bluuebunny/crossref_metadata_2025_split huggingface dataset:
High‐Performance Solid Polymer Electrolytes Filled with Vertically Aligned 2D Materials
Authors: Tang Wenjing , Tang Shan , Guan Xuze , Zhang Xinyue , Xiang Qian , Luo Jiayan 
Published: February 2019

AbstractSolid state lithium metal batteries are the most promising next‐generation power sources owing to their high energy density and safety. Solid polymer electrolytes (SPE) have gained wide attention due to the excellent flexibility, manufacturability, lightweight, and low‐cost processing. However, fatal drawbacks of the SPE such as the insufficient ionic conductivity and Li+ transference number at room temperature restrict their practical application. Here vertically aligned 2D sheets are demonstrated as an advanced filler for SPE with enhanced ionic conductivity, Li+ transference number, mechanical modulus, and electrochemical stability, using vermiculite nanosheets as an example. The vertically aligned vermiculite sheets (VAVS), prepared by the temperature gradient freezing, provide aligned, continuous, run‐through polymer‐filler interfaces after infiltrating with polyethylene oxide (PEO)‐based SPE. As a result, ionic conductivity as high as 1.89 × 10−4 S cm−1 at 25 °C is achieved with Li+ transference number close to 0.5. Along with their enhanced mechanical strength, Li|Li symmetric cells using VAVS–CSPE are stable over 1300 h with a low overpotential. LiFePO4 in all‐solid‐state lithium metal batteries with VAVS–CSPE could deliver a specific capacity of 167 mAh g−1 at 0.1 C at 35 °C and 82% capacity retention after 200 cycles at 0.5 C.
Recent Advances in n‐Type Polymers for All‐Polymer Solar Cells
Authors: Genene Zewdneh , Mammo Wendimagegn , Wang Ergang , Andersson Mats R. 
Published: February 2019

AbstractAll‐polymer solar cells (all‐PSCs) based on n‐ and p‐type polymers have emerged as promising alternatives to fullerene‐based solar cells due to their unique advantages such as good chemical and electronic adjustability, and better thermal and photochemical stabilities. Rapid advances have been made in the development of n‐type polymers consisting of various electron acceptor units for all‐PSCs. So far, more than 200 n‐type polymer acceptors have been reported. In the last seven years, the power conversion efficiency (PCE) of all‐PSCs rapidly increased and has now surpassed 10%, meaning they are approaching the performance of state‐of‐the‐art solar cells using fullerene derivatives as acceptors. This review discusses the design criteria, synthesis, and structure–property relationships of n‐type polymers that have been used in all‐PSCs. Additionally, it highlights the recent progress toward photovoltaic performance enhancement of binary, ternary, and tandem all‐PSCs. Finally, the challenges and prospects for further development of all‐PSCs are briefly considered.
Exciton‐ and Polaron‐Induced Reversible Dipole Reorientation in Amorphous Organic Semiconductor Films
Authors: Deng Chao , Zhang Liwei , Wang Dan , Tsuboi Taiju , Zhang Qisheng 
Published: February 2019

AbstractThe quantum efficiency of organic light‐emitting diodes (OLEDs) employing thermally activated delayed fluorescence (TADF) highly depends on the S1−T1 energy gaps (ΔEST) of the emitters. However, the ΔEST values determined in solution or even in organic thin films through a static approach continuously fail in predicting device performance. Herein, by systematically investigating the time‐resolved emission spectra of several TADF emitters in various matrixes and the dielectric spectra of the matrixes, it is demonstrated that molecular organic semiconductors can undergo reversible and irreversible spatial rearrangements within a few dozen nanoseconds in an electric field created by a polarized charge‐transfer state and can in turn lower the excited‐state energy. In contrast to solution solvation, the polarized microenvironment in films can last for tens of microseconds or more after removing the electric field, leading to a narrowing and a broader distribution of ΔEST. In TADF OLEDs, the large dipole moment of emitter‐based polarons is key for reducing the ΔEST of subsequently generated excitons by inducing the dipole orientation of the surrounding molecules. Understanding the so‐called solid‐state solvation with a dynamic approach can provide deeper insight into the working mechanism in organic semiconductor devices.
Alkylation of Terminal Alkynes under Zinc Lewis Acid Catalysis and Its Mechanistic Studies
Authors: Osano Mana , Kida Takeru , Yonekura Kyohei , Tsuchimoto Teruhisa 
Published: February 2019

