisCA95616 United States Andreessen Horowitz 2865 Sand Hill Rd Menlo ParkCA94025 United States Department of Structural Biology Stanford University StanfordCA94305 United States Charité Universitätsmedizin Berlin In silico Toxicology and Structural Bioinformatics Virchowweg 6 Berlin10117 Germany Laboratory of Computational Biology National Heart Lung and Blood Institute National Institutes of Health BethesdaMD20892 United States Entos Inc. 9310 Athena Circle La Jolla CA92037 United States College of Engineering Virginia Polytechnic Institute State University BlacksburgVA24061 United States Simons Center for Computational Physical Chemistry Center for Data Science New York University 24 Waverly Place New YorkNY10004 United States T

Machine learning plays an important and growing role in molecular simulation. The newest version of the OpenMM molecular dynamics toolkit introduces new features to support the use of machine learning potentials. Arbitrary PyTorch models can be added to a simulation and used to compute forces and energy. A higher-level interface allows users to easily model their molecules of interest with general purpose, pretrained potential functions. A collection of optimized CUDA kernels and custom PyTorch operations greatly improves the speed of simulations. We demonstrate these features on simulations of cyclin-dependent kinase 8 (CDK8) and the green fluorescent protein (GFP) chromophore in water. Taken together, these features make it practical to use machine learning to improve the accuracy of simulations at only a modest increase in cost. Copyright © 2023, The Authors. All rights reserved.

关键词： Machine learning

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Clinical Features and Outcomes of Primary Breast Diffuse Large B-Cell Lymphoma: A Matched-Pair Study

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Clinical Medicine Insights: Oncology 2023年 17卷

作者： Teng, Ling-Chiao Liao, Yu-Min Gau, Jyh-Pyng Hsiao, Tzu-Hung Chen, Tsung-Chih Chen, Mei-Hui Yeh, Su-Peng Teng, Chieh-Lin Jerry Division of Hematology/Medical Oncology Department of Medicine Taichung Veterans General Hospital Taichung Taiwan Department of Hematology and Oncology China Medical University Hospital Taichung Taiwan Division of Hematology and Oncology Department of Medicine Taipei Medical University Hospital Taipei City Taiwan Department of Medical Research Taichung Veterans General Hospital Taichung Taiwan Department of Chemical Engineering National Tsing Hua University Hsinchu Taiwan Department of Public Health Fu Jen Catholic University New Taipei City Taiwan Institute of Genomics and Bioinformatics National Chung Hsing University Taichung Taiwan Department of Nursing Taichung Veterans General Hospital Taichung Taiwan College of Nursing Hung Kuang University Taichung Taiwan School of Medicine China Medical University Taichung Taiwan Department of Post-Baccalaureate Medicine College of Medicine National Chung Hsing University Taichung Taiwan Department of Life Science Tunghai University Taichung Taiwan School of Medicine Chung Shan Medical University Taichung Taiwan Ph.D. Program in Translational Medicine National Chung Hsing University Taichung Taiwan Rong Hsing Research Center for Translational Medicine National Chung Hsing University Taichung Taiwan

Background: The influence of the breast as the primary site on the outcome of diffuse large B-cell lymphoma (DLBCL) and further changes in therapeutic strategies remain unclear. We aimed to compare the outcomes between primary breast and non-breast DLBCL and analyze the genetic profiles of some of the study cohorts using next-generation sequencing. Methods: This matched-pair study reviewed the medical records of 19 patients with stage I and II primary breast DLBCL diagnosed between January 2005 and December 2021 on the basis of the Wiseman and Liao criteria, and we used 1:4 propensity score matching to identify patients with non-breast DLBCL as the control group. The overall response rate, progression-free survival (PFS), and overall survival (OS) were the outcome measures. Results: Patients with primary breast and non-breast DLBCL had a 5-year PFS of 72.6% and 86.9%, respectively (P =.206). These 2 groups also had comparable 5-year OS (86.9% vs 87.8%;P =.772). The breast as the primary site was not associated with inferior PFS (hazard ratio [HR]: 2.14;95% CI: 0.66-6.96;P =.206) and OS (HR: 1.26;95% CI: 0.27-5.93;P =.772). Conclusion: Patients with primary breast DLBCL and those with non-breast DLBCL had comparable PFS and OS under rituximab, cyclophosphamide, doxorubicin, vincristine, and prednisone (R-CHOP) or R-CHOP-like regimens. Further investigations of the mutation profile, its clinical impact, potential central nervous system relapse, and prognosis of primary breast DLBCL are required. © The Author(s) 2023.

