bluuebunny/crossref_metadata_2025_split huggingface dataset:
Toward High‐Performance Triboelectric Nanogenerators by Engineering Interfaces at the Nanoscale: Looking into the Future Research Roadmap
Authors: Ahmed Abdelsalam , Hassan Islam , Pourrahimi Amir Masoud , Helal Ahmed S. , El‐Kady Maher F. , Khassaf Hamidreza , Kaner Richard B. 
Published: August 2020

AbstractTo meet the future need for clean and sustainable energies, there has been considerable interest in the development of triboelectric nanogenerators (TENGs) that scavenge waste mechanical energies. The performance of a TENG at the macroscale is determined by the multifaceted role of surface and interface properties at the nanoscale, whose understanding is critical for the future development of TENGs. Therefore, various protocols from the atomic to the macrolevel for fabrication and tuning of surfaces and interfaces are required to obtain the desired TENG performance. These protocols branch out into three categories: chemical engineering, physical engineering, and structural engineering. Chemical engineering is an affordable and optimal strategy for introducing more surface polarities and higher work functions for the improvement of charge transfer. Physical engineering includes the utilization of surface morphology control, and interlayer interactions, which can enhance the active interfacial area and electron transfer capacity. Structural engineering at the macroscale, which includes device and electrode design/modifications has a considerable effect on the performance of TENGs. Future challenges and promising research directions related to the construction of next‐generation TENG devices, taking into consideration “interfaces” are also presented.
Revisiting Alkaline Pretreatment of Lignocellulose: Understanding the Structural Evolution of Three Components
Authors: Zhu Yuting , Liu Jing , Lv Wei , Pi Qifeng , Zhang Xinghua , Chen Lungang , Liu Qiying , Xu Ying , Zhang Qi , Ma Longlong , Wang Chenguang 
Published: August 2020

AbstractHerein, sodium hydroxide (NaOH) pretreatment of lignocellulose is performed to investigate the structural evolution of lignin, cellulose, and hemicellulose. It is found that most of hemicellulose and part of cellulose are hydrolyzed/converted to monosaccharide, alcohols, and carboxylic acids. Over half of cellulose is stabilized because the reducing end groups of cellulose convert to stable carboxylic groups. In addition, lignin is converted to aromatic monomers (predominately vanillin and acetovanillone) with a highest yield of 6.1 wt%, along with dimers and oligomers with Mw less than 10 000 Da. According to heteronuclear single quantum coherence analysis, no common interlinkages (β‐O‐4, β‐β, β‐5, etc.) appear in lignin oligomers due to lignin fragments condensed during the alkaline pretreatment. Notably, the acidification process is also the cause of lignin condensation since high aromatic monomers yield of 15 wt% (based on original lignin in pine) is achieved by a postoxidation of alkaline solution, while few no aromatic monomers generated by using the isolated lignin oligomers. The direct oxidation of lignocellulose in alkaline solutions to aromatic monomers demonstrates the potential application of lignocellulose alkaline pretreatment for high‐value chemicals production.
Precise Control of Phase Separation Enables 12% Efficiency in All Small Molecule Solar Cells
Authors: Bin Haijun , Angunawela Indunil , Qiu Beibei , Colberts Fallon J. M. , Li Mengmeng , Dyson Matthew J. , Wienk Martijn M. , Ade Harald , Li Yongfang , Janssen René A. J. 
Published: August 2020

AbstractCompared to conjugated polymers, small‐molecule organic semiconductors present negligible batch‐to‐batch variations, but presently provide comparatively low power conversion efficiencies (PCEs) in small‐molecular organic solar cells (SM‐OSCs), mainly due to suboptimal nanomorphology. Achieving precise control of the nanomorphology remains challenging. Here, two new small‐molecular donors H13 and H14, created by fluorine and chlorine substitution of the original donor molecule H11, are presented that exhibit a similar or higher degree of crystallinity/aggregation and improved open‐circuit voltage with IDIC‐4F as acceptor. Due to kinetic and thermodynamic reasons, H13‐based blend films possess relatively unfavorable molecular packing and morphology. In contrast, annealed H14‐based blends exhibit favorable characteristics, i.e., the highest degree of aggregation with the smallest paracrystalline π–π distortions and a nanomorphology with relatively pure domains, all of which enable generating and collecting charges more efficiently. As a result, blends with H13 give a similar PCE (10.3%) as those made with H11 (10.4%), while annealed H14‐based SM‐OSCs have a significantly higher PCE (12.1%). Presently this represents the highest efficiency for SM‐OSCs using IDIC‐4F as acceptor. The results demonstrate that precise control of phase separation can be achieved by fine‐tuning the molecular structure and film formation conditions, improving PCE and providing guidance for morphology design.
Influence of water deficit and defoliation managements on post‐drought recovery and persistence of smooth bromegrass
Authors: Saeidnia Fatemeh , Majidi Mohammad Mahdi , Bakhtiari Mostafa Abdollahi , Mirlohi Aghafakhr 
Published: August 2020

