bluuebunny/crossref_metadata_2025_split huggingface dataset:
Enhanced Charge Transport and Stability Conferred by Iron(III)‐Coordination in a Conjugated Polymer Thin‐Film Transistors
Authors: Wu Hung‐Chin , Rondeau‐Gagné Simon , Chiu Yu‐Cheng , Lissel Franziska , To John W. F. , Tsao Yuchi , Oh Jin Young , Tang Bohan , Chen Wen‐Chang , Tok Jeffery B.‐H. , Bao Zhenan 
Published: June 2018

AbstractA high performance diketopyrrolopyrrole (DPP)–based semiconducting polymer is modified with ligands to enable metal coordination, and its subsequent effect as field‐effect transistors is investigated. In specific, pyridine‐2,6‐dicarboxamide (PDCA) units are incorporated in a DPP–based polymer backbone with a content from 0 to 30 mol%, and the resulting polymers are then mixed with Fe(II) ions. The coordination and spontaneous oxidation converts Fe(II) to Fe(III) ions to result in Fe(III)‐containing metallopolymers. The resulting metallopolymers are observed to show good solubility in organic solvents and can be easily processed as thin films. The charge transport characteristics are subsequently investigated through the fabrication of field–effect transistor devices, in which an enhanced charge carrier mobility with the Fe(III)‐containing metallopolymers is observed. In specific, an almost twofold improvement in the charge carrier mobility is obtained for the 20% PDCA‐containing polymer after Fe coordination (from 0.96 to 1.84 cm2 V−1 s−1). Furthermore, the operation stability of the metallopolymer‐based devices is found to be significantly improved with low bias stress. Its superior electrical characteristics are attributed to the doping effect of the Fe ions. This study indicates that incorporation of appropriate metallic ions to polymer presents a viable approach to enhance the performance of polymer–based transistor devices.
Fine Tuning Electronic Structure of Catalysts through Atomic Engineering for Enhanced Hydrogen Evolution
Authors: Huang Yichao , Hu Jun , Xu Haoxiang , Bian Wei , Ge Jingxuan , Zang Dejin , Cheng Daojian , Lv Yaokang , Zhang Cheng , Gu Jing , Wei Yongge 
Published: June 2018

AbstractAn efficient, durable, and low‐cost hydrogen evolution reaction (HER) catalyst is an essential requirement for practical hydrogen production. Herein, an effective approach to facilitate the HER kinetics of molybdenum carbide (Mo2C) electrocatalysts is presented by tuning its electronic structure through atomic engineering of nitrogen implantation. Starting from the organoimido‐derivatized polyoxometalate nanoclusters with inherent MoN bonds, the formation of N‐implanted Mo2C (N@Mo2C) nanocrystals with perfectly adjustable amounts of N atoms is demonstrated. The optimized N@Mo2C electrocatalyst exhibits remarkable HER performance and good stability over 20 h in both acid and basic electrolytes. Further density functional theory calculations show that engineering suitable nitrogen atoms into Mo2C can regulate its electronic structure well and decrease MoH strength, leading to a great enhancement of the HER activity. It could be believed that this ligand‐controlled atomic engineering strategy might influence the overall catalyst design strategy for engineering the activation sites of nonprecious metal catalysts for energy conversions.
Fluorophosphates from Solid‐State Synthesis and Electrochemical Ion Exchange: NaVPO4F or Na3V2(PO4)2F3?
Authors: Li Long , Xu Youlong , Sun Xiaofei , Chang Rui , Zhang Yuan , Zhang Xiaona , Li Ju 
Published: June 2018

