bluuebunny/crossref_metadata_2025_split huggingface dataset:
Enabling Stable High‐Voltage LiCoO2 Operation by Using Synergetic Interfacial Modification Strategy
Authors: Yang Xuerui , Lin Min , Zheng Guorui , Wu Jue , Wang Xianshu , Ren Fucheng , Zhang Wenguang , Liao Ying , Zhao Weimin , Zhang Zhongru , Xu Ningbo , Yang Wanli , Yang Yong 
Published: September 2020

AbstractStructural and interfacial instability of the LiCoO2 cathode under a voltage exceeding 4.5 V (vs Li/Li+) severely hinders its practical applications for high‐energy‐density lithium batteries. Herein, a modified electrolyte with nitriles (suberonitrile or 1,3,6‐hexanetricarbonitrile) and fluoroethylene carbonate (FEC) coadditives is demonstrated to form an ultrathin and uniform interface layer on LiCoO2 cathode under a synergetic effect. As such, LiCoO2/Li cells display excellent cyclability at a cutoff voltage of 4.6 V with a capacity retention over 72% after 300 cycles and 60% after 200 cycles at 30 and 55 °C, respectively, even achieving operation at a high current rate (10 C) upon 500 cycles as compared to the controls with fast‐falling capacity to zero. Furthermore, an adsorption‐coordination mechanism between nitriles and cobalt and synergetic effect of coadditives are explored by the alliance of spectroscopic analysis and theoretical calculations. The contributed lone‐pairs on the N 2p orbital of nitriles in coordination lowers the real oxidation state of Co3+/4+ so that it decreases its catalysis on electrolytes, and the synergy from nitrile‐derived species regulates FEC to form an LiF‐containing electron‐insulated interface layer. This work shares a new insight to nitriles with the synergy of coadditives and paves a way to refine (ultra)high‐voltage LiCoO2 cathode for high‐energy‐density energy storages.
Achromatic Huygens’ Metalenses with Deeply Subwavelength Thickness
Authors: Fathnan Ashif A. , Liu Mingkai , Powell David A. 
Published: September 2020

AbstractMatching magnetic and electric responses has proven key to achieving high‐efficiency transmissive Huygens’ metasurfaces. However, the complex frequency dependence of the required magnetic and electric responses is difficult to control, causing inevitable mismatch and undesired narrowband responses. Here, a rigorous design methodology is proposed to obtain a metasurface in which the Huygens’ condition is maintained over a broad bandwidth and range of phase tuning. By utilizing three patterned metallic layers separated by dielectrics, it is shown how the resonant modes with electric and magnetic dipole moments can be controlled almost independently, enabling broadband transparency with controllable dispersion. Representing the resonant elements as series and parallel inductance–capacitance configurations, a convenient implementation of a macro‐level design into a realistic geometry is demonstrated. Based on the proposed method, a subwavelength thickness metasurface lens that maintains constant focal length over 11% of fractional bandwidth is designed and characterized. It is also shown that the method can be utilized to achieve specified values of chromatic dispersion of a metasurface lens, enabling various functional devices and applications.
Highly Stable and Scalable Blue QD‐LED via an Evaporated TiO2 Thin Film as an Electron Transport Layer
Authors: Bang Sang Yun , Fan Xiang‐Bing , Jung Sung‐Min , Yang Jiajie , Shin Dong‐Wook , Suh Yo‐Han , Lee Tae Hoon , Lee Sanghyo , Choi Hyung Woo , Occhipinti Luigi G. , Han Soo Deok , Kim Jong Min 
Published: September 2020

