bluuebunny/crossref_metadata_2025_split huggingface dataset:
Impact of Nanoscale Morphology on Charge Carrier Delocalization and Mobility in an Organic Semiconductor
Authors: Ellis Matthew , Yang Hui , Giannini Samuele , Ziogos Orestis G. , Blumberger Jochen 
Published: November 2021

AbstractA central challenge of organic semiconductor research is to make cheap, disordered materials that exhibit high electrical conductivity. Unfortunately, this endeavor is hampered by the poor fundamental understanding of the relationship between molecular packing structure and charge carrier mobility. Here a novel computational methodology is presented that fills this gap. Using a melt‐quench procedure it is shown that amorphous pentacene spontaneously self‐assembles to nanocrystalline structures that, at long quench times, form the characteristic herringbone layer of the single crystal. Quantum dynamical simulations of electron hole transport show a clear correlation between the crystallinity of the sample, the quantum delocalization, and the mobility of the charge carrier. Surprisingly, the long‐held belief that charge carriers form relatively localized polarons in disordered OS is only valid for fully amorphous structures—for nanocrystalline and crystalline samples, significant charge carrier delocalization over several nanometers occurs that underpins their improved conductivities. The good agreement with experimentally available data makes the presented methodology a robust computational tool for the predictive engineering of disordered organic materials.
Stretchable, Soft, and Variable Stiffness Elastomer foam with Positive and Negative Piezoresistivity Enabled by Liquid Metal Inclusion
Authors: Cho Dongkyun , Bhuyan Priyanuj , Sin Dongho , Kim Hyemin , Kim Eunseon , Park Sungjune 
Published: November 2021

AbstractStretchable and soft piezoresistive composites are appealing for application to tactile sensors, artificial skin, and wearable electronics. The ability of the composites to deform the geometries when they are strained can allow the electrical behavior of the composites to be manipulated. Although rigid metal and semiconductor inclusions have been utilized to create piezoresistive composites, they limit the degree of mechanical deformation. Here, liquid metal (gallium, melting point ≈ 29.7 °C) inclusion into elastomeric foam substrate with 3D open cell morphologies is utilized. Gallium is a fluidic conductor, thus it is possible to infiltrate the liquid metal into the 3D interconnected pore, resulting in soft, stretchable, and shape reconfigurable conductive composites that can change shape and function in response to external stimuli. Applying strain can enable deformation of the liquid metal, generating changes of electrical resistance. Interestingly, it is found that this piezoresistivity of the composite can be positively and negatively manipulated by adjusting the geometries of the liquid metal in the foam. Furthermore, the liquid metal in the elastomeric foam can be reversibly actuated by applying compressive force, resulting in manipulation of the restorative electrical activity of the composites.
High Performance Solution‐Processed Deep‐Blue Phosphorescence Organic Light‐Emitting Diodes with EQE Over 24% by Employing New Carbenic Ir(III) Complexes
Authors: Kumaresan Raja , Park Ho‐Yeol , Maheshwaran Athithan , Park Hyungjin , Do Yeongju , Song Myungkwan , Yoon Jinhwan , Ahn Sung Il , Jin Sung‐Ho 
Published: November 2021

AbstractSolution‐processed phosphorescence organic light‐emitting diodes (PHOLEDs) are an increasingly attractive option as compared with vacuum‐processed PHOLEDs due to their lower costs, large areas, and flexible production. Currently, the majority of reported solution‐processed PHOLEDs are produced using red and green triplet emitters. The earlier reports on blue solution‐processed PHOLEDs describe poor Commission International de l'Éclairage color coordinates (CIE(x, y)) and low external quantum efficiencies (EQEs). It is difficult to produce efficient solution‐processed deep‐blue PHOLEDs that meet high EQE and CIE y color coordinate ≤ 0.15 requirements. The authors design and synthesize three new carbenic homoleptic deep‐blue emitting Ir(III) complexes for solution‐processed PHOLEDs. The introduction of bulky tert‐butyl and trifluoromethyl (CF3) substituents at a suitable position on the benzylated pyridoimidazole moiety effectively improves solution‐processed device performance without compromising CIE(x, y) color purity. The deep‐blue PHOLEDs exhibit remarkable maximum EQE (EQEmax) of 25.3% and excellent CIE(x, y) color of (0.16, 0.10) at a mer‐Ir(ptbbp)3 doping ratio of 50 wt%. In particular, deep‐blue PHOLEDs containing mer‐Ir(CF3pbp)3 as dopant exhibit excellent CIE(x, y) color coordinates of (0.16, 0.05) and an EQEmax of 21.2%. This is the first report of deep‐blue solution‐processed PHOLEDs containing carbene‐based Ir(III) complexes with extremely high EQE values and CIE y coordinate requirement.
Precise Diabetic Wound Therapy: PLS Nanospheres Eliminate Senescent Cells via DPP4 Targeting and PARP1 Activation
Authors: Zhao Renliang , Jin Xiangyun , Li Ang , Xu Bitong , Shen Yifan , Wang Wei , Huang Jinghuan , Zhang Yadong , Li Xiaolin 
Published: November 2021

