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arXiv 2021年

作者： Roig, Marta Bofill Krotka, Pavla Burman, Carl-Fredrik Glimm, Ekkehard Gold, Stefan M. Hees, Katharina Jacko, Peter Koenig, Franz Magirr, Dominic Mesenbrink, Peter Viele, Kert Posch, Martin Center for Medical Statistics Informatics and Intelligent Systems Medical University of Vienna Vienna Austria Statistical Innovation Data Science & Artiffcial Intelligence AstraZeneca Gothenburg Sweden Advanced Methodology and Data Science Novartis Pharma AG Basel Switzerland Institute of Biometry and Medical Informatics University of Magdeburg Magdeburg Germany Klinik für Psychiatrie und Psychotherapie Charité - Universitätsmedizin Berlin Campus Benjamin Franklin Berlin Germany Medizinische Klinik m.S. Psychosomatik Charité - Universitätsmedizin Berlin Campus Benjamin Franklin Berlin Germany Zentrum für Molekulare Neurobiologie Universitätsklinikum Hamburg Eppendorf Hamburg Germany Section of Biostatistics Paul-Ehrlich-Institut Langen Germany Lancaster University Lancaster United Kingdom Analytics Global Drug Development Novartis Pharmaceuticals Corporation One Health Plaza East HanoverNJ United States

Background Platform trials can evaluate the efficacy of several experimental treatments compared to a control. The number of experimental treatments is not fixed, as arms may be added or removed as the trial progresses. Platform trials are more efficient than independent parallel group trials because of using shared control groups. However, for a treatment entering the trial at a later time point, the control group is divided into concurrent controls, consisting of patients randomised to control when that treatment arm is in the platform, and non-concurrent controls, patients randomised before. Using non-concurrent controls in addition to concurrent controls can improve the trial's efficiency by increasing power and reducing the required sample size, but can introduce bias due to time trends. Methods We focus on a platform trial with two treatment arms and a common control arm. Assuming that the second treatment arm is added at a later time, we assess the robustness of recently proposed model-based approaches to adjust for time trends when utilizing non-concurrent controls. In particular, we consider approaches where time trends are modeled either as linear in time or as a step function, with steps at time points where treatments enter or leave the platform trial. For trials with continuous or binary outcomes, we investigate the type 1 error rate and power of testing the efficacy of the newly added arm, as well as the bias and root mean squared error of treatment effect estimates under a range of scenarios. In addition to scenarios where time trends are equal across arms, we investigate settings with different time trends or time trends that are not additive in the scale of the model. Results A step function model, fitted on data from all treatment arms, gives increased power while controlling the type 1 error, as long as the time trends are equal for the different arms and additive on the model scale. This holds even if the shape of the time trend deviates from a s

关键词： Additives

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Moisture-Accelerated Precursor Crystallisation in Ambient Air for High-Performance Perovskite Solar Cells toward Mass Production

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Angewandte Chemie 2022年第42期134卷

作者： Weili Fan Dr. Kaimo Deng Ying Shen Prof. Yang Bai Prof. Liang Li Beijing Advanced Innovation Center for Materials Genome Engineering Institute for Advanced Materials and Technology University of Science and Technology Beijing 100083 P. R. China Contribution: Formal analysis (equal) Investigation (equal) Methodology (equal) Software (lead) Writing - original draft (equal) School of Physical Science and Technology Jiangsu Key Laboratory of Thin Films Soochow University Suzhou 215006 P. R. China Contribution: Data curation (equal) Funding acquisition (equal) Methodology (equal) Project administration (equal) Contribution: Methodology (equal) Software (equal) Contribution: Funding acquisition (equal) Methodology (equal) Project administration (equal) Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead)

Phase-pure crystallised perovskite is considered an excellent precursor for fabricating high-stability perovskite films with minimal defects. However, currently available protocols for synthesising crystallised perovskites must be conducted in an inert atmosphere or in the presence of an organic solvent as the reaction medium, which hinders mass production. Here, we report the fast synthesis of α-phase-crystallised perovskite powder assisted by moisture in ambient air. Moisture can promote the reaction between PbI 2 and organic salts and facilitate complete phase transition, as demonstrated in a joint experimental and theoretical study. Perovskite solar cells with a power conversion efficiency of 24.07 % were achieved using phase-pure crystallised perovskite powder as the precursor. This ambient-air-compatible method opens new vistas to reproducible high-quality precursors for large-scale photovoltaic applications.

