bluuebunny/crossref_metadata_2025_split huggingface dataset:
Palladium‐Catalyzed Heck/Insertion/Decarboxylation Domino Sequence: Synthesis of Dihydrocyclohepta[de]naphthalenes
Authors: He Cai , Chen Xiang‐Long , Zhuang Shi‐Yi , Wu Yan‐Dong , Tang Bo‐Cheng , Wu An‐Xin 
Published: May 2021

AbstractA Pd‐catalyzed cascade cyclization for the construction of fused dihydrocyclohepta[de]naphthalene skeletons was developed. The skeleton was assembled from 3‐iodo‐4H‐chromen‐4‐one, norbornene and 8‐bromo‐1‐naphthoic acid. Unlike the classic Catellani reaction, which involves the removal of norbornene, in the present system, norbornene acts as a building block for the construction of rigid nonplanar molecular architectures rather than as an ortho‐directing transient mediator. This synthesis involves the formation of three C−C bonds via a one‐pot process, and it is compatible of a series of substituents.magnified image
Impact of Crystalline and Amorphous Matrices on Successful Spray Drying of siRNA Polyplexes for Inhalation of Nano‐in‐Microparticles
Authors: Keil Tobias W. M. , Zimmermann Christoph , Baldassi Domizia , Adams Friederike , Friess Wolfgang , Mehta Aditi , Merkel Olivia M. 
Published: May 2021

AbstractTo develop stable and inhalable dry powder formulations with long shelf life, polyplexes consisting of siRNA and a polyethylenimine (PEI)‐based block copolymer in presence of mannitol or trehalose are spray dried. The effect of inlet (T‐In) and outlet (T‐Out) temperature on the recovery of siRNA and adsorption effects within the tubing material are investigated. Choosing a low abrasion silicon tubing prevented siRNA loss due to adsorption. Mannitol and trehalose formulations preserved siRNA integrity regardless of excipient concentration and temperature at T‐Out below the siRNA melting temperature. Trehalose formulations allowed full siRNA recovery whereas mannitol formulations resulted in spray drying induced losses of ≈20% siRNA and of 50–60% polymer. Mannitol formulations showed optimal aerodynamic characteristics as confirmed by next generation impaction analysis based upon siRNA content. All spray dried formulations resulted in green fluorescent protein (GFP) silencing comparable or better than freshly prepared polyplexes. To test if the observed results could be transferred, formulations of siRNA and transferrin‐PEI conjugates are spray dried, characterized, and used to transfect primary human T cells ex vivo. Results confirmed successful silencing of the transcription factor GATA3 in primary CD4+ T cells with spray dried formulations as a potential treatment for severe asthma.
Tuning Pressure Drop in Isoporous Membranes: Design with Fabrication Variability
Authors: Ong Shi Ke , Birgersson Erik , Low Hong Yee 
Published: May 2021

AbstractIsoporous membranes consist of well‐defined micro and nanoscale pore architecture comprising uniform pore sizes with straight pore channels. In contrast to traditional random porous membranes with tortuous flow paths, isoporous membranes offer the opportunity to achieve a high degree of membrane customization and low pressure drop. Here, a physics‐based machine learning methodology that enables the predictive design of a single‐layer isoporous membrane in terms of the pressure drop is reported. In short, the methodology consists of a hybrid approach that includes experimental data on the variability of the pore architecture and the resulting pressure drop, training of a neural network with data from validated physics‐based simulations of laminar flow through the membrane, and Monte Carlo simulation (MCS) to stochastically account for the inherent variabilities of the pore architecture of fabricated isoporous membranes. Overall, the neural network and MCS predict the range of Δp for a given single‐layer membrane well. Experimental values fall within 90% of the minimum and maximum predicted Δp values. In addition, a sensitivity analysis with MCS is carried out to quantify how design and operating parameters affect the overall pressure drop. The methodology can be extended to membranes comprising multiple layers and to account for filtration efficiency.
Unparalleled Armour for Aramid Fiber with Excellent UV Resistance in Extreme Environment
Authors: Chen Fengxiang , Zhai Lisha , Yang Huiyu , Zhao Shichao , Wang Zonglei , Gao Chong , Zhou Jingyi , Liu Xin , Yu Zhenwei , Qin Yong , Xu Weilin 
Published: May 2021

