bluuebunny/crossref_metadata_2025_split huggingface dataset:
RhSe2: A Superior 3D Electrocatalyst with Multiple Active Facets for Hydrogen Evolution Reaction in Both Acid and Alkaline Solutions
Authors: Zhong Wenwu , Xiao Beibei , Lin Zhiping , Wang Zongpeng , Huang Liangai , Shen Shijie , Zhang Qinghua , Gu Lin 
Published: January 2021

AbstractLayered 2D materials are a vital class of electrocatalys for the hydrogen evolution reaction (HER), due to their large area, excellent activity, and facile fabrication. Theoretical caculations domenstrate, however, that only the edges of the 2D nanosheets act as active sites, while the much larger basal plane exhibits passive activity. Here, from a distinguishing perspective, RhSe2 is reported as a “3D” electrocatalyst for HER with top‐class activity, synthesized by a facile solid‐state method. Superior to 2D materials, multiple crystal facets of RhSe2 exhibit near‐zero free energy change of hydrogen adsorption (ΔGH), which guarantees high performance in most common morphologies. Density functional theory calculations reveal that the low‐coordinated Rh atoms act as the active sites in acid, which enables the modified Kubas‐mediated pathway, while the Se atoms act as the active sites in an alkaline medium. The overpotentials of HER activity of RhSe2 are measured to be 49.9 and 81.6 mV at 10 mA cm–2 in acid and alkaline solutions, respectively. This work paves the way to new transition metal chalcogenide catalysts.
Synthesis of Perinaphthenones via BF3.Et2O Mediated One‐Pot Cascade 4,5‐Annulation Reactions of 1‐Naphthols and Ynones
Authors: Kuo Chun‐Wei , Rao Naidu Sambasiva , Patil Prakash Bhimrao , Chiang Ting‐Ta , Kavala Veerababurao , Yao Ching‐Fa 
Published: January 2021

AbstractC4‐C5 periannulation of 1‐naphthols and ynones via BF3.Et2O mediated one‐pot cascade under metal and solvent‐free conditions have been developed for the synthesis of perinaphthenones. Furthermore, this strategy features the formation of new periannulation at C4‐C5 positions of α‐naphthol, synthesis of highly substituted perinaphthenones, broad substrate scope, readily available starting materials and good to moderate yields. The perinaphthenones products synthesized here have exhibited interesting photo physical propertiesmagnified image
Understanding the Outstanding High‐Voltage Performance of NCM523||Graphite Lithium Ion Cells after Elimination of Ethylene Carbonate Solvent from Conventional Electrolyte
Authors: Klein Sven , van Wickeren Stefan , Röser Stephan , Bärmann Peer , Borzutzki Kristina , Heidrich Bastian , Börner Markus , Winter Martin , Placke Tobias , Kasnatscheew Johannes 
Published: January 2021

AbstractThe increase of specific energy of current Li ion batteries via further increase of the cell voltage, for example, to 4.5 V is typically accompanied by a sudden and rapid capacity fade, known as “rollover” failure. This failure is the result of Li dendrite formation triggered in the course of electrode cross‐talk, that is, dissolution of transition metals (TMs) from the cathode and deposition on the anode. It is shown herein, that the elimination of ethylene carbonate (EC) from a state‐of‐the‐art electrolyte, that is, from 1.0 m LiPF6 in a 3:7 mixture of EC and ethyl methyl carbonate prevents this failure in high‐voltage LiNi0.5Co0.2Mn0.3O2||graphite cells, even without any electrolyte additives. While the oxidative stability on the cathode side is similar in both electrolytes, visible by a decomposition plateau at 5.5 V versus Li|Li+ during charge, the anode side in the EC‐free electrolyte reveals significantly less TM deposits and Li metal dendrites compared to the EC‐based electrolyte. The beneficial effect of EC‐free electrolytes is related to a significantly increased amount of degraded LiPF6 species, which effectively trap dissolved TMs and suppress the effect of detrimental cross‐talk, finally realizing rollover‐free performance under high voltage conditions.
Experiments and modeling of bubbles colliding head‐on in water
Authors: Song Runci , Han Luchang , Zhang Ling , Tang Shangyu 
Published: January 2021

