bluuebunny/crossref_metadata_2025_split huggingface dataset:
Outside-In Strategy for Peptide-Based Methacrylate and Methacrylamide Zwitterionic Cross-Linkers
Authors: Waynant Kristopher V. , Chakraborty Moubani 
Published: January 2022

AbstractPolyampholyte hydrogels have shown promise as functional biomaterial platforms with resistance to nonspecific protein adsorption (nonbiofouling). Yet there are few zwitterionic cross-linkers available to complement these materials and to provide an extended charge density throughout the 3D network. The recent development of peptide-based zwitterionic cross-linkers has shown merit. Indeed, the use of functionalizable amino acids permits the synthesis of a series of peptide-based zwitterionic methacrylate and methacrylamide cross-linkers. Methacrylate additions prior to peptide coupling provide an outside-in strategy when using natural l-serine or l-lysine as substrates to produce a series of methacrylate and methacrylamide combinations, expanding the library of peptide-based cross-linkers. Here, we describe the preparation of such dipeptide combinations as Ser-Lys, Lys-Ser, and Lys-Lys in zwitterionic bis(methacrylate/methacrylamide) cross-linkers. To highlight the utility of this method and its potential to increase the distance between zwitterionic components, syntheses of the tripeptide Lys-Gly-Lys dimethacrylamide and Ser-Gly-Ser dimethacrylate are reported.
Stereoselective Synthesis of Cyclohexane Derivatives: Tandem Lithium Iodide Mediated Intramolecular Conjugate Addition of Thiols to α,β-Bisenones
Authors: Seo SungYong , Jeon Minseok , Yun Chaeyoung 
Published: January 2022

AbstractA tandem intramolecular conjugate addition reaction was conducted with α,β-bisenones as selected Michael acceptors which were converted into 1,2,3-trisubstituted six-membered rings in the presence of activated sulfur nucleophiles. The products were obtained in good to excellent yields (maximum yield: 99%). Various substituted α,β-bisenones and sulfur nucleophiles were examined to understand the substrate scope of the reaction. Only one diastereomer was isolated, as lithium iodide mediated enolate trapping reactions improve the stereoselectivity of reactions involving 1,2,3-trisubstituted cyclohexanes.
Cascade Reaction of 3-Phenacylideneoxindoles with Trimethylsilyl Cyanide: Synthesis of Furan-Fused 1,3-Benzodiazepin-2-one Derivatives
Authors: Li Xiao-Juan , Ma Jing , Li Shao-Yi , Aisikaer Ailipire 
Published: January 2022

AbstractA cascade reaction of 3-phenacylideneoxindoles with trimethylsilyl cyanide is described. This method provides an efficient route for the synthesis of furan-fused 1,3-benzodiazepin-2-one derivatives by simply refluxing a reaction mixture of various 3-phenacylideneoxindoles with trimethylsilyl cyanide in the presence of H2O and K2CO3.
Synthetic Approach toward (–)-Tetrodotoxin via Construction of the Bicyclo[2.2.2]octane Skeleton
Authors: Fukuyama Tohru , Yokoshima Satoshi , Kobayashi Kazuki , Senoo Yoshiki , Toma Tatsuya 
Published: January 2022

AbstractA synthetic approach toward (–)-tetrodotoxin (TTX) is described. Our approach features a stereoselective construction of the TTX core structure using the bicyclo[2.2.2]octane skeleton which was constructed via intramolecular Diels–Alder reaction of an o-quinone monoketal having the key functional groups. The robust asymmetric synthesis was achieved by an iridium-catalyzed dynamic kinetic resolution (DKR) of the aryl vinyl carbinol that could be easily prepared from a simple aromatic compound.
Recurrent Blistering Skin Lesions and Reversible Monocular Abducens Paralysis in a Patient with CD59 Deficiency
Authors: Güngör Mesut , Demirsoy Evren , Güneş Ayfer Sakarya , Anık Yonca , Kara Bülent 
Published: January 2022

