bluuebunny/crossref_metadata_2025_split huggingface dataset:
Disentangling the neurobiological bases of temporal impulsivity in Huntington's disease
Authors: Pardina‐Torner Helena , De Paepe Audrey E. , Garcia‐Gorro Clara , Rodriguez‐Dechicha Nadia , Vaquer Irene , Calopa Matilde , Ruiz‐Idiago Jesus , Mareca Celia , de Diego‐Balaguer Ruth , Camara Estela 
Published: March 2024

AbstractBackgroundDespite its impact on daily life, impulsivity in Huntington's disease (HD) is understudied as a neuropsychiatric symptom. Our aim is to characterize temporal impulsivity in HD and to disentangle the white matter correlate associated with impulsivity.MethodsForty‐seven HD individuals and 36 healthy controls were scanned and evaluated for temporal impulsivity using a delay‐discounting (DD) task and complementary Sensitivity to Punishment and Sensitivity to Reward Questionnaire. Diffusion tensor imaging was employed to characterize the structural connectivity of three limbic tracts: the uncinate fasciculus (UF), the accumbofrontal tract (NAcc‐OFC), and the dorsolateral prefrontal cortex connectig the caudate nucleus (DLPFC‐cn). Multiple linear regression analyses were applied to analyze the relationship between impulsive behavior and white matter microstructural integrity.ResultsOur results revealed altered structural connectivity in the DLPC‐cn, the NAcc‐OFC and the UF in HD individuals. At the same time, the variability in structural connectivity of these tracts was associated with the individual differences in temporal impulsivity. Specifically, increased structural connectivity in the right NAcc‐OFC and reduced connectivity in the left UF were associated with higher temporal impulsivity scores.ConclusionsThe present findings highlight the importance of investigating the spectrum of temporal impulsivity in HD. As, while less prevalent than other psychiatric features, this symptom is still reported to significantly impact the quality of life of patients and caregivers. This study provides evidence that individual differences observed in temporal impulsivity may be explained by variability in limbic frontostriatal tracts, while shedding light on the role of sensitivity to reward in modulating impulsive behavior through the selection of immediate rewards.
Identification of a 2‐Aminobenzimidazole Scaffold that Potentiates Gram‐Positive Selective Antibiotics Against Gram‐Negative Bacteria
Authors: Nemeth Ansley M. , Young Milah M. , Melander Roberta J. , Smith Richard D. , Ernst Robert K. , Melander Christian 
Published: March 2024

AbstractThe development of novel therapeutic approaches is crucial in the fight against multi‐drug resistant (MDR) bacteria, particularly gram‐negative species. Small molecule adjuvants that enhance the activity of otherwise gram‐positive selective antibiotics against gram‐negative bacteria have the potential to expand current treatment options. We have previously reported adjuvants based upon a 2‐aminoimidazole (2‐AI) scaffold that potentiate macrolide antibiotics against several gram‐negative pathogens. Herein, we report the discovery and structure‐activity relationship (SAR) investigation of an additional class of macrolide adjuvants based upon a 2‐aminobenzimidazole (2‐ABI) scaffold. The lead compound lowers the minimum inhibitory concentration (MIC) of clarithromycin (CLR) from 512 to 2 μg/mL at 30 μM against Klebsiella pneumoniae 2146, and from 32 to 2 μg/mL at 5 μM, against Acinetobacter baumannii 5075. Preliminary investigation into the mechanism of action suggests that the compounds are binding to lipopolysaccharide (LPS) in K. pneumoniae, and modulating lipooligosaccharide (LOS) biosynthesis, assembly, or transport in A. baumannii.
Right disc thrombosis of the new Gore Cardioform ASD Occluder
Authors: Oliva Omar A. , Giugno Luca , Moroni Alice , Sturla Francesco , Piazza Luciane , Saracino Antonio , Micheletti Angelo , d'Aiello Angelo Fabio , Reali Matteo , Chessa Massimo , Carminati Mario 
Published: March 2024