AbstractWith a zinc Lewis acid catalyst and proton sponge in toluene, terminal alkynes were found to undergo the alkylation by alkyl triflates to provide unsymmetrical internal alkynes. This is the first example that a simple alkyl chain other than benzylic and norbornyl units can be introduced onto the alkynyl carbon atom under Lewis acid catalysis. Mechanistic studies revealed that the activation of the alkyne by the zinc Lewis acid and proton sponge is the trigger of the reaction to give a monoalkynylzinc species, which successively reacts with the alkyl triflate to afford the internal alkyne. A radical pathway is unlikely in this system.magnified image
Phosphine‐Catalyzed Intermolecular Annulations of Fluorinated ortho‐Aminophenones with Alkynones – The Switchable [4+2] or [4+2]/[3+2] Cycloaddition
Authors: Zhang Yanshun , Sun Yaoliang , Wei Yin , Shi Min 
Published: February 2019

AbstractA phosphine‐catalyzed intermolecular annulation reaction of functionalized ortho‐aminoacetophenones with alkynones has been disclosed in this paper. A variety of 2‐alkynylquinolines and benzo‐fused indolizine were selectively afforded in moderate to good yields at different reaction temperatures and with different phosphine catalysts via the in situ generated zwitterionic intermediate derived from alkynone and phosphine.magnified image
Synergistic Effect of Co–Ni Hybrid Phosphide Nanocages for Ultrahigh Capacity Fast Energy Storage
Authors: Liang Zibin , Qu Chong , Zhou Wenyang , Zhao Ruo , Zhang Hao , Zhu Bingjun , Guo Wenhan , Meng Wei , Wu Yingxiao , Aftab Waseem , Wang Qian , Zou Ruqiang 
Published: February 2019

AbstractRational design of metal compounds in terms of the structure/morphology and chemical composition is essential to achieve desirable electrochemical performances for fast energy storage because of the synergistic effect between different elements and the structure effect. Here, an approach is presented to facilely fabricate mixed‐metal compounds including hydroxides, phosphides, sulfides, oxides, and selenides with well‐defined hollow nanocage structure using metal–organic framework nanocrystals as sacrificial precursors. Among the as‐synthesized samples, the porous nanocage structure, synergistic effect of mixed metals, and unique phosphide composition endow nickel cobalt bimetallic phosphide (NiCo‐P) nanocages with outstanding performance as a battery‐type Faradaic electrode material for fast energy storage, with ultrahigh specific capacity of 894 C g−1 at 1 A g−1 and excellent rate capability, surpassing most of the reported metal compounds. Control experiments and theoretical calculations based on density functional theory reveal that the synergistic effect between Ni and Co in NiCo‐P can greatly increase the OH− adsorption energy, while the hollow porous structure facilitates the fast mass/electron transport. The presented work not only provides a promising electrode material for fast energy storage, but also opens a new route toward structural and compositional design of electrode materials for energy storage and conversion.
Ruthenium Oxide Nanosheets for Enhanced Oxygen Evolution Catalysis in Acidic Medium
Authors: Laha Sourav , Lee Yonghyuk , Podjaski Filip , Weber Daniel , Duppel Viola , Schoop Leslie M. , Pielnhofer Florian , Scheurer Christoph , Müller Kathrin , Starke Ulrich , Reuter Karsten , Lotsch Bettina V. 
Published: February 2019

AbstractThe fabrication of highly active and robust hexagonal ruthenium oxide nanosheets for the electrocatalytic oxygen evolution reaction (OER) in an acidic environment is reported. The ruthenate nanosheets exhibit the best OER activity of all solution‐processed acid medium electrocatalysts reported to date, reaching 10 mA cm−2 at an overpotential of only ≈255 mV. The nanosheets also demonstrate robustness under harsh oxidizing conditions. Theoretical calculations give insights into the OER mechanism and reveal that the edges are the origin of the high OER activity of the nanosheets. Moreover, the post OER analyses indicate, apart from coarsening, no observable change in the morphology of the nanosheets or oxidation states of ruthenium during the electrocatalytic process. Therefore, the present investigation suggests that ruthenate nanosheets are a promising acid medium OER catalyst with application potential in proton exchange membrane electrolyzers and beyond.
Microstructure‐Controlled Ni‐Rich Cathode Material by Microscale Compositional Partition for Next‐Generation Electric Vehicles
Authors: Kim Un‐Hyuck , Ryu Hoon‐Hee , Kim Jae‐Hyung , Mücke Robert , Kaghazchi Payam , Yoon Chong S. , Sun Yang‐Kook 
Published: February 2019

