bluuebunny/crossref_metadata_2025_split huggingface dataset:
Acceptorless Dehydrogenative Coupling Reactions by Manganese Pincer Complexes
Authors: Nad Pinaki , Mukherjee Arup 
Published: May 2021

AbstractAcceptorless dehydrogenative coupling reactions has emerged as one of the promising technique in synthetic organic chemistry to construct carbon‐carbon and carbon‐heteroatom bonds in an environmentally benign and sustainable way. The methodology is highly atom economical and produces water and hydrogen as the byproducts. This protocol, coupled with the earth‐abundant and less toxic manganese catalyst provides a unique opportunity to construct various synthons and biologically important motifs. In recent years, tremendous progress has been made with manganese catalysis based on the pincer ligands for various homogeneous transformations. This review covers the recent progress in the field of manganese catalyzed acceptorless dehydrogenative coupling reactions, their scope and brief mechanistic discussion.
One‐pot Synthesis of 3‐Acylsilane‐Substituted Isoquinolines via Rhodium (III)‐Catalyzed C−H Activation/Annulation of O‐pivaloyl Oximes With Acryloylsilanes
Authors: Yang Zengbao , Zhou Hui , He Maoyao , Li Jianglian , Yang Zhongzhen , Wu Yong 
Published: May 2021

AbstractA protocol realized by rhodium‐catalyzed C−H functionalization of O‐pivaloyl oximes with acryloylsilane was developed for synthesis of highly functionalized 3‐acylsilane‐substituted isoquinolines. This reaction features mild condition, broad substrate tolerance, operational simplicity and excellent chemoselectivity. Furthermore, 3‐acylsilane‐substituted isoquinoline cores could be further modificated and have important application potential in organic synthesis.
Total Synthesis of Taiwaniaquinoids: A Strategic Account
Authors: Graham Marlowe S. , McErlean Christopher S. P. 
Published: May 2021

AbstractDue to their novel architectures and promising biological activities, the family of taiwaniaquinoid natural products continues to capture the attention of synthetic chemists. This mini‐review highlights recent advances in the total synthesis of taiwaniaquinoids, with a focus on the overarching synthetic strategies that have been employed to access the structural and stereochemical diversity that exists among these plant secondary metabolites.
Copper‐Catalyzed Oxidative C−C Cleavage of Carbohydrates: An Efficient Access to Quinazolinone Scaffolds
Authors: Philips Abigail , Raja Dineshkumar , Arumugam Ajithkumar , Lin Wei‐Yu , Chandru Senadi Gopal 
Published: May 2021

AbstractA copper‐catalyzed oxidative coupling strategy has been developed for the synthesis of 4(3H)‐quinazolinones and benzoimidazoquinazoline using glucose as renewable C1 synthon. Isotope labelling studies using 13C6 D‐glucose and DMSO‐d6 confirmed the role of D‐glucose as C1 source. The significant features of this method include (i) utilization of 0.25 to 0.5 equiv., of D‐glucose as a multi‐C1 synthon; (ii) biomass‐derived platform chemical as carbon synthon; (iii) atom‐economical and benign conditions and; (iv) synthesis of naturally occurring alkaloid and precursor.
Polygenic Risk Score for Alzheimer's Disease in Caribbean Hispanics
Authors: Sariya Sanjeev , Felsky Daniel , Reyes‐Dumeyer Dolly , Lali Ricky , Lantigua Rafael A. , Vardarajan Badri , Jiménez‐Velázquez Ivonne Z. , Haines Jonathan L. , Shellenberg Gerard D. , Pericak‐Vance Margaret A , Paré Guillaume , Mayeux Richard , Tosto Giuseppe 
Published: May 2021

