bluuebunny/crossref_metadata_2025_split huggingface dataset:
Redox‐Neutral Tetrafluoroethylation of Aryl Alkynes with 1,1,2,2‐Tetrafluoroethane Sulfonic Acid Leading to α‐Tetrafluoroethylated Acetophenones
Authors: Kawamoto Takuji , Noguchi Kohki , Takata Ryotaro , Sasaki Rio , Matsubara Hiroshi , Kamimura Akio 
Published: April 2021

AbstractThe redox‐neutral tetrafluoroethylation of alkynes with 1,1,2,2‐tetrafluroroethanesulfonic acid (TFESA) and azobis(isobutyronitrile) (AIBN) proceeds via the formation of vinyl tetrafluoroethanesulfonates followed by a radical tetrafluoroethylation. Experimental and theoretical results support an intermolecular reaction.
Electrostatic Interactions Leading to Hierarchical Interpenetrating Electroconductive Networks in Silicon Anodes for Fast Lithium Storage
Authors: Jiang Min , Chen Junliang , Ma Yuanyuan , Luo Wei , Yang Jianping 
Published: April 2021

AbstractRecently, the frequency of combining MXene, which has unique properties such as metal‐level conductivity and large specific surface area, with silicon to achieve excellent electrochemical performance has increased considerably. There is no doubt that the introduction of MXene can improve the conductivity of silicon and the cycling stability of electrodes after elaborate structure design. However, most exhaustive contacts can only improve the electrode conductivity on the plane. Herein, a MXene@Si/CNTs (HIEN‐MSC) composite with hierarchical interpenetrating electroconductive networks has been synthesized by electrostatic self‐assembly. In this process, the CNTs are first combined with silicon nanoparticles and then assembled with MXene nanosheets. Inserting CNTs into silicon nanoparticles can not only reduce the latter‘s agglomeration, but also immobilizes them on the three‐dimensional conductive framework composed of CNTs and MXene nanosheets. Therefore, the HIEN‐MSC electrode shows superior rate performance (high reversible capacity of 280 mA h−1 even tested at 10 A g−1), cycling stability (stable reversible capacity of 547 mA h g−1 after 200 cycles at 1 A g−1) and applicability (a high reversible capacity of 101 mA h g−1 after 50 cycles when assembled with NCM622 into a full cell). These results may provide new insights for other electrodes with excellent rate performance and long‐cycle stability.
Elucidating the Dual Mode of Action of Dipeptidyl Enoates in the Inhibition of Rhodesain Cysteine Proteases
Authors: Arafet Kemel , González Florenci V. , Moliner Vicent 
Published: April 2021

AbstractA computational study of the two possible inhibition mechanisms of rhodesain cysteine protease by the dipeptidyl enoate Cbz‐Phe‐Leu‐CH=CH−CO2C2H5 has been carried out by means of molecular dynamics simulations with hybrid QM/MM potentials. The low free energy barriers confirm that the Cys25 residue can attack both Cβ and C1 atoms of the inhibitor, confirming a dual mode of action in the inhibition of the rhodesain by enoates. According to the results, the inhibition process through the Cys25 attack on the Cβ atom of the inhibitor is an exergonic and irreversible process, while the inhibition process when Cys25 attacks on the C1 atom of the inhibitor is and exergonic but reversible process. The interactions between the inhibitor and rhodesain suggest that P2 is the most important fragment to consider in the design of new efficient inhibitors of rhodesain. These results may be useful for the design of new inhibitors of rhodesain and other related cysteine proteases based on dipeptidyl enoates scaffolds.
Empowerment or enslavement: The impact of technology‐driven work intrusions on work–life balance
Authors: Senarathne Tennakoon K L Uthpala 
Published: April 2021