AbstractA multicompositional particulate Li[Ni0.9Co0.05Mn0.05]O2 cathode in which Li[Ni0.94Co0.038Mn0.022]O2 at the particle center is encapsulated by a 1.5 µm thick concentration gradient (CG) shell with the outermost surface composition Li[Ni0.841Co0.077Mn0.082]O2 is synthesized using a differential coprecipitation process. The microscale compositional partitioning at the particle level combined with the radial texturing of the refined primary particles in the CG shell layer protracts the detrimental H2 → H3 phase transition, causing sharp changes in the unit cell dimensions. This protraction, confirmed by in situ X‐ray diffraction and transmission electron microscopy, allows effective dissipation of the internal strain generated upon the H2 → H3 phase transition, markedly improving cycling performance and thermochemical stability as compared to those of the conventional single‐composition Li[Ni0.9Co0.05Mn0.05]O2 cathodes. The compositionally partitioned cathode delivers a discharge capacity of 229 mAh g−1 and exhibits capacity retention of 88% after 1000 cycles in a pouch‐type full cell (compared to 68% for the conventional cathode). Thus, the proposed cathode material provides an opportunity for the rational design and development of a wide range of multifunctional cathodes, especially for Ni‐rich Li[NixCoyMn1‐x‐y]O2 cathodes, by compositionally partitioning the cathode particles and thus optimizing the microstructural response to the internal strain produced in the deeply charged state.
Achieving Thickness‐Insensitive Morphology of the Photoactive Layer for Printable Organic Photovoltaic Cells via Side Chain Engineering in Nonfullerene Acceptors
Authors: Lee Seongyu , Park Kwang Hun , Lee Jong‐Hoon , Back Hyungcheol , Sung Min Jae , Lee Jinho , Kim Jehan , Kim Heejoo , Kim Yun‐Hi , Kwon Soon‐Ki , Lee Kwanghee 
Published: February 2019

AbstractAlthough high power conversion efficiency of over 14% has been achieved using nonfullerene acceptors (NFAs) in organic photovoltaics (OPVs), securing their insensitive device performance to the thickness of the photoactive layer remains an indispensable requirement for their successful commercialization via printing technologies. In this study, by synthesizing a new series of ITIC‐based NFAs having alkyl or alkoxy groups, it is found that the bulk heterojunction morphology dependence on the thickness of the photoactive layer becomes more severe as the difference in the surface energy of the donor and acceptor increases. It is believed that this observation is the origin that yields the device performance dependence on the thickness of the photoactive layer. Through sensitive control of the surface energy of these ITIC‐based NFAs, it is demonstrated that thickness‐insensitive OPVs can be achieved even using a doctor blade technique under air without using any additives. It is believed that present approach provides an important insight into the design of photoactive materials and morphology control for the printable OPVs using NFAs.
Building Emergency Medicine Trainee Competency in Pediatric Musculoskeletal Radiograph Interpretation: A Multicenter Prospective Cohort Study
Authors: Lee Michelle Sin , Pusic Martin , Carrière Benoit , Dixon Andrew , Stimec Jennifer , Boutis Kathy 
Published: February 2019

AbstractObjectivesAs residency programs transition from time‐ to performance‐based competency standards, validated tools are needed to measure performance‐based learning outcomes and studies are required to characterize the learning experience for residents. Since pediatric musculoskeletal (MSK) radiograph interpretation can be challenging for emergency medicine trainees, we introduced Web‐based pediatricMSKradiograph learning system with performance endpoints into pediatric emergency medicine (PEM) fellowships and determined the feasibility and effectiveness of implementing this intervention.MethodsThis was a multicenter prospective cohort study conducted over 12 months. The course offered 2,100 pediatricMSKradiographs organized into seven body regions.PEMfellows diagnosed each case and received feedback after each interpretation. Participants completed cases until they achieved a performance benchmark of at least 80% accuracy, sensitivity, and specificity. The main outcome measure was the median number of cases completed by participants to achieve the performance benchmark.ResultsFiftyPEMfellows from nine programs in theUSand Canada participated. There were 301 of 350 (86%) modules started and 250 of 350 (71%) completed to the predefined performance benchmark during the study period. The median (interquartile range [IQR]) number of cases to performance benchmark per participant was 78 (60–104; min = 56, max = 1,333). Between modules, the median number of cases to achieve the performance benchmark was different for the ankle versus other modules (ankle 366 vs. other 76; difference = 290, 95% confidence interval [CI] = 245 to 335). The performance benchmark was achieved for 90.7% of participants in all modules except the ankle/foot, where 34.9% achieved this goal (difference = 55.8%, 95%CI = 45.3 to 66.3). The mean (95%CI) change in accuracy, sensitivity, and specificity from baseline to performance benchmark was +14.6% (13.4 to 15.8), +16.5% (14.8 to 18.1), and +12.6% (10.7 to 14.5), respectively. Median (IQR) time on each case was 31.0 (21.0–45.3) seconds.ConclusionsMost participants completed the modules to the performance benchmark within 1 hour and demonstrated significant skill improvement. Further, there was a large variation in the number of cases completed to achieve the performance endpoint in any given module, and this impacted the feasibility of completing specific modules.
The prognostic value of agonal respiration in refractory cardiac arrest: a case series of non‐shockable cardiac arrest successfully resuscitated through extracorporeal cardiopulmonary resuscitation
Authors: Bunya Naofumi , Wada Kenshiro , Yamaoka Ayumu , Kakizaki Ryuichiro , Katayama Yoichi , Kasai Takehiko , Kyan Ryoko , Murakami Naoto , Kokubu Nobuaki , Uemura Shuji , Narimatsu Eichi 
Published: February 2019