AbstractExperiments and modeling of head‐on collision of a pair of bubbles driven by buoyancy in quiescent water are presented. The experiments showed that two bubbles after contacting for a few milliseconds may coalesce or bounce back depending on the collision velocity. As theoretical comparisons, the influence of velocity boundary conditions on the liquid film drainage and the characteristics of two film drainage models with the assumptions of “partially” and fully mobile interfaces under variable‐velocity approach condition are studied. The “partially” mobile model is found to be easier to predict rebound case and longer drainage time, and could not obtain the drainage process where the film is thinned to the thickness below 10−7 m at both low and relatively high Re. As a whole, the fully mobile model with variable‐velocity approach shows more reasonable prediction results for the coalescence and rebound of bubbles in the ultrapure water.
Direct and correlated responses to artificial selection for growth and water‐use efficiency in a Mediterranean pine
Authors: Suárez‐Vidal Estefanía , Sampedro Luis , Climent Jose , Voltas Jordi , Sin Ester , Notivol Eduardo , Zas Rafael 
Published: January 2021

PREMISEPersistence of tree populations in the face of global change relies on their capacity to respond to biotic and abiotic stressors through plastic or adaptive changes. Genetic adaptation will depend on the additive genetic variation within populations and the heritability of traits related to stress tolerance. Because traits can be genetically linked, selective pressure acting on one trait may lead to correlated responses in other traits.METHODSTo test direct and correlated responses to selection for growth and drought tolerance in Pinus halepensis, we selected trees in a parental population for higher growth and greater water‐use efficiency (WUE) and compared their offspring with the offspring of random trees from the parental population in two contrasting common gardens. We estimated direct responses to selection for growth and WUE and correlated responses for growth and tolerance to abiotic and biotic stressors.RESULTSWe found a strong response to selection and high realized heritability for WUE, but no response to selection for growth. Correlated responses to selection in other life‐history traits were not significant, except for concentration of some chemical defenses, which was greater in the offspring of mother trees selected for growth than in the offspring of unselected control trees.CONCLUSIONSThe empirical evidence of direct responses to selection for high WUE suggests that P. halepensis has the potential to evolve in response to increasing drought stress. Contrary to expectations, the results are not conclusive of a potential negative impact of WUE and growth selection on other key life‐history traits.
Patterns of genetic variation in a prairie wildflower, Silphium integrifolium, suggest a non‐prairie origin and locally adaptive variation
Authors: Raduski Andrew R. , Herman Adam , Pogoda Cloe , Dorn Kevin M. , Van Tassel David L. , Kane Nolan , Brandvain Yaniv 
Published: January 2021

PREMISEUnderstanding the relationship between genetic structure and geography provides information about a species’ history and can be used for breeding and conservation goals. The North American prairie is interesting because of its recent origin and subsequent fragmentation. Silphium integrifolium, an iconic perennial American prairie wildflower, is targeted for domestication, having undergone a few generations of improvement. We present the first application of population genetic data in this species to address the following goals: (1) improve breeding by characterizing genetic structure and (2) identify the species geographic origin and potential targets and drivers of selection during range expansion.METHODSWe developed a reference transcriptome as a genotyping reference for samples from throughout the species range. Population genetic analyses were used to describe patterns of genetic variation, and demographic modeling was used to characterize potential processes that shaped variation. Outlier scans for selection and associations with environmental variables were used to identify loci linked to putative targets and drivers of selection.RESULTSGenetic variation partitioned samples into three geographic clusters. Patterns of variation and demographic modeling suggest that the species origin is in the American Southeast. Breeding program accessions are from the region with lowest observed genetic variation.CONCLUSIONSThis prairie species did not originate within the prairie. Breeding may be improved by including accessions from outside of the germplasm founding region. The geographic structuring and the identified targets and drivers of adaptation can guide collecting efforts toward populations with beneficial agronomic traits.
Rheumatoid arthritis in low‐level toluene‐exposed workers based on nationwide medical surveillance data in Korea
Authors: Min Young‐Sun , Lee Sungho , Kim Mingi , Ahn Yeon‐Soon 
Published: January 2021