AbstractAramid fibers are widely used in many cutting‐edge fields, including space, aviation, military, and electronics. However, their poor UV resistance and surface inertness seriously hinder their utilization, especially in harsh environments. Here, a dual‐layer ultrathin Al2O3–TiO2 coating with a thickness of 70–180 nm is fabricated on aramid fibers by a modified atomic layer deposition (ALD) method. The tenacity of ALD‐coated aramid fibers decreases only by ≈0.85% after exposure to intense UV light (4260 W m−2) under high temperature (>200 ℃) for 90 min, which equals to continuous exposure to sunlight for about 17 500 days. The as‐prepared aramid fibers also show excellent laundering durability, thermal and chemical stabilities. This work presents a green and damage‐free approach to achieve the highly anti‐UV aramid fibers without sacrificing their outstanding performance, which is expected to guide material design for future innovations in functional fibers and devices.
Dual‐Metal Sites Boosting Polarization of Nitrogen Molecules for Efficient Nitrogen Photofixation
Authors: Zhang Yida , Hou Tingting , Xu Quan , Wang Qingyu , Bai Yu , Yang Shaokang , Rao Dewei , Wu Lihui , Pan Haibin , Chen Jiafu , Wang Gongming , Zhu Junfa , Yao Tao , Zheng Xusheng 
Published: May 2021

AbstractConstructing nitrogen (N2) adsorption and activation sites on semiconductors is the key to achieving efficient N2 photofixation. Herein, Mn–W dual‐metal sites on WO3 are designed toward efficient N2 photoreduction via controlled Mn doping. Impressively, the optimal 2.3% Mn‐doped WO3 (Mn‐WO3) exhibits a remarkable ammonia (NH3) production rate of 425 µmol gcat.−1 h−1, representing the best catalytic performance among the ever‐reported tungsten oxide‐based photocatalysts for N2 fixation. Quasi in situ synchrotron radiation X‐ray spectroscopy directly identifies that the Mn–W dual‐metal sites can enhance the polarization of the adsorbed N2, which is beneficial to the N2 activation. Further theoretical calculations reveal that the increased polarization is originated from the electron back‐donation into the antibonding orbitals of the adsorbed N2, hence lowering the reaction energy barrier toward the N2 photofixation. The concept of dual sites construction for inert molecule activation offers a powerful platform toward rational design of highly efficient catalysts for nitrogen fixation and beyond.
Quantifying the Plasmonic Generation Rate of Non‐Thermal Hot Carriers with an AlGaN/GaN High‐Electron‐Mobility Transistor
Authors: Li Chun‐Yu , Liu Chi‐Ching , Lai Wei‐Chih , Lan Yung‐Chiang , Chang Yun‐Chorng 
Published: May 2021

AbstractPlasmonic generation of hot carriers in metallic nanostructures has attracted much attention due to its great potential in several applications. However, it is highly debated whether the enhancement is due to the hot carriers or the thermal effect. Here, the ability to exclude the thermal effect and detect the generation of non‐thermal hot carriers by surface plasmon is demonstrated using an AlGaN/GaN high‐electron‐mobility transistor. This ultrasensitive platform, which demonstrates at least two orders of magnitude more sensitivity compared to the previous reports, can detect the hot carriers generated from discrete nanostructures illuminated by a continuous wave light. The quantitative measurements of hot carrier generation also open a new way to optimize the plasmonic nanoantenna design in many applications.
Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives
Authors: Shi Zixiong , Li Matthew , Sun Jingyu , Chen Zhongwei 
Published: May 2021

