bluuebunny/crossref_metadata_2025_split huggingface dataset:
Heterostructured Metal–Organic Frameworks/Polydopamine Coating Endows Polyetheretherketone Implants with Multimodal Osteogenicity and Photoswitchable Disinfection
Authors: Deng Yi , Shi Jiacheng , Chan Yau Kei , Bai Ding , Shu Rui , Shi Xiuyuan , Li Yunfei , Li Limei , Yang Xiao , Yang Weizhong 
Published: May 2022

AbstractClinically, bacteria‐induced contagion and insufficient osseointegrative property inevitably elicit the failure of orthopedic implants. Herein, a heterostructured coating consisting of simvastatin (SIM)‐laden metal–organic frameworks and polydopamine nanolayers is created on a porous bioinert polyetheretherketone implant. The heterostructured coating significantly promotes cytocompatibility and osteogenic differentiation through multimodal osteogenicity mechanisms of zinc ion (Zn2+) therapy, SIM drug therapy, and surface micro‐/nano‐topological stimulation. Under the illumination of near‐infrared (NIR) light, singlet oxygen (1O2) and local hyperthermia are produced; besides, NIR light dramatically accelerates the release of Zn2+ ions from heterostructured coatings. Gram‐positive and ‐negative bacteria are effectively eradicated by the synergy of photothermal/photodynamic effects and photo‐induced accelerated delivery of Zn2+ ions. The superior osteogenicity and osseointegration, as well as photoswitchable disinfection controlled by NIR light are corroborated via in vivo results. This work highlights the great potential of photoresponsive heterostructured orthopedic implants in treatment of the noninvasive bone reconstruction of bacteria‐associated infectious tissues through multimodal phototherapy and photoswitchable ion‐therapy.
Confined Assembly of Colloidal Nanorod Superstructures by Locally Controlling Free‐Volume Entropy in Nonequilibrium Fluids
Authors: Zhang Jingyuan , Li Xiao , Liu Yawei , Feng Jiangang , Zhao Jinjin , Geng Yue , Gao Hanfei , Wang Tie , Yang Wensheng , Jiang Lei , Wu Yuchen 
Published: May 2022

AbstractLong‐range‐ordered structures of nanoparticles with controllable orientation have advantages in applications toward sensors, photoelectric conversion, and field‐effect transistors. The assembly process of nanorods in colloidal systems undergoes a nonequilibrium process from dispersion to aggregation. A variety of assembly methods such as solvent volatilization, electromagnetic field induction, and photoinduction are restricted to suppress local perturbations during the nonequilibrium concentration of nanoparticles, which are adverse to controlling the orientation and order of assembled structures. Here, a confined assembly method is reported by locally controlling free‐volume entropy in nonequilibrium fluids to fabricate microstructure arrays based on colloidal nanorods with controllable orientation and long‐range order. The unique fluid dynamics of the liquid bridge is utilized to form a local region, where the free volume entropy reduction triggers assembly near the three‐phase contact line (TPCL), allowing nanorods to assemble in 2D closest packing parallel to the TPCL for the maximum Gibbs free energy reduction. By manipulating the orientation of liquid flow, microstructures are assembled with programmable geometry, which sustains polarized photoluminescence and polarization‐dependent photodetection. This confined assembly method opens up perspectives on assemblies of nanomaterials with controllable orientation and long‐range order as a platform for multifunctional integrated devices.
Microstructured Hydrogels to Guide Self‐Assembly and Function of Lung Alveolospheres
Authors: Loebel Claudia , Weiner Aaron I. , Eiken Madeline K. , Katzen Jeremy B. , Morley Michael P. , Bala Vikram , Cardenas‐Diaz Fabian L. , Davidson Matthew D. , Shiraishi Kazushige , Basil Maria C. , Ferguson Laura T. , Spence Jason R. , Ochs Matthias , Beers Michael F. , Morrisey Edward E. , Vaughan Andrew E. , Burdick Jason A. 
Published: May 2022

