bluuebunny/crossref_metadata_2025_split huggingface dataset:
Light‐Driven C−C Coupling for Targeted Synthesis of CH3COOH with Nearly 100 % Selectivity from CO2
Authors: Ding Jinyu , Du Peijin , Zhu Juncheng , Hu Qing , He Dongpo , Wu Yang , Liu Wenxiu , Zhu Shan , Yan Wensheng , Hu Jun , Zhu Junfa , Chen Qingxia , Jiao Xingchen , Xie Yi 
Published: February 2024

AbstractTargeted synthesis of acetic acid (CH3COOH) from CO2 photoreduction under mild conditions mainly limits by the kinetic challenge of the C−C coupling. Herein, we utilized doping engineering to build charge‐asymmetrical metal pair sites for boosted C−C coupling, enhancing the activity and selectivity of CO2 photoreduction towards CH3COOH. As a prototype, the Pd doped Co3O4 atomic layers are synthesized, where the established charge‐asymmetrical cobalt pair sites are verified by X‐ray photoelectron spectroscopy and X‐ray absorption near edge spectroscopy spectra. Theoretical calculations not only reveal the charge‐asymmetrical cobalt pair sites caused by Pd atom doping, but also manifest the promoted C−C coupling of double *COOH intermediates through shortening of the coupled C−C bond distance from 1.54 to 1.52 Å and lowering their formation energy barrier from 0.77 to 0.33 eV. Importantly, the decreased reaction energy barrier from the protonation of two*COOH into *CO intermediates for the Pd‐Co3O4 atomic layer slab is 0.49 eV, higher than that of the Co3O4 atomic layer slab (0.41 eV). Therefore, the Pd‐Co3O4 atomic layers exhibit the CH3COOH evolution rate of ca. 13.8 μmol g−1 h−1 with near 100% selectivity, both of which outperform all previously reported single photocatalysts for CO2 photoreduction towards CH3COOH under similar conditions.
Centering dialog and care in digital Indigenous knowledge stewardship: Of relationality, responsibility, and respect
Authors: Liew Chern Li , Lipscombe Ailsa 
Published: February 2024

AbstractThe question of how to appropriately care for and share Indigenous knowledges is central to cultural heritage documentation and, contemporary archival praxes and discourses. Transforming the standards of Indigenous knowledge management (IKM) necessitates confronting the legacies of colonial control and Indigenous expurgation that settler colonial galleries, libraries, archives, and museums (GLAM) have contributed to (intentionally or not). Writing of and within the Māori context in New Zealand, we argue that a renewed orientation toward dialogic collaboration between institutions and Indigenous communities is crucial for revitalizing archival practices and partnerships in ways that center Indigenous values. Moreover, we purport that aligning institutional practices with Indigenous values is insufficient if Indigenous communities are neither made to feel welcome within archival spaces nor empowered to utilize them. As such, we identify the notions of relationality, responsibility, and respect as vital in supporting this ethical transformation of Indigenous knowledge stewardship both in New Zealand and in other Indigenous contexts. We propose that current efforts to reshape IKM praxes in culturally responsible and responsive ways can be meaningfully expanded through dialogic engagement, and an ethics of care.
Uptake of silicate by pipe scale materials and effects on lead release
Authors: Mishrra Anushka , Wang Ziqi , Giammar Daniel E. 
Published: February 2024

AbstractThe interactions between dissolved silica and corrosion scale on lead pipes such as hydrocerussite (Pb3(CO3)2(OH)2) and aluminum containing amorphous phases can affect the rates of lead release from the pipes to drinking water. Batch experiments that were well mixed to fully suspend these materials complemented previous experiments that were performed with pipes with intact pipe scales. These experiments focused on chemical interactions between the corrosion scale materials and silicate by decreasing the effect of mass transfer processes associated with solute diffusion into and out of intact scales. The findings from the batch experiments help us understand that the benefits of silicate addition in controlling lead release observed in a previous pipe loop study with pipes with intact scale were primarily due to inhibited diffusion of lead through the scale as a result of silicate uptake and not due to chemical interactions between lead‐containing solids and silicate.
Impact of Ionic Liquid Functionalized ZrO2 Nanoparticles on Poly (stearyl methacrylate) Grafted Poly (vinylidene fluoride‐co‐hexafluoropropylene) Based Highly Conductive Gel Polymer Electrolytes for Lithium‐Metal Batteries
Authors: Parui Rittik , Deb Debalina , Bose Pallab , Bhattacharya Subhratanu 
Published: February 2024

