bluuebunny/crossref_metadata_2025_split huggingface dataset:
Visualization of Collagen–Mineral Arrangement Using Atom Probe Tomography
Authors: Lee Bryan E. J. , Langelier Brian , Grandfield Kathryn 
Published: July 2021

AbstractBone is a functional material comprised of mainly two phases: an organic collagenous phase and an inorganic mineral phase. Collagen–mineral arrangement has implications for bone function, aging, and disease. However, theories on collagen‐mineral arrangement have been confined to studies with low spatial and/or compositional resolution resulting in an extensive debate over the location of mineral with respect to collagen. Herein, a strategy is developed to extract a single mineralized collagen fibril from bone and analyze its composition and structure atom‐by‐atom with 3D sub‐nanometer accuracy and compositional clarity using atom probe tomography (APT). It is shown for the first time a method to probe fibril‐level mineralization and collagen–mineral arrangement from an in vivo system with both the spatial and compositional precision required to comment on nanoscale collagen–mineral arrangement. APT of leporine bone shows distinct and helical collagen fibrils with mineralized deposits both encapsulating and incorporated into the collagenous structures. This study demonstrates a novel fibril‐level detection method that can be used to probe the composition of bone and contribute new insights to the structure and organization of mineralized materials such as bones and teeth.
High‐Yield Production, Characterization, and Functionalization of Recombinant Magnetosomes in the Synthetic Bacterium Rhodospirillum rubrum “magneticum”
Authors: Mickoleit Frank , Rosenfeldt Sabine , Toro‐Nahuelpan Mauricio , Schaffer Miroslava , Schenk Anna S. , Plitzko Jürgen M. , Schüler Dirk 
Published: July 2021

AbstractRecently, the photosynthetic Rhodospirillum rubrum has been endowed with the ability of magnetosome biosynthesis by transfer and expression of biosynthetic gene clusters from the magnetotactic bacterium Magnetospirillum gryphiswaldense. However, the growth conditions for efficient magnetite biomineralization in the synthetic R. rubrum “magneticum”, as well as the particles themselves (i.e., structure and composition), have so far not been fully characterized. In this study, different cultivation strategies, particularly the influence of temperature and light intensity, are systematically investigated to achieve optimal magnetosome biosynthesis. Reduced temperatures ≤16 °C and gradual increase in light intensities favor magnetite biomineralization at high rates, suggesting that magnetosome formation might utilize cellular processes, cofactors, and/or pathways that are linked to photosynthetic growth. Magnetosome yields of up to 13.6 mg magnetite per liter cell culture are obtained upon photoheterotrophic large‐scale cultivation. Furthermore, it is shown that even more complex, i.e., oligomeric, catalytically active functional moieties like enzyme proteins can be efficiently expressed on the magnetosome surface, thereby enabling the in vivo functionalization by genetic engineering. In summary, it is demonstrated that the synthetic R. rubrum “magneticum” is a suitable host for high‐yield magnetosome biosynthesis and the sustainable production of genetically engineered, bioconjugated magnetosomes.
From main axes control to flexible body control of large telescope structures
Authors: Kärcher Hans J. 
Published: July 2021

AbstractAstronomers have to point their telescopes with extreme high precision to their targets on the sky. The early craftsmen, which built their telescope mounts, were masters in mechanics and developed sophisticated axis mechanisms based on clockwork motors for the hour angle. The situation changed with the growth of the size of the optical telescopes, the upcoming of large radio telescopes, the related transition to elevation over azimuth mounts and the introduction of electrical main axes drives. The new telescopes were equipped with gears of high transmission ratios, and the dynamics of the motor control was limited by mechanical resonances between the rotors of the motors and the mass of the telescope structure. Early layout tools for the controllers were lumped mass models for the telescope structure including gear stiffnesses and inertias of rotors and brakes, with the free rotor and locked rotor frequencies as critical characteristics influencing the servo loop performance. Nowadays, static and dynamic analysis is performed with the help of finite element models, and the axes controllers are optimized with end‐to‐end models. The emergence of large radio telescopes initiated the development of additional compensation methods for environmental influences as temperature and wind on the shape of the reflectors and their pointing to the sky. Additional active elements on the telescope as surface actuators and subreflector positioners, and additional state sensors on the structure allow the identification and compensation of structural deformations. The method is called flexible body control (FBC). The increasing size of the optical telescopes initiated the development of new mirror technologies as thin meniscus or segmented mirrors in sizes not feasible with the passive supported thick meniscus mirrors. These mirrors need active elements as shape actuators, segment positioners, and wavefront and edge sensors. The method is called active optics (AcO). Astronomical observations in the visible are disturbed by atmospheric blur, and the operability is depending of the active compensation of that blur, based on a fast wavefront sensor analyzing an artificial star and an additional fast wavefront corrector. The method is called adaptive optics (AdO). The following text gives an overview on the historic development of telescope control systems from the viewpoint of the telescope mount and its axes control systems, finally culminating in FBC applications. Actual examples are the large millimeter telescope LMT/GTM in Mexico, the advanced technology solar telescope DKIST in Hawaii, and the airborne telescope of SOFIA, the Stratospheric Observatory for Infrared Astronomy with its base in Palmdale, California.
Stable Light‐Emitting Electrochemical Cells Using Hyperbranched Polymer Electrolyte
Authors: Mardegan Lorenzo , Dreessen Chris , Sessolo Michele , Tordera Daniel , Bolink Henk J. 
Published: July 2021

