bluuebunny/crossref_metadata_2025_split huggingface dataset:
Unveiling the Synergy of O‐Vacancy and Heterostructure over MoO3‐x/MXene for N2 Electroreduction to NH3
Authors: Chu Ke , Luo Yaojing , Shen Peng , Li Xingchuan , Li Qingqing , Guo Yali 
Published: December 2021

AbstractThe electrochemical N2 reduction reaction (NRR) offers a promising approach for sustainable NH3 production, and modulating the structural/electronic configurations of the catalyst materials with optimized electrocatalytic properties is pivotal for achieving high‐efficiency NRR electrocatalysis. Herein, vacancy and heterostructure engineering are rationally integrated to explore O‐vacancy‐rich MoO3‐x anchored on Ti3C2Tx‐MXene (MoO3‐x/MXene) as a highly active and selective NRR electrocatalyst, achieving an exceptional NRR activity with an NH3 yield of 95.8 µg h−1 mg−1 (−0.4 V) and a Faradaic efficiency of 22.3% (−0.3 V). A combination of in situ spectroscopy, molecular dynamics simulations and density functional theory computations is employed to unveil the synergistic effect of O‐vacancies and heterostructures for the NRR, which demonstrates that O‐vacancies on MoO3‐x serve as the active sites for N2 chemisorption and activation, while the MXene substrate can further regulate the O‐vacancy sites to break the scaling relation to effectively stabilize *N2/*N2H while destabilizing *NH2/*NH3, resulting in more optimized binding affinity of NRR intermediates toward reduced energy barriers and an enhanced NRR activity for MoO3‐x/MXene.
Effects of Polymer Coating Mechanics at Solid‐Electrolyte Interphase for Stabilizing Lithium Metal Anodes
Authors: Huang Zhuojun , Choudhury Snehashis , Paul Neelima , Thienenkamp Johannes Helmut , Lennartz Peter , Gong Huaxin , Müller‐Buschbaum Peter , Brunklaus Gunther , Gilles Ralph , Bao Zhenan 
Published: December 2021

AbstractLithium metal batteries are next‐generation energy storage devices that rely on the stable electrodeposition of lithium metal during the charging process. The major challenge associated with this battery chemistry is related to the uneven deposition that leads to dendritic growth and poor coulombic efficiency (CE). A promising strategy for addressing this challenge is utilizing a polymer coating on the anodic surface. While several works in the past have evaluated polymer coatings, the requirements for polymer design are still unclear. In this work, the effect of polymer dynamics on lithium metal deposition is specifically investigated. Electrolyte (solvent) blocking perfluoropolyether polymer networks with evenly spaced H‐bonding sites of various strengths are designed, resulting in significant differences in the molecular ordering, as analyzed by X‐ray scattering measurements. The differences in the H‐bonding strength directly impact the mechanical properties of these materials, thus providing a controlled set of samples with a range of polymer dynamics for electrodeposition studies. Finally, a systematic evaluation of the lithium metal electrodeposition quality with these polymers as anodic coating shows that polymers with flowability or faster polymer dynamics exhibit higher CE. These experimental findings provide rational design principles for soft polymer coatings on lithium metal anodes.
Fine‐Tuning Batch Factors of Polymer Acceptors Enables a Binary All‐Polymer Solar Cell with High Efficiency of 16.11%
Authors: Jia Jianchao , Huang Qiri , Jia Tao , Zhang Kai , Zhang Jie , Miao Jingsheng , Huang Fei , Yang Chuluo 
Published: December 2021

AbstractRandom conjugated polymers, such as typical polymerized small molecular acceptors (PSMAs), concurrently suffer from the dual batch factors of molecular weights (MWs) and regioregularity, which seriously interfere with the study of the relationship between batch factors and polymer properties. Here, four isomer‐free PSMAs, PA‐5 and three members of a PA‐6 series with low (L), medium (M), and high (H) MWs, in which 5 and 6 define linkage position throughout conjugated backbone, are designed and synthesized to clearly investigate polymer batch effects. These studies reveal that PA‐6‐L and PA‐6‐M have ignorable batch differences within deviations, which deliver comparable maximum efficiencies of 14.81% and 14.99%, respectively. The PA‐6‐H based cell is processed from chlorobenzene with its high boiling point, due to the limited solubility in other common solvents, leading to large‐size phase separation during prolonged film drying process, and thereby inferior performance. In contrast, PA‐5 possesses diverse absorption characteristics, and ordered crystallization, which prompts higher short‐circuit current density and fill factor in the cell. As a result, the corresponding device realizes a photovoltaic performance of 16.11%, which is one of the best binary all‐polymer solar cells in the reported literature to date. This study provides a new insight into complicated batch effects of PSMAs on device performance while avoiding cross‐talk between them.
Remembering where we're from: Community‐ and individual‐level predictors of college students' White privilege awareness
Authors: Blevins Emily J. , Todd Nathan R. 
Published: December 2021

