bluuebunny/crossref_metadata_2025_split huggingface dataset:
Die direkte mechanokatalytische Suzuki–Miyaura‐Kupplung kleiner organischer Moleküle
Authors: Pickhardt Wilm , Beaković Claudio , Mayer Maike , Wohlgemuth Maximilian , Kraus Fabien Joel Leon , Etter Martin , Grätz Sven , Borchardt Lars 
Published: May 2022

AbstractIn dieser Arbeit wird die Suzuki–Miyaura‐Reaktion in Abwesenheit von Lösungsmitteln, Liganden und pulverförmiger Katalysatoren vorgestellt. Unter Verwendung einer einzelnen katalytisch aktiven Mahlkugel können quantitative Ausbeuten nach 30 min des Vermahlens isoliert werden. Weiterhin führten Anpassungen der Mahlparameter dazu, dass der Materialverlust durch Kugelabrieb vermieden wurde. Anhand dieses abriebfreien Systems wird durch Röntgenphotoelektronenspektroskopie, in situ Röntgendiffraktrometrie, sowie durch Referenzexperimente bewiesen, dass die katalytische Reaktion auf der Kugeloberfläche stattfindet. Die Vielseitigkeit dieses neuartigen Katalysekonzepts wird anhand verschiedener Edukte verdeutlicht. Aktivierte, deaktivierte, sowie sterisch‐gehinderte Aryliodide und ‐bromide werden innerhalb kurzer Zeit in guten Ausbeuten gekuppelt.
A Practical and Scalable Approach to Fluoro‐Substituted Bicyclo[1.1.1]pentanes
Authors: Bychek Roman , Mykhailiuk Pavel K. 
Published: May 2022

AbstractAfter more than 20 years of trials, a practical scalable approach to fluoro‐substituted bicyclo[1.1.1]pentanes (F‐BCPs) has been developed. The physicochemical properties of the F‐BCPs have been studied, and the core was incorporated into the structure of the anti‐inflammatory drug Flurbiprofen in place of the fluorophenyl ring.
The Direct Mechanocatalytic Suzuki–Miyaura Reaction of Small Organic Molecules
Authors: Pickhardt Wilm , Beaković Claudio , Mayer Maike , Wohlgemuth Maximilian , Kraus Fabien Joel Leon , Etter Martin , Grätz Sven , Borchardt Lars 
Published: May 2022

AbstractThe molecular Suzuki cross‐coupling reaction was conducted mechanochemically, without solvents, ligands, or catalyst powders. Utilizing one catalytically active palladium milling ball, products could be formed in quantitative yield in as little as 30 min. In contrast to previous reports, the adjustment of milling parameters led to the complete elimination of abrasion from the catalyst ball, thus enabling the first reported systematic catalyst analysis. XPS, in situ XRD, and reference experiments provided evidence that the milling ball surface was the location of the catalysis, allowing a mechanism to be proposed. The versatility of the approach was demonstrated by extending the substrate scope to deactivated and even sterically hindered aryl iodides and bromides.
Ultrathin Covalent Organic Framework Anchored on Graphene for Enhanced Organic Pollutant Removal
Authors: Li Changxia , Guggenberger Patrick , Han Seung Won , Ding Wei‐Lu , Kleitz Freddy 
Published: May 2022

AbstractCovalent organic frameworks (COFs) are of great potential as adsorbents owing to their tailorable functionalities, low density and high porosity. However, their intrinsically stacked two‐dimensional (2D) structure limits the full use of their complete surface for sorption, especially the internal pores. The construction of ultrathin COFs could increase the exposure of active sites to the targeted molecules in a pollutant environment. Herein, an ultrathin COF with a uniform thickness of ca. 2 nm is prepared employing graphene as the surface template. The resulting hybrid aerogel with an ultralow density (7.1 mg cm−3) exhibits the ability to remove organic dye molecules of different sizes with high efficiency. The three‐dimensional (3D) macroporous structure and well‐exposed adsorption sites permit rapid diffusion of solution and efficient adsorption of organic pollutants, thereby, greatly contributing to its enhanced uptake capacity. This work highlights the effect of COF layer thickness on adsorption performance.
Comprehensive demetallization of crude oil using spherical polyelectrolyte brushes with submicron polybutadiene latex as a core
Authors: Yang Lianzhou , Shen Kaili , Xu Jun , Ren Mannian , Cao Fahai 
Published: May 2022