AbstractThe choice of an adequate electrolyte is a fundamental aspect in polymer light‐emitting electrochemical cells (PLECs) as it provides the in situ electrochemical doping and influences the performance of these devices. In this study, a hyperbranched polymer (Hybrane DEO750 8500) blended with a Li salt is used as a novel electrolyte in state‐of‐the‐art Super Yellow (a polyphenylenevinylene) based LECs. Due to the desirable properties of the hyperbranched polymer and the homogeneous and smooth films that it forms with the emitting polymer, PLEC with excellent electroluminescent properties are obtained using a pulsed current bias scheme. The devices are very stable, with lifetimes in excess of 2000 h with initial luminance values above 450 cd m−2, a peak efficiency of 12.6 lm W−1, and sub‐minute turn‐on times. The stability of the devices is also studied by measuring the photoluminescence (PL) of the semiconductor during electroluminescent operation. The findings suggest that it is possible to observe the quenching of the PL in vertically stacked devices due to the advancement of the doped fronts in the film and an immediate PL recovery when the bias is removed.
Viral Transduction Enhancing Effect of EF‐C Peptide Nanofibrils Is Mediated by Cellular Protrusions
Authors: Schütz Desiree , Rode Sascha , Read Clarissa , Müller Janis A. , Glocker Bernhard , Sparrer Konstantin M. J. , Fackler Oliver T. , Walther Paul , Münch Jan 
Published: July 2021

AbstractSelf‐assembling peptide nanofibrils (PNF) have gained increasing attention as versatile molecules in material science and biomedicine. One important application of PNF is to enhance retroviral gene transfer, a technology that has been central for gene therapy approaches. The best‐investigated and commercially available PNF is derived from a 12‐mer peptide termed EF‐C. The mechanism of transduction enhancement depends on the polycationic surface of EF‐C PNF, which bind to the negatively charged membranes of viruses and cells, thereby overcoming electrostatic repulsions and increasing virion attachment and fusion. To better understand how EF‐C PNF interact with the cell surface, scanning electron and time‐lapse confocal microscopy were performed. The fibrils are found to be actively engaged by cellular protrusions such as filopodia. Consequently, chemical suppression of protrusion formation abrogates fibril binding and virion delivery to the cell surface of immortalized and primary T cells. Vice versa, induction of plasma membrane blebs result in increased fibril binding. Thus, the mechanism of PNF‐mediated viral transduction enhancement involves an active engagement of virus‐loaded fibrils by cellular protrusions, which may explain its superior performance over soluble transduction enhancers.
Localized Chemotherapy Based on Injectable Hydrogel Boosts the Antitumor Activity of Adoptively Transferred T Lymphocytes In Vivo
Authors: Cao Yue , Zhou Yuhao , Chen Zhixiong , Zhang Zhen , Chen Xuesi , He Chaoliang 
Published: July 2021