AbstractQuantum dot‐based light‐emitting diodes (QD‐LEDs) have excellent optical properties; however, their limitations of stability, reproducibility, and scalability due to the solution process are the major drawback. Herein, blue QD‐LEDs fabricated with the conventional vacuum process using an e‐beam‐evaporated TiO2 thin film as an electron transport layer (ETL) are demonstrated. CdZnS/ZnS‐based blue LEDs with a TiO2 thin film are fabricated under ambient conditions. They exhibit maximum external quantum efficiencies of 3.53% and a peak luminance of 2847 cd m−2. These values are retained, which minimizes performance degradation under high potential bias. In addition, the optimized evaporated TiO2 thin film has a negligible red shift (0.5 nm) of the peak wavelength between the photoluminescence spectrum and electroluminescence spectrum with stable full‐width at half‐maximum changing by less than 2 nm at high voltage. Finally, a blue QD‐LED is fabricated on a scalable emission area of 2 × 2 in. with a patterned cathode accompanied by an evaporated TiO2 thin film, which allows to perform conventional photolithography. A highly stable and reproducible vaporized inorganic thin film as the ETL supports the multilayer architecture to minimize the process damage.
Metal‐Free Synthesis of (E)‐Vinyl Sulfones via An Insertion of Sulfur Dioxide/1,5‐Hydrogen Atom Transfer Sequence
Authors: He Fu‐Sheng , Yao Yanfang , Xie Wenlin , Wu Jie 
Published: September 2020

AbstractA metal‐free three‐component reaction of propargyl alcohols, sodium metabisulfite, and aryldiazonium tetrafluoroborates under mild conditions is described. The reaction proceeds efficiently at room temperature without the need of any catalysts, affording the corresponding (E)‐vinyl sulfones in moderate to good yields with excellent functional group tolerance. Preliminary mechanistic studies show that a vinyl radical‐induced 1,5‐hydrogen atom transfer process and functional group migration are involved, resulting in the cleavage of inert C−H and C−C bonds in sequence.magnified image
7q31.2q31.31 deletion downstream of FOXP2 segregating in a family with speech and language disorder
Authors: Rieger Melissa , Krumbiegel Mandy , Reuter Miriam S. , Schützenberger Anne , Reis André , Zweier Christiane 
Published: September 2020

AbstractChromosomal 7q31 deletions have been described in individuals with variable neurodevelopmental phenotypes including speech and language impairment. These copy number variants usually encompass FOXP2, haploinsufficiency of which represents a widely acknowledged cause for specific speech and language disorders. By chromosomal microarray analysis we identified a 4.7 Mb microdeletion at 7q31.2q31.31 downstream of FOXP2 in three family members presenting with variable speech, language and neurodevelopmental phenotypes. The index individual showed delayed speech development with impaired speech production, reduced language comprehension, and additionally learning difficulties, microcephaly, and attention deficit. His younger sister had delayed speech development with impaired speech production and partially reduced language comprehension. Their mother had attended a school for children with speech and language deficiencies and presented with impaired articulation. The deletion had occurred de novo in the mother, includes 15 protein‐coding genes and is located in close proximity to the 3′ end of FOXP2. Though a novel locus at 7q31.2q31.31 associated with mild neurodevelopmental and more prominent speech and language impairment is possible, the close phenotypic overlap with FOXP2‐associated speech and language disorder rather suggests a positional effect on FOXP2 expression and function.
Long‐term risk of dementia following hospitalization due to physical diseases: A multicohort study
Authors: Sipilä Pyry N , Lindbohm Joni V , Singh‐Manoux Archana , Shipley Martin J. , Kiiskinen Tuomo , Havulinna Aki S , Vahtera Jussi , Nyberg Solja T , Pentti Jaana , Kivimäki Mika 
Published: September 2020

AbstractIntroductionConventional risk factors targeted by prevention (e.g., low education, smoking, and obesity) are associated with a 1.2‐ to 2‐fold increased risk of dementia. It is unclear whether having a physical disease is an equally important risk factor for dementia.MethodsIn this exploratory multicohort study of 283,414 community‐dwelling participants, we examined 22 common hospital‐treated physical diseases as risk factors for dementia.ResultsDuring a median follow‐up of 19 years, a total of 3416 participants developed dementia. Those who had erysipelas (hazard ratio = 1.82; 95% confidence interval = 1.53 to 2.17), hypothyroidism (1.94; 1.59 to 2.38), myocardial infarction (1.41; 1.20 to 1.64), ischemic heart disease (1.32; 1.18 to 1.49), cerebral infarction (2.44; 2.14 to 2.77), duodenal ulcers (1.88; 1.42 to 2.49), gastritis and duodenitis (1.82; 1.46 to 2.27), or osteoporosis (2.38; 1.75 to 3.23) were at a significantly increased risk of dementia. These associations were not explained by conventional risk factors or reverse causation.DiscussionIn addition to conventional risk factors, several physical diseases may increase the long‐term risk of dementia.
Activating the Antibacterial Effect of 4,6‐Diamino‐2‐pyrimidinethiol‐Modified Gold Nanoparticles by Reducing their Sizes
Authors: Xie Yangzhouyun , Yang Junchuan , Zhang Jiangjiang , Zheng Wenfu , Jiang Xingyu 
Published: September 2020