AbstractIn this study, an organic‐inorganic hybrid polymer membrane is successfully designed and developed by grafting stearyl methacrylate (SMA) side chains onto the backbone of the P(VDF‐HFP) copolymer followed by blending with varying amounts of imidazolium ionic liquids functionalized ZrO2 nanoparticles. Different microporous gel polymer electrolytes (MGPEs) are prepared by immersing the membranes into a LiTFSI salt‐dissolved ionic liquid electrolyte. The membranes′ crystallinity, surface morphology, porosity, and thermal stability are investigated using various characterization techniques. The copolymer membrane blended with 60 wt % functionalized nanoparticles exhibits the highest porosity of 64.5 %, which allows it to achieve a maximum electrolyte uptake of 387 wt %. That enables the corresponding MGPE to achieve the highest room temperature lithium ion conductivity of ~5.34×10−3 S cm−1 with a wide electrochemical stability window and good electrochemical stability against Li metal. Leveraging these advantageous characteristics, the lab‐scale truly solid‐state Li|MGPE|LiFePO4 and Li|MGPE|LiNi0.8Mn0.1Co0.1O2 cells demonstrate excellent rate capability and reversible cycling stability while maintaining high specific capacities (up to 154 and 172 mAh g−1, respectively, at 0.5 C) with >99.0 % coulombic efficiency over 100 cycles. Such exceptional interfacial compatibility with both low‐ and high‐voltage cathodes establishes the applicability of these newly developed MGPEs in next‐generation all‐solid‐state lithium‐metal batteries.
Diffusion Models of Mass Transport for the Characterisation of Amperometric Gas Sensors
Authors: Saunders L. , Mudashiru L. K. , Baron R. , Horrocks B. R. 
Published: February 2024

AbstractA diffusion model for the analysis of chronoamperometric data in response to a concentration step is developed for amperometric gas sensors. This analysis avoids the difficulties with standard potentiodynamic measurements at the large specific area, high capacitance electrodes employed in these sensors. Despite the fact that typical devices comprise multiple layers with varying thicknesses and diffusivities, we show that typical chronoamperometric traces can be fitted to a simple diffusion model with a single parameter
where L is an overall effective thickness of the diffusion barrier and D is an effective diffusion coefficient. Through a comparison of the transient and steady‐state current, independent estimates of L and D in the devices can be made. The model is also extended to cover cases with interfacial kinetic barriers; such kinetic limitations lead to a change in the effective values L and D, but the simple diffusion model remains a good fit to the data. This analysis shows that transient sensor responses can be characterised by a single parameter τ and conversely that deviations from this regression model cannot be assigned to (i) complex layer architectures or (ii) interlayer kinetic barriers. Instead, we show that non‐uniform accessibility effects arising from a distribution of diffusion rates across the device lead to deviations from the simple regression model, but that they may be captured approximately by a more complex model in which τ has a probability distribution.
Ultrafast Halogen Dance Reactions of Bromoarenes Enabled by Catalytic Potassium Hexamethyldisilazide
Authors: Inoue Kengo , Mori Atsunori , Okano Kentaro 
Published: February 2024

AbstractLochmann–Schlosser base, a stoichiometric combination of nBuLi and KOtBu, is commonly used as a superbase for deprotonating a wide range of organic compounds. In the present study, we report that catalytic potassium hexamethyldisilazide (KHMDS) exhibits higher catalytic activity than KOtBu for successive bromine–metal exchanges. Accordingly, 1–10 mol% of KHMDS dramatically enhances halogen dance reactions to introduce various electrophiles to bromopyridine, bromoimidazole, bromothiophene, bromofuran, and bromobenzene derivatives with the bromo group translocated from the original position. A dual catalytic cycle is proposed to explain the ultrafast bromine transfer.
Trifluoromethyl Fluorosulfonate (CF3OSO2F) and Trifluoromethoxy Sulfur Pentafluoride (CF3OSF5) – Two Gaseous Sulfur(VI) Compounds with Insulating Properties
Authors: Golz Paul , Dreyhsig Gesa H. , Pernice Holger , Drews Thomas , Nissen Jan H. , Beckers Helmut , Steinhauer Simon , Wiesner Anja , Riedel Sebastian 
Published: February 2024