AbstractEpithelial cell organoids have increased opportunities to probe questions on tissue development and disease in vitro and for therapeutic cell transplantation. Despite their potential, current protocols to grow these organoids almost exclusively depend on culture within 3D Matrigel, which limits defined culture conditions, introduces animal components, and results in heterogenous organoids (i.e., shape, size, composition). Here, a method is described that relies on hyaluronic acid hydrogels for the generation and expansion of lung alveolar organoids (alveolospheres). Using synthetic hydrogels with defined chemical and physical properties, human‐induced pluripotent stem cell (iPSC)‐derived alveolar type 2 cells (iAT2s) self‐assemble into alveolospheres and propagate in Matrigel‐free conditions. By engineering predefined microcavities within these hydrogels, the heterogeneity of alveolosphere size and structure is reduced when compared to 3D culture, while maintaining the alveolar type 2 cell fate of human iAT2‐derived progenitor cells. This hydrogel system is a facile and accessible system for the culture of iPSC‐derived lung progenitors and the method can be expanded to the culture of primary mouse tissue derived AT2 and other epithelial progenitor and stem cell aggregates.
“Water‐in‐Eutectogel” Electrolytes for Quasi‐Solid‐State Aqueous Lithium‐Ion Batteries
Authors: Hou Xu , Pollard Travis P , He Xin , Du Leilei , Ju Xiaokang , Zhao Wenguang , Li Meirong , Wang Jun , Paillard Elie , Lin Hai , Sun Jingyu , Xu Kang , Borodin Oleg , Winter Martin , Li Jie 
Published: May 2022

AbstractThe development of high safety lithium‐ion batteries (LIBs) is greatly impeded by the flammability and leakage concerns of typical organic solvent‐based electrolytes. As one of the alternative classes of electrolytes, hydrogel electrolytes exhibit high safety, high flexibility, low cost, and are benign to the environment. However, the narrow electrochemical stability window (ESW) of typical hydrogel electrolytes restricts the operating voltage of battery cells. Here, a new class of “water‐in‐eutectogel (WiETG)” electrolyte is reported, fabricated by combining a hydrogel with a “deep eutectic solvent” (LiTFSI in acetamide). The obtained WiETG electrolyte exhibits non‐flammability, high ionic conductivity, and a wide ESW. LiMn2O4||Li4Ti5O12 cells with the WiETG electrolyte exhibit good cycling stability, high flexibility, and high safety. This newly developed WiETG electrolyte not only broadens the ESW of typical hydrogel electrolytes, but also opens a new perspective on future directions and guidance for the design of high safety electrolytes for flexible LIBs and beyond.
Thioester‐Assisted Sortase‐A‐Mediated Ligation
Authors: Zuo Chong , Ding Ruichao , Wu Xiangwei , Wang Yuanxia , Chu Guo‐Chao , Liang Lu‐Jun , Ai Huasong , Tong Ze‐Bin , Mao Junxiong , Zheng Qingyun , Wang Tian , Li Zichen , Liu Lei , Sun Demeng 
Published: May 2022

AbstractSortase A (SrtA)‐mediated ligation, a popular method for protein labeling and semi‐synthesis, is limited by its reversibility and dependence on the LPxTG motif, where “x” is any amino acid. Here, we report that SrtA can mediate the efficient and irreversible ligation of a protein/peptide containing a C‐terminal thioester with another protein/peptide bearing an N‐terminal Gly, with broad tolerance for a wide variety of LPxT‐derived sequences. This strategy, the thioester‐assisted SrtA‐mediated ligation, enabled the expedient preparation of proteins bearing various N‐ or C‐terminal labels, including post‐translationally modified proteins such as the Ser139‐phosphorylated histone H2AX and Lys9‐methylated histone H3, with less dependence on the LPxTG motif. Our study validates the chemical modification of substrates as an effective means of augmenting the synthetic capability of existing enzymatic methods.
Charge Separation by Creating Band Bending in Metal–Organic Frameworks for Improved Photocatalytic Hydrogen Evolution
Authors: Zhang Chenxi , Xie Chenfan , Gao Yuying , Tao Xiaoping , Ding Chunmei , Fan Fengtao , Jiang Hai‐Long 
Published: May 2022

AbstractMetal–organic frameworks (MOFs) have been intensively studied as a class of semiconductor‐like materials in photocatalysis. However, band bending, which plays a crucial role in semiconductor photocatalysis, has not yet been demonstrated in MOF photocatalysts. Herein, a representative MOF, MIL‐125‐NH2, is integrated with the metal oxides (MoO3and V2O5) that feature appropriate work functions and energy levels to afford the corresponding MOF composites. Surface photovoltage results demonstrate band bending in the MOF composites, which gives rise to the built‐in electric field of MIL‐125‐NH2, boosting the charge separation. As a result, the MOF composites present 56 and 42 times higher activities, respectively, compared to the pristine MOF for photocatalytic H2production. Upon depositing Pt onto the MOF, ∼6 times higher activity is achieved. This work illustrates band bending of MOFs for the first time, supporting their semiconductor‐like nature, which would greatly promote MOF photocatalysis.
Lewis Acid‐Catalyzed Diastereoselective C−C Bond Insertion of Diazo Esters into Secondary Benzylic Halides for the Synthesis of α,β‐Diaryl‐β‐haloesters
Authors: Wang Fei , Nishimoto Yoshihiro , Yasuda Makoto 
Published: May 2022