ObjectivePolygenic risk scores (PRSs) assess the individual genetic propensity to a condition by combining sparse information scattered across genetic loci, often displaying small effect sizes. Most PRSs are constructed in European‐ancestry populations, limiting their use in other ethnicities. Here we constructed and validated a PRS for late‐onset Alzheimer's Disease (LOAD) in Caribbean Hispanics (CH).MethodsWe used a CH discovery (n = 4,312) and independent validation sample (n = 1,850) to construct an ancestry‐specific PRS (“CH‐PRS”) and evaluated its performance alone and with other predictors using the area under curve (AUC) and logistic regression (strength of association with LOAD and statistical significance). We tested if CH‐PRS predicted conversion to LOAD in a subsample with longitudinal data (n = 1,239). We also tested the CH‐PRS in an independent replication CH cohort (n = 200) and brain autopsy cohort (n = 33). Finally, we tested the effect of ancestry on PRS by using European and African American discovery cohorts to construct alternative PRSs (“EUR‐PRS”, “AA‐PRS”).ResultsThe full model (LOAD ~ CH‐PRS + sex + age + APOE‐ɛ4), achieved an AUC = 74% (ORCH‐PRS = 1.51 95%CI = 1.36–1.68), raising to >75% inAPOE‐ɛ4non‐carriers. CH‐PRS alone achieved an AUC = 72% in the autopsy cohort, raising to AUC = 83% in full model. Higher CH‐PRS was significantly associated with clinical LOAD in the replication CH cohort (OR = 1.61, 95%CI = 1.19–2.17) and significantly predicted conversion to LOAD (HR = 1.93, CI = 1.70–2.20) in the longitudinal subsample. EUR‐PRS and AA‐PRS reached lower prediction accuracy (AUC = 58% and 53%, respectively).InterpretationEnriching diversity in genetic studies is critical to provide an effective PRS in profiling LOAD risk across populations. ANN NEUROL 2021;90:366–376
Hypsochromic Shift of Multiple‐Resonance‐Induced Thermally Activated Delayed Fluorescence by Oxygen Atom Incorporation
Authors: Tanaka Hiroyuki , Oda Susumu , Ricci Gaetano , Gotoh Hajime , Tabata Keita , Kawasumi Ryosuke , Beljonne David , Olivier Yoann , Hatakeyama Takuji 
Published: May 2021

AbstractHerein, we reported an ultrapure blue multiple‐resonance‐induced thermally activated delayed fluorescence (MR‐TADF) material (ν‐DABNA‐O‐Me) with a high photoluminescence quantum yield and a large rate constant for reverse intersystem crossing. Because of restricted π‐conjugation of the HOMO rather than the LUMO induced by oxygen atom incorporation, ν‐DABNA‐O‐Me shows a hypsochromic shift compared to the parent MR‐TADF material (ν‐DABNA). An organic light‐emitting diode based on this material exhibits an emission at 465 nm, with a small full‐width at half‐maximum of 23 nm and Commission Internationale de l'Eclairage coordinates of (0.13, 0.10), and a high maximum external quantum efficiency of 29.5 %. Moreover, ν‐DABNA‐O‐Me facilitates a drastically improved efficiency roll‐off and a device lifetime compared to ν‐DABNA, which demonstrates significant potential of the oxygen atom incorporation strategy.
Simultaneous Regulation on Solvation Shell and Electrode Interface for Dendrite‐Free Zn Ion Batteries Achieved by a Low‐Cost Glucose Additive
Authors: Sun Peng , Ma Liang , Zhou Wanhai , Qiu Meijia , Wang Zilong , Chao Dongliang , Mai Wenjie 
Published: May 2021

AbstractDendrite growth and by‐products in Zn metal aqueous batteries have impeded their development as promising energy storage devices. We utilize a low‐cost additive, glucose, to modulate the typical ZnSO4 electrolyte system for improving reversible plating/stripping on Zn anode for high‐performance Zn ion batteries (ZIBs). Combing experimental characterizations and theoretical calculations, we show that the glucose in ZnSO4 aqueous environment can simultaneously modulate solvation structure of Zn2+ and Zn anode‐electrolyte interface. The electrolyte engineering can alternate one H2O molecule from the primary Zn2+‐6H2O solvation shell and restraining side reactions due to the decomposition of active water. Concomitantly, glucose molecules are inclined to absorb on the surface of Zn anode, suppressing the random growth of Zn dendrite. As a proof of concept, a symmetric cell and Zn‐MnO2 full cell with glucose electrolyte achieve boosted stability than that with pure ZnSO4 electrolyte.
Catalytic Asymmetric Aza‐Diels–Alder Reaction of Ketimines and Unactivated Dienes
Authors: Zhao Qun , Li Yao , Zhang Qing‐Xia , Cheng Jin‐Pei , Li Xin 
Published: May 2021