AbstractAdequately decorated gold nanoparticles (GNPs) have excellent antibiotic activities against multidrug‐resistant (MDR) bacteria. Nanoparticles exhibiting Gram selective antibacterial actions are beneficial to precise therapy. Here, we present a strategy to tune the antibacterial spectrum of a small molecule (4,6‐diamino‐2‐pyrimidinethiol, DAPT)‐modified GNPs (DAPT‐GNPs, DGNPs) by adjusting their sizes. Compared to large (ca. 14 nm diameter) DGNPs (lDGNPs) and medium‐sized (3–4 nm diameter) DGNPs (mDGNPs), which have no antibacterial effect or only target Gram‐negative (G−) bacteria, ultrasmall DGNPs (uDGNPs, <2 nm) have a broad antibacterial spectrum, especially showing an over 60‐fold increase in antibacterial efficacy against Gram‐positive (G+) bacteria. Moreover, the uDGNPs‐functionalized scaffolds (agarose gel) can serve as general wound dressings for healing burnt infections. Our strategy is insightful for exploring properties of the nanomaterials and their applications.
Designing Cascades of Electron Transfer Processes in Multicomponent Graphene Conjugates
Authors: Limosani Francesca , Kaur Ramandeep , Cataldo Antonino , Bellucci Stefano , Micciulla Federico , Zanoni Robertino , Lembo Angelo , Wang Bingzhe , Pizzoferrato Roberto , Guldi Dirk M. , Tagliatesta Pietro 
Published: September 2020

AbstractA novel family of nanocarbon‐based materials was designed, synthesized, and probed within the context of charge‐transfer cascades. We integrated electron‐donating ferrocenes with light‐harvesting/electron‐donating (metallo)porphyrins and electron‐accepting graphene nanoplates (GNP) into multicomponent conjugates. To control the rate of charge flow between the individual building blocks, we bridged them via oligo‐p‐phenyleneethynylenes of variable lengths by β‐linkages and the Prato–Maggini reaction. With steady‐state absorption, fluorescence, Raman, and XPS measurements we realized the basic physico‐chemical characterization of the photo‐ and redox‐active components and the multicomponent conjugates. Going beyond this, we performed transient absorption measurements and corroborated by single wavelength and target analyses that the selective (metallo)porphyrin photoexcitation triggers a cascade of charge transfer events, that is, charge separation, charge shift, and charge recombination, to enable the directed charge flow. The net result is a few nanosecond‐lived charge‐separated state featuring a GNP‐delocalized electron and a one‐electron oxidized ferrocenium.
Enhancing CO2 Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc–Nitrogen–Carbon Tandem Catalyst
Authors: Lin Long , Liu Tianfu , Xiao Jianping , Li Hefei , Wei Pengfei , Gao Dunfeng , Nan Bing , Si Rui , Wang Guoxiong , Bao Xinhe 
Published: September 2020

