bluuebunny/crossref_metadata_2025_split huggingface dataset:
Remarkably Enhanced Hydrogen Generation of Organolead Halide Perovskites via Piezocatalysis and Photocatalysis
Authors: Wang Mengye , Zuo Yunpeng , Wang Jingli , Wang Yi , Shen Xinpeng , Qiu Bocheng , Cai Lejuan , Zhou Feichi , Lau Shu Ping , Chai Yang 
Published: August 2019

AbstractTo alleviate photoinduced charge recombination in semiconducting nanomaterials represents an important endeavor toward high‐efficiency photocatalysis. Here a judicious integration of piezoelectric and photocatalytic properties of organolead halide perovskite CH3NH3PbI3 (MAPbI3) to enable a piezophotocatalytic activity under simultaneous ultrasonication and visible light illumination for markedly enhanced photocatalytic hydrogen generation of MAPbI3 is reported. The conduction band minimum of MAPbI3 is higher than hydrogen generation potential (0.046 V vs normal hydrogen electrode), thereby rendering efficient hydrogen evolution. In addition, the noncentrosymmetric crystal structure of MAPbI3 enables its piezoelectric properties. Thus, MAPbI3 readily responds to external mechanical force, creating a built‐in electric field for collective piezophotocatalysis as a result of effective separation of photogenerated charge carriers. The experimental results show that MAPbI3 powders exhibit superior piezophotocatalytic hydrogen generation rate (23.30 µmol h−1) in hydroiodic acid (HI) solution upon concurrent light and mechanical stimulations, much higher than that of piezocatalytic (i.e., 2.21 µmol h−1) and photocatalytic (i.e., 3.42 µmol h−1) hydrogen evolution rate as well as their sum (i.e., 5.63 µmol h−1). The piezophotocatalytic strategy provides a new way to control the recombination of photoinduced charge carriers by cooperatively capitalizing on piezocatalysis and photocatalysis of organolead halide perovskites to yield highly efficient piezophotocatalysis.
Emerging 2D Layered Materials for Perovskite Solar Cells
Authors: Bati Abdulaziz S. R. , Batmunkh Munkhbayar , Shapter Joseph G. 
Published: August 2019

AbstractPerovskite solar cells (PSCs) are now at the forefront of the state‐of‐the‐art photovoltaic technologies due to their high efficiency and low fabrication costs. To further realize the potential of this fascinating class of solar cells, nanostructured functional materials have been playing important roles. 2D layered materials have attracted a great deal of interest due to their fascinating properties and unique structure. Recently, the exploration of a wide range of novel 2D materials for use in PSCs has seen considerable progress, but still a lot remains to be done in this field. In this progress report, the advancements that have recently been made in the application of these emerging 2D materials, beyond graphene, for PSCs are presented. Both the advantages and challenges of these 2D materials for PSCs are highlighted. Finally, important directions for the future advancements toward efficient, low‐cost, and stable PSCs are outlined.
Benchmarking Treatment Effectiveness of Community‐Delivered Trauma‐Focused Cognitive Behavioral Therapy
Authors: Rudd Brittany N. , Last Briana S. , Gregor Courtney , Jackson Kamilah , Berkowitz Steven , Zinny Arturo , Kratz Hilary E. , Cliggitt Lauren , Adams Danielle R. , Walsh Lucia M. , Beidas Rinad S. 
Published: August 2019

AbstractIt is critical for urban youth with post‐traumatic stress disorder (PTSD) living in poverty to have access to evidence‐based interventions for their traumatic stress. However, there is limited research on the effectiveness of these interventions when provided in urban, community settings. The objectives of the current study are to (a) evaluate the effectiveness of trauma‐focused cognitive behavioral therapy delivered from 2013 to 2016 in 15 behavioral health agencies on youth (N = 114) PTSD as well as general mental health symptoms and functioning, and (b) benchmark these clinical outcomes against other published efficacy and effectiveness trials. Effectiveness data are from the Philadelphia County Community Behavioral Health System, a system that has invested significantly in the training and ongoing support of clinicians providing high‐quality trauma services to youth since 2012. From baseline to last assessment, youth PTSD symptom severity (d = 0.34), PTSD functional impairment (d = 0.38), and overall mental health problem severity (d = 0.29) improved. The effect sizes of improvements were smaller than effect sizes observed in efficacy and effectiveness studies. This study is the first benchmarking study of TF‐CBT and provides preliminary findings with regard to the effectiveness, and transportability, of TF‐CBT to urban community settings that serve youth in poverty.
Density Functional Theory Study of the Mechanisms of Iron‐Catalyzed Regioselective Anti‐Markovnikov Addition of C‐H Bonds in Aromatic Ketones to Alkenes
Authors: Ren Qinghua , An Shanshan , Wang Yuling , Tong Weiqi 
Published: August 2019

