bluuebunny/crossref_metadata_2025_split huggingface dataset:
Thermally‐Drawn Multi‐Electrode Fibers for Bipolar Electrochemistry and Magnified Electrochemical Imaging
Authors: Iwama Tomoki , Guo Yuanyuan , Handa Shoma , Y. Inoue Kumi , Yoshinobu Tatsuo , Sorin Fabien , Shiku Hitoshi 
Published: November 2021

AbstractImaging systems using closed bipolar electrode (cBPE) arrays and electrochemiluminescence (ECL) have attracted great attention in recent years as a 2D imaging platform with high spatiotemporal resolution. However, the fabrication techniques for cBPE arrays involve complicated procedures. Therefore, a new fabrication scheme enabling the mass production of cBPE arrays with high precision, reproducibility, and yield, is desired. Here, the use of a versatile and scalable thermal drawing process as a novel fabrication method for fiber‐based cBPEs with feature sizes down to micro‐/nanoscales is proposed. First, a single‐electrode fiber consisting of a carbon‐based composite as the electrode material is produced by thermal drawing. The fundamental electrical properties of the single‐electrode fiber are characterized, and its applicability to the cBPE‐ECL system is demonstrated. A multielectrode fiber is fabricated by subjecting a bundle of 104 single‐electrode fibers to thermal drawing. Its usability as a cBPE array for ECL imaging is confirmed with a functional rate of 99%. Further the multielectrode fiber, utilizing the principle of thermal drawing, for magnified electrochemical imaging is tapered. This work establishes a novel mass‐production method for cBPE arrays, as well as a proof of concept for magnified electrochemical imaging using a thermally‐drawn electrode array fiber.
Cobalt‐Catalyzed Deoxygenative Hydroboration of Nitro Compounds and Applications to One‐Pot Synthesis of Aldimines and Amides
Authors: Gudun Kristina A. , Zakarina Raikhan , Segizbayev Medet , Hayrapetyan Davit , Slamova Ainur , Khalimon Andrey Y. 
Published: November 2021

AbstractThe commercially available and bench‐stable Co(acac)2 ligated with bis[(2‐diphenylphosphino)phenyl] ether (dpephos) was employed for selective room temperature hydroboration of nitro compounds with HBPin (TOF up to 4615 h−1), tolerating halide, hydroxy, amino, ether, ester, lactone, amide and heteroaromatic functionalities. These reactions offered a direct access to a variety of N‐borylamines RN(H)BPin, which were in situ treated with aldehydes and carboxylic acids to produce a series of aldimines and secondary carboxamides without the need for dehydrating and/or coupling reagents. Combination of these transformations in a sequential one‐pot manner allowed for direct and selective synthesis of aldimines and secondary carboxamides from readily available and inexpensive nitro compounds.magnified image
Update on the Synthesis of N‐Heterocycles via Cyclization of Hydrazones (2017–2021)
Authors: Lv Yunhe , Meng Jianping , Li Chen , Wang Xin , Ye Yong , Sun Kai 
Published: November 2021

AbstractHydrazones, as universal structural units, are useful synthons for the formation of carbon–nitrogen and nitrogen−heteroatom bonds. Thus, they provide new methods of constructing nitrogen‐containing heterocycles. In recent years, especially between 2017 and 2021, many efforts have been made to exploit hydrazone‐based reactions in efforts to develop more powerful and effective pathways towards the synthesis of various multifunctional heterocyclic compounds. However, despite the tremendous amount of work that has been published over the past five years, no review has been published that summarizes the significant progress in the preparation of nitrogen heterocycles via intramolecular cyclization of hydrazones with adjacent unsaturated bonds or intermolecular cyclization of hydrazones with unsaturated systems. Therefore, this review summarizes the hydrazone‐based cyclization strategies used to synthesize nitrogen‐containing heterocycles over the past five years. It discusses the corresponding reaction scopes, limitations, mechanisms, and problems.magnified image
Sortase‐vermittelte Multi‐Fragment‐Kopplung durch Ligationsstellen‐Schaltung
Authors: Bierlmeier Jan , Álvaro‐Benito Miguel , Scheffler Maren , Sturm Kristina , Rehkopf Luisa , Freund Christian , Schwarzer Dirk 
Published: November 2021