AbstractBackgroundThere is growing evidence that exposure to organic solvents can play a role in the etiology of rheumatoid arthritis (RA). This prospective cohort study aimed to investigate the association between RA and toluene exposure.MethodsThe study cohort consisted of Korea Occupational Safety and Health Agency data from male workers exposed to toluene who had undergone a toluene‐associated special medical examination at least once between January 1, 2000 and December 31, 2004 (n = 148,870). The morbidity from RA based on hospital admission records was estimated from 2000 to 2005 using National Health Insurance Claim Data. The standardized admission ratio (SAR) for RA was calculated with reference to the general population. Levels of urinary hippuric acid (HA), a metabolite of toluene, were measured and used for exposure assessment.ResultsToluene‐exposed workers were at an elevated risk of seropositive rheumatoid arthritis (ICD‐10 code M05) with an SAR of 2.38 (95% confidence interval [CI]: 1.14–4.37) and other rheumatoid arthritis (M06) with an SAR of 1.22 (95% CI: 0.91–1.59). When data were stratified according to the duration of toluene exposure and by tertiles of urinary HA level, no significant difference was apparent.ConclusionSARs of the toluene‐exposed workers are higher than that of the general reference population, indicating that exposure to toluene may contribute to an increased risk of RA. Further studies of toluene‐exposed workers with longer follow‐up are needed.
Bildungsmechanismen für Phosphoren und SnIP
Authors: Pielmeier Markus R. P. , Nilges Tom 
Published: January 2021

AbstractPhosphoren – das Einzelschichtmaterial des Elementallotrops schwarzer Phosphor (Pblack) – und SnIP sind 2D‐ und 1D‐Halbleiter und können beide über sehr ähnliche Synthesewege, mithilfe von Gasphasentransportreaktion und Mineralisation, aus amorphem rotem Phosphor und Sn/Sn(IV)‐iodid hergestellt werden. Der Top‐down‐Ansatz über Pblack ist heutzutage der wichtigste Zugangsweg zu Phosphoren. Die beiden Reaktionswege unterscheiden sich hauptsächlich in der Reaktionstemperatur und den Stoffmengenverhältnissen der Reaktanten. Bei der Top‐down‐Synthese von Phosphoren aus schwarzem Phosphor wird über mögliche Intermediate oder Nebenphasen (z. B. Hittorfscher Phosphor oder ein Sn24P19.3I8‐Clathrat) spekuliert. Die Bedeutung P‐basierter 2D‐ und 1D‐Materialien für Energiekonvertierung, ‐speicherung und Katalyse inspirierte uns, den Bildungsmechanismus dieser beiden Stoffe genauer zu untersuchen. Hier stellen wir die intermediatfreien Reaktionsmechanismen von Pblack/Phosphoren und SnIP aus P4 und SnI2 mittels direkter Gasphasenbildung vor.
Spin‐elektrische Kopplung in einem Cobalt(II)‐basierten Spindreieck, gezeigt mithilfe elektrisches‐Feld‐modulierter Elektronenspinresonanzspektroskopie
Authors: Kintzel Benjamin , Fittipaldi Maria , Böhme Michael , Cini Alberto , Tesi Lorenzo , Buchholz Axel , Sessoli Roberta , Plass Winfried 
Published: January 2021

AbstractEin Cobalt(II)‐basiertes Spin‐Dreieck zeigt signifikante Spin‐elektrische Kopplung. Der Komplex [Co3(pytag)(py)6Cl3]ClO4⋅3 py kristallisiert in der azentrischen monoklinen Raumgruppe P21. Eine antiferromagnetische Wechselwirkung von ca. −15 cm−1 (H=−JSaSb) führt zu Spinfrustration. Die zu erwartenden zwei energetisch entarteten Grundzustandsdubletts sind jedoch um einige Wellenzahlen voneinander separiert, was aus der magnetischen Anisotropie und Abweichungen von der ideal dreizähligen Symmetrie resultiert. Die Co3‐Ebenen der symmetrieverwandten Moleküle sind nahezu parallel. Das ermöglicht die Untersuchung Spin‐elektrischer Eigenschaften in Einkristallen durch EFM‐ESR‐Spektroskopie. Der Spin‐elektrische Effekt bei Einwirkung des elektrischen Felds in der Co3‐Ebene zeigte sich in einer Verschiebung des Resonanzfelds. Eine Quantifizierung erfolgte als ΔgE/E=0,11×10−9 m V−1, was ca. 0,3 Hz m V−1 entspricht. Dieser Wert ist vergleichbar mit dem in einem Cu3‐Dreieck gefundenen, wenngleich die antiferromagnetische Wechselwirkung in diesem 20‐mal größer ist.
Formation Mechanisms for Phosphorene and SnIP
Authors: Pielmeier Markus R. P. , Nilges Tom 
Published: January 2021