AbstractThe enantioselective aza‐Diels–Alder reaction is efficient for constructing chiral tetrahydropyridines, but the catalytic asymmetric aza‐Diels–Alder reaction of ketimines with unactivated dienes is still a challenging topic. Herein, guided by computational screening, a highly enantioselective aza‐Diels–Alder reaction of 2‐aryl‐3H‐indol‐3‐ones with unactivated dienes was realized by using a B(C6F5)3/chiral phosphoric acid catalyst system under mild conditions. The reaction has a broad scope with respect to both aza‐Diels–Alder reaction partners and hence offers rapid access to an array of tetrahydropyridine derivatives with pretty outcomes (up to 99 % yield, >20:1 dr and 98:2 er). The reaction is very efficient: lowering catalyst loadings for the model reaction to 0.1 mol %, enantioselectivity is still maintained. The synthetic utility was confirmed by transformations of the products. DFT calculations provide convincing evidence for the interpretation of stereoselection.
A 2D Graphitic‐Polytriaminopyrimidine (g‐PTAP)/Poly(ether‐block‐amide) Mixed Matrix Membrane for CO2 Separation
Authors: Asim Mohd , Khan Abuzar , Helal Aasif , Alshitari Wael , Akbar Usman A. , Khan Mohd Yusuf 
Published: May 2021

AbstractPoly(ether‐block‐amide)/g‐PTAP mixed matrix membranes (MMMs) were developed by incorporating different wt.% (1–10%) of a novel 2D g‐PTAP nanofiller and its effects on membrane structure and gas permeability were studied. The novel 2D material g‐PTAP was synthesized and characterized by various analytical techniques including field‐emission scanning electron microscopy (FESEM), X‐ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC) and Raman spectroscopy. The fabricated MMMs were investigated to study the interaction and compatibility between Pebax and g‐PTAP. The MMMs showed an effective integration of g‐PTAP nanofiller into the Pebax matrix without affecting its thermal stability. Gas permeation experiments with MMMs showed improved CO2 permeability and selectivity (CO2/N2) upon incorporation of g‐PTAP in the Pebax polymer matrix. The maximum CO2 permeability enhancement from 82.3 to 154.6 Barrer with highest CO2/N2 selectivity from 49.5 to 83.5 were found with 2.5 wt.% of nanofiller compared to neat Pebax membranes.
Statistical characteristics of Arctic forecast busts and their relationship to Arctic weather patterns in summer
Authors: Yamagami Akio , Matsueda Mio 
Published: May 2021

AbstractRecently, human activity in the Arctic region, such as trans‐Arctic shipping, has increased due to the reduction in Arctic sea ice. Accurate weather forecasts will become increasingly important as the level of human activity in the Arctic continues to increase. Operational numerical weather predictions (NWPs) have been improved considerably over recent decades; however, they still occasionally generate large forecast errors referred to as “forecast busts.” This study investigates forecast busts over the Arctic between 2008 and 2019 using operational forecasts from five leading NWP centers. Forecasts with an anomaly correlation coefficient below its climatological 10th percentile, and a root‐mean‐square error above its 90th percentile at a lead time of 144 hr, are regarded as “busts.” The occurrence frequency of forecast busts decreased from 2008 (13–7%) to 2012 and was between 2 and 6% for the period 2012–2019. Arctic forecast busts were most frequent in the May and July–September periods (~6 to 7%), but less frequent between December and March (~4%). The summertime forecast bust occurred more frequently when the initial pattern was the Greenland Blocking (GB) or Arctic Cyclone (AC) pattern rather than one of the other patterns. Some busts occurred without the weather pattern transition (~22 to 40%), but the others occurred with the pattern transition. These results help users to be careful when they use the forecasts initialized on GB and AC patterns.
Using technology to improve the management of development impacts on biodiversity
Authors: White Thomas B. , Viana Leonardo R. , Campbell Geneviève , Elverum Claire , Bennun Leon A. 
Published: May 2021