AbstractDie Sortase‐vermittelte Ligation (Engl. sortase‐mediated ligation, SML) ist ein effektives Werkzeug der Proteinchemie, welches die Ligation von Peptiden mit LPxTG‐Sortiermotiven und N‐terminalen Glycin‐Nukleophilen ermöglicht. Die Kopplung mehrerer Fragmente durch SML wird durch den erneuten Einbau eines Sortiermotivs in das Produkt verhindert. Hier beschreiben wir die Multi‐Fragment‐SML auf Grundlage von schaltbaren Sortase‐Substraten. Die Substitution des Leu‐Restes durch disulfidhaltiges Cys(StBu) führt zu aktiven Sortiermotiven, die durch Reduktion inaktiviert werden können. In Kombination mit einem photo‐geschützten N‐Gly‐Nukleophil wird Multi‐Fragment‐SML durch wiederholte Zyklen von SML und Ligationsstellenschaltung ermöglicht. Die Durchführbarkeit dieser Herangehensweise wurde durch eine Proof‐of‐Concept Vier‐Fragment‐Ligation, die Fertigung von Peptidsonden für bivalente chromatinbindende Proteine sowie die Oligomerisierung von Peptidantigenen nachgewiesen. Biochemische und immunologische Assays zeigten die Funktionalität dieser Sonden, was sie zu vielversprechenden Werkzeugen für die Immunologie und Chromatinbiochemie macht.
Vitamin D Inhibits the Early Aggregation of α‐Synuclein and Modulates Exocytosis Revealed by Electrochemical Measurements
Authors: Zhang Yue , Ji Wenliang , Zhang Shuai , Gao Nan , Xu Tianci , Wang Xiaofang , Zhang Meining 
Published: November 2021

AbstractAlpha‐synuclein (α‐Syn) localizes at presynaptic terminal and modulates synaptic functions. Increasing evidence demonstrate that α‐Syn oligomers, forming at the early of aggregation, are cytotoxic and is thus related to brain neurodegenerative diseases. Herein, we find that vitamin D (VD) can reduce neurocytotoxicity. The reduced neurocytotoxicity might be attributed to the less amount of large‐sized α‐Syn oligomers inhibited by VD, measured by electrochemical collision at single particle level, which are not observable with traditionally ensembled method. Single‐cell amperometry (SCA) results show that VD can recover the amount of neurotransmitter release during exocytosis induced by α‐Syn oligomers, further verifying the neuroprotection of VD. Our study reveals the neuroprotective role of VD through inhibiting α‐Syn aggregation, which is envisioned to be of great importance in treatment and prevention of the neurodegenerative diseases.
Stable Isotope Phosphate Labelling of Diverse Metabolites is Enabled by a Family of 18O‐Phosphoramidites**
Authors: Haas Thomas M. , Mundinger Stephan , Qiu Danye , Jork Nikolaus , Ritter Kevin , Dürr‐Mayer Tobias , Ripp Alexander , Saiardi Adolfo , Schaaf Gabriel , Jessen Henning J. 
Published: November 2021

AbstractStable isotope labelling is state‐of‐the‐art in quantitative mass spectrometry, yet often accessing the required standards is cumbersome and very expensive. Here, a unifying synthetic concept for 18O‐labelled phosphates is presented, based on a family of modified 18O2‐phosphoramidite reagents. This toolbox offers access to major classes of biologically highly relevant phosphorylated metabolites as their isotopologues including nucleotides, inositol phosphates, ‐pyrophosphates, and inorganic polyphosphates. 18O‐enrichment ratios >95 % and good yields are obtained consistently in gram‐scale reactions, while enabling late‐stage labelling. We demonstrate the utility of the 18O‐labelled inositol phosphates and pyrophosphates by assignment of these metabolites from different biological matrices. We demonstrate that phosphate neutral loss is negligible in an analytical setup employing capillary electrophoresis electrospray ionisation triple quadrupole mass spectrometry.
Quantifying Intracellular Single Vesicular Catecholamine Concentration with Open Carbon Nanopipettes to Unveil the Effect of L‐DOPA on Vesicular Structure
Authors: Hu Keke , Le Vo Kim Long , Hatamie Amir , Ewing Andrew G. 
Published: November 2021