AbstractInformation and communication technology (ICT) tools have become an integral component of our lives, enabling individuals to seamlessly cross the work/life border with minimal effort. This paper examines the mechanisms through which work‐related ICT use beyond worktime (Wk_ICT) impacts work–life balance (WLB) through four mediator paths: work‐to‐life conflict, life‐to‐work conflict, work‐to‐life enrichment, and life‐to‐work enrichment. Data from 423 professionals from Canada was analyzed using the multiple mediation approach with bootstrapping using the PROCESS add‐on to SPSS. The results allude to a possible downward spiralling effect of diminishing WLB resulting from excessive work ICT use beyond worktime. The findings add to the literature by empirically demonstrating the mechanisms by which Wk_ICT impact WLB through cross‐domain conflict and enrichment.
Water‐Assisted Concerted Proton‐Electron Transfer at Co(II)‐Aquo Sites in Polyoxotungstates With Photogenerated RuIII(bpy)33+ Oxidant
Authors: Rigodanza Francesco , Marino Nadia , Bonetto Alessandro , Marcomini Antonio , Bonchio Marcella , Natali Mirco , Sartorel Andrea 
Published: April 2021

AbstractThe cobalt substituted polyoxotungstate [Co6(H2O)2(α‐B‐PW9O34)2(PW6O26)]17− (Co6) displays fast electron transfer (ET) kinetics to photogenerated RuIII(bpy)33+, 4 to 5 orders of magnitude faster than the corresponding ET observed for cobalt oxide nanoparticles. Mechanistic evidence has been acquired indicating that: (i) the one‐electron oxidation of Co6 involves Co(II) aquo or Co(II) hydroxo groups (abbreviated as Co6(II)−OH2 and Co6(II)−OH, respectively, whose speciation in aqueous solution is associated to a pKa of 7.6), and generates a Co(III)−OH moiety (Co6(III)−OH), as proven by transient absorption spectroscopy; (ii) at pH>pKa, the Co6(II)−OH→RuIII(bpy)33+ ET occurs via bimolecular kinetics, with a rate constant k close to the diffusion limit and dependent on the ionic strength of the medium, consistent with reaction between charged species; (iii) at pH <pKa, the process involves Co6(II)−OH2→Co6(III)−OH transformation and proceeds via a multiple‐site, concerted proton electron transfer (CPET) where water assists the transfer of the proton, as proven by the absence of effect of buffer base concentrations on the rate of the ET and by a H/D kinetic isotope in a range of 1.2–1.4. The reactivity of water is ascribed to its organization on the surface of the polyanionic scaffold through hydrogen bond networking involving the Co(II)−OH2 group.
Dodecacyclic‐Fused Electron Acceptors with Multiple Electron‐Deficient Units for Efficient Organic Solar Cells
Authors: Ma Shanshan , Feng Hexiang , Liu Xiang , Hu Zhicheng , Yang Xiye , Liang Yuanying , Zhang Jie , Huang Fei , Cao Yong 
Published: April 2021

AbstractFused aromatic cores in non‐fullerene electron acceptors (NFEAs) play a significant role in determining their optoelectronic properties and photovoltaic performance. In this work, a dodecacyclic‐fused core with three electron‐deficient units is synthesized through a double intramolecular Cadogan reduction cyclization. Terminal groups with different halogen substitution (F or Cl) are grafted onto the dodecacyclic‐fused core to afford MS‐4F and MS‐4Cl, both of which showed strong and broad absorption, narrow bandgaps around 1.40 eV, and variable molecular packing model in pristine and blend films. Photovoltaic performance of solar cells containing MS‐4F and MS‐4Cl as NFEAs were investigated with resultant power conversion efficiencies (PCEs) of 11.75 % and 11.79 %, respectively. The mechanism study indicates that both of PBDB‐T : MS‐4F‐ and PBDB‐T : MS‐4Cl‐based devices displayed high hole and electron mobility values, efficient charge transfer, and low charge recombination etc. These results indicate that designing multiple‐fused aromatic cores with multiple electron‐deficient units is a promising strategy to obtain high‐performance NFEAs.
Time‐modulated multibeam steered antenna array synthesis with optimally designed switching sequence
Authors: Chakraborty Avishek , Ram Gopi , Mandal Durbadal 
Published: April 2021

