bluuebunny/crossref_metadata_2025_split huggingface dataset:
Patterned Carbon Nitride–Based Hybrid Aerogel Membranes via 3D Printing for Broadband Solar Wastewater Remediation
Authors: He Peisheng , Tang Xingwei , Chen Liao , Xie Peiwen , He Lu , Zhou Han , Zhang Di , Fan Tongxiang 
Published: May 2018

AbstractControlled scalable assembly of 2D building blocks into macroscopic 3D architectures is highly significant. However, the assembly of g‐C3N4 into tailored, 3D architectures is not yet reported. Here, a 3D printing methodology to enable the programmable construction of carbon nitride–based hybrid aerogel membranes with patterned macroscopic architectures is proposed. g‐C3N4 nanosheets (CNNS) are used as the building block, and sodium alginate (SA) increases the viscosity of the ink to obtain the desired rheological properties. Three printing routes, including printing directly in air and in the supporting reservoirs composed of CaCl2/glycerol solution or Pluronic F127, are demonstrated for printing versatility. The printed Au nanobipyramid–CNNS–SA hybrid aerogels exhibit broadband visible‐light absorption and superior solar wastewater remediation performance with excellent cyclic stability and easy manipulation features. Remarkably, the activity of the 3D‐printed aerogel is about 2.5 times of that of the contrast sample, attributing to the enhanced liquid velocity and solution diffusion efficiency because of the 3D‐printed structure, which is demonstrated by experimental and theoretical simulations. This approach can be extended to the macroscopic assembly of other 2D materials for myriad applications.
High‐Performance Triphase Bio‐Photoelectrochemical Assay System Based on Superhydrophobic Substrate‐Supported TiO2 Nanowire Arrays
Authors: Chen Liping , Sheng Xia , Wang Dandan , Liu Jie , Sun Ruize , Jiang Lei , Feng Xinjian 
Published: May 2018

AbstractThe design and fabrication of bio‐photoelectrodes that simultaneously possess rapid charge and gas‐phase mass transport abilities are highly desirable for the development of high‐performance bio‐photoelectrochemical assay systems. Here, a solid–liquid–air triphase bio‐photoelectrode is demonstrated by immobilizing glucose oxidase, a model redox active enzyme, onto 1D single crystalline TiO2 nanowire arrays grown upon a superhydrophobic carbon textile substrate. Based on this triphase bio‐photoelectrode system, oxygen can be directly and constantly supplied from the air phase to sustain enzymatic reactions, leading to much enhanced oxidase kinetics. Further, the photogenerated electrons can transport rapidly and be efficiently collected along the nanowire arrays. The bio‐photoelectrochemical assay system demonstrates a significant wide detection range, high sensitivity, and selectivity as well as a low detection limit. The design principle is generally applicable to the fabrication of other triphase bio‐photoelectrodes, which offers an excellent opportunity for significant advances in environmental analysis and clinical diagnosis.
Mechanotargeting: Mechanics‐Dependent Cellular Uptake of Nanoparticles
Authors: Wei Qiong , Huang Changjin , Zhang Yao , Zhao Tiankai , Zhao Peng , Butler Peter , Zhang Sulin 
Published: May 2018

AbstractTargeted delivery of nanoparticle (NP)‐based diagnostic and therapeutic agents to malignant cells and tissues has exclusively relied on chemotargeting, wherein NPs are surface‐coated with ligands that specifically bind to overexpressed receptors on malignant cells. Here, it is demonstrated that cellular uptake of NPs can also be biased to malignant cells based on the differential mechanical states of cells, enabling mechanotargeting. Owing to mechanotransduction, cell lines (HeLa and HCT‐8) cultured on hydrogels of various stiffness are directed into different stress states, measured by cellular force microscopies. In vitro NP delivery reveals that increases in cell stress suppress cellular uptake, counteracting the enhanced uptake that occurs with increases in exposed surface area of spread cells. Upon prolonged culture on stiff hydrogels, cohesive HCT‐8 cell colonies undergo metastatic phenotypic change and disperse into individual malignant cells. The metastatic cells are of extremely low stress state and adopt an unspread, 3D morphology, resulting in several‐fold higher uptake than the nonmetastatic counterparts. This study opens a new paradigm of harnessing mechanics for the design of future strategies in nanomedicine.
Reverse Saturable Absorption Induced by Phonon‐Assisted Anti‐Stokes Processes
Authors: Tian Xiangling , Wei Rongfei , Guo Qianyi , Zhao Yu‐Jun , Qiu Jianrong 
Published: May 2018