AbstractCongenital CD59 deficiency is an autosomal recessive disease characterized by mild-to-moderate chronic intravascular hemolysis, relapsing demyelinating peripheral neuropathies, and recurrent ischemic central nervous system strokes. We report a 2-year-old Turkish girl with a history of two episodes of Guillain-Barré syndrome-like acute weakness, reversible monocular abducens paralysis, and recurrent blistering skin lesions during periods of upper respiratory tract infections. Reversible monocular abducens palsy and recurrent blistering skin lesions have not been reported previously in cases of congenital CD59 deficiency.
What shapes local health system actors’ thinking and action on social inequalities in health? A meta-ethnography
Authors: McMahon Naoimh E. 
Published: January 2022

AbstractLocal health systems are increasingly tasked to play a more central role in driving action to reduce social inequalities in health. Past experience, however, has demonstrated the challenge of reorienting health system actions towards prevention and the wider determinants of health. In this review, I use meta-ethnographic methods to synthesise findings from eleven qualitative research studies that have examined how ambitions to tackle social inequalities in health take shape within local health systems. The resulting line-of-argument illustrates how such inequalities continue to be problematised in narrow and reductionist ways to fit both with pre-existing conceptions of health, and the institutional practices which shape thinking and action. Instances of health system actors adopting a more social view of inequalities, and taking a more active role in influencing the social and structural determinants of health, were attributed to the beliefs and values of system leaders, and their ability to push-back against dominant discourses and institutional norms. This synthesised account provides an additional layer of understanding about the specific challenges experienced by health workforces when tasked to address this complex and enduring problem, and provides essential insights for understanding the success and shortcomings of future cross-sectoral efforts to tackle social inequalities in health.
The calculated energies and charge and spin distributions of the excited GR1 state in diamond
Authors: Mackrodt William C. , Gentile Francesco S. , Dovesi Roberto 
Published: January 2022

This paper reports the energies and charge and spin distributions of both the vertically excited and fully relaxed GR1 states of the neutral singlet vacancy in diamond obtained from direct Δ-SCF calculations used previously to describe the low-lying excited states in AFII NiO and α-Al2O3. The calculations are based on the B3LYP functional in its standard form, with a C basis set that is identical to that which was used previously in numerous calculations of the ground state properties of defective diamond. Both the vertically excited and thermally relaxed GR1 states are predicted to be excitonic and insulating, with extensive re-distribution of charge and spin density and back-donation to the donor site. The present calculations suggest that the triplet state makes no contribution to the GR1 excitation. The predicted energy of the zero phonon line (1.57 eV) compares with the observed value of 1.67 eV, which also suggests that the GR1 state is neutral. The bandgaps lead to an estimate of the next higher (GR2) excited state energy, which is close to that found in the observed spectra. Similar calculations are used to predict the energies of the higher gap states at (5.0–5.5) eV, including the bulk value of 7.3 eV, which compares with the experimental value of (7.3–7.4) eV. An explanation is suggested as to why only the GR1 luminescence is observed. This paper also suggests an alternative channel for the recovery of the ground state in photoluminescence studies.
Nucleation of glucose isomerase protein crystals in a nonclassical disguise: The role of crystalline precursors
Authors: Van Driessche Alexander E. S. , Ling Wai Li , Schoehn Guy , Sleutel Mike 
Published: January 2022

Significance
The ability of proteins to self-assemble into complex, hierarchical structures has been the inspiration for the bottom-up design of a class of biomaterials with proteins as their building blocks. The earliest stages of formation often involve the passing of an activation barrier under the form of nucleus formation, a quaternary protein complex that templates incoming molecules to proper registry. For protein crystallization, the consensus has emerged that the fastest route toward a nucleus follows a winding path: first, densification, followed by symmetry formation. In this contribution, we show that this need not be the case for the protein glucose isomerase, which seems to follow the simplest path to a nucleus, making crystalline clusters from the earliest detectable beginnings.
In vitro cell cycle oscillations exhibit a robust and hysteretic response to changes in cytoplasmic density
Authors: Jin Minjun , Tavella Franco , Wang Shiyuan , Yang Qiong 
Published: January 2022