AbstractBackgroundThe GCA is a well performing device in terms of efficacy despite complex anatomies (aortic rim <5 mm and ASD diameter >17 mm) with a good safety profile.AimsTo evaluate atrial septal defect (ASD) features impacting on right disc device thrombosis in patients who underwent Gore Cardioform ASD Occluder (GCA) implantation.MethodsA total of 44 consecutive patients undergoing percutaneous ASD with GCA device from January 2020 to September 2022 at our tertiary care Center were evaluated. The minimum follow‐up was 6 months.ResultsThe patients were stratified in two groups according to a cut‐off value of ASD diameter equal to 20 mm at sizing balloon, derived from ROC analysis (AUC = 0.894; p = 0.024). Baseline characteristics were comparable between groups in terms of age, sex, weight, height, and interatrial septum dimensions. Patients with ASD > 20 mm (n = 9) had a higher ASD/device dimension ratio, both at echocardiography (p = 0.009) and at sizing balloon (p = 0.001), longer fluoroscopic time (p = 0.022), and higher incidence of device thrombosis (0.006). Right disc thrombosis was observed in three patients of the ASD > 20 mm group, always in the inferior portion of the right disc. On univariate analysis, ASD diameter at sizing balloon (OR 1.360; p = 0.036) was the only positive predictor of device thrombosis.ConclusionsRight disc thrombosis of the GCA device may be under‐recognized at follow‐up, hence deserving clinical attention, especially in those patients with larger ASD diameters.
Electroreductive Decomplexation and Isomerism of Copper(II) Complexes with Cyclam Ligands for Medical Use
Authors: Koláčná Lucie , Maďar Milan , Kubíček Vojtěch , Ludvík Jiří 
Published: March 2024

AbstractDetailed electrochemical study of copper(II) complexes of cyclam bearing two phosphonate (TE2P), phenolate (TE2PhOH) or carboxylate (TE2A) pendant arms (together with one cross‐bridged‐cyclam derivative cb‐TE2A) was performed using cyclic voltammetry (CV) and polarography. The electrochemical‐heterogeneous measurements were accompanied by UV‐vis spectra describing the situation in homogeneous phase. Reduction of complexes on mercury electrode in buffered aqueous solutions (pH 2–12) occurs generally as a two‐electron process of reductive decomposition. The formed Cu‐amalgam can be (e. g. during the anodic scan of CV) reoxidized to Cu(II) cation which undergoes re‐complexation resulting in the original complex. This process of a square diagram is manifold repeatable. The results also showed presence of several isomers differing in mutual orientation of substituents on cyclam nitrogen atoms. The primary “kinetic”, pentacoordinated isomers are irreversibly transformed to the stable, hexacoordinated “thermodynamic” ones upon heating. The development of isomerization process was followed electrochemically. The cross‐bridged cb‐TE2A derivative forms only one isomer which does not change even after heating. The higher stability of the complex manifests itself at pH>8 when the complex is reversibly reduced in one‐electron step, formally CuII/CuI, without decomposition.
Efficient N2 Electrofixation to NH3 Through Optimizing Binder‐Catalyst Configuration
Authors: Aslambakhsh Amirhamzeh , Kentish Sandra E. , Scholes Colin A. 
Published: March 2024