AbstractDiabetic ulcers, a difficult problem faced by clinicians, are strongly associated with an increase in cellular senescence. Few empirical studies have focused on exploring a targeted strategy to cure diabetic wounds by eliminating senescent fibroblasts (SFs) and reducing side effects. In this study, poly‐l‐lysine/sodium alginate (PLS) is modified with talabostat (PT100) and encapsulates a PARP1 plasmid (PARP1@PLS‐PT100) for delivery to target the dipeptidyl peptidase 4 (DPP4) receptor and eliminate SFs. PARP1@PLS‐PT100 releases encapsulated plasmids, displaying high selectivity for SFs over normal fibroblasts by targeting the DPP4 receptor, decreasing senescence‐associated secretory phenotypes (SASPs), and stimulating the secretion of anti‐inflammatory factors. Furthermore, the increased apoptosis of SFs and the disappearance of cellular senescence alleviates SASPs, accelerates re‐epithelialization and collagen deposition, and significantly induces macrophage M2 polarization, which mediates tissue repair and the inflammatory response. This innovative strategy has revealed the previously undefined role of PARP1@PLS‐PT100 in promoting diabetic wound healing, suggesting its therapeutic potential in refractory wound repair.
The High‐Pressure Processed Cu2S: Phase Intergrowth with Strained Lamella Leading to an Improved Thermoelectric Performance
Authors: Luo Hao , Yang Dongwang , Yu Yimeng , Liang Qi , Peng Haoyang , Xia Fanjie , Tang Xinfeng , Wu Jinsong 
Published: November 2021

AbstractAmong the state‐of‐the‐art thermoelectric materials, Cu2S has attracted much attention because of its nontoxicity, high abundance, and “phonon‐liquid electron‐crystal” characteristics. It is found the thermoelectric performance of Cu2S processed by high‐pressure at room temperature (HPRT) can be greatly improved. However, the underlying mechanism remains unknown due to the complex phase and microstructure formed under high pressure. Herein, the origin of the improved properties is disclosed by investigating the dynamic phase and defect structure evolutions using both ex situ and in situ transmission electron microscopy, and by exploring the high temperature thermal kinetics through differential scanning calorimetry and high temperature Hall test. It is surprising to find that an intergrowth of monoclinic γ‐phase and tetragonal δ‐phase is formed in the HPRT Cu2S. Meanwhile, a strained lamella structure with a large number of dislocations is found within the monoclinic γ‐Cu2S phase. Due to the defected microstructure and thus the increased carrier concentration, conductivities of electron and phonon are decoupled. Notably, the average lattice thermal conductivity of HPRT Cu2S is low in 600–900 K, due to the strongly phonon scattering by nanovoids inside the material. Finally, in 600–900 K, an average ZT value of 0.89 is obtained in the HPRT Cu2S, much higher than that of 0.19 for melting combined with plasma activated sintering processed Cu2S.
Nitrogen and phosphorus uptake and nitrogen fixation estimation of faba bean in western Canada
Authors: Klippenstein Serena Roslyn , Khazaei Hamid , Vandenberg Albert , Schoenau Jeff 
Published: November 2021

AbstractFaba bean (Vicia faba L.) has very efficient dinitrogen (N2) fixation, the greatest among grain legumes. The main aims of this study were to investigate the effect of nitrogen (N) and phosphorus (P) fertilizers on yield, N and P uptake, and biological nitrogen fixation (BNF) potential of faba bean. Four faba bean cultivars (‘CDC Snowdrop’, ‘219‐16’, ‘Snowbird’, and ‘Tabasco’) were grown in a 2‐yr field experiment at four site‐locations in Saskatchewan, Canada, during 2016 and 2017. In addition, a controlled‐environment study was also conducted to address how P fertilization influences growth and proportion of nitrogen derived from the atmosphere (%Ndfa) through BNF in 2017. Yield was not significantly affected by cultivar, fertilization or site‐location, however, N and P uptake were significantly affected to varying degrees by all three effects. The average faba bean grain yield was 5,280 kg ha–1 in field experiments. Average grain N uptake (117–300 kg N ha–1) and P uptake (15–35 kg P ha–1 and 34–80 kg P2O5 ha–1) were significantly greater than straw N and P uptake in the field. An estimated 88% Ndfa was obtained in the controlled‐environment study and 230 kg N ha–1 of N uptake was observed in aboveground biomass (grain and straw) in the field experiments. Results support the efficiency of N2 fixation in this species in western Canada.
Total Synthesis of Shearinines D and G: A Convergent Approach to Indole Diterpenoids
Authors: Hauser Nicole , Imhof Michael A. , Eichenberger Sarah S. , Kündig Tomas , Carreira Erick M. 
Published: November 2021