AbstractIn this work, we analyzed trifluoromethyl fluorosulfonate (CF3OSO2F) and trifluoromethoxy sulfur pentafluoride (CF3OSF5) regarding their potential use as dielectrics by investigating some of their intrinsic and extrinsic properties. Both compounds show a higher breakdown voltage than SF6 with averaged relative breakdown voltages of 1.3±0.2 for CF3OSO2F and 1.4±0.2 for CF3OSF5 compared to SF6 with 1.0. Like the dielectric (CF3)2CFCN, both compounds decompose during the breakdown process. The decomposition products were analyzed by IR spectroscopy and GCIR methods. Furthermore, the molecular structures of both gaseous compounds CF3OSO2F and CF3OSF5 have been determined by in situ crystallization, and their physical properties were determined as well.
Droplet deposition of agrochemical spraying: Comparison of results from a random‐walk model and CFD simulations
Authors: Renaudo Carlos A. , Bucalá Veronica , Bertin D. E. 
Published: February 2024

AbstractThe effectiveness of agricultural spraying processes depends considerably on the ability of the atomized droplets to reach the target site in the desired amount. In this work, two mathematical models to study the trajectories and deposition of atomized droplets are implemented and compared. On the one hand, a computational fluid dynamics (CFD) coupled with discrete phase model (DPM) is implemented to calculate the trajectories of atomized droplets and determine distances at which the droplets are deposited. The continuous phase (atmospheric air) is modelled by continuity, momentum, and energy equations. On the other hand, a Lagrangian random‐walk (LRW) model based on force and energy balances to predict the pulverization process of a nozzle is formulated and implemented in Python. Both models take into account the effects of drag, gravity, buoyancy, and evaporation on individual droplets, as well as the impact of atmospheric stability and dispersion. By tracking a large number of trajectories, meaningful estimates of dispersal statistics can be obtained. The LRW model accurately replicated the trajectories, deposition distances, and final diameters of atomized droplets for three atmospheric stability cases, compared with CFD simulation results. The results of both models agreed that 100 μm droplets were most susceptible to wind‐induced spray drift, depositing at the furthest distances from the nozzle. In addition, 50 μm droplets exhibited a significant tendency to evaporate entirely before reaching the ground. The LRW model is found to be a cost‐effective alternative for estimating spray drift compared to the computationally intensive CFD approach.
Rearrangement of GUV‐confined actin networks in response to micropipette aspiration
Authors: Wubshet Nadab H. , Young Cole J. , Liu Allen P. 
Published: February 2024

AbstractAlthough diverse actin network architectures found inside the cell have been individually reconstituted outside of the cell, how different types of actin architectures reorganize under applied forces is not entirely understood. Recently, bottom‐up reconstitution has enabled studies where dynamic and phenotypic characteristics of various actin networks can be recreated in an isolated cell‐like environment. Here, by creating a giant unilamellar vesicle (GUV)‐based cell model encapsulating actin networks, we investigate how actin networks rearrange in response to localized stresses applied by micropipette aspiration. We reconstitute actin bundles and branched bundles in GUVs separately and mechanically perturb them. Interestingly, we find that, when aspirated, protrusive actin bundles that are otherwise randomly oriented in the GUV lumen collapse and align along the axis of the micropipette. However, when branched bundles are aspirated, the network remains intact and outside of the pipette while the GUV membrane is aspirated into the micropipette. These results reveal distinct responses in the rearrangement of actin networks in a network architecture‐dependent manner when subjected to physical forces.
Urine cytology in the detection of renal cell carcinomas – a territory‐wide multi‐institutional retrospective review of more than 2 decades
Authors: Li Joshua J. X. , Ng Joanna K. M. , Tang Cheuk‐Yin , Chan Bryan C. H. , Chan Sau Yee , Law Jasmine H. N. , Teoh Jeremy Y. , VandenBussche Christopher J. , Tse Gary M. 
Published: February 2024

