bluuebunny/crossref_metadata_2025_split huggingface dataset:
Understanding the Selectivity of the Oxygen Reduction Reaction at the Atomistic Level on Nitrogen‐Doped Graphitic Carbon Materials
Authors: Fernandez‐Escamilla Hector Noe , Guerrero‐Sanchez Jonathan , Contreras Enrique , Ruiz‐Marizcal Jose Manuel , Alonso‐Nunez Gabriel , Contreras Oscar E. , Felix‐Navarro Rosa María , Romo‐Herrera Jose M. , Takeuchi Noboru 
Published: November 2020

AbstractThe oxygen reduction reaction (ORR) is of paramount interest, in the context of both alternative energy applications in fuel cells and for on‐site hydrogen peroxide (H2O2) production in environmental remediation applications. Using theoretical and experimental methods, the mechanism involved in the ORR is studied on nitrogen‐doped graphitic carbon materials. The two principal reaction pathways involved in the ORR are the four‐electron pathway producing water (H2O), or the two‐electron pathway leading to the formation of H2O2. An atomistic step by step ORR mechanism is proposed to understand the selectivity of the reaction toward the two principal pathways. The results show that graphitic N sites favor the two‐electron pathway, in a similar way to three pyridinic N sites. Meanwhile, the one or two pyridinic N sites lead to the four‐electron pathway. The calculations show the importance of dangling bonds and/or pentagonal C rings in selectivity toward the four‐electron pathway. The results are consistent with recent reports on the importance of topological defects in graphitic carbon materials. The understanding of the ORR mechanism is very important for the design and development of novel ORR electrocatalysts to favor the required pathway, according to the application.
Single Ru Atoms Stabilized by Hybrid Amorphous/Crystalline FeCoNi Layered Double Hydroxide for Ultraefficient Oxygen Evolution
Authors: Hu Yidong , Luo Gan , Wang Liguang , Liu Xiaokang , Qu Yunteng , Zhou Yansong , Zhou Fangyao , Li Zhijun , Li Yafei , Yao Tao , Xiong Can , Yang Bo , Yu Zhenqiang , Wu Yuen 
Published: November 2020

AbstractIn view of the sluggish kinetics suppressing the oxygen evolution reaction (OER), developing efficient and robust OER catalysts is urgent and essential for developing efficient energy conversion technologies. Herein, hybrid amorphous/crystalline FeCoNi layered double hydroxide (LDH)‐supported single Ru atoms (Ru SAs/AC‐FeCoNi) are developed for enabling a highly efficient electrocatalytic OER. The amorphous outer layer in Ru SAs/AC‐FeCoNi is composed of abundant defect sites and unsaturated coordination sites, which can serve as anchoring sites to stabilize single Ru atoms. The crystalline inner has a highly symmetric rigid structure, thereby strengthening the stability of support for a long‐lasting OER. The synergistic effects endow this hybrid catalyst with extremely low overpotential (205 mV at 10 mA cm−2). Density functional theory calculation indicates that single Ru atoms stabilized by hybrid amorphous/crystalline FeCoNi LDH facilitate the formation of Ru–O* (rate‐determining step), thus accelerating the OER process.
A Photoregulated Racemase Mimic
Authors: Saha Monochura , Hossain Munshi Sahid , Bandyopadhyay Subhajit 
Published: November 2020

AbstractThe racemase enzymes convert L‐amino acids to their D‐isomer. The reaction proceeds through a stepwise deprotonation–reprotonation mechanism that is assisted by a pyridoxal phosphate (PLP) coenzyme. This work reports a PLP–photoswitch–imidazole triad where the racemization reaction can be controlled by light by tweaking the distance between the basic residue and the reaction centre.
Light‐Activated Electron Transfer and Catalytic Mechanism of Carnitine Oxidation by Rieske‐Type Oxygenase from Human Microbiota
Authors: Shanmugam Muralidharan , Quareshy Mussa , Cameron Alexander D. , Bugg Timothy D. H. , Chen Yin 
Published: November 2020