AbstractLithium–sulfur (Li–S) batteries have stimulated a burgeoning scientific and industrial interest owing to high energy density and low materials costs. The favorable reaction kinetics of sulfur species is a key prerequisite for pursuing their commercialization. Recent years have witnessed a wealth of investigations in terms of boosting sulfur redox via rationalizing redox mediators. Defect engineering, which allows for the effective exposure of active sites and optimization of electronic structure, has emerged expeditiously as an essential strategy to enhance polysulfide modulation, and hence expedite Li–S chemistry. Nevertheless, a comprehensive overview of defect engineering in Li–S realm is still lacking. This review emphasizes the recent advances in the rational design and polysulfide modulation strategies of different types of defective mediators. Their unique morphological configuration, superb electrochemical activity, and underlying catalytic mechanism are comprehensively summarized, aiming to deepen the understanding of defect‐mediated Li–S chemistry. Moreover, in situ evolution of defective mediators is discussed to identify the true active sites under aprotic reaction conditions. Opportunities and an outlook of this fast‐developing frontier that may lead to practical implementations of Li–S batteries are proposed.
Revealing the Impact of Hierarchical Pore Organization in Supercapacitor Electrodes by Coupling Ionic Dynamics at Micro‐ and Macroscales
Authors: Dvoyashkin Muslim , Leistenschneider Desirée , Evans Jack D. , Sander Miriam , Borchardt Lars 
Published: May 2021

AbstractThe rate of charging of supercapacitors depends on how quickly ions can reach and accommodate the surface of electrodes. Diffusivity, a parameter reflecting the speed of ions’ migration, is believed to be crucial in designing supercapacitor electrodes. Herein, this belief is questioned, shedding light on a puzzling and potentially critical feature of ionic dynamics denoted as confinement‐induced ion–solvent separation. This effect can lead to a strong slowdown of the ion mobility inside hierarchical pore networks. Explanations for when such an effect occurs and how it can be circumvented are provided. Furthermore, this microscopic picture of diffusion seen by NMR is bridged with the macroscopic charging behavior of supercapacitors investigated by impedance spectroscopy. Quantifying the average residence time of ions within carbon particles shows that the nanopore environment may not be the rate‐limiting factor for the overall ion mobility and thus performance of a cell—as commonly expected. Combining direct diffusion studies performed with neat and solvated ionic liquids and those on organic electrolytes, the so far lacking criteria for the rational selection of electrolyte–carbon systems is developed and recommendations for the preparation of transport‐optimized materials for supercapacitors to minimize ionic diffusion limitations are given.
Galvanic Couples in Ionic Liquid‐Based Electrolyte Systems for Lithium Metal Batteries—An Overlooked Cause of Galvanic Corrosion?
Authors: Dohmann Jan Frederik , Horsthemke Fabian , Küpers Verena , Bloch Sophia , Preibisch Yves , Kolesnikov Aleksei , Kolek Martin , Stan Marian Cristian , Winter Martin , Bieker Peter 
Published: May 2021

AbstractThe breakthroughs in rechargeable lithium metal‐anode‐based batteries is still challenged by safety and performance limitations. Ionic liquid (IL)‐based electrolytes are in consideration for increased safety but their moderate electrolyte performance and high costs still suppress their usefulness in Li metal‐batteries. In an effort to deepen the understanding of the limited performance, galvanic corrosion as an electrochemical degradation process is herein identified as a contributing factor toward battery cell deterioration. Four different ILs, based on bis(trifluoromethylsulfonyl)imide in combination with the quaternary ammonium cations N‐butyl‐N‐methylpyrrolidinium, N‐methyl‐N‐propyl‐pyrrolidinium, N‐butyl‐N‐methylpiperidinium, and N‐butyltrimethylammonium, respectively, are systematically investigated for such corrosive side reactions. The reaction pathways of this commonly neglected phenomenon are found to be both Hofmann‐type and reductive eliminations. Supported by headspace‐gas chromatography‐mass spectrometry, the evolving gaseous reaction products are characterized. With zero resistance ammetry and Li electrochemical dissolution and deposition experiments, the dependency of galvanic corrosion on the presence of the galvanically coupled materials is elucidated. Variation of the lithium bis(trifluoromethylsulfonyl)imide concentration in the electrolytes is shown to influence the extent of detectable degradation products. Based on these findings, the necessity for more sophisticated electrode designs and electrolyte formulations is emphasized.
Website usability analysis of United States emergency medicine residencies
Authors: Fundingsland Edwin , Fike Joseph , Calvano Joshua , Raja Ali , Lai Deborah , Silacci Sara , Haas Mary , Chan Teresa , He Shuhan 
Published: May 2021