关键词： Moisture Perovskite Solar Cells Precursor Crystallization Stability

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A Versatile Strategy for Screening Custom-Designed Warhead-Armed Cyclic Peptide Inhibitors

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Angewandte Chemie 2022年第7期135卷

作者： Deokhee Kang Do-Wook Kim Joo-Chan Kim Prof. Hee-Sung Park Department of Chemistry Korea Advanced Institute of Science and Technology 291 Daehak-ro Yuseong-gu Daejeon 34141 Korea Contribution: Conceptualization (equal) Data curation (equal) Methodology (equal) Validation (equal) Writing - original draft (equal) Contribution: Conceptualization (equal) Data curation (equal) Methodology (equal) Validation (equal) Writing - original draft (supporting) Contribution: Formal analysis (supporting) Methodology (supporting) Visualization (supporting) Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead)

Demand for peptide-based pharmaceuticals has been steadily increasing, but only limited success has been achieved to date. To expedite peptide-based drug discovery, we developed a general scheme for cell-based screening of cyclic peptide inhibitors armed with a user-designed warhead. We combined unnatural amino acid incorporation and split intein-mediated peptide cyclization techniques and integrated a yeast-based colorimetric screening assay to generate a new scheme that we call the custom-designed warhead-armed cyclic peptide screening platform (CWCPS). This strategy successfully discovered a potent inhibitor, CY5-6Q, that targets human histone deacetylase 8 (HDAC8) with a K D value of 15 nM. This approach can be a versatile and general platform for discovering cyclic peptide inhibitors.

关键词： Cyclic Peptide Inhibitor Genetic Code Expansion Warhead-Bearing Unnatural Amino Acid

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High-Performance Thermoelectric α-Ag9Ga1−xTe6Compounds with Ultralow Lattice Thermal Conductivity Originating from Ag9Te2Motifs

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Angewandte Chemie 2022年第36期134卷

作者： Yingfei Tang Yimeng Yu Na Zhao Keke Liu Haijie Chen Constantinos C. Stoumpos Yixuan Shi Shuo Chen Lingxiao Yu Jinsong Wu Qingjie Zhang Xianli Su Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (equal) Visualization (equal) Writing - original draft (lead) Nanostructure Research Center Wuhan University of Technology Wuhan 430070 China Contribution: Data curation (equal) Software (equal) Visualization (supporting) Contribution: Investigation (equal) Methodology (equal) Contribution: Investigation (equal) Methodology (equal) Visualization (equal) State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China Contribution: Methodology (equal) Visualization (equal) Writing - review & editing (equal) Department of Materials Science and Technology Voutes Campus University of Crete Iraklio Heraklion 70013 Greece Contribution: Methodology (equal) Visualization (equal) Contribution: Investigation (equal) Visualization (equal) Contribution: Conceptualization (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Methodology (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Methodology (equal) Supervision (equal) Writing - review & editing (equal)

We have determined the complex atomic structure of high-temperature α-Ag 9 GaTe 6 phase with a hexagonal lattice ( P 6 3 mc space group, a = b =8.2766 Å, c =13.4349 Å). The structure has outer [GaTe 4 ] 5− tetrahedrons and inner [Ag 9 Te 2 ] 5+ clusters. All of the Ag ions are disorderly distributed in the lattice. Seven types of the Ag atoms constitute the cage-like [Ag 9 Te 2 ] 5+ clusters. The highly disordered Ag ions vibrate in-harmonically, producing strong coupling between low frequency optical phonons and acoustic phonons. This in conjunction with a low sound velocity of 1354 m s −1 leads to an ultralow thermal conductivity of 0.20 W m −1 K −1 at 673 K. Meanwhile, the deficiency of Ga in Ag 9 Ga 1− x Te 6 compounds effectively optimizes the electronic transport properties. Ag 9 Ga 0.91 Te 6 attains a highest power factor of 0.40 mW m −1 K −2 at 673 K. All these contribute to a much-improved ZT value of 1.13 at 623 K for Ag 9 Ga 0.95 Te 6 , which is 41 % higher than that of the pristine Ag 9 GaTe 6 sample.

