bluuebunny/crossref_metadata_2025_split huggingface dataset:
The Second Spacer Cation Assisted Growth of a 2D Perovskite Film with Oriented Large Grain for Highly Efficient and Stable Solar Cells
Authors: Lian Xiaomei , Chen Jiehuan , Qin Minchao , Zhang Yingzhu , Tian Shuoxun , Lu Xinhui , Wu Gang , Chen Hongzheng 
Published: May 2019

AbstractThe fabrication of high‐quality film with large grains oriented along the direction of film thickness is important for 2D Ruddlesden–Popper perovskite‐based solar cells (PVSCs). High‐quality 2D BA2MAn−1PbnI3n+1 (BA+=butylammonium, MA+=methylammonium, n=5) perovskite films were fabricated with a grain size of over 1 μm and preferential orientation growth by introducing a second spacer cation (SSC+) into the precursor solution. Dynamic light scattering showed that SSC+ addition can induce aggregation in the precursor solution. The precursor aggregates are favorable for the formation of large crystal grains by inducing nucleation and decreasing the nucleation sites. Applying phenylethylammonium as SSC+, the optimized inverted planar PVSCs presented a maximum PCE of 14.09 %, which is the highest value of the 2D BA2MAn−1PbnI3n+1 (n=5) PVSCs. The unsealed device shows good moisture stability by maintaining around 90 % of its initially efficiency after 1000 h exposure to air (Hr=25±5 %).
S‐Adamantyl Group Directed Site‐Selective Acylation: Applications in Streamlined Assembly of Oligosaccharides
Authors: Blaszczyk Stephanie A. , Xiao Guozhi , Wen Peng , Hao Hua , Wu Jessica , Wang Bo , Carattino Francisco , Li Ziyuan , Glazier Daniel A. , McCarty Bethany J. , Liu Peng , Tang Weiping 
Published: May 2019

AbstractThe site‐selective functionalization of carbohydrates is an active area of research. Reported here is the surprising observation that the sterically encumbered adamantyl group directed site‐selective acylation at the C2 position of S‐glycosides through dispersion interactions between the adamantyl C−H bonds and the π system of the cationic acylated catalyst, which may have broad implications in many other chemical reactions. Because of their stability, chemical orthogonality, and ease of activation for glycosylation, the site‐selective acylation of S‐glycosides streamlines oligosaccharide synthesis and will have wide applications in complex carbohydrate synthesis.
Non‐natural Photoenzymatic Controlled Radical Polymerization Inspired by DNA Photolyase
Authors: Zhou Fanfan , Li Ruoyu , Wang Xiao , Du Simin , An Zesheng 
Published: May 2019

AbstractInspired by DNA photolyase, a non‐natural photoenzymatic catalysis of common flavoproteins is developed for controlled radical polymerization under irradiation of visible light. This photoenzymatic polymerization is highly efficient under mild conditions, applicable to various monomer families, suitable for both homogeneous and heterogeneous media, and can be externally modulated by switching light on and off. A unique combination of the natural enzymatic deoxygenation with the non‐natural photoenzymatic process enables an unprecedented oxygen‐tolerant, visible‐light‐controlled radical polymerization using a single enzyme to be developed. Visible light activation of non‐natural catalytic functions of the widely distributed flavoproteins is an exciting conceptual advance and may uncover a hitherto underexplored field of photoenzymatic catalysis.
Encapsulating Perovskite Quantum Dots in Iron‐Based Metal–Organic Frameworks (MOFs) for Efficient Photocatalytic CO2 Reduction
Authors: Wu Li‐Yuan , Mu Yan‐Fei , Guo Xiao‐Xuan , Zhang Wen , Zhang Zhi‐Ming , Zhang Min , Lu Tong‐Bu 
Published: May 2019