AbstractNitrogen electrofixation under ambient conditions is a promising approach to synthesize ammonia sustainably but improving the yield and efficiency remains a challenge. This is due to the competition between the nitrogen electrofixation and hydrogen evolution reactions, which can be depressed through appropriate working electrode design. This study investigated the influence of the catalyst‐binder configuration on ammonia yield and Faradic efficiency. A series of working electrodes were tested in an aqueous system, with the proton and electron transfer on the working electrode found to be dependent on the catalyst material, binder material, and binder hydrophobicity. The use of a binder with low proton/electron conductivity increased Faradic efficiency by hindering the hydrogen evolution reaction and reducing charge transfer to the catalytic material. Utilising a hydrophobic binder significantly improved ammonia yield. Furthermore, nitrogen sorption experiments revealed that the catalyst‘s nitrogen affinity exerts a greater influence on ammonia yield than the binder‘s affinity. The best performance was observed for a semi‐conductive catalyst based on vanadium, integrated within a highly hydrophobic perfluorinated binder. At ambient conditions in 0.1 M hydrogen chloride, 39.3±4.3
of ammonia was synthesized with 38.5±4.5 % Faradic efficiency at −0.2 V versus a reversible hydrogen electrode.
Three‐dimensional (3D)‐printed MXene high‐voltage aqueous micro‐supercapacitors with ultrahigh areal energy density and low‐temperature tolerance
Authors: Zhu Yuanyuan , Zhang Qingxiao , Ma Jiaxin , Das Pratteek , Zhang Liangzhu , Liu Hanqing , Wang Sen , Li Hui , Wu Zhong‐Shuai 
Published: March 2024

AbstractThe rapid advancement in the miniaturization, integration, and intelligence of electronic devices has escalated the demand for customizable micro‐supercapacitors (MSCs) with high energy density. However, efficient microfabrication of safe and high‐energy MXene MSCs for integrating microelectronics remains a significant challenge due to the low voltage window in aqueous electrolytes (typically ≤0.6 V) and limited areal mass loading of MXene microelectrodes. Here, we tackle these challenges by developing a high‐concentration (18 mol kg−1) “water‐in‐LiBr” (WiB) gel electrolyte for MXene symmetric MSCs (M‐SMSCs), demonstrating a record high voltage window of 1.8 V. Subsequently, additive‐free aqueous MXene ink with excellent rheological behavior is developed for three‐dimensional (3D) printing customizable all‐MXene microelectrodes on various substrates. Leveraging the synergy of a high‐voltage WiB gel electrolyte and 3D‐printed microelectrodes, quasi‐solid‐state M‐SMSCs operating stably at 1.8 V are constructed, and achieve an ultrahigh areal energy density of 1772 μWh cm−2 and excellent low‐temperature tolerance, with a long‐term operation at −40°C. Finally, by extending the 3D printing protocol, M‐SMSCs are integrated with humidity sensors on a single planar substrate, demonstrating their reliability in miniaturized integrated microsystems.
Delta‐convex structure of the singular set of distance functions
Authors: Miura Tatsuya , Tanaka Minoru 
Published: March 2024

AbstractFor the distance function from any closed subset of any complete Finsler manifold, we prove that the singular set is equal to a countable union of delta‐convex hypersurfaces up to an exceptional set of codimension two. In addition, in dimension two, the whole singular set is equal to a countable union of delta‐convex Jordan arcs up to isolated points. These results are new even in the standard Euclidean space and shown to be optimal in view of regularity.
Synthesis of Deuterated Compounds by Flow Chemistry
Authors: Kamio Shintaro , Okamoto Kazuhiro , Yamagishi Takehiro , Nagaki Aiichiro 
Published: March 2024

AbstractDevelopment of the efficient and practical method for the synthesis of deuterated compounds which occupies the broadest area among stable isotopes is one of the most essential issues toward the industrial advance and building a sustainable society. This review describes recent advances in deuteration reactions, where the continuous flow chemistry plays pivotal roles for the successful installation of deuterium atom into diverse organic frameworks, opening new fields of isotope‐based synthetic chemistry.
Ligand Environment and Light: Two Triggers for Controlling Cytotoxicity of Ruthenium Nitrosyl Complexes
Authors: Yakovlev Ivan A. , Golubeva Julia A. , Klyushova Lyubov S. , Nadolinny Vladimir A. , Kostin Gennadiy A. , Mikhailov Artem A. 
Published: March 2024

