bluuebunny/crossref_metadata_2025_split huggingface dataset:
Interfacial Engineering for Highly Stable and Stretchable Electrodes Enabled by Printing/Writing Surface‐Embedded Silver and Its Selective Alloying with Liquid Metals
Authors: Liu Zelin , Chen Song , Zhang Guangyong , Shi Hang , Chen Xiaochan , Shi Wei , Liu Lan 
Published: February 2022

AbstractEven though intrinsically stretchable liquid metals (LMs) have been widely used in the stretchable electrodes for improving the stretchability, it is still challenging to achieve stable interfaces in these electrodes. A usual approach of adhering the LMs on a substrate is to modify the LMs with an organic surfactant, which is easily ruptured under a dynamic deformation. Herein, a surface‐embedded silver and its selective alloying of LMs are reported to address this problem. Typically, the surface‐embedding structure and the alloying interaction are both robust and stretchable, enabling the high interfacial stability during deformation (the ability to resist peeling, scratching, and sonication). And the cracked silver layer under tensile strains can be well bridged by LMs, enabling the good conducting stability during deformation (resistance change of 0.076 at 50% strain, 0.18 at 100% strain, and 0.4 at 200% strain). It is noted that this interfacial engineering can be facilely organized by directly printing or writing, which is convenient for preparing customized electrodes and circuits. At last, a light‐emitting diode array and a drone remote controller are assembled using the stretchable electrodes, showing their advantages in practical application.
Using δ15N to screen for nitrogen fixation: Reference plant position and species
Authors: Cox Amanda , Boots‐Haupt Laura , Brasier Kyle , Riar Ranjit , Zakeri Hossein 
Published: February 2022

AbstractThe δ15N natural abundance technique is frequently used to quantify the proportion of legume nitrogen derived from atmospheric fixation (%Ndfa). This method compares the δ15N of a legume with a nonlegume reference plant to estimate the %Ndfa. For accurate estimations, it is recommended to pair each legume plot with a nonlegume reference plant to account for spatial variation. However, this pairing scheme is not feasible in large screening trials. Here, we tested the feasibility of eliminating reference plants to screen a faba bean (Vicia faba L.) population for %Ndfa. The first experiment screened 63 faba bean genotypes for %Ndfa by comparing estimates derived from an adjacent wheat (Triticum aestivum L.) reference plant in a nearest neighbor scheme (NN) with an arbitrary δ15N reference value (AR) of 7‰. Average and standard deviation of the genotypes’ %Ndfa were 58 ± 13% in 2019 and 72 ± 8% in 2020 using the NN model and 61 ± 11% in 2019 and 75 ± 7% in 2020 using the AR model. The AR model was able to identify a majority of the high and low %Ndfa genotypes in both years. In a second study, wheat and a dicot weed within the field were used as reference plants to estimate the %Ndfa. The weed reference plant resulted in 3 to 13% higher %Ndfa values compared with the wheat in three out of four testing environments, but the variation did not alter ranking of the genotypes for %Ndfa.
Promoting early management of frailty in the new normal: An updated software tool in addressing the need of virtual assessment of frailty at points of care
Authors: Sepehri Katayoun , Low Hilary , Hoang Jenny , Park Grace , Song Xiaowei 
Published: February 2022

AbstractIntroductionFrailty is a state of diminished physiological reserve and can be assessed using the frailty index. Early management of frailty is crucial for preventing adverse outcomes. Intended for assessing home‐living older adults, the initial release of the eFI‐CGA software was prior to the coronavirus disease 2019 (COVID‐19) pandemic.MethodsIn addressing the increased need of virtual assessment, the eFI‐CGA was upgraded to version 3.0. In this paper, we introduce the updated electronic frailty assessment tool, reporting the newly developed features and validating its use.ResultsEnd‐user experiences with the previous versions are discussed. The updated features include a search function to resume disrupted assessments. The improved user interface enabled clinicians to record care management details.ConclusionThis study represents an example of software solutions in moving from disruption to transformation, benefiting healthcare for older adults during this challenging time.
Small bowel bleeding treated successfully with transcatheter arterial embolization with imipenem/cilastatin
Authors: Arima Takahiro , Morimoto Kohei , Terai Kiyoshi , Kawamoto Ken , Muroya Ken , Koba Yuji , Omura Takashi 
Published: February 2022