AbstractOxidation of quaternary ammonium substrate, carnitine by non‐heme iron containing Acinetobacter baumannii (Ab) oxygenase CntA/reductase CntB is implicated in the onset of human cardiovascular disease. Herein, we develop a blue‐light (365 nm) activation of NADH coupled to electron paramagnetic resonance (EPR) measurements to study electron transfer from the excited state of NADH to the oxidized, Rieske‐type, [2Fe‐2S]2+ cluster in the AbCntA oxygenase domain with and without the substrate, carnitine. Further electron transfer from one‐electron reduced, Rieske‐type [2Fe‐2S]1+ center in AbCntA‐WT to the mono‐nuclear, non‐heme iron center through the bridging glutamate E205 and subsequent catalysis occurs only in the presence of carnitine. The electron transfer process in the AbCntA‐E205A mutant is severely affected, which likely accounts for the significant loss of catalytic activity in the AbCntA‐E205A mutant. The NADH photo‐activation coupled with EPR is broadly applicable to trap reactive intermediates at low temperature and creates a new method to characterize elusive intermediates in multiple redox‐centre containing proteins.
Randomly Distributed Sulfur Atoms in the Main Chains of CO2‐Based Polycarbonates: Enhanced Optical Properties
Authors: Yue Tian‐Jun , Ren Bai‐Hao , Zhang Wen‐Jian , Lu Xiao‐Bing , Ren Wei‐Min , Darensbourg Donald J. 
Published: November 2020

AbstractPolymeric materials possessing both high refractive indices and high Abbe numbers are much in demand for the development of advanced optical devices. However, the synthesis of such functional materials is a challenge because of the trade‐off between these two properties. Herein, a synthetic strategy is presented for enhancing the optical properties of CO2‐based polycarbonates by modifying the polymer's topological structure. Terpolymers with thiocarbonate and carbonate units randomly distributed in the polymers’ main chain were synthesized via the terpolymerization of cyclohexene oxide with a mixture of CO2 and COS in the presence of metal catalysts, most notably a dinuclear aluminum complex. DFT calculations were employed to explain why different structural sequence were obtained with distinct bimetallic catalysts. Varying the CO2 pressure made it possible to obtain terpolymers with tunable carbonate linkages in the polymer chain. More importantly, optical property studies revealed that terpolymers with comparable thiocarbonate and carbonate units exhibited a refractive index of 1.501 with an enhanced Abbe number as high as 48.6, much higher than the corresponding polycarbonates or polythiocarbonates. Additionally, all terpolymers containing varying thiocarbonate content displayed good thermal properties with Tg>109 °C and Td>260 °C, suggesting little loss in the thermal stability compared to the polycarbonate. Hence, modification of the topological structure of the polycarbonate is an efficient method of obtaining polymeric materials with enhanced optical properties without compromising thermal performance.
Olefin‐Supported Cationic Copper Catalysts for Photochemical Synthesis of Structurally Complex Cyclobutanes
Authors: Gravatt Christopher S. , Melecio‐Zambrano Luis , Yoon Tehshik P. 
Published: November 2020

AbstractThe sole method available for the photocycloaddition of unconjugated aliphatic alkenes is the Cu‐catalyzed Salomon–Kochi reaction. The [Cu(OTf)]2⋅benzene catalyst that has been standard in this reaction for many decades, however, is air‐sensitive, prone to photodecomposition, and poorly reactive towards sterically bulky alkene substrates. Using bench‐stable precursors, an improved catalyst system with superior reactivity and photostability has been designed, and it offers significantly expanded substrate scope. The utility of this new catalyst for the preparation of sterically crowded cyclobutane structures is highlighted through the preparation of the cores of the natural products sulcatine G and perforatol.
Light‐Driven Enantioselective Synthesis of Pyrroline Derivatives by a Radical/Polar Cascade Reaction
Authors: Rodríguez Ricardo I. , Mollari Leonardo , Alemán José 
Published: November 2020

AbstractHerein, a light‐driven, atom‐economical process that provides access to enantiomerically enriched substituted chiral 1‐pyrroline derivatives is introduced. The strategy involves the distal functionalization of acyl heterocycles through a hydrogen‐atom transfer (HAT) process and the use of tailor‐made ketimines as reliable electrophilic partners. This transformation is translated into an enantiomerically controlled radical/polar cascade reaction in which water is produced as the sole by‐product and stereoselectivity is dictated by coordination to a chiral‐at‐rhodium catalyst.
Mild and Robust Stille Reactions in Water using Parts Per Million Levels of a Triphenylphosphine‐Based Palladacycle
Authors: Takale Balaram S. , Thakore Ruchita R. , Casotti Gianluca , Li Xaiohan , Gallou Fabrice , Lipshutz Bruce H. 
Published: November 2020

AbstractAn inexpensive and new triphenylphosphine‐based palladacycle has been developed as a pre‐catalyst, leading to highly effective Stille cross‐coupling reactions in water under mild reaction conditions. Only 500–1000 ppm of Pd suffices for couplings involving a variety of aryl/heteroaryl halides with aryl/hetaryl stannanes. Several drug intermediates can be prepared using this catalyst in aqueous nanoreactors formed by 2 wt % Brij‐30 in water.
One‐Step Room‐Temperature Synthesis of Metal(IV) Carboxylate Metal—Organic Frameworks
Authors: Dai Shan , Nouar Farid , Zhang Sanjun , Tissot Antoine , Serre Christian 
Published: November 2020