AbstractIn materials showing reverse saturable absorption (RSA), optical transmittance decreases at intense laser irradiation. One approach to application of these materials is to protect the sensors or human eyes from laser damage. To date, research has mainly concentrated on thin films and suspensions of graphite and its nanostructure (including nanotubes, graphene, and graphene oxides), which are mainly used as an optical limiter for nanosecond laser pulses. Moreover, thin individual pieces of semiconductor usually exhibit increased transmittance due to saturable absorption when the laser energy (Elaser) is higher than the band gap (EB). Here, it is shown that indirect gap semiconductor WSe2 exhibits high RSA on exposure to a femtosecond laser under Elaser > EB near band gap excitation, which is attributed to the longitudinal optical phonon‐assisted anti‐Stokes transition by the annihilation of phonons and the absorption of photons. An optical limiting threshold (≈21.6 mJ cm−2) lower than those reported for other optical‐limiting materials currently for femtosecond laser at 800 nm is observed.
Hypervalent Iodine(III)‐Mediated Solvent‐Free, Regioselective Synthesis of 3,4‐Disubstituted 5‐Imino‐1,2,4‐thiadiazoles and 2‐Aminobenzo[d]thiazoles
Authors: Tumula Nagaraju , Palakodety Radha Krishna , Balasubramanian Sridhar , Nakka Mangarao 
Published: May 2018

AbstractA convenient approach for the synthesis of 3,4‐disubstituted 5‐imino‐1,2,4‐thiadiazoles and 2‐aminobenzo[d]thiazoles has been developed using phenyliodine diacetate (PIDA). This approach involves a metal‐free oxidative C−N, N−S and C−S bond formations under neat conditions. High regioselectivity, solvent‐free conditions, short reaction time and broad functional group compatibility are the notable features of this report.magnified image
Recent Progress on Layered Double Hydroxides and Their Derivatives for Electrocatalytic Water Splitting
Authors: Wang Yanyong , Yan Dafeng , El Hankari Samir , Zou Yuqin , Wang Shuangyin 
Published: May 2018

AbstractLayered double hydroxide (LDH)‐based materials have attracted widespread attention in various applications due to their unique layered structure with high specific surface area and unique electron distribution, resulting in a good electrocatalytic performance. Moreover, the existence of multiple metal cations invests a flexible tunability in the host layers; the unique intercalation characteristics lead to flexible ion exchange and exfoliation. Thus, their electrocatalytic performance can be tuned by regulating the morphology, composition, intercalation ion, and exfoliation. However, the poor conductivity limits their electrocatalytic performance, which therefore has motivated researchers to combine them with conductive materials to improve their electrocatalytic performance. Another factor hampering their electrocatalytic activity is their large lateral size and the bulk thickness of LDHs. Introducing defects and tuning electronic structure in LDH‐based materials are considered to be effective strategies to increase the number of active sites and enhance their intrinsic activity. Given the unique advantages of LDH‐based materials, their derivatives have been also used as advanced electrocatalysts for water splitting. Here, recent progress on LDHs and their derivatives as advanced electrocatalysts for water splitting is summarized, current strategies for their designing are proposed, and significant challenges and perspectives of LDHs are discussed.
Graphene–Polymer Nanocomposite‐Based Redox‐Induced Electricity for Flexible Self‐Powered Strain Sensors
Authors: Wang Yuanming , Wang Yang , Yang Ya 
Published: May 2018