AbstractThe adoptive transfer of antigen‐specific T cells has been successfully applied in the treatment of hematological malignancies. However, its application in the treatment of solid tumors has been overshadowed by the immunosuppressive tumor microenvironment. In this context, a preprocessing strategy is developed to reprogram the immunosuppressive tumor microenvironment using a thermoresponsive hydrogel loaded with doxorubicin (DOX@Gel). Compared with hydrogel‐based chemotherapy alone or adoptive T cell therapy alone, this combination exhibits enhanced anti‐tumor efficacy. In addition to the direct killing of tumor cells, the local chemotherapy releases tumor‐associated antigens which enhance the proliferation and effector function of endogenous and adoptively transferred T cells. Moreover, DOX@Gel significantly reduces the numbers of both myeloid derived suppressor cells and Tregs in tumor microenvironment. It is suggested that DOX@Gel promotes the efficacy of adoptively transferred T cells against solid tumors, overcoming the key limitations of adoptive T cell therapy.
Triarylamine‐Pyridine‐Carbonitriles for Organic Light‐Emitting Devices with EQE Nearly 40%
Authors: Chen Yi‐Kuan , Jayakumar Jayachandran , Hsieh Chia‐Min , Wu Tien‐Lin , Liao Chun‐Cheng , Pandidurai Jayabalan , Ko Chang‐Lun , Hung Wen‐Yi , Cheng Chien‐Hong 
Published: July 2021

AbstractHighly efficient thermally activated delayed fluorescence (TADF) molecules are in urgent demand for solid‐state lighting and full‐color displays. Here, the design and synthesis of three triarylamine‐pyridine‐carbonitrile‐based TADF compounds, TPAPPC, TPAmPPC, and tTPAmPPC, are shown. They exhibit excellent photoluminescence quantum yields of 79−100% with small ΔEST values, fast reverse intersystem crossing (RISC), and high horizontal dipole ratios (Θ// = 86−88%) in the thin films leading to the enhancement of device light outcoupling. Consequently, a green organic light‐emitting diode (OLED) based on TPAmPPC shows a high average external quantum efficiency of 38.8 ± 0.6%, a current efficiency of 130.1 ± 2.1 cd A–1, and a power efficiency of 136.3 ± 2.2 lm W–1. The highest device efficiency of 39.8% appears to be record‐breaking among TADF‐based OLEDs to date. In addition, the TPAmPPC‐based device shows superior operation lifetime and high‐temperature resistance. It is worth noting that the TPA‐PPC‐based materials have excellent optical properties and the potential for making them strong candidates for TADF practical application.
A Robust Narrow Bandgap Vanadium Tetrasulfide Sonosensitizer Optimized by Charge Separation Engineering for Enhanced Sonodynamic Cancer Therapy
Authors: Liang Shuang , Liu Bin , Xiao Xiao , Yuan Meng , Yang Ling , Ma Ping'an , Cheng Ziyong , Lin Jun 
Published: July 2021

AbstractThe development and optimization of sonosensitizers for elevating intratumoral reactive oxygen species (ROS) are definitely appealing in current sonodynamic therapy (SDT). Given this, branched vanadium tetrasulfide (VS4) nanodendrites with a narrower bandgap (compared with the most extensively explored sonosensitizers) are presented as a new source of sonosensitizer, which allows a more effortless separation of sono‐triggered electron–hole pairs for ROS generation. Specifically, platinum (Pt) nanoparticles and endogenous high levels of glutathione (GSH) are rationally engineered to further optimize its sono‐sensitized performance. As cocatalyst, Pt is conducive to trapping electrons, whereas GSH, as a natural hole‐scavenger, tends to capture holes. Compared with the pristine VS4 sonosensitizer, the GSH‐Pt‐VS4 nanocomposite can greatly prolong the lifetime of the charge and confer a highly efficacious ROS production activity. Furthermore, such nanoplatforms are capable of reshaping tumor microenvironments to realize ROS overproduction, contributed by overcoming tumor hypoxia to improve SDT‐triggered singlet oxygen production, catalyzing endogenic hydrogen peroxide into destructive hydroxyl radicals for chemodynamic therapy, and depleting GSH to amplify intratumoral oxidative stress. All these combined effects result in a significantly efficient tumor suppression outcome. This study enriches sonosensitizer research and proves that sonosensitizers can be rationally optimized by charge separation engineering strategy.
Emerging Dual‐Atomic‐Site Catalysts for Efficient Energy Catalysis
Authors: Zhang Weiyu , Chao Yuguang , Zhang Wenshu , Zhou Jinhui , Lv Fan , Wang Kai , Lin Fangxu , Luo Heng , Li Jing , Tong Meiping , Wang Erkang , Guo Shaojun 
Published: July 2021