AbstractVanadium‐based fluorophosphates are promising sodium‐ion battery cathode materials. Different phases of NaVPO4F and Na3V2(PO4)2F3 are reported in the literature. However, experiments in this work suggest that there could be confusions about the single‐phase NaVPO4F in solid‐state synthesis. Here, systematic investigation of the mechanism underlying structural and compositional evolution of solid‐state synthesis (NaF:VPO4 = 1:1) is determined by in situ and ex situ X‐ray diffraction and electrochemical measurements. Three reactions—3NaF + 3VPO4 → Na3V2(PO4)2F3 + VPO4 (up to 500 °C), Na3V2(PO4)2F3 + VPO4 → Na3V2(PO4)3 + VF3↑ (600–800 °C), and 2Na3V2(PO4)3 → 2(VO)2P2O7 + Na4P2O7 + amorphous products (above 800 °C)—are validated by in situ XRD and thermogravimetric analysis/differential scanning calorimetry. None of the products reported in this work is consistent with single‐phase NaVPO4F at any temperature. It is speculated that the assignments of I4/mmm and C2/c NaVPO4F from solid‐state synthesis are incorrect, which are instead multiphase mixtures of Le Meins' Na3V2(PO4)2F3, unreacted VPO4, and hexagonal Na3V2(PO4)3. Liquid‐electrolyte‐based electrochemical ion exchange of LiVPO4F produces a tavorite NaVPO4F structure, which is very different from Le Meins' family of Na3Al2(PO4)2F3 polymorphs.
Bandgap Narrowing in Non‐Fullerene Acceptors: Single Atom Substitution Leads to High Optoelectronic Response Beyond 1000 nm
Authors: Lee Jaewon , Ko Seo‐Jin , Seifrid Martin , Lee Hansol , Luginbuhl Benjamin R. , Karki Akchheta , Ford Michael , Rosenthal Katie , Cho Kilwon , Nguyen Thuc‐Quyen , Bazan Guillermo C. 
Published: June 2018

AbstractTwo narrow bandgap non‐fullerene acceptors (NBG‐NFAs), namely, COTIC‐4F and SiOTIC‐4F, are designed and synthesized for the fabrication of efficient near‐infrared organic solar cells (OSCs). The chemical structures of the NBG‐NFAs contain a D′‐D‐D′ electron‐rich internal core based on a cyclopentadithiophene (or dithienosilole) (D) and alkoxythienyl (D′) core, end‐capped with the highly electron‐deficient unit 2‐(5,6‐difluoro‐3‐oxo‐2,3‐dihydro‐1H‐inden‐1‐ylidene)malononitrile (A), ultimately providing a A‐D′‐D‐D′‐A molecular configuration that enhances the intramolecular charge transfer characteristics of the excited states. One can thereby reduce the optical bandgap (Egopt) to as low as ≈1.10 eV, one of the smallest values for NFAs reported to date. In bulk‐heterojunction (BHJ) OSCs, NBG‐NFA blends with the polymer donor PTB7‐Th yield power conversion efficiencies (PCE) of up to 9.0%, which is particularly high when compared against a range of NBG BHJ blends. Most significantly, it is found that, despite the small energy loss (Egopt − eVOC) of 0.52 eV, the PTB7‐Th/NBG‐NFA bulk heterojunction blends can yield short‐circuit current densities of up to 22.8 mA cm−2, suggesting that the design and application of NBG‐NFA materials have substantial potential to further improve the PCE of OSCs.
Superflexible Multifunctional Polyvinylpolydimethylsiloxane‐Based Aerogels as Efficient Absorbents, Thermal Superinsulators, and Strain Sensors
Authors: Zu Guoqing , Kanamori Kazuyoshi , Maeno Ayaka , Kaji Hironori , Nakanishi Kazuki 
Published: June 2018

AbstractAerogels are porous materials but show poor mechanical properties and limited functionality, which significantly restrict their practical applications. Preparation of highly bendable and processable aerogels with multifunctionality remains a challenge. Herein we report unprecedented superflexible aerogels based on polyvinylpolydimethylsiloxane (PVPDMS) networks, PVPDMS/polyvinylpolymethylsiloxane (PVPMS) copolymer networks, and PVPDMS/PVPMS/graphene nanocomposites by a facile radical polymerization/hydrolytic polycondensation strategy and ambient pressure drying or freeze drying. The aerogels have a doubly cross‐linked organic–inorganic network structure consisting of flexible polydimethylsiloxanes and hydrocarbon chains with tunable cross‐linking density, tunable pore size and bulk density. They have a high hydrophobicity and superflexibility and combine selective absorption, efficient separation of oil and water, thermal superinsulation, and strain sensing.
Metal–Organic Framework Based Microcapsules
Authors: He Ting , Xu Xiaobin , Ni Bing , Lin Haifeng , Li Chaozhong , Hu Wenping , Wang Xun 
Published: June 2018