AbstractWe report a formal carbon–carbon (C−C) bond insertion via the reaction of secondary benzylic halides (fluorides, chlorides, and bromides) with α‐diazo esters catalyzed by Lewis acid catalysts. Secondary benzylic halides underwent elongation to afford α,β‐diaryl‐β‐haloesters diastereoselectively. Density functional theory calculation revealed that the present formal C−C bond insertion was the result of Lewis acid‐promoted cleavage and the re‐formation of a carbon–halogen bond and that the aryl‐migration step determined the diastereoselectivity. Various diarylmethyl halides and α‐diazo esters were applicable to this reaction system. In addition, ring expansion in cyclic benzylic chlorides was accomplished.
Constructing Organic Electroluminescent Material with Very High Color Purity and Efficiency Based on Polycyclization of the Multiple Resonance Parent Core
Authors: Xu Yincai , Wang Qingyang , Wei Jinbei , Peng Xiaomei , Xue Jianan , Wang Zhiheng , Su Shi‐Jian , Wang Yue 
Published: May 2022

AbstractMultiple resonance thermally activated delayed fluorescence (MR‐TADF) compounds have set off an upsurge of research because of their tremendous application prospects in the field of wide color gamut display. Herein, we propose a novel MR‐TADF molecular construction paradigm based on polycyclization of the multiple resonance parent core, and construct a representative multiple resonance polycyclic aromatic hydrocarbon (MR‐PAH) based on thepara‐alignment of boron and nitrogen atoms into a six‐membered ring (p‐BNR). Through the retrosynthesis analysis, a concise synthesis strategy with wide applicability has been proposed, encompassing programmed sequential boron esterification, Suzuki coupling and Scholl oxidative coupling. The target model molecule BN‐TP shows green fluorescence with an emission peak at 523 nm and a narrow full‐width at half‐maximum (FWHM) of 34 nm. The organic light‐emitting diode (OLED) employing BN‐TP as an emitter exhibits ultrapure green emission with Commission Internationale de L'Eclairage (CIE) coordinates of (0.26, 0.70), and achieves a maximum external quantum efficiency (EQE) of 35.1 %.
Controlled Synthesis of Cyclic‐Helical Polymers with Circularly Polarized Luminescence
Authors: Xu Lei , Gao Bao‐Rui , Xu Xun‐Hui , Zhou Li , Liu Na , Wu Zong‐Quan 
Published: May 2022

AbstractCyclic polymers attract attention because of their endless structure and unique properties, which differ from the linear analogs. However, the synthesis of cyclic polymers is difficult and prohibits their functions and applications. In this study, we reported chiral cyclic PdII‐catalysts that initiate a living ring‐expansion polymerization of isocyanides, yielding a single‐handed cyclic‐helical poly(phenyl isocyanide), with predictable molecular weight (Mn) and low dispersity (Mw/Mn), in good yield. Using this method, cyclic bottlebrush polymers were prepared via the grafting‐onto strategy. The cyclic topology was confirmed using various spectroscopic data and atomic force microscope observation. Moreover, the cyclic polymer brushes, comprising of a one‐handed helical backbone, showed interesting photoluminescence and circularly‐polarized luminescence.
Electron Diffraction Enables the Mapping of Coke in ZSM‐5 Micropores Formed during Methanol‐to‐Hydrocarbons Conversion
Authors: Wennmacher Julian T. C. , Mahmoudi Soheil , Rzepka Przemyslaw , Sik Lee Sung , Gruene Tim , Paunović Vladimir , van Bokhoven Jeroen A. 
Published: May 2022

AbstractUnveiling the coke formation in zeolites is an essential prerequisite for tackling the deactivation of these catalysts in the transformations of hydrocarbons. Herein, we present the direct mapping of coke in the micropores of ZSM‐5 catalysts used in methanol‐to‐hydrocarbons conversion by single‐crystal electron diffraction analysis. The latter technique revealed a polycyclic aromatic structure along the straight channel, wherein the high‐quality data permit refinement of its occupancy to about 40 %. These findings were exploited to analyze the evolution of micropore coke during the reaction. Herein, coke‐associated signals, which correlate with the activity loss, indicate that the nucleation of coke commences in the intersections of sinusoidal and straight channels, while the formation of coke in the straight pores occurs in the late stages of deactivation. The findings uncover an attractive method for analyzing coke deposition in the micropore domain.
Remimazolam anaphylaxis confirmed by serum tryptase elevation and skin test
Authors: Yamaoka M. , Kuroda K. , Matsumoto N. , Okazaki Y. , Minami E. , Yamashita C. , Kurasako T. 
Published: May 2022