关键词： α-Ag9GaTe6 Crystal Structure Ga Deficiency Thermoelectrics Ultralow Lattice Thermal Conductivity

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Safe approaching control for spacecraft rendezvous with disturbances: A positive system approach

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Asian Journal of Control 2021年第5期24卷

作者： Yuhan Xu Chenliang Wang Jianzhong Qiao Lei Guo School of Automation Science and Electrical Engineering Beihang University Beijing 100191 China Contribution: Methodology Beijing Advanced Innovation Center for Big Data-Based Precision Medicine Beihang University Beijing 100191 China Contribution: Supervision Contribution: Funding acquisition Investigation Contribution: Conceptualization Project administration Supervision

This paper concerns about the safe approaching in rendezvous with spherical envelops of spacecraft. Based on the nonnegative characteristic of positive systems, a novel strategy of controlling the relative distance positive and convergent is proposed to guarantee no-collision approaching. The dynamics of the relative distance is decoupled from that of the relative angles. A nonlinear disturbance observer is designed, and two anti-disturbance controllers are constructed to reject the effect of disturbances for the subsystems of relative distance and angles. Under the controllers, the closed-loop subsystem of relative distance is a positive and stable system, while that of relative angles is a general stable system satisfying the given time-varying constraints. Particularly, a theorem is proposed to present the conditions of controllers to ensure the system positivity under a class of external inputs without nonnegativity default. Finally, simulation results are presented to illustrate the effectiveness of proposed methods.

关键词： barrier Lyapunov functions nonlinear disturbance observers positive systems safe approaching spacecraft

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Intrinsically Stretchable Electroluminescent Elastomers with Self-Confinement Effect for Highly Efficient Non-Blended Stretchable OLEDs

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Angewandte Chemie 2022年第2期135卷

作者： Xiang-Chun Li Lanqian Yao Wan Song Fang Liu Qian Wang Jin Chen Qian Xue Wen-Yong Lai State Key Laboratory of Organic Electronics and Information Displays (SKLOEID) Institute of Advanced Materials (IAM) Nanjing University of Posts & Telecommunications 9 Wenyuan Road Nanjing 210023 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (equal) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Frontiers Science Center for Flexible Electronics (FSCFE) MIIT Key Laboratory of Flexible Electronics (KLoFE) Northwestern Polytechnical University Xi'an 710072 China Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Resources (lead) Writing - original draft (equal) Writing - review & editing (lead)

Ultra-flexible stretchable organic light-emitting diodes (OLEDs) are emerging as a basic component of flexible electronics and human-machine interfaces. However, the brightness and efficiency of stretchable OLEDs remain still far inferior to their rigid counterparts, owing to the scarcity of satisfactory stretchable electroluminescent materials. Herein, we explore a general concept based on the self-confinement effect to dramatically improve the stretchability of elastomers, without affecting electroluminescent properties. The balanced rigid/flexible chain dynamics under self-confinement significantly reduces the modulus of the elastomers, resulting in the maximum strain reaching 806 %. Ultra-flexible stretchable OLEDs have been constructed based on the resulting ISEEs, achieving unprecedented high-performance non-blended stretchable OLEDs. The results suggest an effective molecular design strategy for highly deformable stretchable displays and flexible electronics.

关键词： Electroluminescent Elastomers Flexible Electronics Organic Emitters Organic Light-Emitting Diodes (OLEDs) Stretchable Electronics

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Rapid Charge Transfer Endowed by Interfacial Ni-O Bonding in S-scheme Heterojunction for Efficient Photocatalytic H2and Imine Production