AbstractMOFs are a type of ideal crystalline material with rigid reticular structures whereas microcapsules are usually prepared from soft mater, such as polymers or supramolecules. The synthesis of MOF‐based microcapsules with novel nanostructures at the molecular scale remains a great challenge. Herein, we develop a competitive coordination strategy to synthesize MOF‐based microcapsules with novel bowl‐like structures. During the competitive coordination process, the infinite structures of MOFs are partially broken by the competitive reagents, thus flexibility is introduced into the rigid skeletons and results in the formation of bowl‐like microcapsules. Owing to the unique structure and composition of these nano‐structures, the microcapsules exhibit excellent performance and stability in adsorbing and removing iodine for both vapor and solution. This work describes new opportunities in designing MOF‐based microcapsules with novel structures.
Modular One‐Step Three‐Component Synthesis of Tetrahydroisoquinolines Using a Catellani Strategy
Authors: Qian Guangyin , Bai Miao , Gao Shijun , Chen Han , Zhou Siwei , Cheng Hong‐Gang , Yan Wei , Zhou Qianghui 
Published: June 2018

AbstractReported is a modular one‐step three‐component synthesis of tetrahydroisoquinolines using a Catellani strategy. This process exploits aziridines as the alkylating reagents, through palladium/norbornene cooperative catalysis, to enable a Catellani/Heck/aza‐Michael addition cascade. This mild, chemoselective, and scalable protocol has broad substrate scope (43 examples, up to 90 % yield). The most striking feature of this protocol is the excellent regioselectivity and diastereoselectivity observed for 2‐alkyl‐ and 2‐aryl‐substituted aziridines to access 1,3‐cis‐substituted and 1,4‐cis‐substituted tetrahydroisoquinolines, respectively. Moreover, this is a versatile process with high step and atom economy.
Catalytic Enantioselective Synthesis of α‐Chiral Azaheteroaryl Ethylamines by Asymmetric Protonation
Authors: Xu Chao , Muir Calum W. , Leach Andrew G. , Kennedy Alan R. , Watson Allan J. B. 
Published: June 2018

AbstractThe direct enantioselective synthesis of chiral azaheteroaryl ethylamines from vinyl‐substituted N‐heterocycles and anilines is reported. A chiral phosphoric acid (CPA) catalyst promotes dearomatizing aza‐Michael addition to give a prochiral exocyclic aryl enamine, which undergoes asymmetric protonation upon rearomatization. The reaction accommodates a broad range of N‐heterocycles, nucleophiles, and substituents on the prochiral centre, generating the products in high enantioselectivity. DFT studies support a facile nucleophilic addition based on catalyst‐induced LUMO lowering, with site‐selective, rate‐limiting, intramolecular asymmetric proton transfer from the ion‐paired prochiral intermediate.
Embedding 1D Conducting Channels into 3D Isoporous Polymer Films for High‐Performance Humidity Sensing
Authors: Shevate Rahul , Haque Md Azimul , Akhtar Faheem Hassan , Villalobos Luis Francisco , Wu Tom , Peinemann Klaus‐Viktor 
Published: June 2018

AbstractIsoporous block copolymer (BCP) films have received exponential interest as highly selective membranes, stemming from their unique morphological features, but their applications in functional devices remain to be realized. Now single‐walled carbon nanotubes (CNTs) were efficiently incorporated into isoporous block copolymer films for chemiresistive sensing at room temperature. Leveraging the efficient charge extraction ability of CNTs together with nanochannel arrays aligned perpendicular to the surface of the films, an ultrafast response time of 0.3 s was achieved for humidity detection with a sensor response of about 800 on changing humidity from 10 % to 95 %. Furthermore, the sensor also responds to various organic vapors, underscoring its promising detection capability.
Recognition of Complex Core‐Fucosylated N‐Glycans by a Mini Lectin
Authors: Cabanettes Aurore , Perkams Lukas , Spies Carolina , Unverzagt Carlo , Varrot Annabelle 
Published: June 2018