SummaryAnaphylactic reactions during the induction of general anaesthesia are rare. Anaesthetists should determine the pathogenesis of anaphylaxis in order to establish appropriate treatment and prevent recurrence. Very little clinical information has been published to date about anaphylaxis induced by the recently launched drug remimazolam. A 78‐year‐old man, scheduled for elective surgery for colon cancer, became profoundly hypotensive and hypoxic shortly following the induction of general anaesthesia with remimazolam, remifentanil and rocuronium. His physiological derangement was successfully managed with adrenaline, vasopressors and intravenous fluid resuscitation. His serum tryptase level was significantly elevated and an intradermal test with diluted remimazolam revealed a positive reaction, confirming the diagnosis of anaphylaxis. We believe this is the first case report of remimazolam‐induced anaphylactic shock diagnosed with a serum tryptase elevation and positive skin test.
Characterization of diterpene metabolism in rats with ingestion of seed products from Euphorbia lathyris L. (Semen Euphorbiae and Semen Euphorbiae Pulveratum) using UHPLC‐Q‐Exactive MS
Authors: Zhang Jingqiu , Jiang Mingrui , Yue Zhuzhu , Wang Zhicheng , Wang Huinan , Chen Mengyu , Wei Xiaotong , Shi Shuanghui , Wang Menglin , Wang Yingzi 
Published: May 2022

AbstractPrevious pharmacological studies have indicated that diterpenoids are the primary effective chemical cluster in the seeds of Euphorbia lathyris L. The seed products are used in traditional Chinese medicine in the forms of Semen Euphorbiae (SE) and Semen Euphorbiae Pulveratum (SEP). However, the metabolism of the plant's diterpenoids has not been well elucidated, which means that the in vivo metabolite products have not been identified. The current study screened the physiological metabolites of six diterpenes [Euphorbia factor L1 (L1), L2 (L2), L3 (L3), L7a (L7a), L7b (L7b), and L8 (L8)] in feces and urine of rats after oral administration of SE and SEP using UHPLC‐Q‐Exactive MS. A total of 22 metabolites were detected in feces and 8 in urine, indicating that the major elimination route of diterpenoids is via the colon. Hydrolysis, methylation, and glucuronidation served as the primary metabolic pathways of these diterpenoids. In sum, this study contributed to the elucidation of new metabolites and metabolic pathways of SE and SEP, and the new chemical identities can be used to guide further pharmacokinetic studies.
The innervation of the cervical facet joints—an anatomical and histological approach
Authors: Büsken Fabian , Lataster Arno , Herrler Andreas 
Published: May 2022

AbstractCervical facet joint pain syndrome accounts for a great amount of cervical pain worldwide. This study aims to provide updated knowledge of cervical facet joint innervation with new anatomical findings. Twenty‐seven cervical facet joints and their innervating structures were dissected from five halves of three human neck specimens. Histologic staining was used to confirm that the samples were nervous tissues, and all samples were documented with photography. Histology: Thirty‐six assumed facet joint branch samples were obtained and stained. Twenty‐two of these were confirmed to be nervous tissue. Therefore, 61% of the samples were identified as facet joint branches. Of all samples, 28% were not nerves. Dissection: At least one medial branch was clearly identified at each dissected cervical level. At some cervical levels, more than one medial branch was found. Anatomical differences, such as a plexus‐like innervation in the high cervical region, were observed. Direct facet joint branches were also discovered. These branches originate directly from the dorsal root of the spinal nerve and were independent from medial branches during their direct pathway toward the facet joint. Direct cervical facet joint branches were identified and a more diverse innervation pattern than previously described of the cervical facet joints was found.
Rapid bilateral visual loss as the initial clinical manifestation in idiopathic hypertrophic cranial pachymeningitis
Authors: Shao Weiyang , Tian Chunyu , Gao Lixiong , Cui Bei , Shi Qian 
Published: May 2022

AbstractA 59‐year‐old patient presented with 4‐day acute painless bilateral visual loss, MRI results showed dura enhancement of the frontal, anterior cranial fossa. The patient was considered to have idiopathic hypertrophic cranial pachymeningitis based on laboratory tests and MRI data. After treatment with hormones, the visual acuity obviously improved.
The relationships among career maturity, motivation, and self‐regulation: A longitudinal study
Authors: Lee Hyemi , Joo HyunGyung 
Published: May 2022