The mechanisms of iron‐catalyzed regioselective anti‐Markovnikov addition of C‐H bonds in the aromatic ketones to alkenes are studied using Density Functional Theory (DFT) calculations with the B3LYP‐D3 method. Our results show that the overall catalytic cycle includes the initial generation of aromatic ketone C‐H activation, the coordination and insertion of a styrene, and finally C‐C reductive elimination. Two different alkylation products are obtained through the linear or branched formation via several different paths. The formation of the linear product is energetically favorable over that of the branched product, which is in agreement with the experimental observation. The rate‐limiting step for the whole catalytic cycle to obtain the main linear product is the reductive elimination step where the Gibbs free energy in solvent THF ΔGsol is 13.5 kcal/mol computed using the SMD method.
Electric field‐driven preparation of elastomer/plastic nanoparticles gradient films with enhanced damping property
Authors: Zhang Yuanfang , Fang Wei , Zhao Yichun , Liu Zhihong , Chen Shaoyun , Hu Chenlong , Liu Jiyan , Liu Xueqing 
Published: August 2019

ABSTRACTPolymeric gradient film consisting of the plastic nanoparticles in addition to an elastomer matrix was created by driving the charged sulfonated polystyrene (PS) nanoparticles in polydimethylsiloxane (PDMS) matrix under direct‐current electric field. The gradient morphology was frozen by thermal curing. The morphology, composition, damping, and mechanical properties of cured PS/PDMS gradient film containing 10 wt % of PS nanoparticles were measured with scanning electron microscopy, energy‐disperse spectroscopy, and dynamic thermal mechanic analysis and tensile test, respectively. In comparison with the isotropic PS/PDMS film, the gradient film shows a better damping property, and a higher tensile strength and elongation at breaking. The interpretation in terms of deformation and fracture mechanism of gradient structure was proposed. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020, 137, 48401.
Effect of co‐agents on adhesion between peroxide cured ethylene–propylene–diene monomer and thermoplastics in two‐component injection molding
Authors: Laing Brittany , De Keyzer Jozefien , Seveno David , Van Bael Albert 
Published: August 2019

ABSTRACTTwo‐component (2K) injection‐molded products combining ethylene–propylene–diene monomer (EPDM) with polar or nonpolar thermoplastics require strong interfacial bonding. To optimize the adhesion, co‐agents trimethylolpropane trimethacrylate (TMPT) and triallyl cyanurate (TAC) are compared and concentrations were varied between 0 and 12 parts per hundred rubber (phr). Changes in material compatibility were characterized by contact angle measurements at high temperature, the adhesion was evaluated by tensile testing, and physicomechanical properties of the EPDM bulk were analyzed. Results show that with polypropylene, the adhesion increases to an optimum (3 phr TAC or 6 phr TMPT) independent of the co‐agent type, while for polyethylene only TAC (1.5 phr) effectively boosts adhesion. It is surmised that these optimal concentrations promote crosslinking reactions at the interface. For polycarbonate and acrylonitrile–butadiene–styrene, increasing TAC concentration causes higher adhesion due to improved compatibility. Furthermore, physicomechanical bulk properties change significantly with co‐agent concentrations, making the optimal curing composition application dependent. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020, 137, 48414.
Targeting Mechanistic Target of Rapamycin Complex 1 Restricts Proinflammatory T Cell Differentiation and Ameliorates Takayasu Arteritis
Authors: Zhang Jifeng , Zhao Lei , Wang Jing , Cheng Zhihua , Sun Mengyao , Zhao Jiayi , Liu Bin , Liu Xiyu , Wen Zhenke , Li Zhibo 
Published: August 2019