AbstractUnderstanding the regulatory mechanisms of exocytosis is essential for uncovering the pathologies of neuronal disorders and developing related pharmaceuticals. In this work intracellular vesicle impact electrochemical cytometry (IVIEC) measurements with different‐sized (50–500 nm radius) open carbon nanopipettes (CNPs) were performed to quantify the vesicular content and release kinetics of specific vesicle populations grouped by orifice sizes. Intracellular vesicles with radius below 100 nm were captured and narrowed between 50 and 100 nm. On the basis of this, single vesicular catecholamine concentrations in the intracellular environment were quantified as 0.23–1.1 M. Our results with L‐3,4‐dihydroxyphenylalanine (L‐DOPA)‐exposure indicate that L‐DOPA regulates exocytosis by increasing the dense core size and vesicular content while catecholamine concentrations did not show obvious alterations. These were all achieved simultaneously and relatively noninvasively with open CNPs.
Air‐Stable PdI Dimer Enabled Remote Functionalization: Access to Fluorinated 1,1‐Diaryl Alkanes with Unprecedented Speed
Authors: Kundu Gourab , Opincal Filip , Sperger Theresa , Schoenebeck Franziska 
Published: November 2021

AbstractWhile remote functionalization via chain walking has the potential to enable access to molecules via novel disconnections, such processes require relatively long reaction times and can be in need of elevated temperatures. This work features a remote arylation in less than 10 min reaction time at room temperature over a distance of up to 11 carbons. The unprecedented speed is enabled by the air‐stable PdI dimer [Pd(μ‐I)(PCy2tBu)]2, which in contrast to its PtBu3 counterpart does not trigger direct coupling at the initiation site, but regioconvergent and chemoselective remote functionalization to yield valuable fluorinated 1,1‐diaryl alkanes. Our combined experimental and computational studies rationalize the origins of switchability, which are primarily due to differences in dispersion interactions.
Rigid Bridge‐Confined Double‐Decker Platinum(II) Complexes Towards High‐Performance Red and Near‐Infrared Electroluminescence
Authors: Zhang Youming , Miao Jingsheng , Xiong Jinfan , Li Kai , Yang Chuluo 
Published: November 2021

AbstractA molecular design to high‐performance red and near‐infrared (NIR) organic light‐emitting diodes (OLEDs) emitters remains demanding. Herein a series of dinuclear platinum(II) complexes featuring strong intramolecular Pt⋅⋅⋅Pt and π–π interactions has been developed by using N‐deprotonated α‐carboline as a bridging ligand. The complexes in doped thin films exhibit efficient red to NIR emission from short‐lived (τ=0.9–2.1 μs) triplet metal‐metal‐to‐ligand charge transfer (3MMLCT) excited states. Red OLEDs demonstrate high maximum external quantum efficiencies (EQEs) of up to 23.3 % among the best PtII‐complex‐doped devices. The maximum EQE of 15.0 % and radiance of 285 W sr−1 m−2 for NIR OLEDs (λEL=725 nm) are unprecedented for devices based on discrete molecular emitters. Both red and NIR devices show very small efficiency roll‐off at high brightness. Appealing operational lifetimes have also been revealed for the devices. This work sheds light on the potential of intramolecular metallophilicity for long‐wavelength molecular emitters and electroluminescence.
Photocleavable Fluorescent Membrane Tension Probes: Fast Release with Spatiotemporal Control in Inner Leaflets of Plasma Membrane, Nuclear Envelope, and Secretory Pathway
Authors: López‐Andarias Javier , Eblighatian Krikor , Pasquer Quentin T. L. , Assies Lea , Sakai Naomi , Hoogendoorn Sascha , Matile Stefan 
Published: November 2021

AbstractMechanosensitive flipper probes are attracting interest as fluorescent reporters of membrane order and tension in biological systems. We introduce PhotoFlippers, which contain a photocleavable linker and an ultralong tether between mechanophore and various targeting motifs. Upon irradiation, the original probe is released and labels the most ordered membrane that is accessible by intermembrane transfer. Spatiotemporal control from photocleavable flippers is essential to access open, dynamic or elusive membrane motifs without chemical or physical interference. For instance, fast release with light is shown to place the original small‐molecule probes into the innermost leaflet of the nuclear envelope to image changes in membrane tension, at specific points in time of membrane trafficking along the secretory pathway, or in the inner leaflet of the plasma membrane to explore membrane asymmetry. These results identify PhotoFlippers as useful chemistry tools to enable research in biology.
Toward role of westerly‐monsoon interplay in linking interannual variations of late spring precipitation over the southeastern Tibetan Plateau
Authors: Song Chengyu , Wang Jing , Liu Yanju , Zhang Ling , Ding Yihui , Li Qiaoping , Shen Xinyong , Song Yanling , Yan Yuping 
Published: November 2021