AbstractThe first total syntheses of the indole diterpenoids (+)‐shearinine G and D are disclosed. The successful routes rely on late‐stage coupling of two complex fragments. Formation of the challenging trans‐hydrindane motif was accomplished by diastereoselective, intramolecular cyclopropanation. A one‐pot sequence consisting of Sharpless dihydroxylation/Achmatowicz reaction was developed to install the dioxabicyclo[3.2.1]octane motif. The indenone subunit was accessed by Prins cyclization. Tuning the electronic nature of the substituents on the parent arylcarboxaldehyde allowed access to divergent products that were further transformed into shearinines G and D. Riley‐type oxidation of a bicyclic enone yielded a surprising stereochemical outcome.
Controlled In‐Cell Generation of Active Palladium(0) Species for Bioorthogonal Decaging
Authors: Konč Juraj , Sabatino Valerio , Jiménez‐Moreno Ester , Latocheski Eloah , Pérez Laura Rodríguez , Day Jason , Domingos Josiel B. , Bernardes Gonçalo J. L. 
Published: November 2021

AbstractOwing to their bioorthogonality, transition metals have become very popular in the development of biocompatible bond‐cleavage reactions. However, many approaches require design and synthesis of complex ligands or formulation of nanoparticles which often perform poorly in living cells. This work reports on a method for the generation of an active palladium species that triggers bond‐cleaving reactions inside living cells. We utilized the water‐soluble Na2PdCl4 as a simple source of PdII which can be intracellularly reduced by sodium ascorbate to the active Pd0 species. Once generated, Pd0 triggers the cleavage of allyl ether and carbamate caging groups leading to the release of biologically active molecules. These findings do not only expand the toolbox of available bioorthogonal dissociative reactions but also provide an additional strategy for controlling the reactivity of Pd species involved in Pd‐mediated bioorthogonal reactions.
A novel UPLC–MS/MS method for simultaneous quantification of trigonelline, 4‐hydroxyisoleucine, and diosgenin from Trigonella foenum‐graecum extract: Application to pharmacokinetic study in healthy and type 2 diabetic rats
Authors: Wadhwa Geetika , Krishna Kowthavarapu Venkata , Taliyan Rajeev , Tandon Neeraj , Yadav Satyapal Singh , Banerjee Dipankar , Narwaria Avinash , Katiyar Chandrakant , Dubey Sunil Kumar 
Published: November 2021

AbstractTrigonelline (TR), 4‐hydroxyisoleucine (4‐HI), and diosgenin (DG) are the main bioactives of the purified standardized extract of the popular plant Trigonella foenum‐graecum L. (TFG), and it has been proven effective for the treatment of various diseases. However, to the best of our knowledge, no study has investigated the pharmacokinetic parameters of purified standardized T. foenum‐graecum extract in normal and diabetic Wistar rats. The present study has developed and validated a rapid, reliable, and sensitive simultaneous ultra‐performance liquid chromatography MS method to estimate these bioactives. The chromatographic separation was achieved using methanol, acetonitrile, and 0.1% formic acid with the ideal gradient flow system on a BEH Shield RP 18 column. A positive electrospray ionization mode was selected to estimate m/z values of TR (138.14 > 94.63), 4‐HI (148.19 > 74.08), and DG (415.54 > 271.33). The method was robust and reproducible over the linearity range of 60–5000, 6–5000, and 15–5000 ng/mL for TR, 4‐HI, and DG, respectively. Using this novel validated method, we investigated the pharmacokinetic parameters of bioactives using Phoenix WinNonlin version 8.0 (Certera) in normal and diabetic rats. The assay was successfully applied for the estimation of pharmacokinetic parameters using noncompartmental analysis. This investigation shows that the absorption rate increased, whereas distribution and elimination processes slowed down in diabetic rats compared with normal rats.
Tailoring the Properties of Optical Force Probes for Polymer Mechanochemistry
Authors: He Siyang , Stratigaki Maria , Centeno Silvia P. , Dreuw Andreas , Göstl Robert 
Published: November 2021