AbstractThe mitigation hierarchy (MH) is a prominent tool to help businesses achieve no net loss or net gain outcomes for biodiversity. Technological innovations offer benefits for business biodiversity management, yet the range and continued evolution of technologies creates a complex landscape that can be difficult to navigate. Using literature review, online surveys, and semi‐structured interviews, we assess technologies that can improve application of the MH. We identify six categories (mobile survey, fixed survey, remote sensing, blockchain, data analysis, and enabling technologies) with high feasibility and/or relevance to (i) aid direct implementation of mitigation measures and (ii) enhance biodiversity surveys and monitoring, which feed into the design of interventions including avoidance and minimization measures. At the interface between development and biodiversity impacts, opportunities lie in businesses investing in technologies, capitalizing on synergies between technology groups, collaborating with conservation organizations to enhance institutional capacity, and developing practical solutions suited for widespread use.
Green apparel buying behaviour: A Stimulus–Organism–Behaviour–Consequence (SOBC) perspective on sustainability‐oriented consumption in Japan
Authors: Dhir Amandeep , Talwar Shalini , Sadiq Mohd , Sakashita Mototaka , Kaur Puneet 
Published: May 2021

AbstractThe green apparel literature has previously examined the disparity between consumers' positive purchase intentions and their actual purchase behaviour. This dichotomous behaviour represents the critical ‘intention–behaviour gap’, which marketers must seek to reduce to increase sales of their products. The current study thus seeks to identify the drivers of green apparel purchase behaviour that may potentially mitigate this gap. The proposed conceptual model is grounded in the Stimulus–Organism–Behaviour–Consequence (SOBC) paradigm and is tested through an analysis of cross‐sectional data collected from 387 green apparel product consumers in Japan who were sourced through Macromill Inc. The findings suggest that optimism as the stimulus is positively associated with labelling satisfaction and labelling desire, which, in turn, are positively associated with purchase intentions, representing behaviour. Furthermore, purchase intentions are positively associated with shopping routine and fully mediate the association between shopping routine and buying behaviour. The study provides interesting strategic inputs for green apparel marketers and retailers.
Nested relationships in pro‐environmental purchasing: A moderated mediation model
Authors: Delistavrou Antonia , Tilikidou Irene , Krystallis Athanasios 
Published: May 2021

AbstractThis paper presents the examination of a particular theoretical framework that incorporated the moderating role of demographics in a mediated by negative attitudes relationship between values and pro‐environmental behaviour. The hypothesised hierarchical impact of Universalism (Un) on pro‐environmental purchasing behaviour (PPB) through the mediation of environmental unconcern (EU) was verified, while age was found to moderate the relationship between attitudes and behaviour. Yet, a clear generational effect was indicated as younger consumers (less than 35 years old), who are less inhibited by environmental unconcern, are more likely to get engaged in PPB than their older counterparts are. The verification of this particular theoretical framework revealed nested, not apparent, aspects of the grid of PPB antecedents. It is implied that the overall effort towards PPB should start by inculcating self‐transcendence values in young people's minds and continue by acknowledging, understanding and facing their unconcern tendency instead of just reporting some alleged direct motives towards PPB.
Cascade Electrochemical Reduction of Carbon Dioxide with Bimetallic Nanowire and Foam Electrodes
Authors: Zhang Benjamin A. , Nocera Daniel G. 
Published: May 2021