AbstractImproving the stability of lead halide perovskite quantum dots (QDs) in a system containing water is the key for their practical application in artificial photosynthesis. Herein, we encapsulate low‐cost CH3NH3PbI3 (MAPbI3) perovskite QDs in the pores of earth‐abundant Fe‐porphyrin based metal organic framework (MOF) PCN‐221(Fex) by a sequential deposition route, to construct a series of composite photocatalysts of MAPbI3@PCN‐221(Fex) (x=0–1). Protected by the MOF the composite photocatalysts exhibit much improved stability in reaction systems containing water. The close contact of QDs to the Fe catalytic site in the MOF, allows the photogenerated electrons in the QDs to transfer rapidly the Fe catalytic sites to enhance the photocatalytic activity for CO2 reduction. Using water as an electron source, MAPbI3@PCN‐221(Fe0.2) exhibits a record‐high total yield of 1559 μmol g−1 for photocatalytic CO2 reduction to CO (34 %) and CH4 (66 %), 38 times higher than that of PCN‐221(Fe0.2) in the absence of perovskite QDs.
Ligand‐Controlled Regiodivergent Enantioselective Rhodium‐Catalyzed Alkene Hydroboration
Authors: Bochat Andrew J. , Shoba Veronika M. , Takacs James M. 
Published: May 2019

AbstractRegiocontrol in the rhodium‐catalyzed boration of vinyl arenes is typically dominated by the presence of the conjugated aryl substituent. However, small differences in TADDOL‐derived chiral monophosphite ligands can override this effect and direct rhodium‐catalyzed hydroboration of β‐aryl and β‐heteroaryl methylidenes by pinacolborane to selectively produce either chiral primary or tertiary borated products. The regiodivergent behavior is coupled with enantiodivergent addition of the borane. The nature of the TADDOL backbone substituents and that of the phosphite moiety function synergistically to direct the sense and extent of regioselectivity and enantioinduction. Twenty substrates are shown to undergo each reaction mode with regioselectivity values reaching greater than 20:1 and enantiomer ratios reaching up to 98:2. A variety of subsequent transformations illustrate the potential utility of each product.
Four‐Coordinate Copper Halonitrosyl {CuNO}10 Complexes
Authors: Bower Jamey K. , Sokolov Alexander Yu. , Zhang Shiyu 
Published: May 2019

AbstractWhile copper nitrosyl complexes are implicated in numerous biological systems, isolable examples remain limited. In this report, we show that [Cl3CuNO]−, with a {CuNO}10 electron configuration, can be generated by nitrite reduction at a copper(I) dichloride anion or by nitric oxide addition to a copper(II) trichloride precursor. The bromide analogue, [Br3CuNO]− was synthesized analogously, and both copper halonitrosyl complexes were characterized by X‐ray diffraction and a variety of spectroscopic methods. Experimental data and multireference (CASSCF/NEVPT2) calculations provide strong evidence for a CuII–NO. ground state. Both [Cl3CuNO]− and [Br3CuNO]− release and recapture NO. reversibly, and exhibit nitrosative reactivities toward a wide range of biological nucleophiles, such as amines, alcohols, and thiols.
Demethylenation of Cyclopropanes via Photoinduced Guest‐to‐Host Electron Transfer in an M6L4 Cage
Authors: Cullen William , Takezawa Hiroki , Fujita Makoto 
Published: May 2019

AbstractUnusual demethylenation reactions of cyclopropanes under UV‐light irradiation were found within a cavity of a photoactive coordination cage. The reaction proceeded via a guest‐to‐host electron transfer owing to the highly electron‐deficient nature of the cage. The reactions were highly chemoselective and enabled late‐stage derivatization of a steroid molecule, which led to a totally new un‐natural steroid.
N‐Linked Glycans in the Variable Domain of IgG Anti–Citrullinated Protein Antibodies Predict the Development of Rheumatoid Arthritis
Authors: Hafkenscheid Lise , de Moel Emma , Smolik Irene , Tanner Stacey , Meng Xiaobo , Jansen Bas C. , Bondt Albert , Wuhrer Manfred , Huizinga Tom W. J. , Toes Rene E. M. , El‐Gabalawy Hani , Scherer Hans U. 
Published: May 2019