AbstractObjectivesThe Council of Residency Directors (CORD) in Emergency Medicine (EM) has recommended that all residency programs should conduct virtual interviews for the 2020 to 2021 application cycle due to the COVID‐19 pandemic. While factors such as geographical region, city, program size, or hospital affiliation are not modifiable, EM residencies can bridge the information gap created by a lack of face‐to‐face interaction by representing themselves digitally. Measuring usability provides an objective method for EM residencies to improve their Web presence and effectively represent themselves to applicants.MethodsOur sample set included 55 U.S. EM residency program websites. Using methodology replicated from previous literature on health care website usability, we divided usability into four categories for quantifiable analysis: accessibility, marketing, content quality, and technology. Analysis was performed on each website and scored in all four categories. A “general usability” score was calculated for each website using a composite of the key factors within the four categories. Using a weighted percentage across all of the factors, an overall score was calculated.ResultsContent quality was the overall highest scoring category (mean ± SD = 5.4, SE = 0.33). The overall lowest performing category was technology (mean ± SD = 0.8 ± 0.09, SE = 0.01).ConclusionsMeasuring usability can help EM residency programs identify ways to improve their Web presence. To effectively promote their programs, residencies need quality content that communicates their key features. Our recommendation is for all residency programs to periodically perform website audits and apply the usability measures outlined to improve their digital presence, especially during times when face‐to‐face interactions will be limited.
Sensitivity of reference evapotranspiration to weather variables across seven regions of Turkey
Authors: Yildirim Tugba , Wagle Pradeep , Gowda Prasanna H. , Mengu Gulay P. 
Published: May 2021

AbstractDaily weather data from 1984 to 2018 for 14 weather stations representing seven regions of Turkey were used to estimate reference evapotranspiration (ETref). We performed sensitivity analyses of input weather variables (air temperature, wind speed, and solar radiation) to determine the relative effects of measurement errors in weather data on the accuracy of calculated grass (ETos) and alfalfa (Medicago sativa L., ETrs) reference ET. In addition, changes in estimated irrigation water requirement for maize (Zea mays L.), a major crop in all regions of Turkey, due to errors in major climatic variables were also determined across seven regions of Turkey. Comparison of the sensitivity coefficients indicated that ETref was most sensitive to wind speed (sensitivities from −2.46 to 5.56 mm d–1), followed by air temperature (sensitivities from −2.13 to 3.1 mm d–1) across Turkey. However, responses of ETos and ETrs to changes in weather variables varied across the regions. For examples, the Marmara region had the largest impact of errors in air temperature but the smallest impact of errors in wind speed on the calculated ETref. Likewise, the Southeastern and Eastern Anatolia regions had the greatest impact of errors in wind speed but the smallest impact of errors in air temperature on the calculated ETref. The errors in weather variables led to substantial over‐ or underestimation of irrigation water requirement for maize. In some cases, irrigation water requirement was overestimated by more than double. These results suggest that different sensor accuracies are needed for weather stations in different regions of Turkey to accurately estimate ETref and irrigation water requirement.
Chemical immobilization of amino acids into robust metal–organic framework for efficient SO2 removal
Authors: Zhu Zhenliang , Zhang Peixin , Li Bei , Chen Shixia , Deng Qiang , Zeng Zheling , Wang Jun , Deng Shuguang 
Published: May 2021

AbstractAdsorptive removal of trace SO2 emissions from flue‐gases can significantly reduce energy and water consumption and minimize the amount of unmanageable waste, however, this remains a great challenge. Herein, we report a universal strategy of chemical immobilization of amino acids into a robust metal–organic framework to enhance deep desulfurization. The grafted amino acid resulted in the formation of pores with compatible pore sizes and created abundant N‐containing moieties for selective SO2 adsorption. MOF‐808‐His (His = l‐histidine) exhibited a top‐ranking SO2 uptake (10.4 mmol g−1) with an excellent SO2/CO2 selectivity (90.5) under ambient conditions; furthermore, MOF‐808‐His could be easily regenerated. Breakthrough curves verified its excellent separation performances with water vapor and real flue‐gas compositions. Computational simulations confirmed the vital role of immobilized amino acids in improving the SO2 capture ability and selectivity. As a proof‐of‐concept, five natural amino acids were immobilized into MOF‐808; all samples displayed improved adsorptive desulfurization performances.
Mathematical approach to compute the molecular composition of hydrothermal liquefaction‐derived renewable crude oil
Authors: Saxena Nikhlesh , Prabhu Vishwas , Chandra Himanshu , Ghadge Rajaram , Bhujade Ramesh , Sapre Ajit 
Published: May 2021