AbstractStable oil‐soluble metals complexes in crude oil bring various problems to the oil processing. In the previous work, four spherical polymer brushes with SiO2 as a core showed high nickel and calcium removal efficiency, but SiO2 has high density and smaller specific surface area, greatly limiting the demetallization efficiency. In the present work, spherical polyelectrolyte brushes (PAA@PB) were synthesized by emulsion grafting polymerization. DLS and TEM show that PAA@PB exhibits a uniform spherical core‐shell structure with a diameter of 526.3 nm, and TGA exhibits that the grafting rate is 20.6%. The demetallization rate and selectivity of PAA@PB were investigated with varying concentration, electrical desalination conditions, pH value, and NaCl concentration. In contrast, the demetallization efficiency of PAA@PB is much greater than that of PAA@SiO2‐G. Notably, PAA@PB exhibits excellent nickel removal efficiency, but a little more selective for iron. The optimal removal rate for calcium, nickel, and iron are 55.3%, 52.6%, and 46.1%, respectively. Compared with P4VP@SiO2‐G, which possesses the highest demetallization efficiency among four polymer brushes with SiO2, to achieve the same nickel removal rate, the concentration of PAA@PB is almost eight times less than that of P4VP@SiO2‐G. Consequently, PAA@PB has great potential as an excellent comprehensive demetallization agent.
Choroid Plexus–Infiltrating T Cells as Drivers of Murine Neuropsychiatric Lupus
Authors: Moore Erica , Huang Michelle W. , Reynolds Cara A. , Macian Fernando , Putterman Chaim 
Published: May 2022

ObjectiveT cells are critical in the pathogenesis of systemic lupus erythematosus (SLE) in that they secrete inflammatory cytokines, help autoantibody production, and form autoreactive memory T cells. Although the contribution of T cells to several forms of organ‐mediated damage in SLE has been previously demonstrated, the role of T cells in neuropsychiatric SLE (NPSLE), which involves diffuse central nervous system manifestations and is observed in 20–40% of SLE patients, is not known. Therefore, we conducted this study to evaluate how behavioral deficits are altered after depletion or transfer of T cells, to directly assess the role of T cells in NPSLE.MethodsMRL/lpr mice, an NPSLE mouse model, were either systemically depleted of CD4+ T cells or intracerebroventricularly injected with choroid plexus (CP)–infiltrating T cells and subsequently evaluated for alterations in neuropsychiatric manifestations. Our study end points included evaluation of systemic disease and assessment of central nervous system changes.ResultsSystemic depletion of CD4+ T cells ameliorated systemic disease and cognitive deficits. Intracerebroventricular injection of CP–infiltrating T cells exacerbated depressive‐like behavior and worsened cognition in recipient mice compared with mice who received injection of splenic lupus T cells or phosphate buffered saline. Moreover, we observed enhanced activation in CP–infiltrating T cells when cocultured with brain lysate–pulsed dendritic cells in comparison to the activation levels observed in cocultures with splenic T cells.ConclusionT cells, and more specifically CP–infiltrating antigen‐specific T cells, contributed to the pathogenesis of NPSLE in mice, indicating that, in the development of more targeted treatments for NPSLE, modulation of T cells may represent a potential therapeutic strategy.
Self‐Assembly of Lanthanide Crescent‐Like and Macrocyclic Clusters from Versatile o‐Vanillin‐Based Ligands
Authors: Yang Qianqian , Li Xiao‐Lei , Ashebr Tesfay G. , Zhao Lang , Tang Jinkui 
Published: May 2022

AbstractThe construction of metallosupramolecules is an interesting but challenging topic for chemists. Dedicated design of multidentate ligands is an effective approach for the construction of novel lanthanide supramolecules. Herein, we report on the stepwise design and syntheses of two flexible and multidentate ligands H2L1 and H4L2 based on the o‐vanillin. By regulating the coordination sites and mode of the ligands, two novel DyIII‐based supramolecules, [Dy4Na(μ2‐OH)2L14(H2O)5(CH3OH)](CF3SO3)3 ⋅ 3H2O ⋅ CH3OH (Dy4) and [Dy8L24(H2L2)4(H2O)4] ⋅ 4CH3OH ⋅ 12H2O (Dy8), have been obtained. Structural studies reveal that Dy4 and Dy8 show different nuclearity and topology: Dy4 shows a crescent‐like structure coordinated by the ligands in different coordination fashions in which two ligands chelate DyIII forming {Dy2} units and linked by the other two ligands; Dy8 is obtained from the supramolecular assembly, in which four completely deprotonated ligands construct the {Dy2} units and the units are linked by four di‐deprotonated ligands, forming a macrocycle topology. Additionally, magnetic measurements reveal that the two complexes exhibit slow magnetic relaxation behavior.
Consumer Response to Boil Water Notifications During Winter Storm Uri
Authors: Day Ashleigh M. , Islam Khairul , O'Shay Sydney , Taylor Kristin , McElmurry Shawn P. , Seeger Matthew W. 
Published: May 2022