SummarySteering the radiation pattern of an antenna array towards the desired spatial angle is beneficial for modern‐age communication systems. The generation of multiple steered patterns by enhancing the first‐order harmonics of a time‐modulated antenna array (TMAA) with controlled radiation features is proposed in this paper. Suitable switching sequences are designed to realize an efficient electronic beam steering with these simultaneously generated narrow directional beam patterns. TMAAs are considered the time‐domain counterparts of phased arrays where high‐speed switches are used to achieve a weighted response by periodically modulating the array elements instead of attenuators or phase shifters. This periodic modulation inherently produces spurious harmonic patterns generally considered as power loss in unintended directions. The beam steering aimed in this paper is accomplished by exploiting the first‐order harmonic patterns in some specific directions keeping the fundamental pattern unaltered. The intended first positive and first negative harmonic components of the TMAA are utilized as steered multibeam patterns, whereas all the remaining harmonic components are suppressed to improve the efficiency of the array. To achieve this, suitable switching sequences are designed by optimizing the ON‐time duration and switching intervals of the elements with a wavelet mutation‐based particle swarm optimization (PSOWM). 16‐element linear TMAA is used to generate the desired patterns with low sidelobe levels (SLLs) for enhanced performance. Numerical results obtained for spatially independent steered patterns are presented and compared with the state‐of‐the‐art literature results.
Usefulness of cut‐off points of International criteria for prediction of post‐partum diabetes and prediabetes among Chinese women with gestational diabetes
Authors: Li Ninghua , Li Jing , Zhang Cuiping , Liu Gongshu , Leng Junhong , Liu Jinnan , Wang Leishen , Li Weiqin , Yu Zhijie , Hu Gang , Chan Juliana C. N. , Yang Xilin 
Published: April 2021

AbstractAimsThis study tests whether cut‐off points of the International Association of Diabetes and Pregnancy Study Group's (IADPSG) criteria had threshold effects on post‐partum prediabetes and diabetes among Chinese pregnant women with gestational diabetes mellitus (GDM).Materials and MethodsA total of 507 out of 1000 women with GDM (948 of them enrolled in a lifestyle trial during pregnancy) turned up for the follow‐up study and underwent a 75‐g 2‐h oral glucose tolerance test. GDM was diagnosed based on the IADPSG's criteria while post‐partum diabetes and prediabetes were defined by the World Health Organization's. Generalized logit model was used to obtain odds ratios (OR) and 95% confidence interval (CI) of fasting, 1‐h and 2‐h plasma glucoses (PGs) for post‐partum diabetes and prediabetes. Restricted cubic spline was used to identify any threshold effects.ResultsAt a median of 9.1 weeks post‐partum, 3.7% (n = 19) women developed post‐partum diabetes and 35.1% (n = 178) developed post‐partum prediabetes. Fasting PG ≥ 5.1 mmol/L was associated with markedly increased risk of post‐partum diabetes without a discernible threshold (adjusted OR: 3.87, 95% CI: 1.03–14.52) while 2‐h PG ≥ 8.5 and ≥ 9.0 mmol/L had threshold effects on post‐partum prediabetes (2.10, 1.33–3.30) and diabetes (4.02, 1.04–15.56). The 1‐h PG also had a threshold at ≥10.0 mmol/L for prediabetes (1.67, 1.06–2.64), but it was not significant for post‐partum diabetes.ConclusionsAmong Chinese women with GDM, fasting PG ≥ 5.1 mmol/L was associated with post‐partum diabetes without any discernible threshold effects while 2‐h PG ≥ 8.5 and ≥ 9.0 mmol/L respectively identified women at high risk of post‐partum prediabetes and diabetes.
Engrailed‐2 is a cell autonomous regulator of neurogenesis in cultured hippocampal neural stem cells
Authors: Durens Madel , Soliman Mai , Millonig James , DiCicco‐Bloom Emanuel 
Published: April 2021