AbstractCascade electrochemical reduction of CO2 has been investigated on nanostructured bimetallic gold‐copper and silver‐copper catalyst nanowire and foam electrode arrays. The bimetallic electrocatalysts allow for the overall carbon dioxide reduction reaction (CO2RR) to be performed, where CO2 to CO conversion occurring at silver (Ag) or gold (Au) is decoupled from conversion to multicarbon species at Cu. The catalyst fabrication methods permit the catalyst orientation to be controlled and thus investigation of catalyst order on the cascade process. Segmentation of bimetallic electrodes is most versatile for nanofoam arrays. Placement of an Ag foam beneath a Cu foam, where CO produced at Ag must pass through the Cu foam, results in an enhancement in methane, ethanol, and propanol production as compared to the reverse electrocatalyst ordering.
Aurophilic Interactions in Multi‐Radical Species: Electronic‐Spin and Redox Properties of Bis‐ and Tris‐[(Nitronyl Nitroxide)‐Gold(I)] Complexes with Phosphine‐Ligand Scaffolds
Authors: Kira Sayaka , Miyamae Takayuki , Yoshida Kohei , Kanzaki Yuki , Sugisaki Kenji , Shiomi Daisuke , Sato Kazunobu , Takui Takeji , Suzuki Shuichi , Kozaki Masatoshi , Okada Keiji 
Published: May 2021

AbstractMultinuclear AuIcomplexes with two or three nitronyl nitroxide‐2‐ide radical anion and phosphine‐ligand scaffolds,(NN‐Au)2‐1 o,(NN‐Au)2‐1 m, and(NN‐Au)2‐1 p, have been synthesized to investigate the influence of AuI−AuI(aurophilic) interactions on the properties of multispin molecular systems. The desired complexes were successfully prepared in moderate yields in a one‐pot synthesis from the corresponding phosphine ligand, AuIsource, parent NN, and sodium hydroxide. Among the prepared complexes,(NN‐Au)2‐1 o, in which an aurophilic interaction was clearly observed by crystal structure analysis, showed characteristic spin−spin interactions, electrochemical properties, and solvatochromic behavior. The results from theoretical calculations also suggested that the differences in properties between complex(NN‐Au)2‐1 oand the other complexes are due to intramolecular aurophilic interactions.
FAM‐Ag‐catalyzed asymmetric synthesis of heteroaryl‐substituted pyrrolidines
Authors: Beksultanova Nurzhan , Gözükara Zeynep , Araz Mihrimah , Bulut Merve , Polat‐Çakır Sıdıka , Aygün Muhittin , Dogan Özdemir 
Published: May 2021

AbstractNew derivatives of FAM (ferrocenyl aziridinyl methanol) ligands NFAM1–4 (naphthyl ferrocenyl aziridinyl methanol) and CFAM1–4 (cyclohexyl ferrocenyl aziridinyl methanol) were synthesized to form a small ligand library and used as chiral catalysts with AgOAc for the asymmetric synthesis of heteroaryl‐substituted pyrrolidines by the 1,3‐dipolar cycloaddition (1,3‐DC) reaction of azomethine ylides. 2‐Thienyl, 2‐furyl, 2‐, 3‐, and 4‐pyridyl aldimines were prepared and used with N‐methylmaleimide, dimethyl maleate, tert‐butyl acrylate, methyl acrylate, and acrylonitrile to form the corresponding heteroaryl‐substituted pyrrolidines. 1,3‐DC reactions yielded the expected cycloadducts in up to 89% yield and up to 76% ee that could be increased up to 95% ee upon crystallization. New chiral ligands NFAM1–4 and CFAM1–4 were fully characterized, and their absolute stereochemistry was determined by single‐crystal X‐ray analysis.
Electrochemically deposited silver nanostructures for use as surface‐enhanced Raman scattering (SERS) substrates in point‐of‐need diagnostic devices
Authors: Wilson Nicholas G. , Khademi Mahmoud , Docoslis Aristides 
Published: May 2021