AbstractIn this study, we used data from the 2013 Korea Education Longitudinal Study to identify longitudinal relationships among motivation, self‐regulation, and career maturity in Korean elementary, middle, and high school students. Data from three waves were used for autoregressive cross‐lagged modeling—wave 2 (12 years old; sixth graders in elementary school), wave 5 (15 years old; ninth graders in middle school), and wave 7 (17 years old; 11th graders in high school). The results were as follows. First, the autoregressive effect was significant at all time points for all latent variables. Second, the cross‐lagged effect displayed the same direction across all time points, but different results were derived for different variables. The implications of the study are discussed.
Foam Drainage Parametric Study Using the Lattice Boltzmann Method Considering the Non‐Newtonian Behavior
Authors: Mobarak Mohammad , Gatternig Bernhard , Delgado Antonio , Bernstein Thomas , McHardy Christopher , Rauh Cornelia 
Published: May 2022

AbstractFoam exists in several food and chemical processes. It often delays, contaminates, and obstructs the industrial process, which affects the product's quality and safety. Liquid drainage in foam is one of the most influencing physical phenomena impacting its behavior, and is characterized by its short time scales. The lattice Boltzmann method (LBM) is applied to develop a consistent method for evaluating the permeability of different foam structures, while considering the non‐Newtonian behavior of its liquid lamella. Foam drainage for non‐Newtonian fluids is not well understood and established in literature. Different geometrical and liquid parameters are thus considered and analyzed, in order to generate a map for the foam permeability.
Recent Progress of Small‐Molecule Ratiometric Fluorescent Probes for Peroxynitrite in Biological Systems
Authors: Ma Qingqing , Xu Shanlin , Zhai Zhaodong , Wang Kai , Liu Xueli , Xiao Haibin , Zhuo Shuping , Liu Yuying 
Published: May 2022

AbstractPeroxynitrite (ONOO−) as a major reactive oxygen species plays important roles in cellular signal transduction and homeostatic regulation. Precise detection of ONOO−in biological systems is vital for exploring its physiological and pathological function. Among numerous detection methods, fluorescence imaging technology using fluorescent probes offers some advantages, including simple operation, high sensitivity and selectivity, as well as real‐time and nondestructive detection. In particular, ratiometric fluorescent probes, in which the built‐in calibration of the two emission bands prevents interference from the biological environment, have been extensively employed to monitor the fluctuation of bioactive species. In this review, we will discuss small‐molecule ratiometric fluorescent probes for ONOO−in live cells or in vivo, which involves chemical structures, response mechanisms, and biological applications. Moreover, the challenges and future prospects of ONOO−‐responsive ratiometric fluorescent probe are also proposed.
The Pursuit of Perphenylterphenyls
Authors: Du Yuchen , McSkimming Alex , Mague Joel T. , Pascal Robert A. 
Published: May 2022

AbstractTetradecaphenyl‐p‐terphenyl (2) was synthesized from 2,3,5,6‐tetraphenyl‐1,4‐diiodobenzene (11) by two methods. Ullmann coupling of 11 with pentaphenyliodobenzene (9) gave compound 2 in 1.7 % yield, and Sonogashira coupling of 11 with phenylacetylene, followed by a double Diels‐Alder reaction of the product diyne 12 with tetracyclone (6), gave 2 in 1.5 % overall yield. The latter reaction also gave the monoaddition product 4‐(phenylethynyl)‐2,2′,3,3′,4′,5,5′,6,6′‐nonaphenylbiphenyl (13) in 4 % overall yield. The X‐ray structures of compounds 2 and 13 show them to possess core aromatic rings distorted into shallow boat conformations. Density functional calculations indicate that these unusual structures are not the lowest energy conformations in the gas phase and may be the result of packing forces in the crystal. In addition, while uncorrected DFT calculations indicate that the strain energy in compound 2 is approximately 50 kcal/mol, dispersion‐corrected DFT calculations suggest that it is essentially unstrained, due to compensating, favorable, intramolecular interactions of its many phenyl rings. An attempted synthesis of tetradecaphenyl‐o‐terphenyl (4) by reaction of diphenylhexatriyne (14) with three equivalents of tetracyclone at 350 °C gave only the diadduct 2‐(phenylethynyl)‐2′,3,3′,4,4′,5,5′,6,6′‐nonaphenylbiphenyl (15) in 17 % yield. Even higher temperatures failed to produce 4 and lowered the yield of 15, perhaps due to rapid decomposition of the starting materials. Ullmann coupling of 3,4,5,6‐tetraphenyl‐1,2‐diiodobenzene (16) and compound 9 also failed to give compound 4.