AbstractAbnormalities in genes that regulate early brain development are known risk factors for neurodevelopmental disorders. Engrailed‐2 (En2) is a homeodomain transcription factor with established roles in cerebellar patterning. En2 is highly expressed in the developing mid‐hindbrain region, and En2 knockout (KO) mice exhibit major deficits in mid‐hindbrain structures. However, En2 is also expressed in forebrain regions including the hippocampus, but its function is unknown. Previous studies have shown that the hippocampus of En2‐KO mice exhibits reductions in its volume and cell numbers due to aberrant neurogenesis. Aberrant neurogenesis is due, in part, to noncell autonomous effects, specifically, reductions of innervating norepinephrine fibers from the locus coeruleus. In this study, we investigate possible cell autonomous roles of En2 in hippocampal neurogenesis. We examine proliferation, survival, and differentiation using cultures of hippocampal neurospheres of P7 wild‐type (WT) and En2‐KO hippocampal neural progenitor cells (NPCs). At 7 days, En2‐KO neurospheres were larger on average than WT spheres and exhibited 2.5‐fold greater proliferation and 2‐fold increase in apoptotic cells, similar to in vivo KO phenotype. Further, En2‐KO cultures exhibited 40% less cells with neurite projections, suggesting decreased differentiation. Lastly, reestablishing En2 expression in En2‐KO NPCs rescued excess proliferation. These results indicate that En2 functions in hippocampal NPCs by inhibiting proliferation and promoting survival and differentiation in a cell autonomous manner. More broadly, this study suggests that En2 impacts brain structure and function in diverse regions outside of the mid‐hindbrain.
Generation of a new mouse line with conditionally activated signaling through the BMP receptor, ACVR1: A tool to characterize pleiotropic roles of BMP functions
Authors: Yang Jingwen , Toda Nakamura Masako , Hallett Shawn A. , Ueharu Hiroki , Zhang Honghao , Kelley Kristen , Fukuda Tomokazu , Komatsu Yoshihiro , Mishina Yuji 
Published: April 2021

SummaryBMP signaling plays pleiotropic roles in various tissues during embryogenesis and after birth. We have previously generated a constitutively activated Acvr1(ca‐Acvr1) transgenic mouse line (line L35) through pronuclei injection to investigate impacts of enhanced BMP signaling in a tissue specific manner. However, line L35 shows a restricted expression pattern of the transgene. Here, we generated another ca‐Acvr1 transgenic line, line A11, using embryonic stem (ES) transgenesis. The generated line A11 shows distinctive phenotypes from line L35, along with very limited expression levels of the transgene. When the transgene is activated in the neural crest cells in a Cre‐dependent manner, line A11 exhibits cleft palate and shorter jaws, while line L35 develops ectopic cartilages and highly hypomorphic facial structures. When activated in limb buds, line A11 develops organized but smaller limb skeletal structures, while line L35 forms disorganized limbs with little mineralization. Additionally, no heterotopic ossification (HO) is identified in line A11 when bred with NFATc1‐Cre mice even after induction of tissue injury, which is an established protocol for HO for line L35. Therefore, the newly generated conditional ca‐Acvr1 mouse line A11 provides an additional resource to dissect highly context dependent functions of BMP signaling in development and disease.
Politics of flood risk management in Switzerland: Political feasibility of instrument mixes
Authors: Glaus Anik 
Published: April 2021