AbstractRoom‐temperature syntheses of metal–organic frameworks (MOFs) are of interest to meet the demand of the sustainable chemistry and are a pre‐requisite for the incorporation of functional compounds in water‐stable MOFs. However, only few routes under ambient conditions have been reported to produce metal(IV)‐based MOFs. Reported here is a new versatile one‐step synthesis of a series of highly porous M6‐oxocluster‐based MOFs (M=Zr, Hf, Ce) at room temperature, including 8‐ or 12‐connected micro/mesoporous solids with different functionalized organic ligands. The compounds show varying degrees of defects, particularly for 12‐connected phases, while maintaining the chemical stability of the parent MOFs. Proposed here are first insights into in situ kinetics observations for efficient MOF preparation. Remarkably, the synthesis has a high space‐time yield and also provides the possibility to tune the particle size, therefore paving the way for their practical use.
A novel cationic waterborne polyurethane coating modified by chitosan biguanide hydrochloride with application potential in medical catheters
Authors: Liu Yuxing , Zou Yalu , Wang Jing , Wang Shuo , Liu Xiaofei 
Published: November 2020

AbstractThis study reported the synthesis and properties of a new cationic waterborne polyurethane coating. In this work, a chitosan derivative, chitosan biguanide hydrochloride (CSGH), was synthesized, which was used as a blocking agent and cross‐linking agent to participate in the copolymerization of waterborne polyurethane (WPU) and a bioactive ingredient to enhance the biocompatibility of the coating. FTIR results demonstrated the reaction of CSGH with WPU. Moreover, the particle size distribution of the emulsion and SEM results showed that CSGH and WPU were well integrated. Benefiting from the formation of the cross‐linking network, the thermodynamic properties of the coating were significantly improved. Furthermore, due to adding 3 wt% CSGH, the water contact angle of the coating surface decreased from 97.01° to 69.30°, indicating that the coating surface changed from hydrophobic to hydrophilic. And a specific resistance toStaphylococcus aureusandEscherichia coliwas exhibited without cytotoxicity, the resistance rates could reach 85% and 91% respectively. It is highlighted that this WPU‐CSGH coating has great application potential in the field of medical interventional catheters.
Protective Effects of Moderate Intensity Static Magnetic Fields on Diabetic Mice
Authors: Li Qin , Fang Yanwen , Wu Ningzi , Gu Lili , Li Hongxing , Liao Zhongcai , Liu Mengyu , Fang Zhicai , Zhang Xinyue 
Published: November 2020

The purpose of this study was to investigate the effects of moderate‐intensity static magnetic field (SMF) on diabetic mice. We studied the effects of SMF on blood glucose of normal mice by starch tolerance and glucose tolerance tests. Then, we evaluated the effects of SMF on blood glucose of diabetic mice by establishing alloxan‐induced type 1 diabetic mice and high‐fat diet + streptozotocin (STZ)‐induced type 2 diabetic mice. The results showed that different magnetic field intensities and blank control did not affect the blood glucose of normal mice. After starch and glucose administration, different magnetic fields could improve the glucose tolerance of normal mice, and this was obvious in the 600 mT group. In the experiment of type 1 diabetic mice induced by alloxan, the results showed that different magnetic field intensities could improve the starch tolerance of mice, and that in the 400 mT group was obvious. In the experiment of type 2 diabetic mice induced by a high‐fat diet + STZ, the 400 mT group could reduce food intake and water consumption in the later period. The 600 mT group could improve the starch tolerance of mice. The 400 and 600 mT groups could reduce fasting blood glucose. At the same time, total cholesterol and triglyceride decreased in different magnetic field intensities, and the 600 mT group could significantly increase the serum insulin content of mice. In summary, the results of this study suggest that SMF has a protective role in diabetic mice. Bioelectromagnetics. © 2020 Bioelectromagnetics Society
Investigation of plasmon‐induced extraction efficiency enhancement in a CdTe‐based LED using FDTD simulation
Authors: Wang HongYu , Shan Dan , Xu Ling 
Published: November 2020