Key TakeawaysBoil water notifications (BWNs) issued during 2021’s Winter Storm Uri were typically followed, especially in households with children present and those with higher income.Cascading failure of interconnected systems (such as power and drinking water) inhibited some individuals from being able to follow boil water guidance.Of the people who boiled their water following BWNs, more than 92% reported boiling it for 2 minutes or more.
Antibody Recognition of Cancer Cells via Glycan Surface Engineering
Authors: Szponarski Mathieu , Gademann Karl 
Published: May 2022

AbstractStimulation of the body's immune system toward tumor cells is now well recognized as a promising strategy in cancer therapy. Just behind cell therapy and monoclonal antibodies, small molecule‐based strategies are receiving growing attention as alternatives to direct immune response against tumor cells. However, the development of small‐molecule approaches to modulate the balance between stimulatory immune factors and suppressive factors in a targeted way remains a challenge. Here, we report the cell surface functionalization of LS174T cancer cells with an abiotic hapten to recruit antibodies to the cell surface. Metabolic glycoengineering followed by covalent reaction with the hapten results in antibody recognition of the target cells. Microscopy and flow cytometry studies provide compelling evidence that metabolic glycoengineering and small molecule stimulators can be combined to direct antibody recognition.
Distortion prediction during sintering using Monte Carlo method implemented with virtual springs
Authors: Matsuda Tetsushi 
Published: May 2022

AbstractA computational simulation for sintering based on the Monte Carlo (MC) method implemented with a virtual spring was developed to predict the shrinkage and deformation of compacts. Conventional MC models do not sufficiently consider the local strain of the cells. The proposed model considered the local strain using a virtual spring in each cell. The model linked with the finite element method enables direct calculation of the deformation of the powder compacts. The results indicate that the distortion tendency of the simulations agreed with the experimental results of the sintering of Al2O3 powder compacts. Furthermore, the results indicate the potential of the model to predict the stress distribution in a microstructure during sintering.
Pressure Effects on 3dn (n=4, 9) Insulating Compounds: Long Axis Switch in Na3MnF6 not Due to the Jahn‐Teller Effect
Authors: Sánchez‐Movellán Inés , Carrasco‐Busturia David , García‐Lastra Juan M. , García‐Fernández Pablo , Aramburu José A. , Moreno Miguel 
Published: May 2022

AbstractThe pressure‐induced switch of the long axis of MnF63− units in the monoclinic Na3MnF6 compound and Mn3+‐doped Na3FeF6 is explored with the help of first principles calculations. Although the switch phenomenon is usually related to the Jahn‐Teller effect, we show that, due to symmetry reasons, it cannot take place in 3dn (n=4, 9) systems displaying a static Jahn‐Teller effect. By contrast, we prove that in Na3MnF6 the switch arises from the anisotropic response of the low symmetry lattice to hydrostatic pressure. Indeed, while the long axis of a MnF63− unit at ambient pressure corresponds to the Mn3+−F3− direction, close to the crystal c axis, at 2.79 GPa the c axis is reduced by 0.29 Å while b is unmodified. This fact is shown to force a change of the HOMO wavefunction favoring that the long axis becomes the Mn3+−F2− direction, not far from crystal b axis, after the subsequent relaxation process. The origin of the different d‐d transitions observed for Na3MnF6 and CrF2 at ambient pressure is also discussed together with changes induced by pressure in Na3MnF6. The present work opens a window for understanding the pressure effects upon low symmetry insulating compounds containing d4 or d9 ions.
Three‐Dimensionalsp2Carbon‐LinkedCovalent Organic Frameworks as a Drug Carrier Combined with Fluorescence Imaging
Authors: Liao Li , Zhang Zerong , Guan Xinyu , Li Hui , Liu Yaozu , Zhang Minghao , Tang Bin , Valtchev Valentin , Yan Yushan , Qiu Shilun , Yao Xiangdong , Fang Qianrong 
Published: May 2022