关键词： breast DLBCL NGS OS PFS

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Cancer Therapy: Adipocyte-Derived Anticancer Lipid Droplets (Adv. Mater. 26/2021)

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Advanced Materials 2021年第26期33卷

作者： Tingxizi Liang Di Wen Guojun Chen Amanda Chan Zhaowei Chen Hongjun Li Zejun Wang Xiao Han Liping Jiang Jun-Jie Zhu Zhen Gu Department of Bioengineering University of California Los Angeles Los Angeles CA 90095 USA State Key Laboratory of Analytical Chemistry and Collaborative Innovation Center of Chemistry for Life Sciences School of Chemistry & Chemical Engineering Nanjing University Nanjing 210023 China Jonsson Comprehensive Cancer Center California NanoSystems Institute Los Angeles CA 90095 USA College of Pharmaceutical Sciences Zhejiang University Hangzhou 310058 China Zhejiang Laboratory of Systems & Precision Medicine Zhejiang University Medical Center Hangzhou 311121 China Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University Hangzhou 310016 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China

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Artificial Peptide-Protein Necrosomes Promote Cell Death

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Angewandte Chemie 2023年第49期135卷

作者： Ruo-Chen Guo Ning Wang Weishu Wang Zeyu Zhang Wendi Luo Yushi Wang Haiqin Du Prof. Yifei Xu Prof. Gongyu Li Prof. Zhilin Yu Key Laboratory of Functional Polymer Materials Ministry of Education State Key Laboratory of Medicinal Chemical Biology Institute of Polymer Chemistry College of Chemistry Nankai University Tianjin 300071 China State Key Laboratory of Medicinal Chemical Biology Research Center for Analytical Science and Tianjin Key Laboratory of Biosensing and Molecular Recognition Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin 300071 China Laboratory of Theoretical and Computational Nanoscience CAS Key Laboratory for Biological Effects of Nanomaterials & Nanosafety CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Beijing 100190 China State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science Fudan University Shanghai 200438 China

The presence of disordered region or large interacting surface within proteins significantly challenges the development of targeted drugs, commonly known as the “undruggable” issue. Here, we report a heterogeneous peptide-protein assembling strategy to selectively phosphorylate proteins, thereby activating the necroptotic signaling pathway and promoting cell necroptosis. Inspired by the structures of natural necrosomes formed by receptor interacting protein kinases (RIPK) 1 and 3, the kinase-biomimetic peptides are rationally designed by incorporating natural or D -amino acids, or connecting D -amino acids in a retro-inverso (DRI) manner, leading to one RIPK3-biomimetic peptide PR3 and three RIPK1-biomimetic peptides. Individual peptides undergo self-assembly into nanofibrils, whereas mixing RIPK1-biomimetic peptides with PR3 accelerates and enhances assembly of PR3 . In particular, RIPK1-biomimetic peptide DRI-PR1 exhibits reliable binding affinity with protein RIPK3, resulting in specific cytotoxicity to colon cancer cells that overexpress RIPK3. Mechanistic studies reveal the increased phosphorylation of RIPK3 induced by RIPK1-biomimetic peptides, elucidating the activation of the necroptotic signaling pathway responsible for cell death without an obvious increase in secretion of inflammatory cytokines. Our findings highlight the potential of peptide-protein hybrid aggregation as a promising approach to address the “undruggable” issue and provide alternative strategies for overcoming cancer resistance in the future.

关键词： Cancer Therapy Necroptosis Peptides Self-Assembly Supramolecular Chemistry

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Green Biomaterials: fundamental principles

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Green Biomaterials 2023年第1期1卷