AbstractIntroductionCompared with urothelial lesions of the upper urinary tract, the diagnostic performance of urine cytology in detection of renal cell carcinomas is underreported. This study aims to establish the role of urine cytology in the assessment of renal carcinomas by a multi‐institute review of urine cytology from nephrectomy confirmed renal cell carcinomas, referenced against renal urothelial and squamous cell carcinomas.MethodsRecords of nephrectomy performed from the 1990s to 2020s at three hospitals were retrieved and matched to urine cytology specimens collected within 1 year prior. Patient demographics, specimen descriptors, and histology and staging parameters were reviewed and compared against cytologic diagnoses.ResultsThere were 1147 cases of urine cytology matched with renal cell carcinomas, with 666 renal urothelial/squamous carcinomas for comparison. The detection rate for urothelial/squamous (atypia or above [C3+]: 63.1%; suspicious or above [C4+]: 24.0%) were higher than renal cell carcinoma (C3+: 13.1%; C4+: 1.5%) (p < 0.001). The positive rate for upper tract urine exceeded other collection methods at 45.0% (C3+) and 10.0% (C4+) (p < .01). Other factors associated with increased positive rates were male sex, collecting duct carcinoma histology, nuclear grade, and renal/sinus involvement (p < .05). Multivariate analysis revealed additional positive correlations with presence of sarcomatoid tumor cells, lymphovascular invasion, and perinephric fat involvement (p < .05). Larger lesion size and higher urine volume did not improve detection rates (p < .05).ConclusionsThe detection rate of renal cell carcinomas is suboptimal compared with urothelial carcinomas, although urine samples collected from cystoscopy or percutaneous nephrostomy significantly outperformed voided urine specimens.
Prediction of lymph node status in patients with surgically treated head and neck squamous cell carcinoma via neck lavage cytology: A pilot study
Authors: Rimbach Hugo , Linxweiler Maximilian , Körner Sandrina , Smola Sigrun , Linxweiler Barbara , Speicher Stefanie , Helfrich Johanna , Solomayer Erich‐Franz , Wagner Mathias , Schick Bernhard , Kühn Jan Philipp 
Published: February 2024

AbstractBackgroundNeck dissection is a standardized surgical procedure for patients with head and neck squamous cell carcinoma (HNSCC) and plays a critical role in the choice of adjuvant treatment based on histopathological findings. Saline irrigation is routinely performed at the end of surgery. However, this irrigant is not used for diagnostic purposes.MethodsIntraoperative irrigation of the neck dissection wound was performed in 56 patients with HNSCC (N = 93 neck dissections), and the cytological suspension obtained was processed via the liquid‐based cytology (LBC) technique, Papanicolaou staining, and immunocytochemical staining. Microscopic preparations were screened for the presence of tumor cells and classified as positive, borderline, or negative. These results were correlated with the histopathological and clinical data.ResultsNeck lavage LBC demonstrated high diagnostic value in detecting lymph node metastases (N+) with extracapsular spread (ECS), with a specificity, sensitivity, negative predictive value, and positive predictive value of 93.1%, 100%, 100%, and 80%, respectively. Tumor cells were detected in 4.8% of N− cases, 20% of N+ cases without ECS, and 100% of N+ cases with ECS. Receiver operating characteristic curve analysis showed an area under the curve of 0.8429 for the prediction of N+ (p < .0001) and 0.9658 for the prediction of N+ with ECS (p < .0001).ConclusionsDifferential lavage cytology can provide valid and rapid information on the lymph node status in patients with HNSCC and showed an excellent correlation with histopathology. Thus, neck lavage LBC may facilitate faster and more reasonable planning of adjuvant treatment and help improve the therapeutic management of patients with HNSCC.
Safety, Tolerability, and Pharmacokinetics of Voriconazole for Injection in Two Preparations in Chinese Healthy Adult Volunteers
Authors: Yu Jin , Wu Yi , Lin Sisi , Wang Ying 
Published: February 2024

AbstractVoriconazole is a second‐generation, synthetic, triazole antifungal drug based on the structure of fluconazole. We compared the safety, tolerability, and pharmacokinetic characteristics of voriconazole for injection (200 mg) manufactured by at a dose of 6 mg/kg in Chinese healthy adult volunteers. This was a single‐center, randomized, open, 2‐preparation, single‐dose, 2‐period, 2‐sequence, crossover bioequivalence clinical trial. Twenty‐four eligible, healthy, male, and female volunteers were assigned randomly to one of 2 dose‐sequence groups (test‐reference group or reference‐test group) in a 1:1 block. The voriconazole concentration in plasma was determined by protein precipitation and high‐performance liquid chromatography‐tandem mass spectrometry. The main PK parameters were calculated on the basis of a noncompartmental model. The ratio of the geometric mean of the maximum plasma drug concentration, area under the plasma concentration–time curve from time 0 to the last time of quantifiable concentration, and area under the plasma concentration‐time curve from time 0 to infinity of the test preparation, and the reference preparation was 100.4%, 102%, and 102.2%, respectively. The 90% confidence intervals were between 80% and 125%, indicating that the 2 preparations were bioequivalent. The adverse events experienced by healthy adult volunteers were mild. Both preparations had a good safety profile.
Wavily Curved Perylene Diimides: Synthesis, Characterization, and Photovoltaic Properties
Authors: Fujimoto Keisuke , Izawa Seiichiro , Yamada Kazuki , Yagi Sota , Inuzuka Toshiyasu , Sanada Kazutaka , Sakamoto Masami , Hiramoto Masahiro , Takahashi Masaki 
Published: February 2024