ObjectiveAnti–citrullinated protein antibodies (ACPAs) are disease‐specific biomarkers in rheumatoid arthritis (RA). More than 90% of IgG ACPAs harbor N‐linked glycans in the antibody variable (V) domain. The corresponding N‐glycosylation sites in ACPA V‐region sequences result from somatic hypermutation, a T cell–dependent process. As ample evidence indicates that T cells drive the maturation of the ACPA response prior to arthritis onset, we undertook this study to investigate whether the presence of glycans in IgG ACPA V domains predicts the transition from predisease autoimmunity to overt RA.MethodsWe analyzed 2 independent sets of serum samples obtained from 126 ACPA‐positive first‐degree relatives (FDRs) of RA patients. Both sets originated from an Indigenous North American population and comprised cross‐sectional and longitudinal samples of individuals who did or did not develop inflammatory arthritis. Serum IgG ACPAs were affinity‐purified and subjected to ultra high‐performance liquid chromatography–based glycan analysis.ResultsIn both data sets, FDR‐derived IgG ACPA displayed markedly lower levels of V domain glycans (<50%) compared to IgG ACPA from RA patients. Notably, FDRs who later developed RA showed extensive V‐domain glycosylation before the onset of arthritis. Moreover, IgG ACPA V‐domain glycosylation was strongly associated with future development of RA (hazard ratio 6.07 [95% confidence interval 1.46–25.2]; P = 0.013).ConclusionExtensive glycosylation of the IgG ACPA V domain is present in a subset of predisposed FDRs of Indigenous North American RA patients. The presence of this feature substantially increases the risk of RA development. Based on these findings, we propose that glycosylation of the IgG ACPA V domain represents a predictive marker for RA development in ACPA‐positive individuals and may serve to better target prevention measures.
GMPP tracking based on model reference LPV control for a PV system with buck converter modelled on bond graph
Authors: Galindo Orozco René , Villa Villaseñor Noé 
Published: May 2019

AbstractA PhotoVoltaic (PV) system with a Linear Parametric Varying (LPV) average model of a buck converter modelled by bond graph methodology, is considered. It is assumed that the voltage generated by the PV panel is a smooth function of time under changes in atmospheric conditions. A model reference is proposed representing the PV system with buck converter operating at the Global Maximum Power Point (GMPP). An LPV control is designed, and an algorithm is proposed in a model reference tracking control configuration assuring that the PV system with buck converter tracks the proposed model reference and hence guaranteeing that this system operates at the GMPP. The proposed algorithm changes the voltage reference based on the power measurement of the PV system assuring that this reference represents the GMPP under shading conditions. The LPV control is designed for an average model of the buck converter solving a feasibility problem based on linear matrix inequalities that assure quadratic stability and minimize a quadratic criterion. The feedback system is tested under shading conditions, and its performance is compared with a standard Perturb and Observe method and with an ideal algorithm based on the irradiance measurement in each section of the PV system.
Aberrant brain network topology in fronto‐limbic circuitry differentiates euthymic bipolar disorder from recurrent major depressive disorder
Authors: Dvorak Jannis , Hilke Marietheres , Trettin Marco , Wenzler Sofia , Hagen Marleen , Ghirmai Naddy , Müller Maximilian , Kraft Dominik , Reif Andreas , Oertel Viola 
Published: May 2019

AbstractIntroductionPrevious studies have established graph theoretical analysis of functional network connectivity (FNC) as a potential tool to detect neurobiological underpinnings of psychiatric disorders. Despite the promising outcomes in studies that examined FNC aberrancies in bipolar disorder (BD) and major depressive disorder (MDD), there is still a lack of research comparing both mood disorders, especially in a nondepressed state. In this study, we used graph theoretical network analysis to compare brain network properties of euthymic BD, euthymic MDD and healthy controls (HC) to evaluate whether these groups showed distinct features in FNC.MethodsWe collected resting‐state functional magnetic resonance imaging (fMRI) data from 20 BD patients, 15 patients with recurrent MDD as well as 30 age‐ and gender‐matched HC. Graph theoretical analyses were then applied to investigate functional brain networks on a global and regional network level.ResultsGlobal network analysis revealed a significantly higher mean global clustering coefficient in BD compared to HC. We further detected frontal, temporal and subcortical nodes in emotion regulation areas such as the limbic system and associated regions exhibiting significant differences in network integration and segregation in BD compared to MDD patients and HC. Participants with MDD and HC only differed in frontal and insular network centrality.ConclusionIn conclusion, our findings indicate that a significantly altered brain network topology in the limbic system might be a trait marker specific to BD. Brain network analysis in these regions may therefore be used to differentiate euthymic BD not only from HC but also from patients with MDD.
Interethnic differences in pancreatic cancer incidence and risk factors: The Multiethnic Cohort
Authors: Huang Brian Z. , Stram Daniel O. , Le Marchand Loic , Haiman Christopher A. , Wilkens Lynne R. , Pandol Stephen J. , Zhang Zuo‐Feng , Monroe Kristine R. , Setiawan Veronica Wendy 
Published: May 2019