AbstractScholars in the field of community psychology have called for more research dedicated to examining White privilege as part of a system of White supremacy in the United States. One branch of this work focuses on awareness of White privilege, yet to date, this research has typically investigated awareness of White privilege at individual levels of analysis instead of also focusing on neighborhoods, schools, and other levels of analysis beyond the individual. In this study, we combine survey and U.S. Census data to explore both individual‐ and community‐level predictors of White privilege awareness. With a sample of 1285 White college students, we found that gender, modern racism, social dominance orientation, and subjective socioeconomic status (SES) significantly predicted White privilege awareness. After accounting for these individual‐level variables, we found that characteristics of students' hometowns (defined by zip code) predicted White privilege awareness. Specifically, greater income inequality was associated with higher White privilege awareness, while greater White racial homogeneity was marginally associated with lower White privilege awareness. There was a significant interaction between community‐level White racial homogeneity and individual‐level subjective SES, such that students with high subjective SES and low White racial homogeneity had the highest White privilege awareness. This study highlights the importance of examining different facets of ecological context in relation to White Americans' racial attitudes.
Synthesis of Benzylidenesuccinates through Rhodium(III)‐Catalyzed C‐H Alkenylation with Itaconate
Authors: Ochiai Shiho , Yoshimoto Risa , Usuki Yoshinosuke , Satoh Tetsuya 
Published: December 2021

AbstractThe dehydrogenative coupling of aromatic amides with dimethyl itaconate proceeds smoothly under rhodium catalysis through ortho C−H bond cleavage directed by their amide group to produce benzylidenesuccinates. Aromatic carboxylic acids including benzoic and phthalic acids also couple with the itaconate to give 1 : 2 coupling products predominantly. Benzylidenesuccinic acid derivatives have been known to show various biological activities. These reactions provide easy access to the important structures.
Clinical reporting following the quantification of cerebrospinal fluid biomarkers in Alzheimer's disease: An international overview
Authors: Delaby Constance , Teunissen Charlotte E. , Blennow Kaj , Alcolea Daniel , Arisi Ivan , Amar Elodie Bouaziz , Beaume Anne , Bedel Aurélie , Bellomo Giovanni , Bigot‐Corbel Edith , Bjerke Maria , Blanc‐Quintin Marie‐Céline , Boada Mercè , Bousiges Olivier , Chapman Miles D , DeMarco Mari L. , D'Onofrio Mara , Dumurgier Julien , Dufour‐Rainfray Diane , Engelborghs Sebastiaan , Esselmann Hermann , Fogli Anne , Gabelle Audrey , Galloni Elisabetta , Gondolf Clémentine , Grandhomme Frédérique , Grau‐Rivera Oriol , Hart Melanie , Ikeuchi Takeshi , Jeromin Andreas , Kasuga Kensaku , Keshavan Ashvini , Khalil Michael , Körtvelyessy Peter , Kulczynska‐Przybik Agnieszka , Laplanche Jean‐Louis , Lewczuk Piotr , Li Qiao‐Xin , Lleó Alberto , Malaplate Catherine , Marquié Marta , Masters Colin L. , Mroczko Barbara , Nogueira Léonor , Orellana Adelina , Otto Markus , Oudart Jean‐Baptiste , Paquet Claire , Paoletti Federico Paolini , Parnetti Lucilla , Perret‐Liaudet Armand , Peoc'h Katell , Poesen Koen , Puig‐Pijoan Albert , Quadrio Isabelle , Quillard‐Muraine Muriel , Rucheton Benoit , Schraen Susanna , Schott Jonathan M. , Shaw Leslie M. , Suárez‐Calvet Marc , Tsolaki Magda , Tumani Hayrettin , Udeh‐Momoh Chinedu T , Vaudran Lucie , Verbeek Marcel M , Verde Federico , Vermunt Lisa , Vogelgsang Jonathan , Wiltfang Jens , Zetterberg Henrik , Lehmann Sylvain 
Published: December 2021