AbstractPhosphorene—the monolayered material of the element allotrope black phosphorus (Pblack)—and SnIP are 2D and 1D semiconductors with intriguing physical properties. Pblack and SnIP have in common that they can be synthesized via short way transport or mineralization using tin, tin(IV) iodide and amorphous red phosphorus. This top‐down approach is the most important access route to phosphorene. The two preparation routes are closely connected and differ mainly in reaction temperature and molar ratios of starting materials. Many speculative intermediates or activator side phases have been postulated especially for top‐down Pblack/phosphorene synthesis, such as Hittorf's phosphorus or Sn24P19.3I8 clathrate. The importance of phosphorus‐based 2D and 1D materials for energy conversion, storage, and catalysis inspired us to elucidate the formation mechanisms of these two compounds. Herein, we report on the reaction mechanisms of Pblack/phosphorene and SnIP from P4 and SnI2 via direct gas phase formation.
Advances in high‐resolution mass spectrometry applied to pharmaceuticals in 2020: A whole new age of information
Authors: Géhin Caroline , Holman Stephen W. 
Published: January 2021

AbstractContinuous improvements in mass spectrometry (MS) have resulted in the widespread availability and adoption of high‐resolution mass spectrometry (HRMS) across laboratories worldwide. The capabilities and the associated advantages of HRMS make it an invaluable analytical tool for analyte characterization, screening, and quantification methodologies for a wide scope of applications across pharmaceutical development. These applications include drug discovery, product characterizations of both small molecules and novel drug modalities,in vitroandin vivometabolism studies, post‐approval quality control, and pharmacovigilance. This review gives an overview of the current capabilities of HRMS and its pharmaceutical applications in 2020, and provides a perspective on the future of HRMS within the pharmaceutical industry.
Black hole mass, jet, and accretion disk connection: An analysis of radio‐loud and radio‐quiet quasars
Authors: Chakraborty Avinanda , Bhattacharjee Anirban 
Published: January 2021

AbstractSurveys have shown radio‐loud (RL) quasars constitute 10–15% of the total quasar population. However, it is unknown if the radio‐loud fraction (RL quasars/Total quasars) remains consistent among different parameter spaces. This study shows that radio‐loud fraction increases for increasing full width half maximum (FWHM) velocity of the Hβ and MgII broad emission line. Our data have been obtained from Shen, Y., Richards, G. T., Strauss, M. A. et al., ApJS, 194(2), 45, 2011 catalogue. To investigate the reason, in this preliminary study we analyze various properties like bolometric luminosity, optical continuum luminosity, black hole (BH) mass, and accretion rate of RL quasars and RQ quasars sample which have FWHM greater than 15,000 km s−1 (High broad line). From the distributions, we can conclude for all the properties in high broad line, RL quasars are having higher values than RQ quasars. We have predicted RL quasars are intrinsically brighter than RQ quasars and also predicted BH mass‐jet connection and accretion disk‐jet connection from our results but to conclude anything more analysis is needed.
Which is preferred for initial treatment of papillary thyroid cancer, total thyroidectomy or lobotomy?
Authors: Wu Zhen , Han Lin , Li Wenlei , Wang Wei , Chen Liqaing , Yao Yumin , Wang Yongkun 
Published: January 2021

AbstractPurposesThe incidence of thyroid cancer has increased annually, and has a heavy psychological and economic burden on society and individuals. Based thyroid cancer data from patients treated in Liaocheng People's Hospital from 2015 to 2018, with Chinese national and regional characteristics, in this study, we addressed the controversy of which initial thyroid surgical mode, lobectomy or total thyroidectomy, is most effective.MethodsClinical and pathological data from 2108 patients with thyroid cancer, who were initially diagnosed and treated surgically, were collected from the Department of Thyroid Surgery. Among them, there were 1001 cases who underwent open operation with total thyroidectomy + central lymph node dissection; meanwhile, 1107 cases were treated with neck lateral lymph node dissection at the same time.ResultsThe overall metastasis rate of all patients was 57.23%. Even the lymph node metastasis of papillary thyroid microcarcinoma (PTMC) was as high as 48.97%. When the mass rose above 2 cm, the proportion of metastasis increased to 77.22%. When the tumor was complicated with bilateral and multiple high‐risk factors, the proportion of metastasis was 65.27% and 72.21%, respectively. When the tumor breaks through the capsule, the metastasis rate was 67.08%. With the increase of tumor diameter, the metastasis of cervical lymph nodes ranged from 22.54% to 73.33%, which showed positive correlation. 49.32% of patients had lymph node metastasis in the lateral cervical region. When the diameter of the tumor reached T1c level, the metastasis of the cervical lymph nodes was 56.91%, and the number of metastatic cases above T1c level accounted for 69.96% of the total metastatic cases.ConclusionThe degree of malignancy of thyroid cancer depends on tumor genome evolution. Rates of neck lymph node metastasis are high, particularly among patients with risk factors for poor prognosis. It is recommended that initial treatment should comprise at least total thyroidectomy + central lymph node dissection in China, to avoid the risks associated with secondary surgery and effects on patient quality of life. When the tumor diameter exceeds 1 cm, the risk of cervical lymph node metastasis is high, and we recommended lateral lymph node dissection.
Rational Design and Synthesis of Selective PRMT4 Inhibitors: A New Chemotype for Development of Cancer Therapeutics**
Authors: Sutherland Mathew , Li Alice , Kaghad Anissa , Panagopoulos Dimitrios , Li Fengling , Szewczyk Magdalena , Smil David , Scholten Cora , Bouché Léa , Stellfeld Timo , Arrowsmith Cheryl H. , Barsyte Dalia , Vedadi Masoud , Hartung Ingo V. , Steuber Holger , Britton Robert , Santhakumar Vijayaratnam 
Published: January 2021