AbstractWhile disparity in pancreatic cancer incidence between blacks and whites has been observed, few studies have examined disparity in other ethnic minorities. We evaluated variations in pancreatic cancer incidence and assessed the extent to which known risk factors account for differences in pancreatic cancer risk among African Americans, Native Hawaiians, Japanese Americans, Latino Americans, and European Americans in the Multiethnic Cohort Study. Risk factor data were obtained from the baseline questionnaire. Cox regression was used to estimate the relative risks (RRs) and 95% confidence intervals (CIs) for pancreatic cancer associated with risk factors and ethnicity. During an average 16.9‐year follow‐up, 1,532 incident pancreatic cancer cases were identified among 184,559 at‐risk participants. Family history of pancreatic cancer (RR 1.97, 95% CI 1.50‐2.58), diabetes (RR 1.32, 95% CI 1.14‐1.54), body mass index ≥30 kg/m2 (RR 1.25, 95% CI 1.08‐1.46), current smoking (<20 pack‐years RR 1.43, 95% CI 1.19‐1.73; ≥20 pack‐years RR 1.76, 95% CI 1.46‐2.12), and red meat intake (RR 1.17, 95% CI 1.00‐1.36) were associated with pancreatic cancer. After adjustment for these risk factors, Native Hawaiians (RR 1.60, 95% CI 1.30‐1.98), Japanese Americans (RR 1.33, 95% CI 1.15‐1.54), and African Americans (RR 1.20, 95% CI 1.01‐1.42), but not Latino Americans (RR 0.90, 95% CI 0.76‐1.07), had a higher risk of pancreatic cancer compared to European Americans. Interethnic differences in pancreatic cancer risk are not fully explained by differences in the distribution of known risk factors. The greater risks in Native Hawaiians and Japanese Americans are new findings and elucidating the causes of these high rates may improve our understanding and prevention of pancreatic cancer.
The role of microRNAs in the involvement of vascular smooth muscle cells in the development of atherosclerosis
Authors: Li Linqing , Li Yongjun , Tang Chengchun 
Published: May 2019

AbstractMicroRNAs (miRNAs) are a class of nonprotein‐encoding RNAs of ~22 nucleotides in length that bind to or complement each other with a target gene messenger RNA (mRNA) to promote mRNA degradation or inhibit translation of the target mRNA. The protein required [such as Toll‐like receptor (TLR) proteins] is controlled at an optimal level. By affecting protein translation, miRNAs have become powerful regulators of biological processes, including development, differentiation, cell proliferation, and apoptosis. MiRNAs are involved in the regulation of proliferation, migration, and apoptosis of vascular smooth muscle cells (VSMCs), thereby affecting the formation of atherosclerosis (AS). In recent years, the role and mechanism of miRNAs involved in AS development in VSMCs have been studied extensively. In the current study, the results and progress in miRNA research are reviewed.
Comparison of drug eluting versus bare metal stents for pulmonary vein stenosis in childhood
Authors: Khan Asra , Qureshi Athar M. , Justino Henri 
Published: May 2019