AbstractIntroductionThe current practice of quantifying cerebrospinal fluid (CSF) biomarkers as an aid in the diagnosis of Alzheimer's disease (AD) varies from center to center. For a same biochemical profile, interpretation and reporting of results may differ, which can lead to misunderstandings and raises questions about the commutability of tests.MethodsWe obtained a description of (pre‐)analytical protocols and sample reports from 40 centers worldwide. A consensus approach allowed us to propose harmonized comments corresponding to the different CSF biomarker profiles observed in patients.ResultsThe (pre‐)analytical procedures were similar between centers. There was considerable heterogeneity in cutoff definitions and report comments. We therefore identified and selected by consensus the most accurate and informative comments regarding the interpretation of CSF biomarkers in the context of AD diagnosis.DiscussionThis is the first time that harmonized reports are proposed across worldwide specialized laboratories involved in the biochemical diagnosis of AD.
Nickel‐Mediated Enantioselective Photoredox Allylation of Aldehydes with Visible Light
Authors: Calogero Francesco , Potenti Simone , Bassan Elena , Fermi Andrea , Gualandi Andrea , Monaldi Jacopo , Dereli Busra , Maity Bholanath , Cavallo Luigi , Ceroni Paola , Cozzi Pier Giorgio 
Published: December 2021

AbstractHere we report a practical, highly enantioselective photoredox allylation of aldehydes mediated by chiral nickel complexes with commercially available allyl acetate as the allylating agent. The methodology allows the clean stereoselective allylation of aldehydes in good to excellent yields and up to 93 % e.e. using a catalytic amount of NiCl2(glyme) in the presence of the chiral aminoindanol‐derived bis(oxazoline) as the chiral ligand. The photoredox system is constituted by the organic dye 3DPAFIPN and a Hantzsch's ester as the sacrificial reductant. The reaction proceeds under visible‐light irradiation (blue LEDs, 456 nm) at 8–12 °C. Compared to other published procedures, no metal reductants (such as Zn or Mn), additives (e.g. CuI) or air‐sensitive Ni(COD)2 are necessary for this reaction. Accurate DFT calculations and photophysical experiments have clarified the mechanistic picture of this stereoselective allylation reaction.
Tuning Exciton Coupling of Merocyanine Nucleoside Dimers by RNA, DNA and GNA Double Helix Conformations
Authors: Dietzsch Julia , Bialas David , Bandorf Johannes , Würthner Frank , Höbartner Claudia 
Published: December 2021

AbstractExciton coupling between two or more chromophores in a specific environment is a key mechanism associated with color tuning and modulation of absorption energies. This concept is well exemplified by natural photosynthetic proteins, and can also be achieved in synthetic nucleic acid nanostructures. Here we report the coupling of barbituric acid merocyanine (BAM) nucleoside analogues and show that exciton coupling can be tuned by the double helix conformation. BAM is a nucleobase mimic that was incorporated in the phosphodiester backbone of RNA, DNA and GNA oligonucleotides. Duplexes with different backbone constitutions and geometries afforded different mutual dye arrangements, leading to distinct optical signatures due to competing modes of chromophore organization via electrostatic, dipolar, π–π‐stacking and hydrogen‐bonding interactions. The realized supramolecular motifs include hydrogen‐bonded BAM–adenine base pairs and antiparallel as well as rotationally stacked BAM dimer aggregates with distinct absorption, CD and fluorescence properties.
Nano‐synthesis, solid‐state structural characterization, and antimicrobial and anticancer assessment of new sulfafurazole azo dye‐based metal complexes for further pharmacological applications
Authors: Khedr Abdalla M. , El‐Ghamry Hoda A. , El‐Sayed Yusif S. 
Published: December 2021