AbstractProtein arginine N‐methyl transferase 4 (PRMT4) asymmetrically dimethylates the arginine residues of histone H3 and nonhistone proteins. The overexpression of PRMT4 in several cancers has stimulated interest in the discovery of inhibitors as biological tools and, potentially, therapeutics. Although several PRMT4 inhibitors have been reported, most display poor selectivity against other members of the PRMT family of methyl transferases. Herein, we report the structure‐based design of a new class of alanine‐containing 3‐arylindoles as potent and selective PRMT4 inhibitors, and describe key structure–activity relationships for this class of compounds.
Ternary Cocrystals with Large Soft Cavities: A 1,4‐diiodotetrafluorobenzene (DITFB)⋅4‐Biphenylpyridine N‐oxide (BPNO) Host Assembled by Inclusion of Planar Aromatic Guests
Authors: Liang Wen Juan , Wang Hui , Chen Xue , Zhang Ting Ting , Bai Yun Feng , Feng Feng , Jin Wei Jun 
Published: January 2021

AbstractA large soft‐cavity host composed of 1,4‐diiodotetrafluorobenzene (DITFB) and 4‐biphenylpyridine N‐oxide (BPNO) is assembled under the mediation of a planar aromatic guest molecule (pyrene or perylene) through C−I⋅⋅⋅−O−N+ halogen bonds and π‐hole⋅⋅⋅π bonds. Single‐crystal X‐ray diffraction reveals that guest molecules can be completely encapsulated in the four‐layer host cavity to assemble ternary host‐guest cocrystals; namely, Pyr@DITFB ⋅ BPNO and Per@DITFB ⋅ BPNO. The luminescence of these ternary cocrystals originates from their discrete guest molecules, which exhibit pure‐blue and yellow emissions, respectively, that are localized at 425 nm and in the range of 485 to 578 nm, respectively. In addition, the contribution of different fragments to the stabilization of the crystal structure is estimated by computational chemistry. These cocrystals have significant potential for use in optical applications or materials, such as photonics or organic light‐emitting diodes, respectively, that require to avoid the aggregation between luminophores.
Löwdin's symmetry dilemma within Green functions theory for the one‐dimensional Hubbard model
Authors: Joost J.‐P. , Schlünzen N. , Hese S. , Bonitz M. , Verdozzi C. , Schmitteckert P. , Hopjan M. 
Published: January 2021

AbstractThe energy gap of correlated Hubbard clusters is well studied for one‐dimensional systems using analytical methods and density‐matrix‐renormalization‐group (DMRG) simulations. Beyond 1D, however, exact results are available only for small systems by quantum Monte Carlo. For this reason and, due to the problems of DMRG in simulating 2D and 3D systems, alternative methods such as Green functions combined with many‐body approximations (GFMBA), that do not have this restriction, are highly important. However, it has remained open whether the approximate character of GFMBA simulations prevents the computation of the Hubbard gap. Here we present new GFMBA results that demonstrate that GFMBA simulations are capable of producing reliable data for the gap which agrees well with the DMRG benchmarks in 1D. An interesting observation is that the accuracy of the gap can be significantly increased when the simulations give up certain symmetry restriction of the exact system, such as spin symmetry and spatial homogeneity. This is seen as manifestation and generalization of the “symmetry dilemma” introduced by Löwdin for Hartree–Fock wave function calculations.