AbstractPhotoinduced nitric oxide (NO) release for complexes [RuNO(L)2(NO2)2OH], where L=methyl isonicotinate (1), ethyl isonicotinate (2), methyl nicotinate (3) and ethyl nicotinate (4) was studied in DMSO, MeCN and water solutions (PBS, CTAB) using spectroscopic methods (UV‐vis, IR, EPR) and spectrometric techniques (ESI‐MS). Additionally, we present methodological evidence for improving the calculation of the quantum yield (QY) of NO release through the utilization of a combined IR‐UV‐vis‐spectroscopy flow‐through setup. According to DFT calculations, the production of nitric oxide occurs through the photoinduced cleavage of the Ru−NO bond, triggered by irradiation at 445 or 532 nm. This cleavage is a consequence of charge transfer from the orbitals of the Ru−OH group and the equatorial ligands (HOMO, HOMO‐1) to the Ru−NO antibonding orbital (LUMO). The cytotoxicity and photoinduced cytotoxicity of the investigated compounds were assessed against the breast adenocarcinoma cell line MCF‐7. Moreover, the investigation of the lipophilic properties of compounds 1–4 unveiled a significant influence of their lipophilicity on cytotoxic behavior, allowing for the modification of cytotoxicity through changes in the ligand L or by light irradiation.
Is developmental plasticity triggered by DNA methylation changes in the invasive cane toad (Rhinella marina)?
Authors: Yagound Boris , Sarma Roshmi R. , Edwards Richard J. , Richardson Mark F. , Rodriguez Lopez Carlos M. , Crossland Michael R. , Brown Gregory P. , DeVore Jayna L. , Shine Richard , Rollins Lee A. 
Published: March 2024

AbstractMany organisms can adjust their development according to environmental conditions, including the presence of conspecifics. Although this developmental plasticity is common in amphibians, its underlying molecular mechanisms remain largely unknown. Exposure during development to either ‘cannibal cues’ from older conspecifics, or ‘alarm cues’ from injured conspecifics, causes reduced growth and survival in cane toad (Rhinella marina) tadpoles. Epigenetic modifications, such as changes in DNA methylation patterns, are a plausible mechanism underlying these developmental plastic responses. Here we tested this hypothesis, and asked whether cannibal cues and alarm cues trigger the same DNA methylation changes in developing cane toads. We found that exposure to both cannibal cues and alarm cues was associated with local changes in DNA methylation patterns. These DNA methylation changes affected genes putatively involved in developmental processes, but in different genomic regions for different conspecific‐derived cues. Genetic background explains most of the epigenetic variation among individuals. Overall, the molecular mechanisms triggered by exposure to cannibal cues seem to differ from those triggered by alarm cues. Studies linking epigenetic modifications to transcriptional activity are needed to clarify the proximate mechanisms that regulate developmental plasticity in cane toads.
Diuretic use and outcomes in patients with heart failure with reduced ejection fraction: Insights from the VICTORIA trial
Authors: Ezekowitz Justin , Alemayehu Wendimagegn , Edelmann Frank , Ponikowski Piotr , Lam Carolyn S.P. , O'Connor Christopher M. , Butler Javed , Corda Stefano , McMullan Ciaran J. , Westerhout Cynthia M. , Voors Adriaan A. , Mentz Robert J. , Armstrong Paul W. ,   for the VICTORIA Study Group
Published: March 2024

AimsIn VICTORIA, vericiguat compared with placebo reduced the risk of cardiovascular death (CVD) and heart failure hospitalization (HFH) in patients enrolled after a worsening heart failure (WHF) event. We examined clinical outcomes and efficacy of vericiguat as it relates to background use of loop diuretics in patients with WHF.Methods and resultsWe calculated the total daily loop diuretic dose equivalent to furosemide dosing at randomization and categorized these as: no loop diuretic, 1–39, 41–80, 40, and >80 mg total daily dose (TDD). The primary composite outcome of CVD/HFH and its components were evaluated based on TDD loop diuretic and expressed as adjusted hazard ratios with 95% confidence intervals. Post‐randomization rates of change in TDD were also examined. Of 4974 patients (98% of the trial) with diuretic dose information available at randomization, 540 (10.8%) were on no loop diuretic, 647 (13.0%) were on 1–39, 1633 (32.8%) were on 40, 1185 (23.8%) were on 41–80, and 969 (19.4%) were on >80 mg TDD. Patients with higher TDD had a higher rate of primary and secondary clinical outcomes. There were no significant interactions with TDD at randomization and efficacy of vericiguat versus placebo for any outcome (all pinteraction > 0.5). Post‐randomization diuretic dose changes for vericiguat and placebo showed similar rates of up‐titration (19.6 and 20.2/100 person‐years), down‐titration (16.8 and 18.1/100 person‐years), and stopping diuretics (22.9 and 24.2/100 person‐years).ConclusionsLoop diuretic TDD at randomization was independently associated with worse outcomes in this high‐risk population. The efficacy of vericiguat was consistent across the range of diuretic doses.
Reduced 2,2’‐Bipyridine Lanthanide Metallocenes Provide Access to Mono‐C5Me5 and Polyazide Complexes
Authors: Stennett Cary R. , Ziller Joseph W. , Evans William J. 
Published: March 2024