Significance
The cytoplasm, where most cellular reactions occur, has a variable density. We currently lack an understanding of how density variations affect cellular functions because of the challenge of controlling it experimentally. Here, we systematically modulate the density of an in vitro cytoplasm using microfluidics and analyze how the cell cycle behaves in turn. We found that mitotic cycles maintain their function across 0.2× to 1.2× of the natural density. Higher densities arrest cell cycles, and dilution recovers oscillations. However, the density at which cycles reappear is lower than the natural density. This behavior suggests a history-dependent mechanism called hysteresis, common in physics, chemistry, and engineering. Our approach paves the way for studying the responses of other processes to density changes.
Distinguishing the molecular diversity, nutrient content, and energetic potential of exometabolomes produced by macroalgae and reef-building corals
Authors: Wegley Kelly Linda , Nelson Craig E. , Petras Daniel , Koester Irina , Quinlan Zachary A. , Arts Milou G.I. , Nothias Louis-Felix , Comstock Jacqueline , White Brandie M. , Hopmans Ellen C. , van Duyl Fleur C. , Carlson Craig A. , Aluwihare Lihini I. , Dorrestein Pieter C. , Haas Andreas F. 
Published: January 2022

Significance
Marine dissolved organic matter (DOM) is one of the most complex and abundant chemical mixtures on earth, comprising thousands of different molecules. The molecular structure of these compounds is one factor structuring the community of microorganisms that metabolize them; in turn, this microbial metabolism mediates the composition of DOM. Decades of coral reef research has established the fundamental importance of microbial biogeochemistry in ecosystem function. This study unveils coral reef DOM by identifying a myriad of specific metabolite classes released into the surrounding waters by reef-building corals and algae, further characterizing their energetic and nutrient content and providing a foundation for linking benthic ecology with microbial processes that influence both the livelihood and demise of coral reefs.
Early life lead exposure from private well water increases juvenile delinquency risk among US teens
Authors: Gibson Jacqueline MacDonald , MacDonald John M. , Fisher Michael , Chen Xiwei , Pawlick Aralia , Cook Philip J. 
Published: January 2022

Significance
Public health agencies worldwide have determined that there is no safe level for children’s exposure to lead, a neurotoxin. This study shows that lead in drinking water from private wells is significantly associated with juvenile delinquency. Compared to children in homes with public water supplies, those relying on private wells have a 21% higher risk of any delinquency and a 38% increased risk of serious delinquency. The steepest increases in risk occur at the lowest exposure levels. The results highlight the need to prevent lead-leaching from well components, plumbing, and fixtures in the 13% of US households relying on private wells. They also suggest the need to decrease blood and environmental lead thresholds currently used to identify at-risk children.
Catalytic role of formaldehyde in particulate matter formation
Authors: Dovrou Eleni , Bates Kelvin H. , Moch Jonathan M. , Mickley Loretta J. , Jacob Daniel J. , Keutsch Frank N. 
Published: January 2022

SignificanceParticulate matter, often formed via cloud processing, strongly influences the Earth’s climate and air quality. Particle composition depends on anthropogenic and biogenic emissions. Thus, in order to understand climate change, knowledge of the difference between preindustrial and current conditions is critical. Under preindustrial conditions, multifunctional organic hydroperoxides, which are strong oxidants and have the ability to contribute to particulate matter formation, are in higher concentrations in the atmosphere. In this work, we focus on the previously unknown importance of hydroxymethyl hydroperoxide, which can be formed by gas-phase reactions and in-cloud reaction of hydrogen peroxide with the simplest aldehyde, formaldehyde, revealing the catalytic role of formaldehyde, and demonstrate that this chemistry is of great importance for particle formation.
Three small vesicular pools in sequence govern synaptic response dynamics during action potential trains
Authors: Tran Van , Miki Takafumi , Marty Alain 
Published: January 2022

Significance
Short-term changes in the strength of synaptic connections underlie many brain functions. The strength of a synapse in response to subsequent stimulation is largely determined by the remaining number of synaptic vesicles available for release. We developed a methodological approach to measure the dynamics of various vesicle pools following synaptic activity. We find that the readily releasable pool, which comprises vesicles that are docked or tethered to release sites, is fed by a small-sized pool containing approximately one to four vesicles per release site at rest. This upstream pool is significantly depleted even after a short stimulation train. Therefore, regulation of the size of the upstream pool emerges as a key factor in determining synaptic strength during and after sustained stimulation.
A nitroaromatic cathode with an ultrahigh energy density based on six-electron reaction per nitro group for lithium batteries
Authors: Chen Zifeng , Su Hai , Sun Pengfei , Bai Panxing , Yang Jixing , Li Mengjie , Deng Yunfeng , Liu Yang , Geng Yanhou , Xu Yunhua 
Published: January 2022