BackgroundAgonal respiration following out‐of‐hospital cardiac arrest is associated with favorable neurological outcomes. Resuscitation using extracorporeal membrane oxygenation could contribute to achieving favorable neurological outcomes in patients with refractory cardiac arrest.Case presentationWe report two cases of refractory cardiac arrest with non‐shockable rhythms and agonal respiration; both patients were successfully resuscitated through extracorporeal cardiopulmonary resuscitation (ECPR). Both patients were breathing spontaneously upon arrival. One patient was asystolic and the other experienced pulseless electrical activity followed by ventricular fibrillation. Agonal respiration was observed in both and ECPR was implemented, leading to a favorable neurological outcome at discharge.ConclusionThe presence of agonal respiration has the potential to confer a favorable neurological outcome in patients with refractory cardiac arrest if maintained, even when the initial cardiac rhythm is not shockable. In these cases, resuscitation should not be abandoned, and ECPR should be considered.
Introduction of two polyvinyl alcohol resins for efficient solid support Cu‐catalyzed N‐arylation of α‐aminoacids with aryl halides in aqueous media
Authors: Kazemnejadi Milad , Sardarian Ali Reza , Esmaeilpour Mohsen 
Published: February 2019

ABSTRACTIn this article, two polyvinyl alcohol (PVA)‐based resins were prepared by crosslinking of epoxidized PVA‐chains using of 4‐(4‐aminobenzyl)benzenamine as a crosslinker and polymerization of acrylated PVA chains in the another approach. The prepared PVA resins showed well hydrophilic and swelling properties in various organic solvents, which are used in solid‐phase organic synthesis (SPOS). Swelling properties of these resins were examined in dimethylformamide, tetrahydrofuran, water, ethanol, methanol, dichloromethane, and dioxane. Furthermore, the both resins were characterized by FTIR and 1H‐NMR and their properties such as epoxy equivalent weight (EEW) of epoxidized PVA and density of the resins were determined by analytical methods. Then, α‐amino acids such as L‐aspartic acid, L‐leucine, L‐alanine, L‐serine, L‐valine, L‐threonine, and L‐tyrosine were immobilized on both resins through esterification reaction between these α‐amino acids with the present hydroxyl groups on PVA resines, to carry out their solid‐phase N‐arylation reaction in the presence of CuI as a catalyst in milder and greener conditions than free resin protocols. Hydrolysis of the correponding N‐arylated α‐amino acids immobilized on the resins gave the N‐arylated α‐amino acids in high to excellent yields. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47597.
Southern right whale (Eubalaena australis), seasonal abundance and distribution at Head of Bight, South Australia
Authors: Charlton Claire , Ward Rhianne , McCauley Robert D. , Brownell Robert L. , Salgado Kent Chandra , Burnell Stephen 
Published: February 2019