AbstractDeveloping copper‐free catalysts for CO2 conversion into hydrocarbons and oxygenates is highly desirable for electrochemical CO2 reduction reaction (CO2RR). Herein, we report a cobalt phthalocyanine (CoPc) and zinc–nitrogen–carbon (Zn‐N‐C) tandem catalyst for CO2RR to CH4. This tandem catalyst shows a more than 100 times enhancement of the CH4/CO production rate ratio compared with CoPc or Zn‐N‐C alone. Density functional theory (DFT) calculations and electrochemical CO reduction reaction results suggest that CO2 is first reduced into CO over CoPc and then CO diffuses onto Zn‐N‐C for further conversion into CH4 over Zn‐N4 site, decoupling complicated CO2RR pathway on single active site into a two‐step tandem reaction. Moreover, mechanistic analysis indicates that CoPc not only generates CO but also enhances the availability of *H over adjacent N sites in Zn‐N4, which is the key to achieve the high CH4 production rate and understand the intriguing electrocatalytic behavior which is distinctive to copper‐based tandem catalysts.
Overcoming Symmetry Mismatch in Vaccine Nanoassembly through Spontaneous Amidation
Authors: Rahikainen Rolle , Rijal Pramila , Tan Tiong Kit , Wu Hung‐Jen , Andersson Anne‐Marie C. , Barrett Jordan R. , Bowden Thomas A. , Draper Simon J. , Townsend Alain R. , Howarth Mark 
Published: September 2020

AbstractMatching of symmetry at interfaces is a fundamental obstacle in molecular assembly. Virus‐like particles (VLPs) are important vaccine platforms against pathogenic threats, including Covid‐19. However, symmetry mismatch can prohibit vaccine nanoassembly. We established an approach for coupling VLPs to diverse antigen symmetries. SpyCatcher003 enabled efficient VLP conjugation and extreme thermal resilience. Many people had pre‐existing antibodies to SpyTag:SpyCatcher but less to the 003 variants. We coupled the computer‐designed VLP not only to monomers (SARS‐CoV‐2) but also to cyclic dimers (Newcastle disease, Lyme disease), trimers (influenza hemagglutinins), and tetramers (influenza neuraminidases). Even an antigen with dihedral symmetry could be displayed. For the global challenge of influenza, SpyTag‐mediated display of trimer and tetramer antigens strongly induced neutralizing antibodies. SpyCatcher003 conjugation enables nanodisplay of diverse symmetries towards generation of potent vaccines.
Anionic Aliovalent Substitution from Structure Models of ZnS: Novel Defect Diamond‐like Halopnictide Infrared Nonlinear Optical Materials with Wide Band Gaps and Large SHG Effects
Authors: Chen Jindong , Lin Chensheng , Zhao Dan , Luo Min , Peng Guang , Li Bingxuan , Yang Shunda , Sun Yingshuang , Ye Ning 
Published: September 2020

AbstractTo design pnictide nonlinear optical materials with wide band gap and large second‐harmonic generation, the heavy halogen I was introduced into pnictides through anionic aliovalent substitution with diamond‐like ZnS as templates. Thus, four excellent halopnictide‐based infrared nonlinear optical crystals, MII3PnI3 (MII=Zn, Cd; Pn=P, As), were obtained. They all exhibited defect diamond‐like structures with highly parallel‐oriented [MIIPnI3] mixed‐anionic tetrahedral groups, leading to excellent physical properties including wide band gaps (2.38–2.85 eV), large second harmonic generation responses (2.7–5.1×AgGaS2), high laser‐induced damage thresholds (5.5–10.7×AgGaS2), and good IR transparency. In particular, Cd3PI3 and Cd3AsI3 achieved phase‐matching (Δn=0.035 and 0.031) that their template β‐ZnS could not do. Anionic aliovalent substitution provides a feasible strategy to design novel promising halopnictide IR NLO materials.
Design and Atroposelective Construction of IAN analogues by Organocatalytic Asymmetric Heteroannulation of Alkynes
Authors: Zhang Lei , Shen Jiahua , Wu San , Zhong Guofu , Wang Yong‐Bin , Tan Bin 
Published: September 2020