AbstractExploration of the reduction chemistry of the 2,2’‐bipyridine (bipy) lanthanide metallocene complexes Cp*2LnCl(bipy) and Cp*2Ln(bipy) (Cp* = C5Me5) resulted in the isolation of a series of complexes with unusual composition and structure including complexes with a single Cp* ligand, multiple azide ligands, and bipy ligands with close parallel orientations. These results not only reveal new structural types, but they also show the diverse chemistry displayed by this redox‐active platform. Treatment of Cp*2NdCl(bipy) with excess KC8 resulted in the formation of the mono‐Cp* Nd(III) complex, [K(crypt)]2[Cp*Nd(bipy)2], 1, as well as [K(crypt)][Cp*2NdCl2], 2, and the previously reported [K(crypt)][Cp*2Nd(bipy)]. A mono‐Cp* Lu(III) complex, Cp*Lu(bipy)2, 3, was also found in an attempt to make Cp*2Lu(bipy) from LuCl3, 2 equiv. of KCp*, bipy, and K/KI. Surprisingly, the (bipy)1− ligands in neighboring molecules in the structure of 3 are oriented in a parallel fashion with intermolecular C⋅⋅⋅C distances of 3.289(4) Å, which are shorter than the sum of van der Waals radii of two carbon atoms, 3.4 Å. Another product with one Cp* ligand per lanthanide was isolated from the reaction of [K(crypt)][Cp*2Eu(bipy)] with azobenzene, which afforded the dimeric Eu(II) complex, [K(crypt)]2[Cp*Eu(THF)(PhNNPh)]2, 4. Attempts to make 4 from the reaction between Cp*2Eu(THF)2 and a reduced azobenzene anion generated instead the mixed‐valent Eu(III)/Eu(II) complex, [K(crypt)][Cp*Eu(THF)(PhNNPh)]2, 5, which allows direct comparison with the bimetallic Eu(II) complex 4. Mono‐Cp* complexes of Yb(III) are obtained from reactions of the Yb(II) complex, [K(crypt)][Cp*2Yb(bipy)], with trimethylsilylazide, which afforded the tetra‐azido [K(crypt)]2[Cp*Yb(N3)4], 6, or the di‐azido complex [K(crypt)]2[Cp*Yb(N3)2(bipy)], 7 a, depending on the reaction stoichiometry. A mono‐Cp* Yb(III) complex is also isolated from reaction of [K(crypt)][Cp*2Yb(bipy)] with elemental sulfur which forms the mixed polysulfido Yb(III) complex [K(crypt)]2[Cp*Yb(S4)(S5)], 8 a. In contrast to these reactions that form mono‐Cp* products, reduction of Cp*2Yb(bipy) with 1 equiv. of KC8 in the presence of 18‐crown‐6 resulted in the complete loss of Cp* ligands and the formation of [K(18‐c‐6)(THF)][Yb(bipy)4], 9. The (bipy)1− ligands of 9 are arranged in a parallel orientation, as observed in the structure of 3, except in this case this interaction is intramolecular and involves pairs of ligands bound to the same Yb atom. Attempts to reduce further the Sm(II) (bipy)1− complex, Cp*2Sm(bipy) with 2 equiv. of KC8 in the presence of excess 18‐crown‐6 led to the isolation of a Sm(III) salt of (bipy)2− with an inverse sandwich Cp* counter‐cation and a co‐crystallized K(18‐c‐6)Cp* unit, [K2(18‐c‐6)2Cp*]2[Cp*2Sm(bipy)]2 ⋅ [K(18‐c‐6)Cp*], 10.
Boron‐Based Enantiomerism
Authors: Braun Manfred 
Published: March 2024