AbstractThe mini fungal lectin PhoSL was recombinantly produced and characterized. Despite a length of only 40 amino acids, PhoSL exclusively recognizes N‐glycans with α1,6‐linked fucose. Core fucosylation influences the intrinsic properties and bioactivities of mammalian N‐glycoproteins and its level is linked to various cancers. Thus, PhoSL serves as a promising tool for glycoprofiling. Without structural precedence, the crystal structure was solved using the zinc anomalous signal, and revealed an interlaced trimer creating a novel protein fold termed β‐prism III. Three biantennary core‐fucosylated N‐glycan azides of 8 to 12 sugars were cocrystallized with PhoSL. The resulting highly resolved structures gave a detailed view on how the exclusive recognition of α1,6‐fucosylated N‐glycans by such a small protein occurs. This work also provided a protein consensus motif for the observed specificity as well as a glimpse into N‐glycan flexibility upon binding.
Green synthesis of silver nanoparticles using Thymus kotschyanus extract and evaluation of their antioxidant, antibacterial and cytotoxic effects
Authors: Hamelian Mona , Zangeneh Mohammad Mahdi , Amisama Abbas , Varmira Kambiz , Veisi Hojat 
Published: June 2018

Present study used ecofriendly, cost efficient and easy method for synthesis of silver nanoparticles (Ag NPs) at the room temperature by Thymus Kotschyanus extract as reducing and capping agent. Various analytical technique including UV–Vis absorption spectroscopy determined presence of Ag NPs in the solution, the functional groups of Thymus Kotschyanus extract in the reduction and capping process of Ag NPs are approved by FT‐IR, crystallinity with the fcc plane approved from the X‐ray diffraction (XRD) pattern, energy dispersive spectroscopy (EDS) determined existence of elements in the sample, surface morphology, diverse shapes and size of present Ag NPs were showed by using scanning electron microscopy (SEM), atomic force microscopy (AFM) and high resolution transmission electron microscopy (HRTEM). Beginning and end destroy temperature of present silver nanoparticles were determined by thermal gravimetric spectroscopy (TGA). In addition, antibacterial, antioxidant and cytotoxicity properties of Ag NPs were studied. Agar disk and agar well diffusion are the methods to determined antibacterial properties of synthesized Ag NPs. Also MIC (Minimum Inhibitory Concentration) and MBC (Minimum Bactericidal Concentration) were recognized by macro broth dilution assay. DPPH free radical scavenging assay was used for antioxidant property and compare to butylated hydroxytoluene (BHT) as standard antioxidant that showed high antioxidant activity more than BHT. Synthesized Ag NPs have great cell viability in a dose depended manner and demonstrate that this method for synthesis silver nanoparticles provided nontoxic. The average diameter of synthesized Ag NPs was about 50–60 nm.
Hydrothermal leather waste by hydrothermal method for uranium (VI) removal from a Simulated Saline Solution
Authors: Deng Guohong , Zhang Yu , Luo Xuegang , Yang Jiayi 
Published: June 2018

Hydrothermal leather waste was prepared by hydrothermal method, using leather waste as the precondition and applying the adsorption of uranium (VI) in solution. The effects of pH value, adsorption time and initial concentration of uranium (VI) on the adsorption efficiency were investigated. The adsorption process was in accordance with the pseudo‐second‐order kinetic model and Freundlich adsorption isotherm model. Kinetic and thermodynamic studies showed that the adsorption process was endothermic and spontaneous, and it reached adsorption equilibrium in 240 min. In the simulated high salinity environment, the adsorbent exhibited excellent adsorption rate on the trace of uranium (VI). The adsorbent was characterized by scanning electron microscopy, flourier transform infrared spectroscopy and X‐ray photoelectron spectroscopy, and it was found that the adsorption mechanism was coordinated complex.
Brummer‐dependent lipid mobilization regulates starvation resistance in Nilaparvata lugens
Authors: Zhou Jinming , Chen Xia , Yan Jing , You Keke , Yuan Zhineng , Zhou Qiang , Lu Kai 
Published: June 2018