ObjectiveTakayasu arteritis (TAK) is a progressive autoimmune large vessel vasculitis with infiltration of proinflammatory T cells, with a largely unknown etiology. This study was undertaken to explore the involvement of mechanistic target of rapamycin (mTOR) in proinflammatory T cell differentiation and disease progression in TAK.MethodsNinety‐five patients with TAK, 26 patients with small vessel vasculitis, and 40 healthy donors were enrolled. Naive and memory CD4+ T cells were activated with anti‐CD3/CD28 beads and analyzed for lineage differentiation. The mTORC1 activity was determined by quantifying intracellular phospho–S6 kinase 1 and phospho–S6 ribosomal protein. Rapamycin and lentiviral regulatory‐associated protein of mTOR short hairpin RNA were used to block mTORC1 activity. Human artery–NSG mouse chimeras representing human TAK were established for targeting mTORC1 in disease treatment.ResultsTAK CD4+ T cells were selectively prepositioned with hyperactivity of mTORC1 (P < 0.001), resulting in spontaneous maldifferentiation of Th1 and Th17 cells (P < 0.001). Activity of mTORC1high in circulating CD4+ T cells predicted elevated frequencies of proinflammatory T cells and active disease in TAK patients (P < 0.001). Blockade of mTORC1 with rapamycin efficiently abrogated the maldifferentiation of Th1 and Th17 cells (P < 0.01) and ameliorated vasculitis in humanized TAK chimeras (P < 0.001). Inhibition of mTORC1 using RNA interference technology is sufficient to reduce proinflammatory T cell frequencies (P < 0.01) and restrict TAK disease progression in vivo (P < 0.01).ConclusionOur findings indicate that hyperactivity of mTORC1 is a critical cell‐intrinsic mechanism underlying spontaneous maldifferentiation of proinflammatory T cells in TAK patients. Targeting mTORC1 is a promising therapeutic strategy against TAK.
A dual‐readout nanosensor based on biomass‐based C‐dots and chitosan@AuNPs with hyaluronic acid for determination of hyaluronidase
Authors: Liu Wei , Ding Fang , Wang Yanying , Lu Zhiwei , Zou Ping , Wang Xianxiang , Zhao Qingbiao , Rao Hanbing 
Published: August 2019

AbstractA dual‐signal strategy is proposed based on fluorescent biomass‐based carbon dots (BC‐dots) and chitosan stabilized AuNPs (CS@AuNPs) to determine hyaluronidase (HAase). BC‐dots can induce aggregation of CS@AuNPs nanoparticles with a colour change from red to blue. Positively charged CS@AuNPs interacted with the negatively charged hyaluronic acid (HA) through electrostatic adsorption, and CS@AuNPs maintained stability due to the semirigid coil conformation of HA. However, in the presence of HAase, due to enzymatic hydrolysis of HA by HAase, the CS@AuNPs agglomerated. Based on the change of fluorescence and colour, quantitative analysis of HAase was achieved. Linear ranges for the fluorometric and colorimetric determinations were 2.0–70 U mL−1 and 8–60 U mL−1, respectively, with a detection limit of 0.27 U mL−1. This dual‐signal sensing system possesses high potential for determination of HAase in biological matrices.
Achieving a high‐density oleaginous yeast culture: Comparison of four processing strategies using Metschnikowia pulcherrima
Authors: Abeln Felix , Chuck Christopher J. 
Published: August 2019

AbstractMicrobial lipids have the potential to displace terrestrial oils for fuel, value chemical, and food production, curbing the growth in tropical oil plantations and helping to reduce deforestation. However, commercialization remains elusive partly due to the lack of suitably robust organisms and their low lipid productivity. Extremely high cell densities in oleaginous cultures are needed to increase reaction rates, reduce reactor volume, and facilitate downstream processing. In this investigation, the oleaginous yeast Metschnikowia pulcherrima, a known antimicrobial producer, was cultured using four different processing strategies to achieve high cell densities and gain suitable lipid productivity. In batch mode, the yeast demonstrated lipid contents more than 40% (w/w) under high osmotic pressure. In fed‐batch mode, however, high‐lipid titers were prevented through inhibition above 70.0 g L−1 yeast biomass. Highly promising were a semi‐continuous and continuous mode with cell recycle where cell densities of up to 122.6 g L−1 and maximum lipid production rates of 0.37 g L−1 h−1 (daily average), a nearly two‐fold increase from the batch, were achieved. The findings demonstrate the importance of considering multiple fermentation modes to achieve high‐density oleaginous yeast cultures generally and indicate the limitations of processing these organisms under the extreme conditions necessary for economic lipid production.
Cell free biosynthesis of isoprenoids from isopentenol
Authors: Ward Valerie C.A. , Chatzivasileiou Alkiviadis Orfefs , Stephanopoulos Gregory 
Published: August 2019