AbstractBoron‐based enantiomerism is fragile due to the inherent tendency of a dissociation of a ligand from tetra‐coordinate chiral boron complexes under formation of the achiral tri‐coordinate species. This review will present the different approaches in overcoming the inherent tendency of racemization in boron‐stereogenic compounds. When embedded in an environment of chiral ligands or substituents, configurationally stable boron stereogenic centers can form in a diastereoselective manner. Compounds incorporating boron as the exclusive stereogenic center are obtained by resolution of the racemic mixtures. The recently developed – much more efficient – methods of a catalytic, enantioselective creation of boron stereogenic compounds are highlighted in this review. Finally the chiroptical properties of enantiomerically pure boron complexes that makes them promising materials or devices are addressed.
Objectively measured activity is not associated with average pain intensity 1 week after surgery: A cross‐sectional study
Authors: Komann M. , Dreiling J. , Baumbach P. , Weinmann C. , Kalso E. , Stamer U. , Volk T. , Pogatzki‐Zahn E. , Kehlet H. , Meissner W. 
Published: March 2024

AbstractBackgroundMeasures of physical activity and pain‐related patient‐reported outcomes are important components of patient recovery after surgery. However, little is known about their association in the early post‐operative period. This study aims to increase this knowledge. Our primary objective was to determine the association between average pain intensity and activity (in steps) 1 week after surgery. Secondary objectives were the association of activity with other patient‐reported outcomes, age, sex, comorbidities and body mass index.MethodsData were obtained from the PROMPT sub‐project of IMI‐PainCare. Patients after breast and endometriosis‐related surgery, sternotomy and total knee arthroplasty completed pain‐related outcomes questionnaires and wore an ActiGraph activity‐tracking device. We correlated steps with average pain intensity on post‐operative days 6 and 7. Secondary analyses were done using correlations and t‐tests.ResultsIn 284 cases, there was no statistically significant correlation between steps and average pain intensity. In addition, none of the 28 secondary analyses showed a statistically significant result.ConclusionsPain‐related patient‐reported outcome measures and physical activity are separate entities. Both should be measured after surgery to assess patient recovery and to identify treatment deficiencies.Significance StatementMeasuring recovery is a multi‐dimensional challenge. After surgery, clinicians need to be aware that neither pain intensity nor activity levels tell the whole story. Each can hint to problems and treatment requirements.
Employee voice in times of crisis: A conceptual framework exploring the role of Human Resource practices and Human Resource system strength
Authors: Nyfoudi Margarita , Kwon Bora , Wilkinson Adrian 
Published: March 2024

AbstractDespite extensive developments in the field of Human Resource Management, we still have limited and fragmented knowledge of how the external and internal environment of an organization influences direct employee voice. In this conceptual paper, we draw on signaling theory and theorize on whether and, if so, how direct employee voice and organizational voice climate are shaped at times of macro and organizational turbulence. Specifically, we introduce the concepts of solidary, utilitarian, and opportunistic crisis‐related Human Resource (HR) practices and propose that they send different signals to employees, influencing their voice perceptions in distinctive ways. We also theorize that employees interpret these signals vis‐à‐vis the experienced meso‐ and macroturbulence, a process that affects HR system strength and the subsequent formulation of voice perceptions and voice climate emergence. With this work, we contribute to the voice and strategic HR literature by offering an integrated and multilayered understanding of how top‐down processes at turbulent times such as crisis‐related HR practices can influence bottom‐up emergent phenomena.