AbstractAn organocatalytic atroposelective strategy for accessing enantioenriched axially chiral IAN analogues was developed for the first time. A class of novel atropisomeric C2‐arylquinoline skeletons were synthesized with high enantiocontrol via chiral phosphoric‐acid‐catalyzed heteroannulation of in situ generated vinylidene ortho‐quinone methide (VQM) intermediates with ortho‐aminophenones. The strategy tolerated a broad substrate scope, providing a facile organocatalytic approach to IAN analogues in good yields and excellent enantioselectivities under mild reaction conditions. Moreover, the synthetic utility of this methodology was illustrated through further transformations into IAN‐type ligand and axially chiral thiourea.
Fluoro Nitrenoid Complexes FN=MF2 (M=Co, Rh, Ir): Electronic Structure Dichotomy and Formation of Nitrido Fluorides N≡MF3
Authors: Stüker Tony , Hohmann Thomas , Beckers Helmut , Riedel Sebastian 
Published: September 2020

AbstractThe fluoronitrenoid metal complexes FNCoF2 and FNRhF2 as well as the first ternary RhVI and IrVI complexes NIrF3 and NRhF3 are described. They were obtained by the reaction of excited Group‐9 metal atoms with NF3 and their IR spectra, isolated in solid rare gases (neon and argon), were recorded. Aided by the observed 14/15N isotope shifts and quantum‐chemical predictions, all four stretching fundamentals of the novel complexes were safely assigned. The F−N stretching frequencies of the fluoronitrenoid complexes FNCoF2 (1056.8 cm−1) and FNRhF2 (872.6 cm−1) are very different and their N−M bonds vary greatly. In FNCoF2, the FN ligand is singly bonded to Co and bears considerable iminyl/nitrene radical character, while the N−Rh bond in FNRhF2 is a strong double bond with comparatively strong σ‐ and π‐bonds. The anticipated rearrangement of FNCoF2 to the nitrido CoVI complex is predicted to be endothermic and was not observed.
Bio‐based and Degradable Block Polyester Pressure‐Sensitive Adhesives
Authors: Chen Thomas T. D. , Carrodeguas Leticia Peña , Sulley Gregory S. , Gregory Georgina L. , Williams Charlotte K. 
Published: September 2020

AbstractA new class of bio‐based fully degradable block polyesters are pressure‐sensitive adhesives. Bio‐derived monomers are efficiently polymerized to make block polyesters with controlled compositions. They show moderate to high peel adhesions (4–13 N cm−1) and controllable storage and loss moduli, and they are removed by adhesive failure. Their properties compare favorably with commercial adhesives or bio‐based polyester formulations but without the need for tackifier or additives.
A Multiple Chirality Switching Device for Spatial Light Modulators
Authors: Yang Guojian , Yu Yang , Yang Baige , Lu Tong , Cai Yiru , Yin Hang , Zhang Huiqi , Zhang Ning‐Ning , Li Li , Zhang Yu‐Mo , Zhang Sean Xiao‐An 
Published: September 2020

AbstractA new and simple strategy towards electric‐field‐driven multiple chirality switching device has been designed and fabricated by combining a newly synthesized base‐responsive chiroptical polymer switch (R‐FLMA) and p‐benzoquinone (p‐BQ) via proton‐coupled electron transfer (PCET) mechanism. Clear and stable triple chirality states (silence, positive, negative) of this device in visible band can be regulated reversibly (>1000 cycles) by adjusting voltage programs. Furthermore, such chiral switching phenomena are also accompanied by apparent changes of color and fluorescence. More importantly, the potential application of this device for a spatial light modulator has also been demonstrated.
Rhodium(III)‐Catalyzed Asymmetric [4+1] and [5+1] Annulation of Arenes and 1,3‐Enynes: A Distinct Mechanism of Allyl Formation and Allyl Functionalization
Authors: Sun Jiaqiong , Yuan Weiliang , Tian Rong , Wang Peiyuan , Zhang Xue‐Peng , Li Xingwei 
Published: September 2020