AbstractCell‐free systems are growing in importance for the biosynthesis of complex molecules. These systems combine the precision of traditional chemistry with the versatility of biology in creating superior overall processes. Recently, a new synthetic pathway for the biosynthesis of isoprenoids using the substrate isopentenol, dubbed the isopentenol utilization pathway (IUP), was demonstrated to be a promising alternative to the native 2C‐methyl‐d‐erythritol‐4‐phosphate (MEP) and mevalonate (MVA) pathways. This simplified pathway, which contains a minimum of four enzymes to produce basic monoterpenes and only depends on ATP and isopentenol as substrates, allows for a highly flexible approach to the commercial synthesis of isoprenoid products. In this work, we use metabolic reconstitution to characterize this new pathway in vitro and demonstrate its use for the cell‐free synthesis of mono‐, sesquit‐, and diterpenoids. Kinetic modeling and sensitivity analysis were also used to identify the most significant parameters for taxadiene productivity, and metabolic control analysis was employed to elucidate protein‐level interactions within this pathway, which demonstrated that the IUP enzymatic system is primarily controlled by the concentration and kinetics of choline kinase (CK) and not regulated by any pathway intermediates. This is a significant advantage over the natural MEP or MVA pathways as it greatly simplifies future metabolic engineering efforts, both in vitro and in vivo, aiming at improving the kinetics of CK. Finally, we used the insights gathered to demonstrate an in vitro IUP system that can produce 220 mg/L of the diterpene taxadiene, in 9 hr, almost 3‐fold faster than any system reported thus far.
Escherichia coli “TatExpress” strains export several g/L human growth hormone to the periplasm by the Tat pathway
Authors: Guerrero Montero Isabel , Richards Kirsty L. , Jawara Chillel , Browning Douglas F. , Peswani Amber R. , Labrit Mickael , Allen Matthew , Aubry Cedric , Davé Emma , Humphreys David P. , Busby Stephen J. W. , Robinson Colin 
Published: August 2019

AbstractEscherichia coli is a heavily used platform for the production of biotherapeutic and other high‐value proteins, and a favored strategy is to export the protein of interest to the periplasm to simplify downstream processing and facilitate disulfide bond formation. The Sec pathway is the standard means of transporting the target protein but it is unable to transport complex or rapidly folding proteins because the Sec system can only transport proteins in an unfolded state. The Tat system also operates to transport proteins to the periplasm, and it has significant potential as an alternative means of recombinant protein production because it transports fully folded proteins. Here, we have tested the Tat system's full potential for the production of biotherapeutics for the first time using fed‐batch fermentation. We expressed human growth hormone (hGH) with a Tat signal peptide in E. coli W3110 “TatExpress” strains that contain elevated levels of the Tat apparatus. This construct contained four amino acids from TorA at the hGH N‐terminus as well as the initiation methionine from hGH, which is removed in vivo. We show that the protein is efficiently exported to the periplasm during extended fed‐batch fermentation, to the extent that it is by far the most abundant protein in the periplasm. The protein was shown to be homogeneous, disulfide bonded, and active. The bioassay showed that the yields of purified periplasmic hGH are 5.4 g/L culture whereas an enzyme‐linked immunosorbent assay gave a figure of 2.39 g/L. Separate analysis of a TorA signal peptide linked to hGH construct lacking any additional amino acids likewise showed efficient export to the periplasm, although yields were approximately two‐fold lower.
Screening of oleaginous algal strains from Chlamydomonas reinhardtii mutant libraries via density gradient centrifugation
Authors: Sung Young Joon , Choi Hong Il , Lee Jeong Seop , Hong Min Eui , Sim Sang Jun 
Published: August 2019

AbstractMicroalgae have a high potential to be utilized as feedstock for biofuels because they have high growth rates and do not compromise food production. Commercialized algae‐based biofuel production relies on the development of strains with high lipid content. Based on the relatively low density of lipids compared to other cellular components, density gradient centrifugation was used to isolate high lipid content algal strains from Chlamydomonas reinhardtii mutant libraries. The correlation between cell density and lipid content was confirmed by analysis of Nile red fluorescence intensity, total lipids, and total fatty acid methyl ester content. A strain isolated by this screening method had 50% higher lipid content and 7% lower cell density than the parent wild‐type strain. Consequently, we demonstrated that screening of algal strains with low cell density via continuous density gradient centrifugation allows simple, rapid, and inexpensive screening for high lipid content strains.
Development and validation of an ultra‐high‐performance liquid chromatography–tandem mass spectrometry method to determine the bioavailability of warfarin and its major metabolite 7‐hydroxy warfarin in rats dosed with oral formulations containing different polymorphic forms
Authors: Shakleya Diaa , Rahman Ziyaur , Faustino Patrick J. 
Published: August 2019