AbstractAtomically dispersed metal catalysts with well‐defined structures have been the research hotspot in heterogeneous catalysis because of their high atomic utilization efficiency, outstanding activity, and selectivity. Dual‐atomic‐site catalysts (DASCs), as an extension of single‐atom catalysts (SACs), have recently drawn surging attention. The DASCs possess higher metal loading, more sophisticated and flexible active sites, offering more chance for achieving better catalytic performance, compared with SACs. In this review, recent advances on how to design new DASCs for enhancing energy catalysis will be highlighted. It will start with the classification of marriage of two kinds of single‐atom active sites, homonuclear DASCs and heteronuclear DASCs according to the configuration of active sites. Then, the state‐of‐the‐art characterization techniques for DASCs will be discussed. Different synthetic methods and catalytic applications of the DASCs in various reactions, including oxygen reduction reaction, carbon dioxide reduction reaction, carbon monoxide oxidation reaction, and others will be followed. Finally, the major challenges and perspectives of DASCs will be provided.
First‐Principles Multiscale Modeling of Mechanical Properties in Graphene/Borophene Heterostructures Empowered by Machine‐Learning Interatomic Potentials
Authors: Mortazavi Bohayra , Silani Mohammad , Podryabinkin Evgeny V. , Rabczuk Timon , Zhuang Xiaoying , Shapeev Alexander V. 
Published: July 2021

AbstractDensity functional theory calculations are robust tools to explore the mechanical properties of pristine structures at their ground state but become exceedingly expensive for large systems at finite temperatures. Classical molecular dynamics (CMD) simulations offer the possibility to study larger systems at elevated temperatures, but they require accurate interatomic potentials. Herein the authors propose the concept of first‐principles multiscale modeling of mechanical properties, where ab initio level of accuracy is hierarchically bridged to explore the mechanical/failure response of macroscopic systems. It is demonstrated that machine‐learning interatomic potentials (MLIPs) fitted to ab initio datasets play a pivotal role in achieving this goal. To practically illustrate this novel possibility, the mechanical/failure response of graphene/borophene coplanar heterostructures is examined. It is shown that MLIPs conveniently outperform popular CMD models for graphene and borophene and they can evaluate the mechanical properties of pristine and heterostructure phases at room temperature. Based on the information provided by the MLIP‐based CMD, continuum models of heterostructures using the finite element method can be constructed. The study highlights that MLIPs were the missing block for conducting first‐principles multiscale modeling, and their employment empowers a straightforward route to bridge ab initio level accuracy and flexibility to explore the mechanical/failure response of nanostructures at continuum scale.
Preparation of Ultrablack Composite Sheets with Excellent Mechanical and Chemical Stability from Sandpaper‐Based Template‐Imprinting
Authors: Chen Hai Tao , Li Chao Qun , Zhan Hang , Mo Run Wei , Zhang Yu , Wang Jian Nong 
Published: July 2021

AbstractUltrablack materials have applications in wide areas such as visible stealth, solar cells, and sea water evaporation. However, their high production cost, low mechanical property, and poor chemical stability have restricted their wide applications. Herein, a low‐cost method is reported for preparing large‐area ultrablack composite sheets with excellent mechanical and chemical stability. This is achieved by mixing a light absorber and transparent resin, and then copying and molding microconvex structures of sandpaper. The result shows that the absorption rate of the prepared composite sheet can reach more than 99% in the visible light range. More importantly, its performance remains almost unchanged after many cycles of mechanical stretching and long‐term chemical soaking. This excellent ultrablack performance is mainly attributed to the light‐trap effect of the subwavelength convex structure with the light absorber embedded in the resilient resin. Such composite sheets open a new pathway to developing high‐performance ultrablack materials with practical applications.
1,3‐Difunctionalization of Imino‐Carbenes via Rhodium‐Catalyzed Reactions of Triazoles with Acyl Selenides
Authors: Li Fang , Pei Chao , Quaranta Calogero , Koenigs Rene M. 
Published: July 2021

AbstractHerein, we report on the rhodium‐catalyzed reaction of triazoles with acyl selenides. Under thermal reaction conditions and in the presence of a rhodium catalyst, a rapid 1,3‐difunctionalization reaction occurs to provide valuable α‐seleno enamides with high stereoselectivity and broad functional group tolerance, which was demonstrated in 35 examples with up to 95% yield. Computational calculations suggest a reaction pathway that gives a direct access to the 1,3‐difunctionalization without intermittent formation of ylide intermediates.magnified image
MRI‐Active Metal‐Organic Frameworks: Concepts for the Translation from Lab to Clinic
Authors: Peller Michael , Lanza Arianna , Wuttke Stefan 
Published: July 2021