Abstract

Seasonal trends in the distribution and relative abundance of southern right whales (SRWs) Eubalaena australis, were assessed in Australia's largest calving aggregation ground at the Head of the Great Australian Bight, in the Commonwealth Marine Reserve, South Australia. Annual cliff‐based surveys were undertaken between June and October from 1992 to 2016.
SRWs were primarily distributed in a 15 km by 2 km area within the 10 m depth contour (with 95% of whale sightings made within a 10 km2 area). The distribution of SRWs at Head of Bight varied within an individual season but was consistent among the years. The composition of SRW sightings was 70% female–calf pairs and 30% unaccompanied whales.
Peak abundance occurred between mid‐July and end‐August for female–calf pairs and unaccompanied whales (juveniles or adults not accompanied by a calf), earlier than previously reported. A mean of 16% (range 8–28%, SD = 6.5, 95% CI = 0.15) of calving females were present at the site in mid‐June and a mean of 37% (range 13–61%, SD = 15.8, 95% CI = 0.37) remained at the site at the end of September.
Based on nearest‐neighbour distances of 150 m, the area occupied by 95% of SRWs at Head of Bight could reach carrying capacity at 68 female and calf pairs. Results suggest that the primary aggregation area at Head of Bight may have reached saturation capacity and that habitat expansion can be expected as the population increases.
This study provides information on SRW seasonal trends in distribution and abundance, timing of arrival and departure from the site and peak abundance periods relevant to application to conservation and marine park management.
As management requirements increase with a growing population, there is a need to complete an Australia‐wide assessment of SRW connectivity and habitat expansion.
Pim‐1 as a Therapeutic Target in Lupus Nephritis
Authors: Fu Rong , Xia Yong , Li Meirong , Mao Renxiang , Guo Chaohuan , Zhou Mianjing , Tan Hechang , Liu Meiling , Wang Shuang , Yang Niansheng , Zhao Jijun 
Published: February 2019

ObjectiveLupus nephritis (LN) is a major determinant of morbidity and mortality in systemic lupus erythematosus (SLE). Pim‐1 regulates lymphocyte proliferation and activation. The role of Pim‐1 in autoimmune disease remains unclear. This study was undertaken to test the hypothesis that inhibition of Pim‐1 would have therapeutic potential in patients with LN.MethodsPim‐1 expression was analyzed in lupus‐prone (NZB × NZW)F1 mice (n = 6), human peripheral blood mononuclear cells (PBMCs) from SLE patients (n = 10), and glomeruli from patients with LN (n = 8). The therapeutic effect of the Pim‐1 inhibitor AZD1208 was assessed in the same murine lupus model (n = 10 mice per group). In vitro analysis was conducted to explore the mechanisms of action of Pim‐1 in mouse and human podocytes after Pim‐1 expression had been induced by anti–double‐stranded DNA (anti‐dsDNA) antibody–positive serum. Finally, MRL/lpr mice were used to confirm the therapeutic effects of Pim‐1 inhibition in vivo (n = 10 mice per group).ResultsUp‐regulation of Pim‐1 was seen in renal lysates from diseased (NZB × NZW)F1 mice and in PBMCs from patients with SLE and renal biopsy tissue from patients with LN, relative to their control counterparts (each P < 0.05). The Pim‐1 inhibitor AZD1208 reduced the severity of proteinuria, glomerulonephritis, renal immune complex deposits, and serum anti‐dsDNA antibody levels, concomitant with the suppression of NFATc1 expression and NLRP3 inflammasome activation, in diseased (NZB × NZW)F1 mice (each P < 0.05 versus controls). Moreover, in mouse and human podocytes, Pim‐1 knockdown with targeted small interfering RNA (siRNA) suppressed NFATc1 and NLRP3 inflammasome signaling in the presence of anti‐dsDNA–positive serum (each P < 0.05 versus control siRNA). Mechanistically, Pim‐1 modulated NLRP3 inflammasome activation through intracellular Ca2+ (P < 0.05 versus normal controls). The therapeutic effect of Pim‐1 blockade was replicated in MRL/lpr mice.ConclusionThese data identify Pim‐1 as a critical regulator of LN pathogenesis in patients with SLE. Targeting of the Pim‐1/NFATc1/NLRP3 pathway might therefore have therapeutic potential in human LN.
Orthogonal Oriented Bisanthrancene‐Bridged Bis(Triarylamine) Diradical Dications: Isolation, Characterizations and Crystal Structures
Authors: Wang Lei , Zhang Li , Fang Yong , Zhao Yue , Tan Gengwen , Wang Xinping 
Published: February 2019

AbstractTwo bis(triarylamine) diradical dication salts 12+2[Al(ORF)4]− and 22+2[Al(ORF)4]− bridged with an orthogonal oriented bisanthrancene motif were synthesized. Their solid state and electronic structures were investigated by various experimental approaches in conjunction with theoretical calculations. Superconducting quantum interference device measurements and density functional theory calculations reveal that both of 12+ and 22+ feature open‐shell singlet ground states with rather small singlet‐triplet energy gaps; thus, they can be regarded as nearly pure diradicals (biradicals). Their diradical characters are enhanced by the orthogonal configuration of the bisanthrancene moiety which demonstrates the importance of the geometry of bridging units in turning the electronic structures of bis(triarylamine) dications.