AbstractInvited for the cover of this issue are Robert Göstl and co‐workers at DWI–Leibniz Institute for Interactive Materials, RWTH Aachen University and Heidelberg University. The image depicts the tailoring of optical force probes for analyzing polymer materials. Read the full text of the article at 10.1002/chem.202102938.
Lactic acidosis, a potential toxicity from drug–drug interaction related to concomitant ribociclib and metformin in preexisting renal insufficiency: A case report
Authors: Lagampan Chalita , Poovorawan Nattaya , Parinyanitikul Napa 
Published: November 2021

AbstractBackgroundRibociclib, one of the cyclin‐dependent kinases (CDK) 4 and 6 inhibitors, in combination with endocrine therapies has been approved in the treatment of hormonal receptor positive, HER‐2 negative metastatic breast cancer worldwide. Long‐term usage of ribociclib with concomitant drugs, potential drug–drug interaction may develop which can limit the therapeutic value of CDK4/6 inhibitor.CaseA 62‐year‐old with history of non‐insulin dependent diabetic, dyslipidemia, and essential hypertension was diagnosed with HR‐positive, HER‐2 negative metastatic breast cancer and treated with fulvestrant plus ribociclib. Four weeks after administration, elevated serum creatinine was observed, and then severe lactic acidosis with acute respiratory failure was subsequently reported. Ribociclib and fulvestrant were temporarily discontinued. Three days after renal replacement therapy, her clinical was stabilized. Combination ribociclib with metformin resulted in high plasma metformin levels and dangerous consequences. Hence, special precaution should be considered during concomitant treatment with sensitive transporter substrates.ConclusionMetformin associated lactic acidosis may potentially occur after combination with ribocilib, an uncommon but lethal complication from the interaction of these drugs, especially in patients who had preexisting renal impairment.
Facile Synthesis of Amorphous MoCo Lamellar Hydroxide for Alkaline Water Oxidation
Authors: Qian Shengtai , Huang Gang , Zhu Tong , Zhang Yue , Tang Wukui , Yu Ronghai 
Published: November 2021

AbstractTo find an oxygen evolution reaction (OER) catalyst with satisfactory catalytic performance and affordable cost is of great importance to the development of many new energy devices. In this work, a simple and effective strategy was developed to synthesize a series of amorphous MoCo lamellar hydroxide through one‐step chemical co‐precipitation. Systematic investigations showed that different functional agents (2‐methylimidazole, NaOH, NH4OH) in the fabrication process resulted in different micromorphology of the catalyst, thus influencing its electrocatalytic performance. Also, adding various amounts of Mo could influence the intrinsic catalytic properties. Samples synthesized with appropriate functional agent addition and optimized Mo addition exhibited amorphous nature and bent nanosheet morphology, as well as highest intrinsic catalytic activity, showing a low overpotential of 290 mV at 10 mA cm−2 and a small Tafel slope of 55 mV dec−1 in 1 m KOH solution. Additionally, the catalytic performance of the sample showed just small decay after 50 h chronopotentiometry test and 3000 cyclic voltammetry cycles, exhibiting the ultra‐stable catalytic activity of the catalyst. This work provides a possible large‐scale commercial production strategy of OER catalysts with promising performance and low fabrication cost.
Electrochemical Proton Reduction over Nickel Foam for Z‐Stereoselective Semihydrogenation/deuteration of Functionalized Alkynes
Authors: Valiente Alejandro , Martínez‐Pardo Pablo , Kaur Gurpreet , Johansson Magnus J. , Martín‐Matute Belén 
Published: November 2021

AbstractSelective reduction strategies based on abundant‐metal catalysts are very important in the production of chemicals. In this paper, a method for the electrochemical semihydrogenation and semideuteration of alkynes to form Z‐alkenes was developed, using a simple nickel foam as catalyst and H3O+ or D3O+ as sources of hydrogen or deuterium. Good yields and excellent stereoselectivities (Z/E up to 20 : 1) were obtained under very mild reaction conditions. The reaction proceeded with terminal and nonterminal alkynes, and also with alkynes containing easily reducible functional groups, such as carbonyl groups, as well as aryl chlorides, bromides, and even iodides. The nickel‐foam electrocatalyst could be recycled up to 14 times without any change in its catalytic properties.
Serological and cellular inflammatory signatures in end‐stage kidney disease and latent tuberculosis
Authors: McLean Milla R , Wragg Kathleen M , Lopez Ester , Kiazyk Sandra A , Ball Terry Blake , Bueti Joe , Kent Stephen J , Juno Jennifer A , Chung Amy W 
Published: November 2021