BackgroundSmall bowel bleeding is an uncommon cause of lower gastrointestinal bleeding, which may require different management.Case PresentationA 37‐year‐old man presenting with hematochezia was promptly diagnosed with small bowel bleeding by computed tomography angiography. Transcatheter arterial embolization was carried out because the patient's hemodynamic status deteriorated. Hemostasis was achieved by embolization with imipenem/cilastatin, although superselective embolization failed. Capsule endoscopy revealed multiple ulcers and erosions. Drug‐induced small bowel injury was suspected to be the cause of small bowel bleeding.ConclusionComputed tomography angiography can facilitate the management of lower gastrointestinal bleeding. Considering transcatheter arterial embolization and choosing an optimal embolic agent depending on the situation are important in the management of hemodynamically unstable patients.
Multiple Emission of Phosphonium Fluorophores Harnessed by the Pathways of Photoinduced Counterion Migration
Authors: Belyaev Andrey , Su Bo‐Kang , Cheng Yu‐Hsuan , Liu Zong‐Ying , Khan Nasrulla Majid , Karttunen Antti J. , Chou Pi‐Tai , Koshevoy Igor O. 
Published: February 2022

AbstractIn the emerging field of intramolecular charge transfer induced counterion migration, we report the new insights into photophysical features of luminescent donor–acceptor phosphonium dyes (D−π−)nA+[X−] (π=−(C6H4)x−). The unique connectivity of the phosphorus atom affords multipolar molecules with a variable number of arms and the electronic properties of the acceptor group. In the ion‐paired form, the transition from dipolar to quadrupolar configuration enhances the low energy migration‐induced band by providing the additional pathways for anion motion. The multipolar architecture, adjustable lengths of the π‐spacers and the nature of counterions allow for efficient tuning of the emission and achieving nearly pure white light with quantum yields around 30 %. The methyl substituent at the phosphorus atom reduces the rate of ion migration and suppresses the red shifted bands, simultaneously improving total emission intensity. The results unveil the harnessing of the multiple emission of phosphonium fluorophores by anion migration via structure and branching of donor–acceptor arms.
Synthesis of a π‐Extended Azacorannulenophane Enabled by Strain‐Induced 1,3‐Dipolar Cycloaddition
Authors: Zhang Xinjiang , Mackinnon Marc R. , Bodwell Graham J. , Ito Shingo 
Published: February 2022

AbstractThe first example of a cyclophane bearing a nitrogen‐containing buckybowl was synthesized via sequential 1,3‐dipolar cycloaddition and palladium‐catalyzed intramolecular cyclization. The key to the successful synthesis is the strain‐induced 1,3‐dipolar cycloaddition of a polycyclic aromatic azomethine ylide to theK‐region of [7](2,7)pyrenophane. The resulting π‐extended azacorannulenophane exhibits intriguing structural and physical properties, including unique variation of bowl depth, extraordinarily high‐field chemical shifts in its1H NMR spectrum, a decreased HOMO–LUMO gap, and a red shift in the absorption/emission spectrum, when compared to those of the parent azacorannulene. These characteristics are derived from both the π‐extension to the polycyclic aromatic system in the cyclophane structure and the increased curvature enforced by the seven‐carbon aliphatic chain.
From Structural Design to Functional Construction: Amine Molecules in High‐Performance Formamidinium‐Based Perovskite Solar Cells
Authors: Fu Chunpeng , Gu Zhenkun , Tang Yan , Xiao Qian , Zhang Shasha , Zhang Yiqiang , Song Yanlin 
Published: February 2022

AbstractFormamidinium (FA) based perovskites are considered as one of the most promising light‐absorbing perovskite materials owing to their narrower band gap and better thermal stability compared to conventional methylammonium‐based perovskites. Constant improvement by using various additives stimulates the potential application of these perovskites. Amine molecules with different structures have been widely used as typical additives in FA‐based perovskite solar cells, and decent performances have been achieved. Thus, a systematic review focusing on structural regulation and functional construction of amines in FA‐based perovskites is of significance. Herein, we analyze the construction mechanism of different structural amines on the functional perovskite crystals. The influence of amine molecules on specific perovskite properties including defect conditions, charge transfer, and moisture resistance are evaluated. Finally, we summarize the design rules of amine molecules for the application in high‐performance FA‐based perovskites and propose directions for the future development of additive molecules.
A Calix[3]acridan‐Based Host–Guest Cocrystal Exhibiting Efficient Thermally Activated Delayed Fluorescence
Authors: Zhou He‐Ye , Zhang Da‐Wei , Li Meng , Chen Chuan‐Feng 
Published: February 2022