AbstractA new azo dye ligand (abbreviated as H3L) derived from coupling of sulfafurazole diazonium salt with 2,4‐dihydroxybenzaldehyde was prepared and characterized applying different spectroscopic and analytical techniques. The novel nanosized trivalent Cr and Fe alongside with divalent Mn, Co, Ni, and Cd complexes with H3L have been synthesized for further promising pharmaceutical uses. All complexes were totally characterized by investigating various analytical and spectral tools such as microanalysis, FT‐IR, 1H NMR, UV‐Vis, powder XRD, and TEM spectra as well as magnetic moment and molar conductance measurements. Microanalysis, TGA, and conductance studies confirmed the formation of all metal complexes in 1:1 (L: M) molar ratio with covalent mode. The FT‐IR and 1H NMR investigation asserted the chelation of H3L to different metal ions through azo nitrogen and phenolic deprotonated hydroxy oxygen in the o‐position. UV‐Vis, ESR, and magnetic moment studies revealed octahedral geometry around Cr and Fe ions, whereas Mn, Co, Ni, and Cd complexes displayed tetrahedral configurations. XRD patterns and TEM images proved homogeneous distribution over the chelates surfaces and nanometric size of complexes particles. Molecular modeling was used to optimize the complexes' geometric structure showing good harmonity with the experimental results. The antifungal and antibacterial efficiencies were strongly enhanced upon complex formation. Cr(III) and Ni(II) complexes showed the strongest and promising anticancer activities (IC50 = 7.64 and 6.99 μg/ml) among the tested compounds, whereas Cd(II) complex showed moderate anticancer efficiency (IC50 = 12.10 μg/ml), compared with the 5‐fluorouracil (applied standard drug) with IC50 = 6.44 μg/ ml.
Inhibition of adhesion of CaCO3 scale by polydopamine/polytetrafluoroethylene coating with stability and anticorrosion properties
Authors: Wang Bing‐Bing , Wang Xin , Xu Zhi‐Ming , Zhao Qi , Wang Xiao‐Dong 
Published: December 2021

AbstractReduction of calcium carbonate (CaCO3) scale formation on the equipment surface is essential in a wide variety of industrial fields. In this work, polydopamine/polytetrafluoroethylene (PDA/PTFE) coating prepared by the simple immersion on stainless steel (SS) surfaces was developed to suppress the CaCO3 scale adhesion. The PDA/PTFE‐coated surface showed the higher hydrophobicity (water contact angle = 133.50°) and lower surface free energy (11.92 mN/m) than the stainless‐steel surface. The scale inhibiting rate of the coated surface was up to 76.8% after 12‐hour immersion in the CaCO3 solution in comparison with the untreated SS. More bubbles were observed on the PDA/PTFE‐coated surfaces, and the number of bubbles increased with increasing solution temperature leading to less area for the scale adhesion. As a result, the PDA/PTFE coated surfaces have the higher antiscale ability at the higher solution temperature. Furthermore, the stripping and electrochemical corrosion tests demonstrated that the PDA/PTFE coating has the better stability and anticorrosion ability. The PDA/PTFE coating with the superior properties has potential application for the long‐lasting reduction of the scale formation.
Observer‐based finite‐time congestion control for TCP/AQM network system with time‐varying delays and UDP flows
Authors: Shen Jindong , Jing Yuanwei , Ren Tao , Bai Yun 
Published: December 2021

AbstractIn this paper, the problem of observer‐based finite‐time congestion control for transmission control protocol (TCP)/active queue management (AQM) network systems with time‐varying delay and nonresponsive flows such as UDP is studied. The congestion control problem of TCP/AQM network system with time delay and external disturbances observer‐based finite‐time control is solved for the first time, and a theorem proved by the Lyapunov function of TCP/AQM network systems finite‐time bounded is given to ensure that the closed‐loop system is finite‐time bounded. Finally, the control gain and observer gain are obtained by linear matrix inequality (LMI) technique. Simulation results show the effectiveness and superiority of the proposed method.
Comparison of metabolic kinetics during high and low solids anaerobic digestion of fecal sludge
Authors: Kinyua Maureen , Stuart Kara 
Published: December 2021

AbstractHigh solids anaerobic digestion (HS‐AD) is an attractive energy‐producing technology; however, high total solids (TS) content may inhibit methanogens due to high volatile fatty acid (VFA) and total ammonia nitrogen concentrations. The objective of this paper is to quantify rate‐limiting metabolic kinetic parameters to determine the influence of TS content during anaerobic digestion of fecal sludge. Two TS content: 11% and 17% microcosms were analyzed. Good performance was observed in both systems, with volatile solid (VS) removal greater than 50%, CH4 yield between 0.44 and 0.56 m3 CH4/g VS added and cumulative CH4 production between 1.78 and 2.03 m3 CH4/m3 digester‐day. At 11% TS VFA consumption and VS removal had a positive correlation to CH4 production while the 17% TS microcosm had a negative correlation with both. This is the first study to determine the kinetic parameters for hydrolysis, VFA consumption, and methanogenesis during digestion of fecal sludge. These kinetic parameters are necessary in the design and operation of anaerobic digestion systems treating fecal sludge.
Fast Feet Forward: Early intervention protocol using bilateral movements to reduce stress and increase positive cognitions in adopted children with complex trauma presentation
Authors: Draper Ana , Marcellino Elisa , Ogbonnaya Comfort 
Published: December 2021