AbstractSolubility enhancement is a key issue for developing the perylene diimide‐based functional materials. Introduction of curved structure proved an effective solubilizing method without employing steric repulsion. In this work, wavily curved perylene diimides were developed as a new family of highly soluble curved perylene diimides. Moreover, their conformational dynamics, aggregating properties, electronic properties, and photovoltaic performances were thoroughly examined in comparison to the previously reported isomer exhibiting an arched curvature. The waved isomer demonstrated heightened rigidity and a greater propensity for aggregation compared to the arched isomer, likely attributed to its more planar structure. Each benzoxepin unit played a role in cancelling out the curvature on the opposite side. While the difference in the molecular curvature did not cause significant alterations in the photophysical and electron‐accepting properties, we identified that the modulation of the curved structure is effective in controlling the morphology of the photoelectric conversion layer.
Protection‐Free, Two‐step Synthesis of C5‐C Functionalized Pyrimidine Nucleosides
Authors: Podskoczyj Karolina , Kuszczynska Anna , Dziergowska Agnieszka , Leszczynska Grazyna 
Published: February 2024

AbstractA simple, reliable, and efficient method for the gram‐scale chemical synthesis of pyrimidine nucleosides functionalized with C5‐carboxyl, nitrile, ester, amide, or amidine, starting from unprotected uridine and cytidine, is described. The protocol involves the synthesis of 5‐trifluoromethyluridine and 5‐trifluoromethylcytidine with Langlois reagent (CF3SO2Na) in the presence of tert‐butyl hydroperoxide and subsequent transformation of the CF3 group to the C5‐C ‘carbon substituents’ under alkaline conditions. © 2024 Wiley Periodicals LLC.Basic Protocol 1: Synthesis and characterization of 5‐trifluoromethyluridine (5‐CF3U) and 5‐trifluoromethylcytidine (5‐CF3C)Basic Protocol 2: Conversion of 5‐CF3U and 5‐CF3C to several C5‐substituted ribonucleosides
Uranium Cyanides from Reactions in Liquid Ammonia Solution
Authors: Graubner Tim , Rudel Stefan S. , Ivlev Sergei I. , Karttunen Antti J. , Kraus Florian 
Published: February 2024

AbstractReactions of uranium tri‐ and tetrahalides, UBr3, UI3, UCl4, and UI4, with different cyanides MCN (M=K, Ag) in liquid anhydrous ammonia led to three novel uranium(IV) cyanide compounds. The reaction of UCl4 in the presence of KCN resulted in the compound [U(CN)(NH3)8]Cl3 ⋅ 3NH3, while UBr3 and UI3 were oxidized in the presence of AgCN to form the compounds
(μ‐CN){(H3N)5U(μ‐NH2)3U(NH3)5}]Br4 ⋅ 2NH3, and
(μ‐CN){(H3N)5U(μ‐NH2)3U(NH3)5}]I4 ⋅ 2NH3. The reaction of UI4 with KCN in aNH3 also yielded the compound
(μ‐CN){(H3N)5U(μ‐NH2)3U(NH3)5}]I4 ⋅ 2NH3. The compounds
(μ‐CN){(H3N)5U(μ‐NH2)3U(NH3)5}]X4 ⋅ 2NH3 (X=Br, I) crystallize in different space groups, Pmn21 (no. 31) and Imm2 (no. 44), respectively. In both cases, the
(μ‐CN){(H3N)5U(μ‐NH2)3U(NH3)5}]4+ cation forms infinite strands. We conducted quantum‐chemical calculations and Intrinsic Bond Orbital analyses on the observed [U(CN)(NH3)8]3+ cation and the [(μ‐CN)2{(H3N)5U(μ‐NH2)3U(NH3)5}]3+ model cation to gain insight into the bonding situation.