AbstractObjectiveComparison of outcomes using bare metal (BMS) and drug‐eluting (DES) stents in pulmonary vein stenosis (PVS).BackgroundPVS is a serious condition with frequent restenosis after surgical and percutaneous interventions. After experiencing encouraging results with DES, we sought to compare outcomes of BMS and DES in native and post‐surgical PVS.Methods and ResultsA retrospective review of all patients who underwent stent implantation between 08/93 and 11/17 for PVS at Texas Children's Hospital was performed. BMS were used to treat 58 lesions in 37 patients and 105 DES used to treat 105 lesions in 41 patients. Mean age at first stent implant was 2.9 ± 3.5 years in BMS and 16.2 ± 18.8 months in DES group. Of those with follow‐up catheterization, mean lumen loss rate from stent implant to first follow‐up catheterization was 0.85 ± 1.47 mm/month over 6.4 ± 6.4 months in the BMS group (n = 44 lesions) compared to 0.16 ± 0.31 mm/month over 6.8 ± 7.4 months in the DES group (n = 86 lesions), p < .01. Follow‐up for the BMS group was 14 months (6 days–22.3 years), with 13 mortalities, eight lesions were re‐stented and six complete occlusions were noted. Follow‐up for DES group (including four cross‐overs) was 17.5 months (3 days‐9 years), with 10 mortalities, seven lesions were re‐stented, 11 had complete occlusion, 20 new adjacent lesions in the same vessel underwent stenting and 12 stents were intentionally fractured.ConclusionDES have significantly lowered lumen loss rate when compared to BMS at medium term follow‐up and can be fractured to enable larger diameters. Availability of larger diameter DES would be ideal.
Light chain lambda myeloma with fatal AL cardiac amyloidosis in a 21‐year‐old patient: A case report and review
Authors: Camus Vincent , Dubois Sydney , Thiébaut Pierre‐Alain , Lepretre Stéphane , Lenain Pascal , Picquenot Jean‐Michel , Veresezan Elena‐Liana , François Arnaud , Penther Dominique , Bauer Fabrice , Jaccard Arnaud , Jardin Fabrice 
Published: May 2019

Abstract
Multi‐organ AL amyloidosis is a therapeutic challenge because of light chain deposits severely damaging the function of concerned organs. Cardiac involvement, which leads to concentric hypertrophy of both ventricles, is particularly severe and leads to poor prognosis regardless of combination chemotherapy. This case pinpoints the relevance of combining clinical, histological, and echocardiographic information in the management of this complex and life‐threatening disease.
Mesoporous Aluminosilicate Nanofibers with a Low Si/Al Ratio as Acidic Catalyst for Hydrodeoxygenation of Phenol
Authors: Haynes Tommy , D'hondt Thibaut , Morritt Alexander L. , Khimyak Yaroslav Z. , Desmecht Didier , Dubois Vincent , Hermans Sophie 
Published: May 2019

AbstractMesoporous aluminosilicate nanofibers (mASNF) were prepared using hard and soft dual templates approach. The mesoporous material was fully characterized and its acidic nature was confirmed by FTIR spectroscopy of pyridine adsorption and 27Al/29Si solid state NMR. Thanks to the incorporated aluminum atoms, the acidic material showed high hydrothermal stability which is an essential property for biomass conversion applications. The catalytic performance of Pd supported on mASNF for hydrodeoxygenation (HDO) of lignin model compound was also investigated. A complete conversion and a high selectivity towards cyclohexane (up to 95 %) starting from phenol were achieved with this bifunctional catalyst. In comparison, no cyclohexane has been produced with a non‐acidic material which underlines the importance of acidic sites in HDO process selectivity control. Moreover, the catalyst can be recycled without losing its initial structure.
Magnetization Slow Dynamics in Ferrocenium Complexes
Authors: Ding Mei , Hickey Anne K. , Pink Maren , Telser Joshua , Tierney David L. , Amoza Martin , Rouzières Mathieu , Ozumerzifon Tarik J. , Hoffert Wesley A. , Shores Matthew P. , Ruiz Eliseo , Clérac Rodolphe , Smith Jeremy M. 
Published: May 2019