AbstractLight‐emitting diodes (LED) based on silicon platforms and CdTe quantum dots (QDs) are an important area of research. Due to poor charge balance in QD layers, reduced graphene oxide (RGO) was introduced between the P–Si substrate and CdTe QDs. To further improve the performance of the QDs‐LED, Au nanorods (NRs) were incorporated into the hole transport layer. A finite‐difference time‐domain simulation was used to discuss theoretically the influence of RGO and Au NRs on the LED performance, and investigate the influence of substrate on the localized surface plasmon resonance (LSPR) coupling wavelength. Simulated results demonstrated that the LSPR peaks for Au NRs red shifted with increase in substrate refractive index, and the electric field along the x–y plane was mostly concentrated near the interface. RGO incorporation enhanced the emission of the QDs‐LED. This may be attributed to improvement in conductivity and hole mobility in the hole transport layer and reduction in the energy barrier for injection of holes. After introduction of Au NRs, there was a significant enhancement in emission, and light extraction efficiency was enhanced about 10‐fold.
Tocilizumab‐induced cytomegalovirus colitis in a patient with COVID‐19
Authors: Khatib Mohamad Y. , Shaik Karimulla S. , Ahmed Amna A. , Alwraidat Mohammad A. , Mohamed Ahmed S. , Abou Kamar Mohamad R. , Sharaf Eldean Mouhammad Z. , Aldaraiseh Bashar K. , Nashwan Abdulqadir J. 
Published: November 2020

AbstractThe authors urge clinicians to observe for early signs of CMV reactivation in patients presenting with gastrointestinal bleeding and intestinal perforation after receiving tocilizumab or other immunosuppressive therapy as a treatment for COVID 19. Early recognition of CMV infection and treatment will prevent life‐threatening bleeding and mortality.
Maternal death of a hemophilic patient due to the inhaling of a mixture of industrial bleach and detergents—A case study
Authors: Abedi Parvin , Mohaghegh Zaynab , Faramazi Nahid , Aghamiri Zahra Biygom Seyyed 
Published: November 2020

AbstractUse of detergents and cleaning products puts women at risk due to hazardous chemical substances. Education of all women, especially pregnant and high‐risk women about the proper use of detergents, is a necessity.
Role of mineralocorticoid receptor antagonists in kidney diseases
Authors: Patel Vishal , Joharapurkar Amit , Jain Mukul 
Published: November 2020

AbstractMineralocorticoid receptor (MR) antagonists, for example, spironolactone and eplerenone, are in clinical use to treat hypertension. Increasing evidence suggests that mineralocorticoid receptor activation causes the pathogenesis and progression of chronic kidney disease. Aldosterone‐induced MR activation increases inflammation, fibrosis, and oxidative stress in the kidney. MR antagonists (MRAs) have demonstrated therapeutic actions in chronic kidney disease (CKD), diabetic nephropathy (DN), renal fibrosis, and drug‐induced renal injury in preclinical and clinical studies. We have summarized and discussed these studies in this review. The nonsteroidal MRA, esaxerenone, recently received approval for the treatment of hypertension. It has also shown a positive therapeutic effect in phase 3 clinical trials in patients with DN. Other nonsteroidal MRA such as apararenone, finerenone, AZD9977, and LY2623091 are in different clinical trials in patients with hypertension suffering from renal or hepatic fibrotic diseases. Hyperkalemia associated with MRA therapy has frequently led to the discontinuation of the treatment. The new generation nonsteroidal MRAs like esaxerenone are less likely to cause hyperkalemia at therapeutic doses. It appears that the nonsteroidal MRAs can provide optimum therapeutic benefit for patients suffering from kidney diseases.
Impact of heart failure on the clinical course and outcomes of patients hospitalized for COVID‐19. Results of the Cardio‐COVID‐Italy multicentre study
Authors: Tomasoni Daniela , Inciardi Riccardo M. , Lombardi Carlo M. , Tedino Chiara , Agostoni Piergiuseppe , Ameri Pietro , Barbieri Lucia , Bellasi Antonio , Camporotondo Rita , Canale Claudia , Carubelli Valentina , Carugo Stefano , Catagnano Francesco , Dalla Vecchia Laura A. , Danzi Gian Battista , Di Pasquale Mattia , Gaudenzi Margherita , Giovinazzo Stefano , Gnecchi Massimiliano , Iorio Annamaria , La Rovere Maria Teresa , Leonardi Sergio , Maccagni Gloria , Mapelli Massimo , Margonato Davide , Merlo Marco , Monzo Luca , Mortara Andrea , Nuzzi Vincenzo , Piepoli Massimo , Porto Italo , Pozzi Andrea , Sarullo Filippo , Sinagra Gianfranco , Volterrani Maurizio , Zaccone Gregorio , Guazzi Marco , Senni Michele , Metra Marco 
Published: November 2020