AbstractGraphene as a powerful inorganic material such as excellent conductivity and ideal mechanical strength has recently been extensively utilized to develop flexible strain sensors. However, graphene‐based strain sensors usually suffer from the deficiencies of stretchability, sensitivity, and sensing range, which can restrict their applications in wearable devices. Here, a novel strain sensor is designed by integrating graphene/ecoflex film and meandering zinc wire into the flexible base. The constructed strain sensor not only possesses high stretchability of up to 150% strain but can also self‐generates current signals from redox‐induced electricity, where the stable current and voltage signals of about 75 µA and 0.83 V can be obtained, respectively. Furthermore, the self‐powered sensor presents a broad and linear sensing range of 25% to 150% strains and a fast response time of less than 0.11 s. Attached on human body, the sensor has been utilized to realize the motion detection of knee joint.
The critical role of fossils in inferring deep‐node phylogenetic relationships and macroevolutionary patterns in Cornales
Authors: Atkinson Brian A. 
Published: May 2018

Premise of the StudyThe basal asterid order, Cornales, experienced a rapid radiation during the Cretaceous, which has made it difficult to elucidate the early evolution of the order using extant taxa only. Recent paleobotanical studies, however, have begun to shed light on the early diversification of Cornales. Herein, fossils are directly incorporated in phylogenetic and quantitative morphological analyses to reconstruct early cornalean evolution.MethodsA morphological matrix of 77 fruit characters and 58 taxa (24 extinct) was assembled. Parsimony analyses including and excluding fossils were conducted. A fossil inclusive tree was time‐scaled to visualize the timing of the initial cornalean radiation. Disparity analyses were utilized to infer the morphological evolution of cornaleans with drupaceous fruits.Key ResultsFossil inclusive and exclusive parsimony analyses resulted in well‐resolved deep‐node relationships within Cornales. Resolution in the fossil inclusive analysis is substantially higher, revealing a basal grade including Loasaceae, Hydrangeaceae, Hydrostachyaceae, Grubbiaceae, a Hironoia+Amersinia clade, and Curtisiaceae, respectively, that leads to a “core” group containing a clade comprising a Cretaceous grade leading to clade of Nyssaceae, Mastixiaceae, and Davidiaceae that is sister to a Cornaceae+Alangiaceae clade. The time‐scaled tree indicates that the initial cornalean diversification occurred before 89.8 Ma. Disparity analyses suggest the morphological diversity of Cornales peaked during the Paleogene.ConclusionsPhylogenetic analyses clearly demonstrate that novel character mosaics of Cretaceous cornaleans play a critical role in resolving deep‐node relationships within Cornales. The post‐Cretaceous increase of cornalean disparity is associated with a shift in morphospace occupation, which can be explained from ecological and developmental perspectives.
Proteomic Analysis of Single Mammalian Cells Enabled by Microfluidic Nanodroplet Sample Preparation and Ultrasensitive NanoLC‐MS
Authors: Zhu Ying , Clair Geremy , Chrisler William B. , Shen Yufeng , Zhao Rui , Shukla Anil K. , Moore Ronald J. , Misra Ravi S. , Pryhuber Gloria S. , Smith Richard D. , Ansong Charles , Kelly Ryan T. 
Published: May 2018

AbstractWe report on the quantitative proteomic analysis of single mammalian cells. Fluorescence‐activated cell sorting was employed to deposit cells into a newly developed nanodroplet sample processing chip, after which samples were analyzed by ultrasensitive nanoLC‐MS. An average of circa 670 protein groups were confidently identified from single HeLa cells, which is a far greater level of proteome coverage for single cells than has been previously reported. We demonstrate that the single‐cell proteomics platform can be used to differentiate cell types from enzyme‐dissociated human lung primary cells and identify specific protein markers for epithelial and mesenchymal cells.
Selective ortho C−H Cyanoalkylation of (Diacetoxyiodo)arenes through [3,3]‐Sigmatropic Rearrangement
Authors: Tian Junsong , Luo Fan , Zhang Chaoshen , Huang Xin , Zhang Yage , Zhang Lei , Kong Lichun , Hu Xiaochun , Wang Zhi‐Xiang , Peng Bo 
Published: May 2018