作者： Navid Rabiee Mehmet R. Dokmeci Ali Zarrabi Pooyan Makvandi Mohammad Reza Saeb Hassan Karimi-Maleh Shima Jafarzadeh Ceren Karaman Yusuke Yamauchi Majid Ebrahimi Warkiani Sidi A. Bencherif Geeta Mehta Miharu Eguchi Ajeet Kaushik Mohammad-Ali Shahbazi Ana Cláudia Paiva-Santos Jacek Ryl Eder C. Lima Michael R. Hamblin Rajender S. Varma YunSuk Huh A. T. Ezhil Vilian Piyush Kumar Gupta Sandeep Kumar Lakhera Kavindra Kumar Kesari Yu-Ting Liu Mohammadreza Tahriri Ganji Seeta Rama Raju Mohsen Adeli Ali Mohammadi Jianglin Wang Mohd Zahid Ansari Tejraj Aminabhavi Houman Savoji Gautam Sethi Tomasz Bączek Agata Kot-Wasik Marcela Elisabeth Penoff Abdorreza Mohammadi Nafchi Justyna Kucinska-Lipka Masoumeh Zargar Mohsen Asadnia Amir Reza Aref Moein Safarkhani Milad Ashrafizadeh Reddicherla Umapathi Amir Ghasemi Milica Radisic a Centre for Molecular Medicine and Innovative Therapeutics Murdoch University Perth WA Australiab School of Engineering Macquarie University Sydney New South Wales Australia c Terasaki Institute for Biomedical Innovation (TIBI) Los Angeles CA90024 USA d Department of Biomedical Engineering Faculty of Engineering and Natural Sciences Istinye University Sariyer Istanbul Turkey e The Quzhou Affiliated Hospital of Wenzhou Medical University Quzhou People’s Hospital Zhejiang Quzhou Chinaf School of Engineering Institute for Bioengineering The University of Edinburgh Edinburgh United Kingdom g Department of Polymer Technology Faculty of Chemistry Gdańsk University of Technology Gdańsk Poland h School of Resources and Environment University of Electronic Science and Technology of China 611731 Xiyuan Ave Chengdu P. R. Chinai School of Engineering Lebanese American University Byblos Lebanon j School of Engineering Edith Cowan University Joondalup WA Australia k Department of Electricity and Energy Akdeniz University Antalya Turkey l Australian Institute for Bioengineering and Nanotechnology (AIBN) and School of Chemical Engineering The University of Queensland Brisbane QLD Australiam Department of Materials Process Engineering Graduate School of Engineering Nagoya University Nagoya Japan n School of Biomedical Engineering University of Technology Sydney Sydney NSW Australiao Faculty of Science Institute for Biomedical Materials and Devices (IBMD) University of Technology Sydney Sydney NSW Australia p Chemical Engineering Department Northeastern University Boston MA USAq Department of Bioengineering Northeastern University Boston MA USAr Harvard John A. Paulson School of Engineering and Applied Sciences Harvard University Cambridge MA USA s Department of Biomedical Engineering University of Michigan Ann Arbor MI USAt Department of Materials Science and Engineering University of Michigan Ann Arbor MI USAu Macromolecular Science and Engineering

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Improvement of extracellular polysaccharides production from Cordyceps militaris immobilized alginate beads in repeated-batch fermentation

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LWT 2024年 193卷

作者： Hou, Shi-Jing Cheng, Kuan-Chen Lin, Shyh-Hsiang Hsiao, I-Lun Santoso, Shella Permatasari Singajaya, Stephanie Chou, Yu-Chieh Lin, Shin-Ping Master Program in Food Safety Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan Institute of Biotechnology National Taiwan University 1 Roosevelt Rd. Sec. 4 Taipei10617 Taiwan Graduate Institute of Food Science and Technology National Taiwan University 1 Roosevelt Rd. Sec. 4 Taipei10617 Taiwan Department of Medical Research China Medical University Hospital China Medical University 91 Hsueh-Shih Rd. Taichung40402 Taiwan Department of Optometry Asia University 500 Lioufeng Rd. Wufeng Taichung41354 Taiwan School of Nutrition and Health Sciences Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan School of Food Safety Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan Department of Chemical Engineering Widya Mandala Surabaya Catholic University Kalijudan 37 East Java Surabaya60114 Indonesia Collaborative Research Center for Sustainable and Zero Waste Industries Kalijudan 37 East Java Surabaya60114 Indonesia Ph.D. Program in Drug Discovery and Development Industry Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan Research Center of Biomedical Device Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan TMU Research Center for Digestive Medicine Taipei Medical University 250 Wu-Hsing Street Taipei11031 Taiwan