AbstractIn arid and semiarid regions, successful recovery from drought may be of more economic significance than plant productivity during a dry season. This research was conducted to investigate the effects of pre‐drought irrigation and defoliation managements (seed and forage managements) on post‐drought recovery of diverse smooth bromegrass (Bromus inermis Leyss.) genotypes, and to identify growth traits associated with persistence and recovery as indices for selecting superior genotypes. Thirty‐six genotypes were field evaluated in two separate experiments of seed and forage managements during 2013–2015 under well‐watered and deficit irrigation regimes. In the fourth year (2016), irrigation was withheld from both moisture regimes for two months (almost complete senescence) and then plants were re‐watered to find the effect of prolonged drought stress on post‐drought recovery. Pre‐drought irrigation increased persistence of genotypes relative to the well‐watered treatment in the seed management experiment. In the seed management trial, genotypes had greater recovery under deficit irrigation when compared to forage management counterpart. There was no significant difference between seed and forage management experiments under the well‐watered regime in this respect. Positive correlations were observed between recovery after prolonged drought and total aerial biomass, persistence, and winter growth vigor under both irrigation regimes. Superior genotypes were identified as having more productivity, better recovery, higher persistence, and drought tolerance.
Microcephalic osteodysplastic primordial dwarfism type II and pachygyria: Morphometric analysis in a 2‐year‐old girl
Authors: Rossi‐Espagnet Maria C. , Dentici Maria L. , Pasquini Luca , Carducci Chiara , Lucignani Martina , Longo Daniela , Agolini Emanuele , Novelli Antonio , Gonfiantini Michaela V. , Digilio Maria C. , Napolitano Antonio , Bartuli Andrea 
Published: August 2020

AbstractMicrocephalic osteodysplastic primordial dwarfism (MOPD) type II is a rare disorder characterized by skeletal dysplasia, severe proportionate short stature, insulin resistance and cerebrovascular abnormalities including cerebral aneurysms and moyamoya disease. MOPD type II is caused by mutations in the pericentrin (PCNT) gene, which encodes a protein involved in centrosomes function. We report a 2 year old girl affected by MOPD type II caused by two compound heterozygous loss‐of‐function variants in PCNT gene, of which one is a novel variant (c.5304delT; p.Gly1769AlafsTer34). The patient presented atypical brain magnetic resonance imaging (MRI) findings consistent with pachygyria. This was confirmed by morphometric analysis of cortical thickness (CT) and gyrification index by comparing MRI data of the patient with a group of eight age‐matched healthy controls. The statistical analysis revealed a significant and diffuse increase of CT with an anterior‐predominant pattern and diffuse reduced gyrification (p < .05). These findings provide new evidences to the emergent concept that malformations of cortical development are complex disorders and that new genetic findings contribute to the fading of classification borders.
Early life stress and HPA axis function independently predict adult depressive symptoms in metropolitan Cebu, Philippines
Authors: Kim Andrew Wooyoung , Adam Emma K. , Bechayda Sonny A. , Kuzawa Christopher W. 
Published: August 2020

AbstractObjectivesAlterations in adult hypothalamic–pituitary–adrenal (HPA) axis activity have increasingly been linked with early life stress and adult depression, but a limited number of studies have used longitudinal data to explore HPA axis dysregulation as an underlying mechanism driving the long‐term depressive impacts of early stressors. Here we address potential long‐term impacts of early life, family‐based stress on depressive symptoms among young adults in a longitudinal birth cohort study begun in 1983 in the Philippines.Materials and methodsWe relate a composite measure of family‐based stressors experienced between birth and adolescence to circadian dynamics in adult salivary cortisol and depressive risk measured at 21–22 years of age. Multiple regression analyses were conducted to examine the relationship between early life stress levels and risk of adult depressive symptoms, as well as the role of adult diurnal cortisol activity in this relationship.ResultsGreater levels of early life familial stress predicted more severe depressive symptomatology at age 21–22 in a dose–response fashion (p < .0001) independent of adult diurnal cortisol patterns. Flatter diurnal cortisol slopes are directly associated with higher adult depressive symptoms, an effect mostly driven by evening cortisol levels (p = .004). When considering the cumulative effects of early life stress measures, however, exposure to more of these stressors during development is associated with even higher depressive symptoms.DiscussionThe long‐term depressive effects of early life familial stress extend to this large sample of Cebuano young adults, and early life stress and HPA axis function may shape adult depressive symptoms through independent pathways in this sample. Our findings provide further evidence that HPA axis activity is shaped by early life conditions and is associated with depressive symptoms.
SERS‐Active MIL‐100(Fe) Sensory Array for Ultrasensitive and Multiplex Detection of VOCs
Authors: Fu Jing‐Hao , Zhong Zhen , Xie Dan , Guo Yan‐Jun , Kong De‐Xuan , Zhao Zhong‐Xing , Zhao Zhen‐Xia , Li Min 
Published: August 2020