Comprehensive SummaryThree‐dimensional (3D) covalent organic frameworks (COFs) are crystalline porous polymers with potential in numerous high‐tech applications, but the linkages involved in their synthesis are still rather limited. Herein, we report novel 3D sp2carbon‐linked COFs fabricated by the formation reaction of C=C bonds and their application in fluorescence imaging. These new COFs, namely JUC‐580 and JUC‐581, show high stability and excellent light‐emitting properties in solid state and dispersed in various solvents. Furthermore, we investigate the potential application of JUC‐581 as a drug carrier combined with fluorescence imaging. These results indicate that 3D sp2carbon‐linked COFs are not only potential drug‐loaded and sustained release materials but also promising cell fluorescent stains. This study thus expands the structural categories of 3D COFs based on different linkages, and promotes their prospective applications for biomedicine and fluorescent materials.
Towards Innovative Antibacterial Correctors for Cystic Fibrosis Targeting the Lung Microbiome with a Multifunctional Effect
Authors: Martina Maria Grazia , Sannio Filomena , Crespan Emmanuele , Pavone Marialaura , Simoncini Alice , Barbieri Francesca , Perini Cecilia , Pesce Emanuela , Maga Giovanni , Pedemonte Nicoletta , Docquier Jean‐Denis , Radi Marco 
Published: May 2022

AbstractCystic fibrosis (CF) is a genetic disease caused by loss‐of‐function mutations in the CFTR gene, which codes for a defective ion channel. This causes an electrolyte imbalance and results in a spiral of negative effects on multiple organs, most notably the accumulation of thick mucus in the lungs, chronic respiratory tract infections and inflammation leading to pulmonary exacerbation and premature death. Progressive decline of lung function is mainly linked to persistent or recurring infections, mostly caused by bacteria, which require treatments with antibiotics and represent one of the major life‐limiting factors in subjects with CF. Treatment of such a complex disease require multiple drugs with a consequent therapeutic burden and complications caused by drug‐drug interactions and rapid emergence of bacterial drug resistance. We report herein our recent efforts in developing innovative multifunctional antibiotics specifically tailored to CF by a direct action on bacterial topoisomerases and a potential indirect effect on the pulmonary mucociliary clearance mediated by ΔF508‐CFTR correction. The obtained results may pave the way for the development of a simplified therapeutic approach with a single agent acting as multifunctional Antibacterial‐Corrector.
Human perceptual responses to multiple colors II: A study of the correlation between multiple colors and emotion
Authors: Wang Shuang , Yao Man , Liu Jingyu , Jiang Yujian , Jiang Wei 
Published: May 2022

AbstractThis article constructs the hierarchical model of multicolor‐emotion generation network (MCEG‐Net) to investigate human emotional responses to multiple colors based on the research of multicolor perceptual features modeling, which reveals the generation mechanism of multicolor emotion from the perspective of hierarchy of visual features. First, the 164 multicolor samples were evaluated by 30 subjects based on PAD emotion space. On this basis, the correlation analysis was carried out among color basic attributes, multicolor physical features, multicolor perceptual features and emotion. Then, a mathematical model of multicolor emotion was constructed by using multiple linear regression (MLR) algorithm. It was observed that, the multiple colors was strongly correlated with emotion. Finally, the MCEG‐Net was constructed, which reveals the generation mechanism of the process the “the basic attributes of color stimulate human's perceptual reflex and then generate emotion” under the interaction of multiple colors from the perspective of information science. The results showed that the mathematical model could predict color emotion well. In addition, the MCEG‐Net provides a new way to reveal the generation mechanism of color‐emotion associations.
Perovskite Materials and Devices
Authors: Lewiński Janusz , Deleporte Emmanuelle , Zakeeruddin Shaik M. 
Published: May 2022

AbstractThis special collection presents research articles and reviews on the preparation of new perovskite and perovskite‐related materials, and various aspects of their physicochemical properties as well as case studies on the development and characterization of perovskite‐based devices. These works serve as an illustration of the richness and directions of current research in the vibrant and fertile landscape of metal halide perovskites and perovskite‐based photovoltaics.
Changes in quantitative sensory testing and patient perspectives following spinal cord stimulation for persistent spinal pain syndrome: An observational study with long‐term follow‐up
Authors: Plantaz Yannick J. G. M. , van Dongen Robert T. M. , Witkam Richard L. , Vissers Kris C. P. , Timmerman Hans 
Published: May 2022