AbstractEnergy homeostasis is an essential characteristic of all organisms, requiring fluctuation in energy accumulation, mobilization, and exchange with the external environment. In insects, energy mobilization is under control of the lipase brummer (bmm), which regulates nutritional status by hydrolyzing the ester bonds in triacylglycerol (TAG). In the present study, we investigated the role of bmm in the lipid mobilization and starvation resistance in the brown planthopper (BPH; Nilaparvata lugens), which is economically one of the most important rice pests in Asia. A severe decrease in TAG and glyceride contents was observed in the starved BPHs, while there was a partial rescue after refeeding. The starvation condition caused a significant increase in the expression levels of Nlbmm, and supplement of food after starvation dramatically reduced the Nlbmm expression. Sucrose rescue after starvation significantly suppressed the expression of Nlbmm, while caused an accumulation of TAG and glyceride. Knockdown of Nlbmm by double‐stranded RNA treatment extended the lifespan to starvation, whereas it increased the level of TAG and glyceride in the BPHs. The decreased lipolysis rate by dsNlbmm‐treated BPHs eventually resulted in increase of starvation resistance. These data demonstrated that the regulation of energy homeostasis by Nlbmm affects starvation resistance, probably through lipid mobilization control in N. lugens.
Baseline Plasma Cell Gene Signature Predicts Improvement in Systemic Sclerosis Skin Scores Following Treatment With Inebilizumab (MEDI‐551) and Correlates With Disease Activity in Systemic Lupus Erythematosus and Chronic Obstructive Pulmonary Disease
Authors: Streicher Katie , Sridhar Sriram , Kuziora Mike , Morehouse Christopher A. , Higgs Brandon W. , Sebastian Yinong , Groves Christopher J. , Pilataxi Fernanda , Brohawn Philip Z. , Herbst Ronald , Ranade Koustubh 
Published: June 2018

ObjectiveB cells impact the progression of systemic sclerosis (SSc; scleroderma) through multiple pathogenic mechanisms. CD19 inhibition in mice reduced skin thickness, collagen production, and autoantibody levels, consistent with CD19 expression on plasma cells (PCs), the source of antibody production. PC depletion could effectively reduce collagen deposition and inflammation in SSc; therefore, we investigated the effects of PC depletion on SSc disease activity.MethodsA PC gene signature was evaluated in SSc skin biopsy samples in 2 phase I clinical trials. We assessed microarray data from tissue from public studies of chronic obstructive pulmonary disease (COPD), idiopathic pulmonary fibrosis (IPF), dermatomyositis (DM), systemic lupus erythematosus (SLE), and atopic dermatitis, as well as blood from a phase IIb clinical trial in SLE.ResultsThe PC signature was elevated in SSc skin specimens compared to healthy donor skin (P = 2.28 × 10−6) and correlated with the baseline modified Rodnan skin thickness score (MRSS) (r = 0.64, P = 0.0004). Patients with a high PC signature at baseline showed greater improvement in the MRSS (mean ± SD change 35 ± 16%; P = 6.30 × 10−4) following anti‐CD19 treatment with inebilizumab (MEDI‐551) than did patients with a low PC signature at baseline (mean ± SD change 8 ± 12%; P = 0.104). The PC signature was overexpressed in tissue from patients with SLE, DM, COPD, interstitial lung disease, and IPF relative to controls (all fold change >2; P < 0.001). The PC signature also differed significantly between SLE patients with mild‐to‐moderate disease and those with severe disease (SLE Disease Activity Index cutoff at 10) (fold change 1.44; P = 3.90 × 10−3) and correlated significantly with the degree of emphysema in COPD (r = 0.53, P = 7.55 × 10−8).ConclusionOur results support the notion that PCs have a role in the pathogenesis of SSc and other autoimmune or pulmonary indications. An elevated pretreatment PC signature was associated with increased benefit from MEDI‐551 in SSc.
A regulatory mutant on TRIM26 conferring the risk of nasopharyngeal carcinoma by inducing low immune response
Authors: Lyu Xiao‐Ming , Zhu Xiao‐Wei , Zhao Manli , Zuo Xian‐Bo , Huang Zhong‐Xi , Liu Xiao , Jiang Tao , Yang Xue‐Xi , Li Xin , Long Xiao‐Bing , Wang Jian‐Guo , Li Jin‐Bang , Han Ming‐Yu , Wang Shuang , Liu Teng‐Fei , Zhang Bo , Sun Tao , Cheng Zhi , Qiu Mo‐Chang , Dong Lei , Zheng Lu , Zhang Long‐Cheng , Wang Jia‐Hong , Wei Gan‐Guan , Yao Kaitai , Wang Qian , Zheng Hou‐Feng , Li Xin 
Published: June 2018