AbstractA supramolecular strategy to construct thermally activated delayed fluorescence (TADF) materials through host–guest charge transfer interactions was proposed. Consequently, a new class of macrocycle namely calix[3]acridan was conveniently synthesized in 90 % yield. The host–guest cocrystal formed by calix[3]acridan and 1,2‐dicyanobenzene exhibited efficient TADF properties due to intense intermolecular charge transfer interactions. Moreover, the spatially separated highest occupied molecular orbital and lowest unoccupied molecular orbital resulted in a very small singlet–triplet energy gap of 0.014 eV and hence guaranteed an efficient reverse intersystem crossing for TADF. Especially, a high photoluminescence quantum yield of 70 % was achieved, and it represents the highest value among the reported intermolecular donor–acceptor TADF materials.
Elektrochemische Carborankäfig‐Aktivierung
Authors: Yang Long , Zhang Zi‐Jing , Bongsuiru Jei Becky , Ackermann Lutz 
Published: February 2022

AbstractCarborane sind Bor‐Kohlenstoff‐Molekülcluster, welche einzigartige Eigenschaften aufweisen, wie ihre ikosaedrische Geometrie, einen hohen Bor‐Anteil und eine dreidimensional delokalisierte Aromatizität. Diese machen Carborane zu wertvollen Bausteinen in verschiedenen Anwendungsbereichen, wie supramolekularem Design, Nanomaterialien, Optoelektronik, Bor‐Neutroneneinfangtherapeutika (BNCT) und metallorganischer sowie Koordinationschemie. Trotz weitreichender Fortschritte auf diesem Forschungsgebiet werden stöchiometrische Mengen chemischer Redox‐Reagenzien weiterhin für die oxidative Aktivierung der Carborankäfige benötigt. In diesem Kontext ist die elektrochemische Synthese eine vielversprechende und nachhaltige Alternative. In den vergangenen Jahren konnte erheblicher Fortschritt in der elektrochemischen Käfig‐Funktionalisierung an Carboranen erzielt werden, welcher hier zusammengefasst wurde. Wir erwarten, dass die Elektrokatalyse innerhalb der aktuellen Renaissance der Carboran‐Elektrochemie einen immer stärkeren Impuls geben wird.
Hierarchical Assembly of Coordination Macromolecules with Atypical Geometries: Gd44Co28 Crown and Gd95Co60 Cage
Authors: Du Ming‐Hao , Wang Dong‐Hui , Wu Ling‐Wei , Jiang Lin‐Peng , Li Jun‐Ping , Long La‐Sheng , Zheng Lan‐Sun , Kong Xiang‐Jian 
Published: February 2022

AbstractThe discovered giant clusters are always highly symmetric owing to the spontaneous assembly of one or two basic units. Herein we report the Gd44Co28 crown and Gd95Co60 cage, formulated as [Gd44Co28(IDA)20 (OH)72(CO3)12(OAc)28(H2O)64]⋅(ClO4)24 and [Na4Gd95 Co60(IDA)40(OH)150(CO3)40(OAc)58(H2O)164] ⋅ (ClO4)41 (H2IDA=iminodiacetic acid), respectively, by providing a library containing multiple low‐nuclearity units. The heart‐like units and crown‐like tetramer found in both compounds indicate unprecedented assembly levels, leading to an atypical geometry characteristic compared to the giant clusters directly assembled by regular units. These two clusters not only significantly increase the size of Ln−Co clusters but also exhibit the enhanced magnetic entropy change at ultra‐low temperatures. This work provided an effective way to fabricate cluster compounds with giant size and geometry complexity simultaneously.
Ceria‐Supported Gold Nanoparticles as a Superior Catalyst for Nitrous Oxide Production via Ammonia Oxidation
Authors: Tang Zhenchen , Surin Ivan , Rasmussen Asbjörn , Krumeich Frank , Kondratenko Evgenii V. , Kondratenko Vita A. , Pérez‐Ramírez Javier 
Published: February 2022

AbstractThe production of nitrous oxide, N2O, via NH3 oxidation is not on a practical scale due to the lack of a suitable catalyst. Instead, it is produced via thermal decomposition of NH4NO3, rendering N2O too costly and limiting its prospective uses. Herein, we report CeO2‐supported Au nanoparticles (2–3 nm) as a highly selective catalyst for low‐temperature NH3 oxidation to N2O, exhibiting two orders of magnitude higher space–time yield than the state‐of‐the‐art Mn−Bi/α‐Al2O3 and remarkable stability over 70 h on stream. The reaction proceeds via a Mars–van Krevelen mechanism, with the density of interfacial Auδ+ species and the oxygen storage capacity of CeO2 identified as the key performance descriptors. The latter could be enhanced by cobalt doping, improving the catalytic activity and setting a new benchmark for N2O productivity. These findings establish NH3 oxidation as an efficient process for N2O manufacture and facilitate its broader utilization in selective oxidations.
Nickel‐Catalyzed Intermolecular Asymmetric Addition of Aryl Iodides across Aldehydes
Authors: Zhu Ziqi , Xiao Jieshuai , Li Mingjie , Shi Zhuangzhi 
Published: February 2022