AbstractAimsTo assess the prognostic value of a history of heart failure (HF) in patients with coronavirus disease 2019 (COVID‐19).Methods and resultsWe enrolled 692 consecutive patients admitted for COVID‐19 in 13 Italian cardiology centres between 1 March and 9 April 2020. Mean age was 67.4 ± 13.2 years, 69.5% of patients were males, 90 (13.0%) had a history of HF, median hospitalization length was 14 days (interquartile range 9–24). In‐hospital death occurred in 37 of 90 patients (41.1%) with HF history vs. 126 of those with no HF history (20.9%). The increased risk of death associated with HF history remained significant after adjustment for clinical variables related to COVID‐19 and HF severity, including comorbidities, oxygen saturation, lymphocyte count and plasma troponin [adjusted hazard ratio (HR) for death: 2.25; 95% confidence interval (CI) 1.26–4.02; P = 0.006 at multivariable Cox regression model including 404 patients]. Patients with a history of HF also had more in‐hospital complications includingacute HF (33.3% vs. 5.1%, P < 0.001), acute renal failure (28.1% vs. 12.9%, P < 0.001), multiorgan failure (15.9% vs. 5.8%, P = 0.004) and sepsis (18.4% vs. 8.9%, P = 0.006). Other independent predictors of outcome were age, sex, oxygen saturation and oxygen partial pressure at arterial gas analysis/fraction of inspired oxygen ratio (PaO2/FiO2). In‐hospital treatment with corticosteroids and heparin had beneficial effects (adjusted HR for death: 0.46; 95% CI 0.29–0.74; P = 0.001; n = 404 for corticosteroids, and adjusted HR 0.41; 95% CI 0.25–0.67; P < 0.001; n = 364 for heparin).ConclusionsHospitalized patients with COVID‐19 and a history of HF have an extremely poor outcome with higher mortality and in‐hospital complications. HF history is an independent predictor of increased in‐hospital mortality.
Autonomous dishwasher loading from cluttered trays using pre‐trained deep neural networks
Authors: Voysey Isobel , George Thuruthel Thomas , Iida Fumiya 
Published: November 2020

AbstractAutonomous dishwasher loading is a benchmark problem in robotics that highlights the challenges of robotic perception, planning, and manipulation in an unstructured environment. Current approaches resort to a specialized solution, however, these technologies are not viable in a domestic setting. Learning‐based solutions seem promising for a general purpose solutions; however, they require large amounts of catered data to be applied in real‐world scenarios. This article presents a novel learning‐based solution without a training phase using pre‐trained object detection networks. By developing a perception, planning, and manipulation framework around an off‐the‐shelf object detection network, we are able to develop robust pick‐and‐place solutions that are easy to develop and general purpose requiring only a RGB feedback and a pinch gripper. Analysis of a real‐world canteen tray data is first performed and used for developing our in‐lab experimental setup. Our results obtained from real‐world scenarios indicate that such approaches are highly desirable for plug‐and‐play domestic applications with limited calibration. All the associated data and code of this work are shared in a public repository.
On the border between land and water: The environmental conditions of the Neolithic occupation from 4.3 until 1.6 ka BC at Serteya, Western Russia
Authors: Kittel Piotr , Mazurkevich Andrey , Wieckowska‐Lüth Magda , Pawłowski Dominik , Dolbunova Ekaterina , Płóciennik Mateusz , Gauthier Emilie , Krąpiec Marek , Maigrot Yolaine , Danger Maxime , Mroczkowska Agnieszka , Okupny Daniel , Szmańda Jacek , Thiebaut Eva , Słowiński Michał 
Published: November 2020

AbstractThe paper presents the results of a palaeoecological study of Neolithic archaeological layers from a wetland, multilayer site, Serteya II (Western Russia). It contains, domestic structures, rich organic artefacts, skeletons, and ecofacts preserved within lacustrine deposits that are extremely important on a European scale. We employed a set of specialised palaeoecological analyses and accelerator mass spectrometry radiocarbon dating to identify the principal environmental conditions which attracted Neolithic hunter‐fisher‐gatherer communities from 4300 to 1600 cal. BC. The distinct impact of communities using a nonproductive economy on the ecology of the palaeolake shore zone was recorded. Also, palaeolake water level changes influenced the palaeoeconomic activity of local Neolithic societies, such as gathering of plants (for the medicinal use or serving as dietary components), fishing activities, and possible funeral practices. In addition, the identified phases of high‐water level changes, which were responses to climatic oscillations, were correlated with supraregional climatic events, especially ca. 6.2, 5.9, and 4.2 ka cal. BP. Thus, our results allowed for the reconstruction of environment transformations and conditions of Neolithic communities' activity, as well as for a better understanding of the relationships between local Neolithic communities' way of life and neolithisation processes in Eastern Europe.