AbstractComplex environmental problems affect multiple policy sectors, decision‐making levels and territories simultaneously and, as such, call for encompassing policy solutions. However, no consensus exists on how encompassing policy solutions are designed. A trade‐off persists between single instruments, leading to sectoral “silo” thinking and complex instrument mixes, constituting the risk of not being implemented due to actors' objections. Policy designs, including balanced policy mixes, can fulfil various goals, interests and priorities; address numerous challenges; and involve multiple actors. Such balanced policy mixes, however, can only manage complex environmental problems successfully when supported by actors belonging to different sectors, levels and territories. This study therefore analyses the political feasibility of balanced instrument mixes via actors' policy preferences in the case of Swiss flood risk management. Public and private actors involved in flood risk management are surveyed on their preferred instrument mixes. Based on these preference data, the political feasibility of instrument mixes is evaluated by combining the number (density) and coerciveness (intensity) of instruments with the balance of different instrument types (balance) in an index. Results indicate that actors' preferences for a balanced instrument mix are weak. In particular, actors' roles and sectoral interests in the policy design process influence their preferences. These findings suggest that policy mixes, including simple, minimally intervening and sector‐specific flood risk management instruments, are more likely to be politically feasible than balanced instrument mixes. Therefore, traditional “silo” thinking continues to outweigh encompassing policy solutions and impedes possible steps towards an integrated flood risk management approach in Switzerland.
An Isomeric Copper‐Diisophthalate Framework Platform for Storage and Purification of C2H2and Exploration of the Positional Effect of the Methyl Group
Authors: Lin Shengjie , Fan Lihui , Zhou Ping , Xu Tingting , Jiang Zhenzhen , Hu Simin , Chen Jingxian , He Yabing 
Published: April 2021

AbstractThree isostructural metal‐organic frameworks (MOFs) based on dicopper paddlewheels and dimethyl‐functionalized linear diisophthalate ligands were solvothermally constructed, with the aim to investigate their performance regarding acetylene (C2H2) storage as well as separation and purification and to further understand the positional effect of the weakly polarized methyl functionality. Isotherm measurements and IAST selectivity analyses revealed that the three compounds exhibited the promising potential for storing C2H2and recovering C2H2from carbon dioxide (CO2) and methane (CH4) at ambient conditions. Furthermore, their C2H2adsorption properties can be tailored and optimized by altering the relative position of the methyl substituents immobilized in the organic linkers. At 298 K and 1 atm, the C2H2uptake capacities vary from 173.0 to 183.6 cm3 (STP) g−1, while the C2H2/CH4and C2H2/CO2adsorption selectivities are in the range of 24.5–26.6 and 4.34–4.70 for the equimolar gas mixtures. Theortho‐dimethyl‐modified MOF outperformed better than the other two MOF isomers. The results indicate that rational arrangement of functional groups can to some extent improve gas adsorption properties. Although the property discrepancy caused by the less‐polar methyl group is not as large as that by Lewis‐basic nitrogen atoms, this is the first experimental demonstration of the positional effect of methyl group on C2H2adsorption.
The Effect of TCNE and TCNQ Acceptor Units on Triphenylamine‐Naphthalenediimide Push‐Pull Chromophore Properties
Authors: Srinivasa Rao Pedada , Brixi Samantha , Shaikh Dada B. , Al Kobaisi Mohammad , Lessard Benoît H. , Bhosale Sidhanath V. , Bhosale Sheshanath V. 
Published: April 2021

AbstractAsymmetrical and symmetrical push‐pull chromophore‐based on triphenylamine (TPA) donors and naphthalenediimide (NDI) acceptors are designed and successfully synthesized via [2+2] cycloaddition‐retroelectrocyclization (CA‐RE) reaction with well‐known electron‐accepting tetracyanoethylene (TCNE) and 7,7,8,8, ‐tetracyanoquinodimethane (TCNQ) groups. The novel series of compounds NDI‐TPA‐1 to NDI‐TPA‐6 were characterized to identify the influence of the TCNE and TCNQ π‐conjugated linkers on the optical, electrochemical, and electronic properties of these molecules. We found that in dichloromethane the NDI‐TPAs 1, 4, 5, and 6 display absorbance peaks at increasing wavelengths 605, 641, 646, and 645 nm, respectively. We demonstrated that through simple chemical modification we could drop the lowest occupied molecular orbital of NDI‐TPA‐1 to 6. Furthermore, NDI‐TPA‐1 to 6 were integrated into organic thin‐film transistors (OTFTs) via spin‐coating technique, and charge transfer properties were investigated. We found that the choice of the functional group led to either p‐type, n‐type, or ambipolar characteristics.
Formal Aza‐Diels−Alder Reactions of Spiroindolenines with Electronrich Dienes
Authors: Brambilla Elisa , Leoni Sara , Abbiati Giorgio , Pirovano Valentina , Rossi Elisabetta 
Published: April 2021