AbstractThe single‐molecule magnet (SMM) properties of a series of ferrocenium complexes, [Fe(η5‐C5R5)2]+ (R=Me, Bn), are reported. In the presence of an applied dc field, the slow dynamics of the magnetization in [Fe(η5‐C5Me5)2]BArF are revealed. Multireference quantum mechanical calculations show a large energy difference between the ground and first excited states, excluding the commonly invoked, thermally activated (Orbach‐like) mechanism of relaxation. In contrast, a detailed analysis of the relaxation time highlights that both direct and Raman processes are responsible for the SMM properties. Similarly, the bulky ferrocenium complexes, [Fe(η5‐C5Bn5)2]BF4 and [Fe(η5‐C5Bn5)2]PF6, also exhibit magnetization slow dynamics, however an additional relaxation process is clearly detected for these analogous systems.
Manganese‐Mediated Formic Acid Dehydrogenation
Authors: Anderson Nickolas H. , Boncella James , Tondreau Aaron M. 
Published: May 2019

AbstractA robust and rapid manganese formic acid (FA) dehydrogenation catalyst is reported. The manganese is supported by the recently developed, hybrid backbone chelate ligand tBuPNNOP (tBuPNNOP=2,6‐(di‐tert‐butylphosphinito)(di‐tert‐butylphosphinamine)pyridine) (1) and the catalyst is readily prepared with MnBrCO5 to form [(tBuPNNOP)Mn(CO)2][Br] (2). Dehydrohalogenation of 2 generated the neutral five coordinate complex (tBuPNNOP)Mn(CO)2 (3). Dehydrogenation of FA by 2 and 3 was found to be highly efficient, exhibiting turnover frequencies (TOFs) exceeding 8500 h−1, rivaling many noble metal systems. The parent chelate, tBuPONOP (tBuPONOP=2,6‐bis(di‐tert‐butylphosphinito)pyridine) or tBuPNNNP (tBuPNNNP=2,6‐bis (di‐tert‐butylphosphinamine)pyridine), coordination complexes of Mn were synthesized, respectively affording [(tBuPONOP)Mn(CO)2][Br] (4) and [(tBuPNNNP)Mn(CO)2][Br] (5). FA dehydrogenation with the hybrid‐ligand supported 2 exhibits superior catalysis to 4 and 5.
N‐Substituted Benzene‐1‐Urea‐3,5‐Biscarboxamide (BUBA): Easily Accessible C2‐Symmetric Monomers for the Construction of Reversible and Chirally Amplified Helical Assemblies
Authors: Li Yan , Dubreucq Ludovic , Alvarenga Bruno G. , Raynal Matthieu , Bouteiller Laurent 
Published: May 2019

AbstractNon‐C3‐symmetric supramolecular helices are gaining interest for the design of hierarchical assemblies, for the compartmentalisation or the self‐assembly of polymer chains and for application in asymmetric catalysis. Herein, N‐substituted benzene‐1‐urea‐3,5‐biscarboxamide (BUBA) monomers, which consist of one urea and two carbon‐connected amide functions linked to an aromatic ring, are introduced as an easily accessible class of C2‐symmetric supramolecular synthons. In apolar solvents, BUBA monomers assemble into long helical assemblies by means of hydrogen‐bonding and aromatic interactions, as assessed by several analytical techniques. To probe the influence of the urea function, BUBA and related benzene‐1,3,5‐tricarboxamide (BTA) helical polymers have been compared, in terms of their thermodynamics of formation, stability, reversibility and chiral amplification properties. Similar to BTA, BUBA monomers form long helices reversibly through a highly cooperative mechanism and the helicity of their assemblies is governed by chiral amplification effects. However, precise quantification of their properties reveals that BUBA monomers assemble in a more cooperative manner. Also, chiral amplification operates to a higher extent in BUBA helices, as probed by both sergeants‐and‐soldiers and majority‐rules experiments. Compatibility between urea and amide functions also allows the formation of co‐assemblies that incorporate both BUBA and BTA monomers. Importantly, a small amount of chiral BUBA monomers in these co‐assemblies is sufficient to obtain single‐handed helices; thus paving the way towards the development of functional supramolecular helices.