AbstractWe herein report a robust catalyst‐free cross‐coupling between ArI(OAc)2 and α‐stannyl nitriles, aided by TMSOTf. The transformation introduces a cyanoalkyl group to the ortho position of ArI(OAc)2 and simultaneously reduces the aryl iodine(III) to iodide, thus providing α‐(2‐iodoaryl) nitrile as the product. This transformation could be completed within 5 min at −78 °C and features superb functional‐group tolerance and efficient scalability. DFT calculations indicate that the formation of a ketenimine(aryl)iodonium intermediate and subsequent [3,3]‐sigmatropic rearrangement are involved as key steps.
MnI/AgI Relay Catalysis: Traceless Diazo‐Assisted C(sp2)–H/C(sp3)–H Coupling to β‐(Hetero)Aryl/Alkenyl Ketones
Authors: Lu Qingquan , Mondal Shobhan , Cembellín Sara , Glorius Frank 
Published: May 2018

AbstractAn unprecedented MnI/AgI‐relay‐catalyzed C(sp2)−H/C(sp3)−H coupling of (vinyl)arenes with α‐diazoketones is reported, wherein the diazo group was exploited as a traceless auxiliary for control of regioselectivity. Challenging β‐(hetero)aryl/alkenyl ketones were obtained through this operationally simple approach. The cascade process merges denitrogenation, carbene rearrangement, C−H activation, and hydroarylation/hydroalkenylation. The robustness of this method was demonstrated at preparative scale and applied to late‐stage diversification of natural products.
Metal‐ and Reagent‐Free Dehydrogenative Formal Benzyl–Aryl Cross‐Coupling by Anodic Activation in 1,1,1,3,3,3‐Hexafluoropropan‐2‐ol
Authors: Imada Yasushi , Röckl Johannes L. , Wiebe Anton , Gieshoff Tile , Schollmeyer Dieter , Chiba Kazuhiro , Franke Robert , Waldvogel Siegfried R. 
Published: May 2018

AbstractA selective dehydrogenative electrochemical functionalization of benzylic positions that employs 1,1,1,3,3,3‐hexafluoropropan‐2‐ol (HFIP) has been developed. The electrogenerated products are versatile intermediates for subsequent functionalizations as they act as masked benzylic cations that can be easily activated. Herein, we report a sustainable, scalable, and reagent‐ and metal‐free dehydrogenative formal benzyl–aryl cross‐coupling. Liberation of the benzylic cation was accomplished through the use of acid. Valuable diarylmethanes are accessible in the presence of aromatic nucleophiles. The direct application of electricity enables a safe and environmentally benign chemical transformation as oxidizers are replaced by electrons. A broad variety of different substrates and nucleophiles can be employed.
Numerical investigation of drop formation in a co‐current liquid–liquid flow for ice slurry making system
Authors: Zhang Tiantian , Xin Yi , Geng Fan , Han Dongtai , Peng Zhengbiao , Chai Hongli , Luo Gang , Ding Haiyan 
Published: May 2018