AbstractA recent study reported a notable westerly‐monsoon interplay (WMI) to the northeast of the Tibetan Plateau in boreal summer. However, this study introduces another striking and unique WMI over the southeastern TP (SETP) in late spring (May), emphasizing the critical roles of the upstream mid‐latitude westerly and the downstream Bay of Bengal (BOB) summer monsoon (BOBSM) in linking interannual variations of precipitation over SETP. In this study, the research SETP domain (22.5°–27.5°N, 87.5°–97.5°E) as well as a westerly index (WI) over the pivotal upstream westerly domain (22.5°–30°N, 65°–80°E) and a monsoon index (MI) over the pivotal downstream BOBSM domain (12.5°–22.5°N, 87.5°–100°E) are defined to investigate connections between the westerly and BOBSM and their combined effects on precipitation over SETP. The results indicate that the mid‐latitude westerly and BOBSM show opposite effects on precipitation over SETP. The weaker westerly and the stronger BOBSM correspond to enhanced SETP precipitation, and vice versa. The enhanced BOBSM acts as a predominant role on the strengthening of precipitation, while the decelerated westerly plays a secondary dynamical amplification role. To quantify their synergistic roles in linking SETP precipitation, a WMI index is defined. Statistical analysis suggests that this newly defined WMI index has a higher positive correlation with the precipitation over SETP. The correlation has a prominent increase compared to individual correlations between WI/MI and SETP precipitation, and dynamic conditions in high WMI index years are more favorable for the formation of SETP precipitation. The possible mechanism is that the BOBSM southerly strengthens and the southern branch of the upstream mid‐latitude westerly weakens in high WMI index years, resulting in an anomalous cyclone over the northwestern BOB and an anomalous anticyclone over the western TP. The anomalous cyclone resembles a Rossby wave response to the increased precipitation over SETP, and the precipitation in turn contributes to maintaining the BOB cyclonic anomaly and the above anticyclonic anomaly via the latent heating release. This positive feedback effect is conducive to enhanced SETP precipitation.
More autosomal dominant SPG18 cases than recessive? The first AD‐SPG18 pedigree in Chinese and literature review
Authors: Chen Shuai , Zou Jin‐Long , He Shuang , Li Wei , Zhang Jie‐Wen , Li Shu‐Jian 
Published: November 2021

AbstractObjectiveHereditary spastic paraplegia (HSP) due to ERLIN2 gene mutations was designated as spastic paraplegia 18 (SPG18). To date, SPG18 families/cases are still rarely reported. All early reported cases shared the autosomal recessive (AR) inheritance pattern. Over the past 3 years, autosomal dominant (AD) or sporadic SPG18 cases had been continuously reported. Here, we reported the clinical and genetic features of the first autosomal dominant SPG18 pedigree in Chinese.MethodsWe conducted detailed medical history inquiry, neurological examinations of the proband and his family members, and charted the family tree. The proband underwent brain and cervical magnetic resonance imaging (MRI), electromyography (EMG), and whole exome sequencing. Sanger sequencing was performed to verify the genetic variation in the proband and some family members. A literature review of all reported SPG18 families/cases was carried out to summarize the clinical‐genetic characteristics of SPG18 under different inheritance patterns.ResultsFour patients were clinically diagnosed as chronic spastic paraplegia in three consecutive generations with the autosomal dominant inheritance model. All the patients presented juvenile‐adolescent onset and gradually worsening pure HSP phenotype. Clinical phenotypes were consistent within the family. Whole exome sequencing in the proband identified a previously reported heterozygous c.502G > A (p.V168M) mutation in exon 8 of ERLIN2 gene. This mutation was cosegregated with the phenotype in the family and was classified as likely pathogenic according to American College of Medical Genetics and Genomics (ACMG) guidelines. To date, eight AR‐SPG18 families, five AD‐SPG18 families, and three sporadic cases had been reported. Clinical phenotype of AD‐SPG18 was juvenile‐adolescent onset pure HSP, while the phenotype of AR‐SPG18 was mostly complicated HSP with earlier onset and more severe conditions. In rare cases, the initial spastic paraplegia could evolve to rapidly progressive amyotrophic lateral sclerosis (ALS).ConclusionsWe reported the first autosomal dominant SPG18 pedigree in Chinese Han population, which added more pathogenic evidence for V168M mutation. As more SPG18 cases reported, the essentials of SPG18 need to be updated in clinical practice. Special attentions should be given in gene test for upper motor neuron disorders in case of missing heterozygous mutations in ERLIN2.
Reinforcing or counterproductive behaviors for sustainable entrepreneurship? The influence of causation and effectuation on sustainability orientation
Authors: Johnson Matthew P. , Hörisch Jacob 
Published: November 2021