AbstractEnantioenriched alcohols comprise much of the framework of organic molecules. Here, we first report that chiral nickel complexes can catalyze the intermolecular enantioselective addition of aryl iodides across aldehydes to provide diverse optically active secondary alcohols using zinc metal as the reducing agent. This method shows a broad substrate scope under mild reaction conditions and precludes the traditional strategy through the pre‐generation of organometallic reagents. Mechanistic studies indicate that an in situ formed arylnickel, instead of an arylzinc, adds efficiently to aldehydes, forming a new C−C bond and a chiral nickel alkoxide that may be turned over by zinc powder.
Linker Molecules Convert Commercial Fluorophores into Tailored Functional Probes during Biolabelling
Authors: Zhang Lei , Isselstein Michael , Köhler Jens , Eleftheriadis Nikolaos , Huisjes Nadia M. , Guirao‐Ortiz Miguel , Narducci Alessandra , Smit Jochem H. , Stoffels Janko , Harz Hartmann , Leonhardt Heinrich , Herrmann Andreas , Cordes Thorben 
Published: February 2022

AbstractMany life‐science techniques and assays rely on selective labeling of biological target structures with commercial fluorophores that have specific yet invariant properties. Consequently, a fluorophore (or dye) is only useful for a limited range of applications, e.g., as a label for cellular compartments, super‐resolution imaging, DNA sequencing or for a specific biomedical assay. Modifications of fluorophores with the goal to alter their bioconjugation chemistry, photophysical or functional properties typically require complex synthesis schemes. We here introduce a general strategy that allows to customize these properties during biolabelling with the goal to introduce the fluorophore in the last step of biolabelling. For this, we present the design and synthesis of ‘linker’ compounds, that bridge biotarget, fluorophore and a functional moiety via well‐established labeling protocols. Linker molecules were synthesized via the Ugi four‐component reaction (Ugi‐4CR) which facilitates a modular design of linkers with diverse functional properties and bioconjugation‐ and fluorophore attachment moieties. To demonstrate the possibilities of different linkers experimentally, we characterized the ability of commercial fluorophores from the classes of cyanines, rhodamines, carbopyronines and silicon‐rhodamines to become functional labels on different biological targets in vitro and in vivo via thiol‐maleimide chemistry. With our strategy, we showed that the same commercial dye can become a photostable self‐healing dye or a sensor for bivalent ions subject to the linker used. Finally, we quantified the photophysical performance of different self‐healing linker–fluorophore conjugates and demonstrated their applications in super‐resolution imaging and single‐molecule spectroscopy.
A General Concurrent Template Strategy for Ordered Mesoporous Intermetallic Nanoparticles with Controllable Catalytic Performance
Authors: Lv Hao , Qin Huaiyu , Ariga Katsuhiko , Yamauchi Yusuke , Liu Ben 
Published: February 2022

AbstractWe report a general concurrent template strategy for precise synthesis of mesoporous Pt‐/Pd‐based intermetallic nanoparticles with desired morphology and ordered mesostructure. The concurrent template not only supplies a mesoporous metal seed for re‐crystallization growth of atomically ordered intermetallic phases with unique atomic stoichiometry but also provides a nanoconfinement environment for nanocasting synthesis of mesoporous nanoparticles with ordered mesostructure and rhombic dodecahedral morphology under elevated temperature. Using the selective hydrogenation of 3‐nitrophenylacetylene as a proof‐of‐concept catalytic reaction, mesoporous intermetallic PtSn nanoparticles exhibited remarkably controllable intermetallic phase‐dependent catalytic selectivity and excellent catalytic stability. This work provides a very powerful strategy for precise preparation of ordered mesoporous intermetallic nanocrystals for application in selective catalysis and fuel cell electrocatalysis.
Active Mechanical Threading by a Molecular Motor**
Authors: Bach Nicolai N. , Josef Verena , Maid Harald , Dube Henry 
Published: February 2022