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Bowen He Dr. Peng Xiao Dr. Sijie Wan Dr. Jianjun Zhang Prof. Tao Chen Prof. Liuyang Zhang Prof. Jiaguo Yu Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street Wuhan 430078 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Methodology (lead) Writing - original draft (equal) Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China Hefei Anhui 230026 China Contribution: Data curation (equal) Formal analysis (equal) State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Contribution: Formal analysis (supporting) Methodology (supporting) Software (lead) Contribution: Methodology (supporting) Validation (supporting) Contribution: Methodology (supporting) Resources (supporting) Contribution: Formal analysis (equal) Funding acquisition (equal) Supervision (supporting) Writing - review & editing (lead)

Cooperative coupling of H 2 evolution with oxidative organic synthesis is promising in avoiding the use of sacrificial agents and producing hydrogen energy with value-added chemicals simultaneously. Nonetheless, the photocatalytic activity is obstructed by sluggish electron-hole separation and limited redox potentials. Herein, Ni-doped Zn 0.2 Cd 0.8 S quantum dots are chosen after screening by DFT simulation to couple with TiO 2 microspheres, forming a step-scheme heterojunction. The Ni-doped configuration tunes the highly active S site for augmented H 2 evolution, and the interfacial Ni−O bonds provide fast channels at the atomic level to lower the energy barrier for charge transfer. Also, DFT calculations reveal an enhanced built-in electric field in the heterojunction for superior charge migration and separation. Kinetic analysis by femtosecond transient absorption spectra demonstrates that expedited charge migration with electrons first transfer to Ni 2+ and then to S sites. Therefore, the designed catalyst delivers drastically elevated H 2 yield (4.55 mmol g −1 h −1 ) and N-benzylidenebenzylamine production rate (3.35 mmol g −1 h −1 ). This work provides atomic-scale insights into the coordinated modulation of active sites and built-in electric fields in step-scheme heterojunction for ameliorative photocatalytic performance.

关键词： Benzylamine Coupling Oxidation Hydrogen Production Interfacial Charge Transfer S-Scheme Photocatalyst

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Efficient adaptive designs for clinical trials of interventions for COVID-19

arXiv

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arXiv 2020年

作者： Stallard, Nigel Hampson, Lisa Benda, Norbert Brannath, Werner Burnett, Tom Friede, Tim Kimani, Peter K. Koenig, Franz Krisam, Johannes Mozgunov, Pavel Posch, Martin Wason, James Wassmer, Gernot Whitehead, John Faye Williamson, S. Zohar, Sarah Jaki, Thomas Statistics and Epidemiology Division of Health Sciences Warwick Medical School University of Warwick United Kingdom Advanced Methodology and Data Science Novartis Pharma AG Basel Switzerland Bonn Germany Institute for Statistics University of Bremen Bremen Germany Department of Mathematics and Statistics Lancaster University United Kingdom Department of Medical Statistics University Medical Center Göttingen Germany Section of Medical Statistics CeMSIIS Medical University of Vienna Austria Institute of Medical Biometry and Informatics University of Heidelberg Germany Population Health Sciences Institute Newcastle University Newcastle upon Tyne United Kingdom MRC Biostatistics Unit University of Cambridge Cambridge United Kingdom RPACT GbR Sereetz Germany INSERM Centre de Recherche des Cordeliers Sorbonne Université Université de Paris France

The COVID-19 pandemic has led to an unprecedented response in terms of clinical research activity. An important part of this research has been focused on randomized controlled clinical trials to evaluate potential therapies for COVID-19. The results from this research need to be obtained as rapidly as possible. This presents a number of challenges associated with considerable uncertainty over the natural history of the disease and the number and characteristics of patients affected, and the emergence of new potential therapies. These challenges make adaptive designs for clinical trials a particularly attractive option. Such designs allow a trial to be modified on the basis of interim analysis data or stopped as soon as sufficiently strong evidence has been observed to answer the research question, without compromising the trial’s scientific validity or integrity. In this paper we describe some of the adaptive design approaches that are available and discuss particular issues and challenges associated with their use in the pandemic setting. Our discussion is illustrated by details of four ongoing COVID-19 trials that have used adaptive designs. Copyright © 2020, The Authors. All rights reserved.