AbstractA simple, sensitive and rapid ultra‐high‐performance liquid chromatography–electrospray ionization–tandem mass spectrometry method was developed and validated for the quantification of warfarin and 7‐hydroxy warfarin in Sprague Dawley (SD) rats. Animals were administered a single dose of warfarin sodium formulations (crystalline and amorphous) at 12 mg/kg via oral gavage and blood was drawn over a 96‐h time course. Sample process recoveries, matrix effect and analyte stability were determined. The linearity for warfarin and 7‐hydroxy warfarin was from 5 to 2000 ng/mL in blank SD rat plasma. Correlation coefficients (r2) for standard calibration curves were >.98 and analytes quantified within ±15% of target at all calibrator concentrations. The average percent accuracy and precision for intra‐ and inter‐day were 93.7%–113.8% and ≤12.1%, respectively, for warfarin and 7‐hydroxy warfarin, across the quality control standards (5, 10, 500, 1800 and 2000 ng/mL). Acceptable analytical recovery (>55%) was achieved with process efficiencies >41.5% and matrix effects <139.9% over the analytical range. Both analytes were stable in stock solution, autosampler, benchtop and three cycles of freeze–thaw with percent accuracy ≥90.2% and precision (percent relative standard deviation) ≤14%. The validated method was successfully applied to a pre‐clinical bioavailability study of crystalline and amorphous warfarin sodium formulations in SD rats.
Three‐Step Total Synthesis of Ramelteon via a Catellani Strategy
Authors: Gao Shijun , Qian Guangyin , Tang Hao , Yang Zuo , Zhou Qianghui 
Published: August 2019

AbstractRamelteon is the first medicine in human history that treat insomnia as a melatonin receptor agonist. Herein, we report an efficient three‐step synthetic route to access it from commercially available 2,3‐dihydrobenzofuran‐4‐amine, which represents as the shortest racemic synthesis to date with a 26 % overall yield. Key to the success is the application of the intermolecular Catellani‐type alkylation and intramolecular redox‐relay Heck cyclization cascade for preparation of the key indane‐containing aldehyde. The unique primary amide‐involved reductive amination of aldehyde is another feature of this route. New process of ramelteon can be developed based on this chemistry.
Comparison of Exergy Losses for Reformers Involved in Hydrogen and Synthesis Gas Production
Authors: Behroozsarand Alireza , Wood David A. 
Published: August 2019

AbstractA user‐coded, customized methodology for exergy balance and analysis of chemical and thermal processes is developed with the Aspen HYSYS process simulator, to assess and explain exergy loss in steam methane reforming. Exergy analysis is presented for four configurations of primary and secondary reformers to produce synthesis gas: (1) an autothermal reformer (ATR) alone, (2) a top‐fired reformer (TFR) alone, (3) ATR‐TFR configured in parallel, and (4) ATR‐TFR configured in series. The same states and feed conditions, i.e., mass flow rate, temperature, pressure, and feed gas composition, are applied to the four reformer configurations considered, with the single ATR showing the lowest exergy loss of about 0.43 W kg−1 of dry productivity.
Copper‐Metal Organic Frameworks Electrodeposited on Carbon Paper as an Enhanced Cathode for the Hydrogen Evolution Reaction
Authors: Li Xiao‐Feng , Lu Miao‐Yu , Yu Hai‐Yang , Zhang Tian‐Heng , Liu Jiao , Tian Jing‐Hua , Yang Ruizhi 
Published: August 2019

AbstractMetal organic framework (MOF)‐based materials have been widely studied and reported as efficient electrocatalysts for the hydrogen evolution reaction (HER), owing to their high surface areas, controllable structures, and tunable pore sizes. However, the intrinsically poor electrical conductivity of most MOFs hinders their directly applications as electrocatalysts. Herein, copper‐centered MOFs (HKUST‐1) have been electrodeposited directly onto the current collector. These electrochemically prepared HKUST‐1@carbon paper hybrids exhibited significantly enhanced electrocatalytic performances for the HER, including a positively shifted of onset potential, a lower overpotential, and a smaller Tafel slope, as compared to the conventional hydrothermally prepared HKUST‐1. The proposed electrodeposited synthesis strategy for MOF‐based electrocatalysts is fast, efficient, mild, and environmentally friendly. This work may also extend to other MOF materials and any conductive substrate, thus providing a facile strategy for the preparation of MOF‐based catalysts with high efficiency and low cost.