AbstractMolecular motors transform external energy input into directional motions and offer exquisite precision for nano‐scale manipulations. To make full use of molecular motor capacities, their directional motions need to be transmitted and used for powering downstream molecular events. Here we present a macrocyclic molecular motor structure able to perform repetitive molecular threading of a flexible tetraethylene glycol chain through the macrocycle. This mechanical threading event is actively powered by the motor and leads to a direct translation of the unidirectional motor rotation into unidirectional translation motion (chain versus ring). The mechanism of the active mechanical threading is elucidated and the actual threading step is identified as a combined helix inversion and threading event. The established molecular machine function resembles the crucial step of macroscopic weaving or sewing processes and therefore offers a first entry point to a “molecular knitting” counterpart.
Step‐by‐step protocol for the isolation and transient transformation of hornwort protoplasts
Authors: Neubauer Anna , Ruaud Stéphanie , Waller Manuel , Frangedakis Eftychios , Li Fay‐Wei , Nötzold Svenja I. , Wicke Susann , Bailly Aurélien , Szövényi Péter 
Published: February 2022

AbstractPremiseA detailed protocol for the protoplast transformation of hornwort tissue is not yet available, limiting molecular biological investigations of these plants and comparative analyses with other bryophytes, which display a gametophyte‐dominant life cycle and are critical to understanding the evolution of key land plant traits.Methods and ResultsWe describe a detailed protocol to isolate and transiently transform protoplasts of the model hornwort Anthoceros agrestis. The digestion of liquid cultures with Driselase yields a high number of viable protoplasts suitable for polyethylene glycol (PEG)‐mediated transformation. We also report early signs of protoplast regeneration, such as chloroplast division and cell wall reconstitution.ConclusionsThis protocol represents a straightforward method for isolating and transforming A. agrestis protoplasts that is less laborious than previously described approaches. In combination with the recently developed stable genome transformation technique, this work further expands the prospects of functional studies in this model hornwort.
Synthesis of azulenolactones through sequential C(2)‐bromoarylation and intramolecular CO bond formation from azulene‐1‐carboxylic acids and di(2‐bromoaryl)iodonium salts in one pot
Authors: Maeng Chanyoung , Lee Phil Ho 
Published: February 2022

AbstractSequential C(2)‐bromoarylation reaction and intramolecular CO bond formation from azulene‐1‐carboxylic acids and di(2‐bromoaryl)iodonium salts produced azulenolactones in one pot. The sequential reaction proceeded smoothly through the copper(I)‐mediated cyclization of 2‐(2‐bromoaryl)azulene‐1‐carboxylic acids derived from the regioselective iridium(III)‐catalyzed C(2)‐bromoarylation reaction without decarboxylation.
Engineering Formaldehyde Dehydrogenase from Pseudomonas putida to Favor Nicotinamide Cytosine Dinucleotide
Authors: Wang Junting , Guo Xiaojia , Wan Li , Liu Yuxue , Xue Haizhao , Zhao Zongbao K. 
Published: February 2022

AbstractThe enzyme formaldehyde dehydrogenase (FalDH) from Pseudomonas putida is of particular interest for biotechnological applications as it catalyzes the oxidation of formaldehyde independent of glutathione. However, the consumption of a stoichiometric amount of nicotinamide adenine dinucleotide (NAD) can be challenging at the metabolic level as this may affect many other NAD‐linked processes. A potential solution is to engineer FalDH to utilize non‐natural cofactors. Here we devised FalDH variants to favor nicotinamide cytosine dinucleotide (NCD) by structure‐guided modification of the binding pocket for the adenine moiety of NAD. Several mutants were obtained and the best one FalDH 9B2 had over 150‐fold higher preference for NCD than NAD. Molecular docking analysis indicated that the cofactor binding pocket shrunk to better fit NCD, a smaller‐sized cofactor. FalDH 9B2 together with other NCD‐linked enzymes offer opportunities to assemble orthogonal pathways for biological conversion of C1 molecules.
Treatment‐induced neuropathy of diabetes in an adolescent with rapid reduction in HbA1c and weight loss: Persistent neuropathic findings at follow‐up after 1.5 years
Authors: Rasmussen Vinni Faber , Thrysøe Mathilde , Tankisi Hatice , Karlsson Páll , Vestergaard Esben Thyssen , Kristensen Kurt , Nyengaard Jens Randel , Krogh Klaus , Brock Christina , Terkelsen Astrid Juhl 
Published: February 2022

AbstractTreatment‐induced neuropathy of diabetes (TIND) is a condition occurring within weeks after a rapid decline in blood glucose. This case report illustrates consequences in an adolescent with TIND. Gold standard methods diagnosing large fiber, small fiber, and autonomic neuropathy were abnormal at 1.5 years of follow‐up. Awareness of TIND is important.