AbstractIn a world that increasingly demands answers in real‐time, there exists a distinct need for chemical sensors that can quickly and efficiently detect substances with high sensitivity and selectivity. To address this need, we use surface‐enhanced Raman scattering (SERS) as a powerful analytical technique that can provide ultrasensitive and versatile chemical detection on a mobile platform when implemented on a handheld Raman spectrometer. However, the large laser spot size of handheld Raman spectrometers requires SERS substrates of sufficient surface area. Here, we present a facile method for electrodepositing nanostructured silver (Ag) SERS substrates onto silicon microchips. In this method, silver ions are continuously reduced from a large volume of solution in an apparatus resembling a batch electrochemical reactor. The straightforward protocol is scalable, fast, and reproducible. Further, we investigate the influence of temperature and fluid agitation on the growth of Ag nanostructures with the intention of maximizing surface area coverage. We observe an increase in lateral nanostructure growth from heating due to an increase in the diffusion coefficient. However, no significant increase in lateral nanostructure growth is observed from stirring the reagent solution. Despite the absence of trends in lateral growth, we find that high agitation levels promote the growth of extraneous Ag structures on top of the nanostructured film, indicating the presence of a boundary layer at the silicon surface. Further, we find that increased diffusion rates at high temperatures shift the reaction towards the limits of the mass transfer‐controlled regime.
Progressive tricuspid regurgitation and elevated pressure gradient after transvenous permanent pacemaker implantation
Authors: Lee Wei‐Chieh , Fang Hsiu‐Yu , Chen Huang‐Chung , Chen Yung‐Lung , Tsai Tzu‐Hsien , Pan Kuo‐Li , Lin Yu‐Sheng , Liu Wen‐Hao , Chen Mien‐Cheng 
Published: May 2021

AbstractBackgroundThe association of postimplant tricuspid regurgitation (TR) and heart failure (HF) hospitalization in patients without HF and preexisting abnormal TR and TR pressure gradient (PG) remain unclear.HypothesisThis study aimed to explore the clinical outcomes of progressive postimplant TR after permanent pacemaker (PPM) implantation.MethodsA total of 1670 patients who underwent a single ventricular or dual‐chamber transvenous PPM implantation at our hospital between January 2003 and December 2017 were included in the study. Patients with prior valvular surgery, history of HF, and baseline abnormal TR and TRPG were excluded. Finally, a total of 1075 patients were enrolled in this study. Progressive TR was defined as increased TR grade of ≥2 degrees and TRPG of >30 mmHg after implant.ResultsIn 198 (18.4%) patients (group 1) experienced progressive postimplant TR and elevated TRPG, whereas 877 patients (group 2) did not have progressive postimplant TR. Group 1 had larger change in postimplant TRPG (group 1 vs. group 2; 12.8 ± 9.6 mmHg vs. 1.1 ± 7.6 mmHg; p < .001) than group 2. Group 1 had a higher incidence of HF hospitalization compared to group 2 (13.6% vs. 4.7%; p < .001). Preimplant TRPG (HR: 1.075; 95% confidence interval [CI]: 1.032–1.121; p = .001) was an independent predictor of progressive postimplant TR.ConclusionsAfter a transvenous ventricular‐based PPM implantation, 18.4% of patients experienced progressive postimplant TR and elevated TRPG. Higher preimplant TRPG was an independent predictor of progressive postimplant TR.
QoS‐aware big service composition using distributed co‐evolutionary algorithm
Authors: Dutta Avik , Jatoth Chandrashekar , Gangadharan G. R. , Fiore Ugo 
Published: May 2021

AbstractBig services are collections of interrelated web services across virtual and physical domains, processing Big Data. Existing service selection and composition algorithms fail to achieve the global optimum solution in a reasonable time. In this paper, we design an efficient quality of service‐aware big service composition methodology using a distributed co‐evolutionary algorithm. In our proposed model, we develop a distributed NSGA‐III for finding the optimal Pareto front and a distributed multi‐objective Jaya algorithm for enhancing the diversity of solutions. The distributed co‐evolutionary algorithm finds the near‐optimal solution in a fast and scalable way.