AbstractEffectuation, as an emerging theoretical approach in entrepreneurship, is receiving increasing attention in research and practice. Still, the integration of effectuation in sustainable entrepreneurship literature is sparse, and its influence on the sustainability orientation of ventures has so far not been examined in the academic literature. This article, therefore, investigates the influence that causal and effectual behaviors have on the sustainability orientation of established entrepreneurial ventures. This is important to consider, especially if entrepreneurial behaviors were to influence sustainability orientation negatively, this could potentially thwart the venture's ability to create lasting sustainability value. Based on a quantitative survey among 140 sustainable ventures, we find support for the hypothesis that causal behaviors reinforce sustainability orientation. We demonstrate that effectual behaviors exert a positive influence on sustainability orientation as well. Thus, the experimentation and flexibility of goals that ventures possess reflect that effectual behaviors are not at the expense of sustainability orientation. These results can inform sustainable entrepreneurs and educators to use both behaviors purposefully and highlight causal and effectual behaviors are equally important elements for sustainable entrepreneurship education.
Sustainability risk and portfolio management—A strategic scenario method for sustainable product development
Authors: Villamil Carolina , Schulte Jesko , Hallstedt Sophie 
Published: November 2021

AbstractCompanies need to strategically develop their portfolio and find the balance between being proactive and passive in relation to sustainability. In this study, a strategic perspective based on backcasting from overarching socio‐ecological sustainability principles was used as a lens to understand how companies might adapt their product portfolios to avoid threats and exploit opportunities on increasingly sustainability‐driven markets. The study shows that sustainability performance, market success, and time are key areas to be considered in the product portfolio process to ensure short‐term profitability and long‐term competitiveness. A novel method was developed and tested in one academic group and two companies to explore how such a strategic sustainability perspective can support the product portfolio process in practice. The results indicate that the strategic layered double‐flow scenario method, including different time horizons, was supportive in identifying opportunities and avoid risks in the sustainable development process at the company.
Age‐specific prevalence of human papillomavirus and abnormal cytology at baseline in a diverse statewide prospective cohort of individuals undergoing cervical cancer screening in Mississippi
Authors: Clarke Megan A. , Risley Carolann , Stewart Mary W. , Geisinger Kim R. , Hiser Laree M. , Morgan Jody C. , Owens Kenyata J. , Ayyalasomayajula Krishna , Rives Rhonda M. , Jannela Ashish , Grunes Dianne E. , Zhang Lei , Schiffman Mark , Wagner Sarah , Boland Joseph , Bass Sara , Wentzensen Nicolas 
Published: November 2021

AbstractBackgroundMississippi (MS) has among the highest rates of cervical cancer incidence and mortality in the United States, with disproportionately higher rates among Blacks compared to Whites. Here, we evaluate the prevalence of high‐risk human papillomavirus (HPV) and abnormal cytology in a representative baseline sample from a diverse statewide cohort of individuals attending cervical screening in MS from the STRIDES Study (STudying Risk to Improve DisparitiES in cervical cancer).MethodsWe included individuals aged 21–65 years undergoing screening at the University of Mississippi Medical Center (UMMC) and the Mississippi State Department of Health (MSDH) from May to November 2018. We calculated age‐specific HPV prevalence, overall and by partial HPV16/18 genotyping, and abnormal cytology by race.ResultsA total of 6871 individuals (mean age 35.7 years) were included. HPV prevalence was 25.6% and higher in Blacks (28.0%) compared to Whites (22.4%). HPV prevalence was significantly higher in Blacks aged 21–24 years (50.2%) and 30–34 years (30.2%) compared to Whites in the same age groups (32.1% and 20.7%; p < 0.0001, respectively). The prevalence of high‐grade cytologic abnormalities, a cytologic sign of cervical precancer, peaked earlier in Blacks (ages 25–29) compared to Whites (35–39). For comparison, we also analyzed HPV prevalence data from the National Health and Nutrition Examination Survey (NHANES, 2013–2016) and observed similar racial differences in HPV prevalence among women aged 21–24 years.ConclusionsOur findings suggest that Blacks undergoing cervical cancer screening in MS have higher prevalence of other high‐risk 12 HPV types at younger ages and experience an earlier peak of high‐grade cytologic abnormalities compared to Whites.