AbstractThe application of metal–organic frameworks (MOFs) as SERS‐active platforms in multiplex volatile organic compounds (VOCs) detection is still unexplored. Herein, we demonstrate that MIL‐100 (Fe) serves as an ideal SERS substrate for the detection of VOCs. The limit of detection (LOD) of MIL‐100(Fe) for toluene sensing can reach 2.5 ppm, and can be even further decreased to 0.48 ppb level when “hot spots” in between Au nanoparticles are employed onto MIL‐100 (Fe) substrate, resulting in an enhancement factor of 1010. Additionally, we show that MIL‐100(Fe) substrate has a unique “sensor array” property allowing multiplex VOCs detection, with great modifiability and expandability by doping with foreign metal elements. Finally, the MIL‐100(Fe) platform is utilized to simultaneously detect the different gaseous indicators of lung cancer with a ppm detection limit, demonstrating its high potential for early diagnosis of lung cancer in vivo.
An Acid‐Activatable Fluorescence Probe for Imaging Osteocytic Bone Resorption Activity in Deep Bone Cavities
Authors: Hashimoto Ryu , Minoshima Masafumi , Kikuta Junichi , Yari Shinya , Bull Steven D. , Ishii Masaru , Kikuchi Kazuya 
Published: August 2020

AbstractA rationally designed pH‐activatable fluorescent probe (pHocas‐RIS) has been used to measure localised pH levels in osteocytic lacunae in bone tissue. Conjugation of the moderate bone‐binding drug risedronate to a pH‐activatable BODIPY fluorophore enables the probe to penetrate osteocytic lacunae cavities that are embedded deep within the bone matrix. After injection of pHocas‐RIS, any osteocytic lacunae caused by bone‐resorbing osteocytes cause the probe to fluoresce in vivo, thus allowing imaging by intravital two‐photon excitation microscopy. This pH responsive probe enabled the visualization of the bone mineralizing activities of acid producing osteocytes in real time, thus allowing the study of their central role in remodeling the bone‐matrix in healthy and disease states.
An Integrated Microfluidic Probe for Mass Spectrometry Imaging of Biological Samples**
Authors: Li Xiangtang , Yin Ruichuan , Hu Hang , Li Yingju , Sun Xiaofei , Dey Sudhansu K. , Laskin Julia 
Published: August 2020

AbstractAmbient ionization based on liquid extraction is widely used in mass spectrometry imaging (MSI) of molecules in biological samples. The development of nanospray desorption electrospray ionization (nano‐DESI) has enabled the robust imaging of tissue sections with high spatial resolution. However, the fabrication of the nano‐DESI probe is challenging, which limits its dissemination to the broader scientific community. Herein, we describe the design and performance of an integrated microfluidic probe (iMFP) for nano‐DESI MSI. The glass iMFP, fabricated using photolithography, wet etching, and polishing, shows comparable performance to the capillary‐based nano‐DESI MSI in terms of stability and sensitivity; a spatial resolution of better than 25 μm was obtained in these first proof‐of‐principle experiments. The iMFP is easy to operate and align in front of a mass spectrometer, which will facilitate broader use of liquid‐extraction‐based MSI in biological research, drug discovery, and clinical studies.
Radical‐Cation Cascade to Aryltetralin Cyclic Ether Lignans Under Visible‐Light Photoredox Catalysis
Authors: Xiang Jia‐Chen , Wang Qian , Zhu Jieping 
Published: August 2020