AbstractAdopted children are a vulnerable group that have often experienced multiple traumatic events such as maltreatment, neglect and the perpetuation of abuse. These early traumatic experiences can result in compromised resilience which impacts both psychological and biological development (Cicchetti & Banny, 2014). This study used the systemic model approach, method and technique to gain an understanding of the complexity of presentation and formulation being made (Harris & Burnham, 1985). It also expanded on an early intervention sports protocol, named fast feet forward, that was previously used with unaccompanied asylum‐seeking minors with significant results. The use of running as a bilateral stimulus resulted in a rise in VOC (validity of cognition) and a reduction in SUD (subjective units of distress) scores, both after a single session and after 12 sessions. The data reported from this study replicated the previous findings of Draper et al., 2020) and showed the benefits of using fast feet forward with adopted children. The results further evidence the potential efficacy of this protocol for adopted children displaying complex trauma and show promising results for future enquiry. Future research should aim to replicate these findings with a larger sample size.
Phytochemical Composition and Anti‐Aging Activity of Butanol Extract of Hedyotis diffusa in Caenorhabditis elegans
Authors: Li Jing , Liu Di , Li Danqing , Guo Yujie , Du Hongzhi , Cao Yan 
Published: December 2021

AbstractHedyotis diffusa Willd. (H. diffusa), a kind of traditional Chinese medicine, has been evaluated to potential display antioxidant and anti‐aging effects in vitro experiments. In this work, we investigated the effects on lifespan and stress resistance of the butanol extract from H. diffusa (NHD) in vivo using a Caenorhabditis elegans (C. elegans) model. The phytochemicals of NHD were identified by UPLC‐ESI‐qTOF‐MS/MS method. NHD‐treated wild‐type N2 worms showed an increase in survival time under both normal and stress conditions. Meanwhile, NHD promoted the healthspan of nematodes by stimulating growth and development, reducing the deposition of age pigment, increasing the activities of superoxide dismutase (SOD) and glutathione peroxidase dismutase (GSH‐Px), and decreasing the level of ROS without impairing fertility. Moreover, the upregulating of the expression of daf‐16, gst‐4, sod‐3, hsp12.6 genes and the downregulating of the expression of daf‐2 were involved in the NHD‐mediated lifespan extension. Finally, the increasing of the expression of GST‐4::GFP in CL2166 transgenic nematodes and the life‐span‐extending activity of NHD was completely abolished in daf‐2 and daf‐16 mutants further revealed that the potential roles for these genes in NHD‐induced longevity in C. elegans. Collectively, our findings suggest that NHD may have an active effect in healthy aging and age‐related diseases.
A novel nonsense variant in MED12 associated with malformations in a female fetus
Authors: Faergeman Soren Lejsted , Becher Naja , Andreasen Lotte , Christiansen Marianne , Frost Lise , Vogel Ida 
Published: December 2021

AbstractPathogenic variants in the MED12 gene located on the X‐chromosome have primarily been reported in males with Lujan‐Fryns syndrome, Ohdo syndrome and the Opits‐Kaveggia syndrome. However, earlier reports of female patients and female mice suggest that MED12 deficiency causes severe malformations. We report a novel example of a MED12 de novo nonsense variant in a female fetus with severe malformations identified by trio‐exome sequencing. This finding further expands the clinical spectrum of MED12‐related disorders, which is vital for prenatal diagnosis and genetic counselling of couples.
Chemoenzymatic Cascades Enabled by Combining Catalytically Active Emulsions and Biocatalysts
Authors: Sun Zhiyong , Zhao Qingcai , Haag Rainer , Wu Changzhu 
Published: December 2021

AbstractThe compartmentalization of chemo‐ and enzymatic reactions is an elegant strategy for one‐pot synthesis while avoiding reaction incompatibility issues. However, chemoenzymatic compartments developed to date are limited to complicated preparation. Herein, a simple, catalytically active polymer that stabilizes diverse types of emulsions for the encapsulation of active enzymes is presented. This design combines two distinct catalysts for cascade reaction while creating separate micro‐environments with a large interfacial area for high reactivity. Moreover, the system is developed for solvent‐free reactions, benefiting the “green” synthesis.