Significance
Organic electrode materials have shown great potential in lithium batteries in terms of easy synthesis, raw materials abundance, and environmental friendliness. However, the traditional organic electrodes typically experience single-electron reaction per active group, leading to limited specific capacities and energy densities. Herein, we report a battery chemistry of a nitroaromatic cathode, in which six-electron transfer occurs on each nitro group, resulting in an ultrahigh specific capacity and energy density, higher than all existing organic electrode materials and even most inorganic electrode materials.
(Re)conceptualizing “Language” in CLIL
Authors: Liu Jiajia Eve , Lin Angel M. Y. 
Published: January 2022

AbstractCLIL focuses on the integration of content learning and additional language learning. However, it is increasingly recognized that the re/presentation and communication of discipline-specific content involve not only language, but also other semiotic modes (such as visuals and gestures). This is accelerated by the advancement of digital technologies and multiplicity of communication channels in recent years. This article points out the urgent need to revisit and reconceptualize the roles of “language” in CLIL. It argues that, to prepare students for the multimodal communication landscape in today’s societies and to truly value their linguistic and semiotic diversity in learning, the “language” dimension in CLIL needs to be reconceptualized as a multimodal dimension, and CLIL classroom practices need to adopt an updated pedagogy of multiliteracies (New London Group, 1996) rather than focusing on “mere language” practice. The article reviews the recent development of theories and studies of multimodality and trans-semiotics and discusses their implications for what to teach and how to teach in today’s CLIL classrooms. It proposes the notions of translanguaging and trans-semiotizing to emphasize a dynamic and dialogic process of meaning (co)making process drawing on multiple linguistic and semiotic resources to enable students to both gain access to and critically engage in meaning/knowledge co-making/co-design. Ultimately, it aims at reconceiving CLIL to contribute to a more equitable school and classroom culture.
Second language acquisition of evidentiality in French and English in a narrative task
Authors: Leclercq Pascale , Mélac Eric 
Published: January 2022

AbstractEvidentiality, i.e. the linguistic encoding of the mode of access to information (direct perception, inference, hearsay), despite not being fully grammaticalized in English and French, is expressed through a variety of means. This paper seeks to determine how a relatively non-salient concept in the source and target languages can be acquired by L2 learners. Using an oral elicited narrative task, we determine what markers of direct perception and inference are commonly used by native speakers of French (n = 10) and English (n = 10) and L2 learners of those two languages (at three levels of proficiency,n = 10 per group), and at which level they emerge. Our results point to a much more frequent use of inferential markers than direct perception markers, to slightly different patterns of evidential marking in French and in English, and to a late emergence of evidential markers in the speech of learners, who display sensitivity to their discursive functions, with types and tokens increasing as a function of proficiency level.
Nominal determination in Moroccan Arabic
Authors: Maas Utz , Procházka Stephan 
Published: January 2022

AbstractMany studies on Moroccan Arabic presuppose the existence of a determination system organized along the lines of definiteness and indefiniteness. Hence, they postulate a ‘definite article’ with the form /l-/ and an ‘indefinite article’ as its counterpart in the form /waħd.l-/.This study shows that the so-called ‘definite article’ /l-/ is actually a general referential marker that mainly marks a noun as [−predicative]. The marker /l-/ and its augmented forms are specific and allow different readings ranging from anaphoric definiteness to specific indefiniteness. The marker /waħd.l-/ is less an ‘indefinite article’ but marks ‘mirativity’, i.e. pragmatic salience. Thus it often has a cataphoric function. Demonstratives are used in deictic function but also to evoke an already existing knowledge in the hearer. The system is extended by the referential marker /ʃi-/ restricted to mark non-specific items. The complexity of nominal determination is partly the result of the juxtaposition of typically Moroccan linguistic innovations and retentions of “common Arabic” structures.
Assessment of activity energy expenditure during competitive golf: The effects of bag carrying, electric or manual trolleys
Authors: Kasper Andreas M. , O'Donnell Amy , Langan‐Evans Carl , Jones Adam , Lindsay Alex , Murray Andrew , Close Graeme L. 
Published: January 2022