AbstractObjectivesTuberculosis comorbidity with chronic diseases including diabetes, HIV and chronic kidney disease is of rising concern. In particular, latent tuberculosis infection (LTBI) comorbidity with end‐stage kidney disease (ESKD) is associated with up to 52.5‐fold increased risk of TB reactivation to active tuberculosis infection (ATBI). The immunological mechanisms driving this significant rise in TB reactivation are poorly understood. To contribute to this understanding, we performed a comprehensive assessment of soluble and cellular immune features amongst a unique cohort of patients comorbid with ESKD and LTBI.MethodsWe assessed the plasma and cellular immune profiles from patients with and without ESKD and/or LTBI (N = 40). We characterised antibody glycosylation, serum complement and cytokine levels. We also assessed classical and non‐classical monocytes and T cells with flow cytometry. Using a systems‐based approach, we identified key immunological features that discriminate between the different disease states.ResultsIndividuals with ESKD exhibited a highly inflammatory plasma profile and an activated cellular state compared with those without ESKD, including higher levels of inflammatory antibody Fc glycosylation structures and activated CX3CR1+ monocytes that correlate with increased inflammatory plasma cytokines. Similar elevated inflammatory signatures were also observed in ESKD+/LTBI+ compared with ESKD−/LTBI+, suggesting that ESKD induces an overwhelming inflammatory immune state. In contrast, no significant inflammatory differences were observed when comparing LTBI+ and LTBI− individuals.ConclusionOur study highlights the highly inflammatory state induced by ESKD. We hypothesise that this inflammatory state could contribute to the increased risk of TB reactivation in ESKD patients.
Fingerprinting Arctic and North Atlantic Macroalgae with eDNA – Application and perspectives
Authors: Ørberg Sarah B. , Krause‐Jensen Dorte , Geraldi Nathan R. , Ortega Alejandra , Díaz‐Rúa Rubén , Duarte Carlos M. 
Published: November 2021

AbstractMacroalgae are key primary producers in North Atlantic and Arctic coastal ecosystems, and tracing their fate and distribution is vital to improve our understanding of their ecological role and provision of ecosystem services. Recent advances from environmental DNA (eDNA) have added a new capacity to fingerprint and trace macroalgae. However, further development of resources for amplifying and identifying macroalgal eDNA are much needed. Here, we examined the performance in terms of resolution and specificity of two 18S primers (18S‐V7 and 18S‐V9) recently applied in identifying macroalgae from eDNA. We also built a local barcode database for primer 18S‐V7 with 31 widespread Arctic and North Atlantic macroalgal species to complement the existing DNA databases. Furthermore, we applied metabarcoding of eDNA to identify macroalgae in Arctic marine sediments (Disko Bay, W. Greenland) and evaluated the contributions from our local barcode database. We identified macroalgal DNA from 19 families across 11 orders in surface (0–1 cm, with both primers) and sub‐surface (5–10 cm, with 18S‐V7 primer) sediments. The barcode database developed here with the 18S‐V7 primer improved the identification of unique families, from 16 to 19 families, thereby strengthening the taxonomic assignment possible relative to pre‐existing barcode reference sequences. Overall, this study demonstrates the feasibility of eDNA to resolve contributions of macroalgae in Arctic marine sediments, and enhances the fingerprinting resolution. We thereby document a novel pathway to answer key questions on the ecological role and fate of macroalgae in the Arctic.
Copper‐Catalyzed N1 Coupling of 3‐Aminoindazoles and Related Aminoazoles with Aryl Bromides
Authors: Cyr Patrick , Joseph‐Valcin Eve‐Marline , Boissarie Patrick , Simoneau Bruno , Marinier Anne 
Published: November 2021

AbstractThe N1‐selective arylation of 3‐aminoindazoles using copper catalysis is herein reported. The reaction uses readily accessible aryl bromides as coupling partners, including those from heterocycles, and allows easy access to a broad variety of substituted 3‐aminoindazoles. The methodology was also examined on other aminoazoles of interest for the pharmaceutical industry.
Pd/Gorlos‐Phos‐Catalyzed Chemoselective Amination of Bromophenyl Chlorides with Primary Arylamines
Authors: Duan Xinyu , Song Yulong , Fu Chunling , Ma Shengming 
Published: November 2021

AbstractWith the readily available Gorlos‐Phos as a ligand, halogenated diarylamines were prepared efficiently from Pd‐catalyzed monoamination of bromophenyl chlorides and primary arylamines, tolerating functional groups such as aldehyde, ketone, nitrile, fluorine, sulphonyl and trifluoromethyl groups. The formation of the amination of the C−Cl bond and diamination products were not observed.