关键词： Clinical research

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Engineering Fluorine-rich Double Protective Layer on Zn Anode for Highly Reversible Aqueous Zinc-ion Batteries

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Angewandte Chemie 2023年第51期135卷

作者： Titi Li Sanlue Hu Chenggang Wang Dun Wang Minwei Xu Caiyun Chang Xijin Xu Cuiping Han School of Physics and Technology University of Jinan Shandong 250022 China Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Resources (lead) Writing - original draft (lead) Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China Contribution: Methodology (lead) Software (lead) Writing - review & editing (equal) Contribution: Supervision (lead) Writing - review & editing (equal) Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Contribution: Resources (lead) Supervision (lead) Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Methodology (lead) Resources (equal) Writing - review & editing (equal) Contribution: Resources (lead) Supervision (lead) Writing - review & editing (lead) Contribution: Methodology (lead) Resources (lead) Supervision (lead) Writing - review & editing (lead)

The high thermodynamic instability and side reactions of Zn-metal anode (ZMA), especially at high current densities, greatly impede the commercialization of aqueous zinc-ion batteries (AZIBs). Herein, a fluorine-rich double protective layer strategy is proposed to obtain the high reversibility of AZIBs through the introduction of a versatile tetradecafluorononane-1,9-diol (TDFND) additive in aqueous electrolyte. TDFND molecule with large adsorption energy (−1.51 eV) preferentially absorbs on the Zn anode surface to form a Zn(OR) 2 − (R=−CH 2 −(CF 2 ) 7 −CH 2 −) cross-linking complex network, which balances space electric field and controls the Zn 2+ ion flux, thus enabling the uniform and compact deposition of Zn (002) crystal planes. Meanwhile, TDFND with low Lowest unoccupied molecular orbital (LUMO, 0.10 eV) energy level is priorly decomposed to regulate the interfacial chemistry of ZMA by building a ZnF 2 -rich solid electrode/electrolyte interface (SEI) layer. It is found that a 14 nm-thick SEI layer delivers excellent structural integrity to suppress parasitic reactions by blocking the direct contact of active water and ZMA. Consequently, the Zn electrode exhibits a superior cycling life over 430 h at 10 mA cm −2 and a high average Coulombic efficiency of 99.8 % at 5 mA cm −2 . Furthermore, a 68 mAh pouch cell delivers 80.3 % capacity retention for 1000 cycles.

关键词： Cross-Linking Network Solid-Electrolyte Interface Zinc Anode Zinc-Ion Battery ZnF2

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A Compartmentalized Nanoreactor Formed by Interfacial Hydrogelation for Cascade Enzyme Catalytic Therapy

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Angewandte Chemie 2023年第15期135卷

作者： Xingyue He Qing Wu Chen Hou Min Hu Qigang Wang Xia Wang School of Chemical Science and Engineering Tongji University Shanghai 200092 China Translational Research Institute of Brain and Brain-Like Intelligence Shanghai Fourth People's Hospital School of Medicine Tongji University Shanghai 200434 China Contribution: Data curation (lead) Formal analysis (lead) Methodology (lead) Writing - original draft (lead) School of Materials Science and Engineering Shanghai University Shanghai 200444 China Contribution: Formal analysis (equal) Investigation (equal) Methodology (equal) Shanghai Synchrotron Radiation Facility (SSRF) from Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Software (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Contribution: Conceptualization (lead) Project administration (lead) Supervision (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Writing - original draft (equal) Writing - review & editing (lead)

Some cellular enzymatic pathways are located within a single organelle, while most others involve enzymes that are located within multiple compartmentalized cellular organelles to realize the efficient multi-step enzymatic process. Herein, bioinspired by enzyme-mediated biosynthesis and biochemical defense, a compartmented nanoreactor (Burr-NCs@Gl SOD ) was constructed through a self-confined catalysis strategy with burr defect-engineered molybdenum disulfide/Prussian blue analogues (MoS 2 /PBA) and an interfacial diffusion-controlled hydrogel network. The specific catalytic mechanism of the laccase-like superactivity induced hydrogelation and cascade enzyme catalytic therapy were explored. The confined hydrogelation strategy introduces a versatile means for nanointerface functionalization and provides insight into biological construction of simulated enzymes with comparable activity and also the specificity to natural enzymes.

关键词： Cascade Catalysis Enzymatic Hydrogelation Interfacial Functionalization Tumor Therapy

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