AbstractMetal‐organic frameworks (MOFs) are an emerging class of synthetic materials obtained by combining organic and inorganic chemistry. MOFs show peculiar properties such as well‐defined crystalline structures, systematic structural variation, high porosity and the possibility to chemically functionalize the pores. These properties are especially promising for designing MOF nanoparticles (NPs) with special functions. The desired functions can be introduced and modified with a chemical approach, by the choice of the inorganic and organic building blocks. All these features and the highest surface area of any porous material make MOF NPs ideal for the use as nanocarrier in biomedicine. So far, a wide variety of biomedical applications of MOF NPs have been already envisioned being supported by promising first in vitro and in vivo results. The ongoing development of MOF NPs is at the edge of basic science to biomedical applications. A major focus of biomedical research is already in cancer therapy using MOF NPs as theranostic nanocarrier. In this article, NP designs and MRI‐labelling concepts are pointed out and discussed in the perspective of facilitating their translation to clinical use. Clinical application is envisioned with a major focus on theranostic MOF NPs and MRI as the most promising imaging method.
TLR7/8 Agonist and SHP2 Inhibitor Loaded Nanoparticle Enhances Macrophage Immunotherapy Efficacy
Authors: Malik Vaishali , Ramesh Anujan , Kulkarni Ashish A. 
Published: July 2021

AbstractTumor‐associated macrophages (TAMs) are among the most abundant immune cells in the solid tumor microenvironment, making them an attractive target for cancer immunotherapy. However, there are two important challenges. First, tumors repolarize the TAMs predominantly to M2 tumor‐aiding phenotype by secreting various immunosuppressive cytokines. Second, CD47 on cancer cells interacts with signal‐regulating protein a (SIRPa) expressed on macrophages. This crosstalk provides a downregulatory signal in the form of activation of SHP1/2 that inhibits cancer cell phagocytosis. These challenges can be overcome by engineering a nanoparticle that can deliver a rationale combination of immunomodulatory agents to the TAMs that can repolarize the M2 macrophages to M1 phenotype efficiently and concurrently block CD47‐SIRPa interactions by inhibiting SHP2 signaling. A lipid nanoparticle (LNP) system loaded with amphiphilic R848‐cholesterol (TLR7/8 agonist) and SHP099 (SHP2 inhibitor) in a predefined ratio has been designed. In vitro studies show that the LNPs system repolarized to M2 macrophages to M1 phenotype and expressed co‐stimulatory molecules while enhancing phagocytic potential. In vivo efficacy studies in 4T1 tumor‐bearing mice show that LNPs exhibit superior anti‐tumor efficacy than other treatments. Thus, the lipid nanoparticle‐mediated co‐delivery of a rational combination of TLR7/8 agonist and SHP2 inhibitor in the TAMs can enhance macrophage immunotherapy.
Harnessing CURATE.AI for N‐of‐1 Optimization Analysis of Combination Therapy in Hypertension Patients: A Retrospective Case Series
Authors: Truong Anh T. L. , Tan Lester W. J. , Chew Kimberly A. , Villaraza Steven , Siongco Paula , Blasiak Agata , Chen Christopher , Ho Dean 
Published: July 2021

AbstractHypertension is a global public health challenge that imposes a significant burden on patients and healthcare systems. Conventional treatment involves dose escalation of an antihypertensive drug, and if the desired response is not achieved, patients are prescribed another drug, often in combination with other therapies. Importantly, drug synergy is dose‐, time‐ and patient‐dependent. Coupled with the challenges of intra‐ and inter‐individual variability, standard care can lead to sub‐optimal outcomes, additional visits, and adherence issues. Furthermore, these factors can cause the additional complication of patients being misperceived as refractory to regimens that are sub‐optimally administered. A scalable strategy that can longitudinally optimize patient response would be a powerful advance for chronic disease management. This four‐patient case series reports the application of CURATE.AI as a mechanism‐independent and disease‐agnostic platform for a retrospective N‐of‐1 (personalized) dose optimization using each patient's own data, including drug doses and corresponding changes in blood pressures. This approach may enable the rapid prediction of treatment response and the identification of optimal doses that may yield improved outcomes. CURATE.AI can be implemented in clinical workflows without creating additional burden of extensive data collection. The findings from this study support the prospective validation of CURATE.AI to optimize hypertension management.