AbstractBackgroundSpinal cord stimulation (SCS) can impact sensory, pain and tolerance thresholds in various ways, which can be accessed via quantitative sensory testing (QST). The objectives of this study were to (1) assess the subjective sensory responses using QST in patients following SCS therapy for PSPS and (2) to get a clinical impression of the results of SCS during an interview of these patients with PSPS and SCS during long term follow‐up.MethodsForty patients with PSPS who received SCS treatment underwent QST via electrical and mechanical pressure stimuli. QST was performed at four different moments (1) pre‐implantation SCS, (2) two weeks postoperatively, (3) three months after permanent SCS implantation and (4) six months after permanent SCS implantation. Patients’ perspectives on pain, use of drugs and quality of life were assessed via semi‐structured interviews during a follow‐up between 5 and 11 years.ResultsWe found statistical significant differences in the changes of sensory, pain and tolerance thresholds. A decrease in pain complaints and analgesics use were reported by the patients during follow‐up. The quality of life in patients increased from three to eight (NRS 0 [worst QoL imaginable] ‐10 [best QoL imaginable]) after receiving SCS.ConclusionsThe increased thresholds on areas without pain or being covered by the SCS induced paresthesias may indicate that there are central changes contributing to these deviations in thresholds. The overall QoL in patients improved greatly after receiving SCS.SignificanceThis study provides an overview of the effect of SCS on sensory, pain and tolerance thresholds in patients with PSPS throughout the SCS treatment process. In addition, this study presents data from 40 patients with PSPS treated with SCS, analysing several long‐term patient‐reported outcome measures. The results serve to give more insight into the mechanism of SCS and document SCS as a possible treatment for PSPS.
The effect of duloxetine on mechanistic pain profiles, cognitive factors and clinical pain in patients with painful knee osteoarthritis—A randomized, double‐blind, placebo‐controlled, crossover study
Authors: Petersen Kristian Kjær‐Staal , Drewes Asbjørn Mohr , Olesen Anne Estrup , Ammitzbøll Nadia , Bertoli Davide , Brock Christina , Arendt‐Nielsen Lars 
Published: May 2022

AbstractBackgroundDuloxetine is indicated in the management of pain in osteoarthritis. Evidence suggests that duloxetine modulates central pain mechanisms and cognitive factors, and these factors are assumed contributing to the analgesic effect. This proof‐of‐mechanism, randomized, placebo‐controlled, crossover, double‐blinded trial evaluated the effect of duloxetine on quantitative sensory testing (QST), cognitive factors and clinical pain in patients with osteoarthritis and to predict the analgesic effect.MethodsTwenty‐five patients completed this cross‐over study with either 18‐week duloxetine (maximum 60 mg/daily) followed by placebo or vice‐versa. Pressure pain thresholds, temporal summation of pain and conditioned pain modulation were assessed using cuff algometry. The Hospital Anxiety and Depression Scale and the Pain Catastrophizing Scale evaluated cognitive factors. Clinical pain was assessed using Brief Pain Inventory and Western Ontario and McMaster Universities Osteoarthritis Index. Linear regression models were used to predict the analgesic effect of duloxetine.ResultsDepending on the clinical pain outcome, 40%–68% of patients were classified as responders to duloxetine. Linear regression models predicted the analgesic effect (predictive value of 45%–75% depending on clinical pain outcome parameter) using a combination of pretreatment QST parameters, cognitive factors and clinical pain. No significant changes were found for QST, cognitive factors or clinical pain on a group level when comparing duloxetine to placebo.ConclusionA combination of pretreatment QST, cognitive factors and clinical pain was able to predict the analgesic response of duloxetine. However, in this relatively small study, duloxetine did not selectively modulate QST, cognitive factors or clinical pain intensity when compared with placebo.SignificanceDuloxetine is proposed as a treatment for chronic pain. Pre‐clinical trials suggest that duloxetine provides analgesia through modulation of descending pain inhibitory pathways or through improvements in cognitive factors. The current study demonstrates that pretreatment mechanistic pain profiling, cognitive factors and clinical pain can predict the analgesic effect of duloxetine and that only a subset of patients might benefit from duloxetine treatment.