AbstractThe development of concise, sustainable, and cost‐effective synthesis of aryltetralin lignans, bearing either a fused lactone or cyclic ether, is of significant medicinal importance. Reported is that in the presence of Fukuzumi's acridinium salt under blue LED irradiation, functionalized dicinnamyl ether derivatives are converted into aryltetralin cyclic ether lignans with concurrent generation of three stereocenters in good to high yields with up to 20:1 diastereoselectivity. Oxidation of an alkene to the radical cation is key to the success of this formal Diels–Alder reaction of electronically mismatched diene and dienophile. Applying this methodology, six natural products, aglacin B, aglacin C, sulabiroin A, sulabiroin B, gaultherin C, and isoshonanin, are synthesized in only two to three steps from readily available biomass‐derived monolignols. A revised structure is proposed for gaultherin C.
Direct Observation of Defect‐Aided Structural Evolution in a Nickel‐Rich Layered Cathode
Authors: Li Shuang , Yao Zhenpeng , Zheng Jianming , Fu Maosen , Cen Jiajie , Hwang Sooyeon , Jin Huile , Orlov Alexander , Gu Lin , Wang Shun , Chen Zhongwei , Su Dong 
Published: August 2020

AbstractNi‐rich LiNi1−x−yMnxCoyO2 (NMC) layered compounds are the dominant cathode for lithium ion batteries. The role of crystallographic defects on structure evolution and performance degradation during electrochemical cycling is not yet fully understood. Here, we investigated the structural evolution of a Ni‐rich NMC cathode in a solid‐state cell by in situ transmission electron microscopy. Antiphase boundary (APB) and twin boundary (TB) separating layered phases played an important role on phase change. Upon Li depletion, the APB extended across the layered structure, while Li/transition metal (TM) ion mixing in the layered phases was detected to induce the rock‐salt phase formation along the coherent TB. According to DFT calculations, Li/TM mixing and phase transition were aided by the low diffusion barriers of TM ions at planar defects. This work reveals the dynamical scenario of secondary phase evolution, helping unveil the origin of performance fading in Ni‐rich NMC.
Single Atoms of Iron on MoS2 Nanosheets for N2 Electroreduction into Ammonia
Authors: Su Hongyang , Chen Lanlan , Chen Yizhen , Si Rui , Wu Yuting , Wu Xiaonan , Geng Zhigang , Zhang Wenhua , Zeng Jie 
Published: August 2020

AbstractEfforts have been devoted to achieving a highly efficient artificial synthesis of ammonia (NH3). Reported herein is a novel Fe‐MoS2 catalyst with Fe atomically dispersed onto MoS2 nanosheets, imitating natural nitrogenase, to boost N2 electroreduction into NH3 at room temperature. The Fe‐MoS2 nanosheets exhibited a faradic efficiency of 18.8 % with a yield rate of 8.63 μg
mgcat.−1 h−1 for NH3 at −0.3 V versus the reversible hydrogen electrode. The mechanism study revealed that the electroreduction of N2 was promoted and the competing hydrogen evolution reaction was suppressed by decorating the edge sites of S in MoS2 with the atomically dispersed Fe, resulting in high catalytic performance for the electroreduction of N2 into NH3. This work provides new ideas for the design of catalysts for N2 electroreduction and strengthens the understanding about N2 activation over Mo‐based catalysts.
Hoch regioselektive Addition von allylischen Zinkhalogeniden und verschiedenen Zinkenolaten an [1.1.1]Propellan
Authors: Schwärzer Kuno , Zipse Hendrik , Karaghiosoff Konstantin , Knochel Paul 
Published: August 2020

AbstractWir berichten über eine Reihe von hoch regioselektiven Öffnungen von [1.1.1]Propellan mit verschiedenen allylischen Zinkhalogeniden, sowie mit Zinkenolaten von Ketonen, Estern und Nitrilen. Die resultierenden zinkierten Bicyclopentane (BCPs) wurden mit einer Reihe von Elektrophilen abgefangen, einschließlich Carbonsäurechloriden, Sulfonothioaten, Hydroxylaminobenzoaten, Tosylcyanid sowie Aryl‐ und Allylhalogeniden. Dadurch wurden hochfunktionalisierte BCP‐Derivate erzeugt. Die ungewöhnlich hohe Regioselektivität dieser Reaktionen wurde mittels DFT‐Berechnungen rationalisiert. Ein Bioisoster des synthetischen Opioids Pethidin wurde mit Hilfe dieser Methodik in einem Schritt in 95 % Ausbeute hergestellt.
K2Sb(P2O7)F: Cairo Pentagonal Layer with Bifunctional Genes Reveal Optical Performance
Authors: Deng Yalan , Huang Ling , Dong Xuehua , Wang Lei , Ok Kang Min , Zeng Hongmei , Lin Zhien , Zou Guohong 
Published: August 2020