AbstractWe report chiral RhIII cyclopentadienyl‐catalyzed enantioselective synthesis of lactams and isochromenes through oxidative [4+1] and [5+1] annulation, respectively, between arenes and 1,3‐enynes. The reaction proceeds through a C−H activation, alkenyl‐to‐allyl rearrangement, and a nucleophilic cyclization cascade. The mechanisms of the [4+1] annulations were elucidated by a combination of experimental and computational methods. DFT studies indicated that, following the C−H activation and alkyne insertion, a RhIII alkenyl intermediate undergoes δ‐hydrogen elimination of the allylic C−H via a six‐membered ring transition state to produce a RhIII enallene hydride intermediate. Subsequent hydride insertion and allyl rearrangement affords several rhodium(III) allyl intermediates, and a rare RhIII η4 ene‐allyl species with π‐agostic interaction undergoes SN2′‐type external attack by the nitrogen nucleophile, instead of C−N reductive elimination, as the stereodetermining step.
1D Coordination π–d Conjugated Polymers with Distinct Structures Defined by the Choice of the Transition Metal: Towards a New Class of Antiaromatic Macrocycles
Authors: Santhini Vijai M. , Wäckerlin Christian , Cahlík Aleš , Ondráček Martin , Pascal Simon , Matěj Adam , Stetsovych Oleksandr , Mutombo Pingo , Lazar Petr , Siri Olivier , Jelínek Pavel 
Published: September 2020

AbstractRecently π–d conjugated coordination polymers have received a lot of attention owing to their unique material properties, although synthesis of long and defect‐free polymers remains challenging. Herein we introduce a novel on‐surface synthesis of coordination polymers with quinoidal ligands under ultra‐high vacuum conditions, which enables formation of flexible coordination polymers with lengths up to hundreds of nanometers. Moreover, this procedure allows the incorporation of different transition‐metal atoms with four‐ or two‐fold coordination. Remarkably, the two‐fold coordination mode revealed the formation of wires constituted by (electronically) independent 12‐membered antiaromatic macrocycles linked together through two C−C single bonds.
Effect of coalbed methane airflow with optimum action concentration on coal oxidation under low temperatures
Authors: Xu Qin , Yang Shengqiang , Yang Wenming , Tang Zongqing , Song Wanxin , Zhou Buzhuang , Yang Kai 
Published: September 2020

AbstractTo explore the effect of coalbed methane (CBM) airflow on coal oxidation under low temperatures, an experimental apparatus was developed and applied to simulate coal oxidation under different oxidizing atmospheres. The formation of carbon monoxide CO, the index gas, in CBM airflow was analyzed to obtain the optimum concentration of CH4 that exerted the strongest influence on coal oxidation. Then, a comparison experiment was performed on coal oxidation in dry air and in CH4 at the optimum concentration by using electron spin resonance (ESR) and Fourier transform infrared (FTIR) technology. The results suggest that 25% of CH4 has the strongest effect on coal oxidation at low temperatures. The free radical concentration (Ng) in coal increases with temperature in both dry air and 25% CH4. At this concentration, CH4 can inhibit the reactivity of coal substantially while raising the excitation temperature. The oxidation of aliphatic hydrocarbons is severely inhibited by 25% CH4, which reduces its consumption rate and abates its decrement in the initial phase. Although 25% CH4 restricts the consumption of –OH and –COOH in oxidation, it promotes the formation of –C–O.
Resveratrol isoforms and conjugates: A review from biosynthesis in plants to elimination from the human body
Authors: Riccio Bruno V. F. , Spósito Larissa , Carvalho Gabriela C. , Ferrari Priscileila C. , Chorilli Marlus 
Published: September 2020

AbstractThe natural isomers of resveratrol, cis‐ and trans‐resveratrol, are natural phenolic substances synthetized via the shikimate pathway and found in many sources, including grapes, peanuts, blackberries, pistachios, cacao, cranberries, and jackfruits. They have functional and pharmacological properties such as anticarcinogenic, antidiabetic, anti‐inflammatory, and cardioprotective activities. The aim of this article is to review the data published on resveratrol and its isomers, and their biosynthesis in plants, food sources, health and toxic effects, and the excretion of their metabolites. Due to its contribution to the promotion of human health, it is convenient to gather more knowledge about its functional properties, food sources, and the interactions with the human body during the processes of eating, digestion, absorption, biotransformation, and excretion, to combine this information to improve the understanding of these substances.