AbstractHydrothermal liquefaction (HTL), a thermo‐chemical conversion process, uses water as a reaction medium at elevated pressure and temperature, to convert biomass to renewable liquid fuel and recovers fertilizer‐rich water. To assess the techno‐economic screening of HTL oils from various feedstock, it is crucial to have information on molecular composition of the feed and products. There are limitations of existing analytical methods to identify and quantify all the molecules present in the bio‐fuel. Therefore, there is a need to find alternate ways to quantify the molecular composition of feed and expected products. The modeling work on bio‐oil is developed and validated on mathematical approach using simple analytical results like CHNO along with structural analysis of oil like Fourier‐transform infrared, nuclear magnetic resonance analysis for HTL derived oil from microalgae. This mathematical framework is further extended to predict the molecular composition of oil obtained from HTL of feedstocks like mixed plastic waste, sludge, and so on. A multi‐dimensional molecular matrix is developed based on the distributions of side chains, aromatic rings, and olefinic carbon on top of core molecules. The parameters of the distributions are estimated computationally using global optimization algorithm (genetic algorithm) and local optimization algorithm to predict a mixture composition that matches closely with bulk properties of the product.
The Roles of Settings in Supporting Immigrants’ Resistance to Injustice and Oppression: A Policy Position Statement by the Society for Community Research and Action
Authors: Buckingham Sara L. , Langhout Regina Day , Rusch Dana , Mehta Tara , Rubén Chávez Noé , Ferreira van Leer Kevin , Oberoi Ashmeet , Indart Monica , Paloma Virginia , King V. Elizabeth , Olson Bradley 
Published: May 2021

AbstractIn 2018, in response to increasingly oppressive and widespread federal immigration enforcement actions in the United States (U.S.) and around the globe – including family separation, immigration raids, detention, deportation of people who have lived in the country for much of their lives – the Society for Community Research & Action produced a statement on the effects of deportation and forced separation on immigrants, their families, and communities (SCRA, 2018). The statement focused exclusively on the impacts of deportation and forced family separation, documenting the damage done by oppressive U.S. policies and practices. We felt it was imperative to document this harm, and yet were uncomfortable producing a narrow paper that focused solely on harm. There are multiple ways immigrants and their allies resist deportation and other forms of oppression. This resistance is done individually, collectively, and in settings that vary in size and scope, including community‐based, faith‐based, direct care, and educational settings, as well as entire municipalities and transnational organizing settings. Settings facilitate resistance in many ways, focusing on those who are oppressed, their oppressors, and systems of oppression. In this statement, we describe the unique and overlapping ways in which settings facilitate resistance. We situate this review of the scientific and practice literature in the frameworks of change through social settings, empowering settings, healing justice, and decolonization. We also document recommendations for continued resistance.
A new syndrome of moyamoya disease, kidney dysplasia, aminotransferase elevation, and skin disease associated with de novo variants in RNF213
Authors: Strong Alanna , O'Grady Gina , Shih Evelyn , Bishop Jonathan R. , Loomes Kathleen , Diamond Tamir , Hartung Erum A. , Wong William , Cuddapah Sanmati , Cahill Anne Marie , Hou Cuiping , Slater Diana , Vaccaro Courtney , Watson Deborah , Li Dong , Hakonarson Hakon 
Published: May 2021

AbstractRing‐finger protein 213 (RNF213) encodes a protein of unknown function believed to play a role in cellular metabolism and angiogenesis. Gene variants are associated with susceptibility to moyamoya disease. Here, we describe two children with moyamoya disease who also demonstrated kidney disease, elevated aminotransferases, and recurrent skin lesions found by exome sequencing to have de novo missense variants in RNF213. These cases highlight the ability of RNF213 to cause Mendelian moyamoya disease in addition to acting as a genetic susceptibility locus. The cases also suggest a new, multi‐organ RNF213‐spectrum disease characterized by liver, skin, and kidney pathology in addition to severe moyamoya disease caused by heterozygous, de novo C‐terminal RNF213 missense variants.