AbstractIce slurry is used widely as phase change materials (PCMs) to reduce the peak demand for power system. Drop formation plays a key role during ice slurry production in liquid–liquid circulating fluidized bed. In the present work, drop formation in a co‐current liquid–liquid flow was investigated via a 3D model. Volume of fluid method was adopted to study drop characteristics by tracking the interface. Major influences of the water velocity, the oil velocity, the jet size, and the jet number on drop formation were analyzed for drop characteristics. The results indicate that properties of drop formation vary significantly according to the different conditions. The drop size was distributed mainly as the normal distribution, and the average drop diameter varies with different conditions. The drop size varies from 0.7 to 1.9 mm at the water velocity of 0.5 m/s, whereas the size of drop size varies from 1.8 to about 2.65 mm at the water velocity of 1.5 m/s. Furthermore, the residence time of drop decreases obviously with the increase of the oil velocity. When the oil velocity is 0.1 m/s, a drop leaves the top outlet at about 0.44 s. When the oil velocity is 0.3 m/s, a drop reaches the outlet at about 0.15 s. Additionally, the simulated results were compared with the relevant experimental results and the previous simulated results. Reasonable agreements have been gained, which can validate the established model to some extent.
Synthesis, evaluation, and molecular docking studies of aryl urea‐triazole‐based derivatives as anti‐urease agents
Authors: Moghimi Setareh , Goli‐Garmroodi Fereshteh , Allahyari‐Devin Maryam , Pilali Hedieh , Hassanzadeh Malihe , Mahernia Shabnam , Mahdavi Mohammad , Firoozpour Loghman , Amanlou Massoud , Foroumadi Alireza 
Published: May 2018

AbstractConsidering the importance of urease inhibitors in the treatment of ureolytic bacterial infections, in this work, the synthesis of novel, aryl urea‐triazole‐based derivatives as effective urease inhibitors is described. Dichloro‐substituted derivative 4o, with IC50 = 22.81 ± 0.05 μM, is found to be the most potent urease inhibitor, determined by Berthelot colorimetric assay. Docking studies were also carried out for compound 4o to confirm the effective interactions with the urease active site.
Development and validation of a UPLC–MS/MS method for determination of Sarsasapogenin‐AA22 in rat plasma and its application to a pharmacokinetic study
Authors: Pei Lixia , Ge Songlan , Ye Yiyi , Jiang Ziwei , Liang Xiaoqiang , Zhao Wenshu , Ma Lei 
Published: May 2018

AbstractA sarsasapogenin derivative, sarsasapogenin‐AA22 (AA22), with cyclobutylamine at the 3‐hydroxyl position of sarsasapogenin, has great neuroprotective activity in PC12 cells and NO production inhibitory activity in RAW264.7 cell lines. A method was developed to determine AA22 in rat plasma which was further applied to evaluate the pharmacokinetics of AA22 after taking a single dose of AA22. Liquid chromatography tandem mass spectrometry was used in the method, while diosgenin was used as internal standard. A simple protein precipitation based on acetonitrile was utilized. A simple sample cleanup promoted the throughput of the method considerably. The method was validated over the range of 1–1000 ng/mL with a correlation coefficient > 0.99. The lower limit of quantification was 1 ng/mL for AA22 in plasma. Intra‐ and inter‐day accuracies for AA22 were 92–111 and 100–103%, respectively, and the inter‐day precision was <15%. After a single oral dose of 25 mg/kg of AA22, the mean peak plasma concentration of AA22 was 2114 ± 362 ng/mL at 6 h. The area under the plasma concentration–time curve was 196,098 ± 69,375 h ng/mL, and the elimination half‐life was 8.7 ± 2.2 h.
Multivariate optimization and characterization of simultaneous removal of binary mixture of Cu(II) and Pb(II) using Fe3O4@MoS2 nanoparticles
Authors: Zolgharnein Javad , Rastgordani Mahdieh 
Published: May 2018