AbstractThe major histocompatibility complex (MHC) is most closely associated with nasopharyngeal carcinoma (NPC), but the complexity of its genome structure has proven challenging for the discovery of causal MHC loci or genes. We conducted a targeted MHC sequencing in 40 Cantonese NPC patients followed by a two‐stage replication in 1065 NPC cases and 2137 controls of Southern Chinese descendent. Quantitative RT‐PCR analysis (qRT‐PCR) was used to detect gene expression status in 108 NPC and 43 noncancerous nasopharyngeal (NP) samples. Luciferase reporter assay and chromatin immunoprecipitation (ChIP) were used to assess the transcription factor binding site. We discovered that a novel SNP rs117565607_A at TRIM26 displayed the strongest association (OR = 1.909, Pcombined = 2.750 × 10−19). We also observed that TRIM26 was significantly downregulated in NPC tissue samples with genotype AA/AT than TT. Immunohistochemistry (IHC) test also found the TRIM26 protein expression in NPC tissue samples with the genotype AA/AT was lower than TT. According to computational prediction, rs117565607 locus was a binding site for the transcription factor Yin Yang 1 (YY1). We observed that the luciferase activity of YY1 which is binding to the A allele of rs117565607 was suppressed. ChIP data showed that YY1 was binding with T not A allele. Significance analysis of microarray suggested that TRIM26 downregulation was related to low immune response in NPC. We have identified a novel gene TRIM26 and a novel SNP rs117565607_A associated with NPC risk by regulating transcriptional process and established a new functional link between TRIM26 downregulation and low immune response in NPC.
Gold Nanoparticles Incorporated in a Zinc‐Based Metal‐Organic Framework as Multifunctional Catalyst for the Oxygen Reduction and Hydrogen Evolution Reactions
Authors: Yadav Dharmendra K. , Gupta Rupali , Ganesan Vellaichamy , Sonkar Piyush K. , Yadav Mamta 
Published: June 2018

AbstractSuccessful synthesis of gold nanoparticles incorporated in a zinc‐based metal‐organic framework (Au@Zn‐MOF) is reported in this paper. The synthesis of Au@Zn‐MOF is confirmed by UV‐Vis, FT‐IR and X‐ray photoelectron spectroscopy (XPS) studies. The Au@Zn‐MOF catalyst demonstrates electrocatalytic activity towards the oxygen reduction reaction (ORR) and the hydrogen evolution reaction (HER). The relative catalytic performance of Au@Zn‐MOF towards ORR and HER has been studied under acidic condition. ORR proceeds via a two electron and two proton mechanism with hydrogen peroxide as the end product, while HER follows the Volmer mechanism i. e., adsorption of H+ on the catalyst's active sites. Au@Zn‐MOF exhibits an ORR onset potential of 0.45 V (vs. RHE) with two different Tafel slopes, −93 and −103.6 mV in acidic solution. Further, an excellent catalytic activity is observed for HER with an onset potential of 0.02 V (vs. RHE) and a Tafel slope of 87 mV in N2 saturated 0.1 M HClO4 solution. However, in O2 saturated 0.1 M HClO4 solution, a HER onset potential of 0.04 V (vs. RHE) is observed with two different Tafel slopes, 610 and 220 mV. The value of Tafel slopes in the presence of O2 advocates the diminution of the ORR activity because of the HER. Thus, Tafel slope values of HER and ORR suggest that protons and O2 compete to reach the electrode surface for getting reduced.