AbstractDiscovering new functional genes, designing perfect crystal structures, and developing high‐performance materials are the goals being pursued by scientists. Herein, the first antimony pyrophosphate, K2Sb(P2O7)F, possessing an optimal layered structure, is reported, where the perfect structural arrangement induces excellent optical properties. K2Sb(P2O7)F not only displays a sharply enhanced birefringence (0.157@546 nm) compared to the existing phosphate optical materials, but also exhibits a strong second‐harmonic generation response (4.0×KDP). Remarkably, a new bifunctional gene, the square‐pyramidal SbO4F group, was discovered, and a unique two‐dimensional arrangement of Cairo pentagonal tiling units was observed in inorganic compounds for the first time.
Self‐Assembled Anion‐Binding Cryptand for the Selective Liquid–Liquid Extraction of Phosphate Anions
Authors: Andrews Rebecca , Begum Sabera , Clemett Christopher J. , Faulkner Robert A. , Ginger Michael L. , Harmer Jane , Molinari Marco , Parkes Gareth M. B. , Qureshi Zuhlqurnain M. H. , Rice Craig R. , Ward Michael D. , Williams Howard M. , Wilson Philippe B. 
Published: August 2020

AbstractThe ligands L1 and L2 form trinuclear self‐assembled complexes with Cu2+ (i.e. [(L1)2Cu3]6+ or [(L2)2Cu3]6+) both of which act as a host to a variety of anions. Inclusion of long aliphatic chains on these ligands allows the assemblies to extract anions from aqueous media into organic solvents. Phosphate can be removed from water efficiently and highly selectively, even in the presence of other anions.
Nanoimpacts at Active and Partially Active Electrodes: Insights and Limitations
Authors: Roehrich Brian , Sepunaru Lior 
Published: August 2020

AbstractWhile the electrochemical nanoimpact technique has recently emerged as a method of studying single entities, it is limited by requirement of a catalytically active particle impacting an inert electrode. We show that an active particle‐active electrode can provide mechanistic insight into electrochemical reactions. When an individual Pt electrocatalyst adsorbs to the surface of a partially active electrode, further reduction of electrode‐produced species can proceed on the nanocatalyst. Current transients obtained during hydrogen evolution allow simultaneous measurement of the Pt catalyst over different length scales, size dependency suggests H atom intercalation as a catalytic deactivation mechanism. Although results show that outer‐sphere redox probes are unproductive for particle characterization, the breadth of inner‐sphere electrochemical reactions makes this a promising method for understanding the properties of catalytic nanomaterials, one at a time.
A Photoaffinity‐Based Fragment‐Screening Platform for Efficient Identification of Protein Ligands
Authors: Grant Emma K. , Fallon David J. , Hann Michael M. , Fantom Ken G. M. , Quinn Chad , Zappacosta Francesca , Annan Roland S. , Chung Chun‐wa , Bamborough Paul , Dixon David P. , Stacey Peter , House David , Patel Vipulkumar K. , Tomkinson Nicholas C. O. , Bush Jacob T. 
Published: August 2020

AbstractAdvances in genomic analyses enable the identification of new proteins that are associated with disease. To validate these targets, tool molecules are required to demonstrate that a ligand can have a disease‐modifying effect. Currently, as tools are reported for only a fraction of the proteome, platforms for ligand discovery are essential to leverage insights from genomic analyses. Fragment screening offers an efficient approach to explore chemical space. Presented here is a fragment‐screening platform, termed PhABits (PhotoAffinity Bits), which utilizes a library of photoreactive fragments to covalently capture fragment–protein interactions. Hits can be profiled to determine potency and the site of crosslinking, and subsequently developed as reporters in a competitive displacement assay to identify novel hit matter. The PhABit platform is envisioned to be widely applicable to novel protein targets, identifying starting points in the development of therapeutics.
Highly Regioselective Addition of Allylic Zinc Halides and Various Zinc Enolates to [1.1.1]Propellane
Authors: Schwärzer Kuno , Zipse Hendrik , Karaghiosoff Konstantin , Knochel Paul 
Published: August 2020

AbstractWe report a range of highly regioselective openings of [1.1.1]propellane with various allylic zinc halides, as well as zinc enolates of ketones, esters and nitriles. The resulting zincated bicyclopentanes (BCPs) were trapped with a range of electrophiles including acyl chlorides, sulfonothioates, hydroxylamino benzoates, tosyl cyanide as well as aryl and allyl halides, generating highly functionalized BCP‐derivatives. The unusually high regioselectivity of these reactions has been rationalized using DFT calculations. A bioisostere of the synthetic opioid pethidine was prepared in 95 % yield in one step using this method.