Cordyceps militaris (C. militaris) is a unique medicinal fungus of the genus Cordyceps. It has high economic value due to various biological functions from the extracellular polysaccharides (EPSs) it produces. The aim of this study was to establish a mycelium-immobilization system for EPS production in a bubble column system. First, EPS production was optimized by 90.2% (from 0.72 to 1.37 g/L) using response surface methodology under an alginate-immobilized mycelium system with 6 days of cultivation. The highest EPS production was obtained (5.3 g/L) in a flask system through elongation to 15 days of cultivation. EPS production subsequently further increased to 10.42 g/L utilizing a bubble column reactor. Furthermore, the system can be reused for at least three rounds. In the EPS characteristics analysis, the produced EPSs were mainly composed of glucose and galactose. They presented strong antibacterial activity against Staphylococcus aureus. In terms of antioxidant activity, respective the EPS concentration that caused 50% scavenging of DPPH and ABTS free radicals values (IC50) were 4.65 and 7.92 mg/mL. In summary, these findings should be helpful for establishing a suitable industrial fermentation system for C. militaris and can be studied in the food and medical industries in future work. © 2024 The Authors

关键词： Mycelium

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Ultrafast Formation of Charge Transfer Trions at Molecular-Functionalized 2D MoS2Interfaces

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Angewandte Chemie 2024年第30期136卷

作者： Yuancheng Jing Kangkai Liang Nicole S. Muir Hao Zhou Zhehao Li Joseph M. Palasz Jonathan Sorbie Chenglai Wang Scott K Cushing Clifford P. Kubiak Zdeněk Sofer Shaowei Li Wei Xiong Department of Chemistry and Biochemistry University of California San Diego 9500 Gilman Drive MC 0358 La Jolla California 92093-0358 United States Material Science and Engineering Program University of California San Diego 9500 Gilman Drive MC 0418 La Jolla California 92093-0418 United States Division of Chemistry and Chemical Engineering California Institute of Technology 1200 E California Blvd MC 127–72 Pasadena California 91125 United States Department of Inorganic Chemistry University of Chemistry and Technology Prague Technická 5 166 28 Prague 6 Czech Republic

In this work, we investigate trion dynamics occurring at the heterojunction between organometallic molecules and a monolayer transition metal dichalcogenide (TMD) with transient electronic sum frequency generation (tr-ESFG) spectroscopy. By pumping at 2.4 eV with laser pulses, we have observed an ultrafast hole transfer, succeeded by the emergence of charge-transfer trions. This observation is facilitated by the cancellation of ground state bleach and stimulated emission signals due to their opposite phases, making tr-ESFG especially sensitive to the trion formation dynamics. The presence of charge-transfer trion at molecular functionalized TMD monolayers suggests the potential for engineering the local electronic structures and dynamics of specific locations on TMDs and offers a potential for transferring unique electronic attributes of TMD to the molecular layers.

关键词： charge transfer trion Time-resolved interfacial-sensitive spectroscopy sum frequency generation molecular- functionalized monolayer TMD

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Mixed-linker strategy for suppressing structural flexibility of metal-organic framework membranes for gas separation

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Communications Chemistry 2023年第1期6卷 1-12页

作者： Chung-Kai Chang Yen-Chun Lin Yi-Pei Li Dun-Yen Kang Ting-Rong Ko Tsai-Yu Lin Heng-Liang Wu Hyun Jung Yu Jong Suk Lee Department of Chemical Engineering National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei 10617 Taiwan International Graduate Program of Molecular Science and Technology National Taiwan University (NTU-MST) No. 1 Sec. 4 Roosevelt Road Taipei 10617 Taiwan Center of Atomic Initiative for New Materials National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei 10617 Taiwan Center for Condensed Matter Sciences National Taiwan University No. 1 Sec. 4 Roosevelt Road Taipei 10617 Taiwan Department of Chemical and Biomolecular Engineering Sogang University Baekbeom-ro 35 Mapo-gu Seoul 04107 Republic of Korea

Structural flexibility is a critical issue that limits the application of metal-organic framework (MOF) membranes for gas separation. Herein we propose a mixed-linker approach to suppress the structural flexibility of the CAU-10-based (CAU = Christian-Albrechts-University) membranes. Specifically, pure CAU-10-PDC membranes display high separation performance but at the same time are highly unstable for the separation of CO2/CH4. A partial substitution (30 mol.%) of the linker PDC with BDC significantly improves its stability. Such an approach also allows for decreasing the aperture size of MOFs. The optimized CAU-10-PDC-H (70/30) membrane possesses a high separation performance for CO2/CH4(separation factor of 74.2 and CO2permeability of 1,111.1 Barrer under 2 bar of feed pressure at 35°C). A combination of in situ characterization with X-ray diffraction (XRD) and diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy, as well as periodic density functional theory (DFT) calculations, unveils the origin of the mixed-linker approach to enhancing the structural stability of the mixed-linker CAU-10-based membranes during the gas permeation tests.

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