ABSTRACTGolf is a sport played around the globe, with an estimated 42.6 million people playing within the United Kingdom and United States of America alone. To date, there is limited data on the energy expenditure of golf. The present study assessed the activity energy expenditure (AEE) of 16 high‐standard (handicap under 5) golfers who completed three rounds of competitive golf either carrying the golf bag (BC), using a manual push trolley (MT) or an electric trolley (ET) (Stewart Golf, Gloucester, UK). Prior to each round, participants were fitted with an Actiheart® accelerometer (Camntech, Fenstanton, UK) to estimate AEE, whilst ratings of perceived exertion (RPE) and enjoyment were collected following each round. Data were analysed using a one‐way repeated measures ANOVA, with Hedges g effect sizes (ES) calculated. Mean (SD) AEE was 688 ± 213 kcal for BC, 756 ± 210 kcal for MT and 663 ± 218 kcal for ET (p = .05) although these differences were deemed small or less. The ET condition resulted in the lowest mean heart rate, moderate or very large from BC or MT, respectively. There were no significant differences in enjoyment although perceived exertion was lowest in the ET condition. In summary, we report meaningful differences in AEE between the three conditions (p = .05), with perceived exertion and maximum HR being lowest when using the electric trolley. Golf may be considered as an effective intervention to increase step count and improve physical activity levels across the general population regardless of transportation methods of clubs.
Pentaheptite diamond: a new carbon allotrope
Authors: Zhang Chuang , Yang Xigui , Lv Ruoyun , Lv Chaofan , Qin Jinxu , Liu Hang , Zang Jinhao , Dong Lin , Shan Chong-Xin 
Published: January 2022

Abstract
The search for sp
3-hybridized carbon allotropes other than diamond has attracted extensive interest because of their fascinating properties. In this paper, an orthorhombic carbon phase in sp
3 bonding, named pentaheptite diamond, by combining the particle swarm optimization method with first-principles calculations has been predicted. The phonon spectra, total energy and elastic constants calculations of the pentaheptite diamond confirm its dynamical, thermal and mechanical stability at zero pressure, respectively. It possesses a high bulk modulus of 385 GPa and Vickers hardness of 72.6 GPa, comparable to diamond. Electronic band structure calculations show that the pentaheptite diamond has a direct band gap of 4.18 eV.
Development of the temperature-dependent interatomic potential for molecular dynamics simulation of metal irradiated with an ultrashort pulse laser
Authors: Tanaka Yuta , Tsuneyuki Shinji 
Published: January 2022

Abstract
Laser ablation is often explained by a two-temperature model (TTM) with different electron and lattice temperatures. To realize a classical molecular dynamics simulation of the TTM, we propose an extension of the embedded atom method to construct an interatomic potential that is dependent on the electron temperature. This method is applied to copper, and its validity is demonstrated by comparison of several physical properties, such as the energy–volume curve, phonon dispersion, electronic heat capacity, ablation threshold, and mean square displacement of atoms, with those of finite-temperature density functional theory.
Iterative weighted fidelity and hybrid regularization-based algorithm for ECT
Authors: Cui Liqin , Tian Peng , Wang Chao , Jia Bin , Wang Yaoxuan , Qin Long , Deng Xiao , Zhang Li , Qin Jianmin 
Published: January 2022

Abstract
A new image reconstruction algorithm for electrical capacitance tomography based on iterative weighted fidelity and hybrid regularization is proposed. Specifically, an improved cost function model with the weighted data fidelity term and non-convex regularization term can better describe the sparsity of images and strengthen the anti-noises ability compared with the L1-norm or L2-norm regularization methods. In order to solve the proposed model efficiently, the alternating direction method of multipliers is used to divide the complex optimization problem into several simple iterative sub-problems. Moreover, the iterative shrinkage thresholding algorithm and the iterative p-shrinkage algorithm are also adopted to solve the sub-problems. Besides, simulation and experiments for different permittivity distributions are investigated with noise-free and noise-contaminated cases respectively. The research results verify that reconstruction images with the proposed algorithm have fewer artifacts and deformations, clearer edges, and better noise robustness than the other methods considered.