AbstractSpiroindolenines were employed as cyclic imine substrates in formal aza‐Diels−Alder reactions with Danishefsky's diene or silyloxy‐substituted electron‐rich dienes for the synthesis of the corresponding tetrahydropyrido[1,2‐a]spiroindolinones. The reactions occur under mild conditions in the presence of ytterbium triflate as Lewis acidic catalyst delivering the desired compounds in good yield. The reaction results in the preparation of a small library of a new class of conformational constrained heterocyclic derivatives that easily undergo selective and efficient manipulations.
Assessment of public hospitals performance in Gaza governorates using the Pabón Lasso Model
Authors: Shaqura Iyad Ibrahim , Gholami Masoomeh , Akbari Sari Ali 
Published: April 2021

AbstractBackgroundMeasuring hospital performance can be undertaken in different areas including efficiency, productivity, and quality. Many studies have been conducted using several indicators in this regard.AimThis study aimed at measuring efficiency of obstetrics and gynaecology, and paediatrics departments at the public hospitals affiliated with the Palestinian Ministry of Health in 2016, 2017 and 2018.MethodThis descriptive study includes 12 hospitals; four (A–D) and eight (E–L) providing obstetrics and gynaecology, and paediatrics services, respectively. Data were collected from health annual reports for the 3‐year study period. Pabón Lasso charts were drawn using Microsoft Excel 2013.Results and conclusionDuring the 3 years, hospitals B, D and C lied in zones 3, 1 and 2, respectively. Hospital A was in Zone 4 in 2016 and 2018, but in Zone 1 in 2017. In 2016, hospitals E, F and H were in Zone 3, while, hospitals I, J, K, and L were in Zone 1. In 2017, hospital G shifted from Zone 2 to Zone 3, and backed to Zone 2 in 2018. Hospital L has moved from Zone 1 to Zone 2 in 2018, whereas other hospitals have remained in the same zones. Inefficiency in hospitals provides an important opportunity for addressing the gaps in a quality and less costly manner. Emphasis antenatal care in primary healthcare is important. Further researches are required to cover other types of hospitals through employing frontier techniques of efficiency measurement.
Sub millimetre flexible fibre probe for background and fluorescence free Raman spectroscopy
Authors: Yerolatsitis Stephanos , Kufcsák András , Ehrlich Katjana , Wood Harry A. C. , Fernandes Susan , Quinn Tom , Young Vikki , Young Irene , Hamilton Katie , Akram Ahsan R. , Thomson Robert R. , Finlayson Keith , Dhaliwal Kevin , Stone James M. 
Published: April 2021

AbstractUsing the shifted‐excitation Raman difference spectroscopy technique and an optical fibre featuring a negative curvature excitation core and a coaxial ring of high numerical aperture collection cores, we have developed a portable, background and fluorescence free, endoscopic Raman probe. The probe consists of a single fibre with a diameter of less than 0.25 mm packaged in a sub‐millimetre tubing, making it compatible with standard bronchoscopes. The Raman excitation light in the fibre is guided in air and therefore interacts little with silica, enabling an almost background free transmission of the excitation light. In addition, we used the shifted‐excitation Raman difference spectroscopy technique and a tunable 785 nm laser to separate the fluorescence and the Raman spectrum from highly fluorescent samples, demonstrating the suitability of the probe for biomedical applications. Using this probe we also acquired fluorescence free human lung tissue data.