AbstractIn this study, a facile hydrothermal method was used for the synthesis of Fe3O4@MoS2 magnetic nanoparticles. Then, this compound was used as an efficient adsorbent for the simultaneous removal of Cu(II) and Pb(II) ions from water. The prepared nanoparticles were characterized by scanning electron microscopy, X‐ray diffraction, vibrating sample magnetometer, and Fourier transform infrared spectroscopy. In addition, the effect of operational parameters on the adsorption process, such as initial pH, the concentration of metal ions, and sorbent mass, was investigated. The results of response surface methodology, obtained from Box‐Behnken design, was used to optimize the removal percent (%R) of Cu(II) and Pb(II). The effect of the different variables and their interactions was displayed by a regression model. A good agreement was seen between the proposed quadratic model resulting from Box‐Behnken design approach and the experimental data. According to the obtained results, the optimized conditions for the removal of metal ions were as follows: pH = 3, sorbent dose = 0.05 g, CPb (initial Pb(II) concentration) = 240.70 mg/L, and CCu (initial Cu(II) concentration) = 198 mg/L. The adsorption of both Freundlich and Langmuir isotherm models and pseudo‐second‐order kinetic model described the adsorption process well (R2 > 0.99). The obtained amounts of the thermodynamic parameters, such as ∆G°, ∆S°, and ∆H°, have proved that the adsorption of Pb(II) and Cu(II) ions on the surface of Fe3O4@MoS2 nanoparticles is spontaneous, feasible, and endothermic in nature.
Radical Cation π‐Dimers of Conjugated Oligomers as Molecular Wires: An Analysis Based on Nitronyl Nitroxide Spin Labels
Authors: Nishinaga Tohru , Kanzaki Yuki , Shiomi Daisuke , Matsuda Kenji , Suzuki Shuichi , Okada Keiji 
Published: May 2018

AbstractNitronyl nitroxide (NN)‐substituted conjugated oligomers, which were expected to self‐associate in biradical cation states, were designed to analyze the capability of π‐dimers as molecular wires. The oligomer moieties were composed of dithienyl‐N‐methylpyrrole with methoxy substituents at the inner β‐position of thiophene rings (DTP‐NN.) and its propylenedioxythiophene (ProDOT) inserted derivative (DTP‐P‐NN.), or two ethylenedioxythiophene (EDOT) and two ProDOT units (E2P2‐NN.). Among them, chemical one‐electron oxidation gave biradical cations (DTP‐P).+‐NN. and (E2P2).+‐NN. that formed π‐dimers (DTP‐P‐NN.)22+ and (E2P2‐NN.)22+ in dichloromethane at low temperatures. ESR studies of (DTP‐P‐NN.)22+ and (E2P2‐NN.)22+ showed the presence of a relatively strong exchange interaction between two NN radicals through the radical cation π‐dimer moieties. DFT calculations supported these experimental results and predicted that exchange interactions between two NN radicals were comparable or stronger than those through covalently linked quaterthiophene. Thus, the conjugated oligomer radical cation π‐dimers acted as efficient molecular wires for electronic communication.
Spiro‐epoxyglycosides as Activity‐Based Probes for Glycoside Hydrolase Family 99 Endomannosidase/Endomannanase
Authors: Schröder Sybrin P. , Kallemeijn Wouter W. , Debets Marjoke F. , Hansen Thomas , Sobala Lukasz F. , Hakki Zalihe , Williams Spencer J. , Beenakker Thomas J. M. , Aerts Johannes M. F. G. , van der Marel Gijsbert A. , Codée Jeroen D. C. , Davies Gideon J. , Overkleeft Herman S. 
Published: May 2018

AbstractN‐Glycans direct protein function, stability, folding and targeting, and influence immunogenicity. While most glycosidases that process N‐glycans cleave a single sugar residue at a time, enzymes from glycoside hydrolase family 99 are endo‐acting enzymes that cleave within complex N‐glycans. Eukaryotic Golgi endo‐1,2‐α‐mannosidase cleaves glucose‐substituted mannose within immature glucosylated high‐mannose N‐glycans in the secretory pathway. Certain bacteria within the human gut microbiota produce endo‐1,2‐α‐mannanase, which cleaves related structures within fungal mannan, as part of nutrient acquisition. An unconventional mechanism of catalysis was proposed for enzymes of this family, hinted at by crystal structures of imino/azasugars complexed within the active site. Based on this mechanism, we developed the synthesis of two glycosides bearing a spiro‐epoxide at C‐2 as electrophilic trap, to covalently bind a mechanistically important, conserved GH99 catalytic residue. The spiro‐epoxyglycosides are equipped with a fluorescent tag, and following incubation with recombinant enzyme, allow concentration, time and pH dependent visualization of the bound enzyme using gel electrophoresis.