bluuebunny/crossref_metadata_2025_split huggingface dataset:
Photo(electro)catalytic Nitrogen Fixation: Problems and Possibilities
Authors: Vu Manh‐Hiep , Sakar Mohan , Hassanzadeh‐Tabrizi Sayed Ali , Do Trong‐On 
Published: May 2019

AbstractPhoto(electro)catalytic nitrogen fixation is considered as a competing alternative for the Haber–Bosch (HB) process due to the direct production of ammonia (NH3) from nitrogen and water with zero carbon dioxide emission, which has made it a very hot research topic in recent years. Particularly, photo‐driven nitrogen reduction has been attracted to a specific focus in the scientific community since it can be powered by limitless solar energy at ambient conditions. However, unsolved challenges have remained to date such as, electron–hole separation, low quantum efficiency, weak visible light harvesting, catalytic selectivity, N2 adsorption, and activation. In this Review, the recent achievements and related approaches toward nitrogen fixation are presented. In addition, the discussions on mechanistic photofixation of nitrogen, catalytic engineering design, and the outlook for enhancing the photocatalytic performance of ammonia photosynthesis are also devoted. Finally, the emerging trend of advanced photo(electro)catalysts for nitrogen fixation is proposed.
Mussel‐Glue Inspired Adhesives: A Study on the Relevance of l‐Dopa and the Function of the Sequence at Nanomaterial‐Peptide Interfaces
Authors: Venkatareddy Narendra L. , Wilke Patrick , Ernst Natalia , Horsch Justus , Weber Marcus , Dallmann Andre , Börner Hans G. 
Published: May 2019

AbstractMussel glue‐proteins undergo structural transitions at material interfaces to optimize adhesive surface contacts. Those intriguing structure responses are mimicked by a mussel‐glue mimetic peptide (HSY*SGWSPY*RSG (Y* = l‐Dopa)) that was previously selected by phage‐display to adhere to Al2O3 after enzymatic activation. Molecular level insights into the full‐length adhesion domain at Al2O3 surfaces are provided by a divergent‐convergent analysis, combining nuclear Overhauser enhancement based 2D NOESY and saturation transfer difference NMR analysis of submotifs along with molecular dynamics simulations of the full‐length peptide. The peptide is divided into two submotifs, each containing one Dopa “anchor” (Motif‐1 and 2). The analysis proves Motif‐1 to constitute a dynamic Al2O3 binder and adopting an “M”‐structure with multiple surface contacts. Motif‐2 binds stronger by two surface contacts, forming a compact “C”‐structure. Taking these datasets as constraints enables to predict the structure and propose a binding process model of the full‐length peptide adhering to Al2O3.
Catalyst‐Free and Morphology‐Controlled Growth of 2D Perovskite Nanowires for Polarized Light Detection
Authors: Ghoshal Debjit , Wang Tianmeng , Tsai Hsin‐Zon , Chang Shao‐Wen , Crommie Michael , Koratkar Nikhil , Shi Su‐Fei 
Published: May 2019

AbstractRuddleson–Popper (RP) perovskites have emerged as a class of material inheriting the superior optoelectronic properties of two materials: perovskites and 2D materials. The large exciton binding energy and natural quantum well structure not only make these materials ideal platforms to study light–matter interactions but also render them suitable for fabrication of various functional optoelectronic devices. Nanoscale structuring and morphology control have led to semiconductors with enhanced functionalities. Nanowires of semiconducting materials are extensively used for important applications like lasing and sensing. However, catalyst and template‐free scalable growth of nanowires of 2D perovskites has remained elusive. In this paper, a facile approach for morphology‐controlled growth of nanowires of 2D perovskite, (BA)2PbI4, is demonstrated. Additionally, it is shown that the photoluminescence (PL) from the nanowires is highly polarized with a polarization ratio as large as ≈0.73, which is one of the largest reported for perovskites. It is further shown that the photocurrent from the hybrid nanowire/graphene device is also sensitive to the polarization of the incident light with the photocurrent anisotropy ratio of ≈3.62 (much larger than the previously reported value of 2.68 for perovskites), thus demonstrating the potential of these nanowires as highly efficient photodetectors for polarized light.
A Highly Sensitive Perovskite/Organic Semiconductor Heterojunction Phototransistor and Its Device Optimization Utilizing the Selective Electron Trapping Effect
Authors: Luo Lin‐Bao , Wu Guo‐An , Gao Yang , Liang Lin , Xie Chao , Zhang Zhi‐Xiang , Tong Xiao‐Wei , Wang Tao , Liang Feng‐Xia 
Published: May 2019

AbstractHybrid organic–inorganic perovskite materials have recently attracted attention due to their impressive physical properties and promising application in future optoelectronic devices and systems. In this study, a high‐performance and broadband photodetector comprising vertically stacked Cs‐doped formanidinium lead iodide (FAPbI3) perovskite/dinaphtho[2,3‐b:2′,3′‐f]thieno[3,2‐b]thiophene heterojunction, which shows a high responsivity of 778 A W−1 and a specific detectivity of 1.04 × 1013 Jones, is reported. In addition, the photodetector displays excellent stability and broadband responsivity to illumination ranging from deep‐ultraviolet to near‐infrared light. It is interesting to note that doping a small amount of [6,6]‐phenyl‐C61‐butyric acid methyl ester (PCBM) into the perovskite film results in a substantial increase in responsivity, specific detectivity, and photoconductive gain. Specifically, the specific detectivity is as high as 7.96 × 1013 Jones, which is much higher than that of other devices with similar geometries. The device optimization can be ascribed to an enhanced electron–hole separation ability and increase in electron accepting sites that can selectively trap electrons in the perovskite–PCBM bulk heterojunction, according to results from the experimental analyses.
Momentum‐Resolved Surface Enhanced Raman Scattering from a Nanowire–Nanoparticle Junction Cavity
Authors: Vasista Adarsh B. , Chaubey Shailendra K. , Gosztola David J. , Wiederrecht Gary P. , Gray Stephen K. , Kumar G. V. Pavan 
Published: May 2019

AbstractHerein experimental evidence of directional surface enhanced Raman scattering from molecules situated inside a single nanowire–nanoparticle junction cavity is reported. The emission is confined to a narrow range of wavevectors perpendicular to the axis of the cavity. In addition to this, the molecules excite multiple guided modes of the nanowire which are imaged using leakage radiation Fourier microscopy. The emission wavevectors are further characterized as a function of output polarization. The excited guided modes of the wire show interesting polarization signatures. All the results are corroborated using finite element method based numerical simulations. Essentially, an important connection between gap‐cavity enhanced Raman scattering and its directionality of emission is provided. The results may be of relevance in understanding the cavity electrodynamics at the nanoscale and molecular coupling to extremely small gaps between a 1D and a 0D plasmonic nanostructure.
Boron Nanosheets for Efficient All‐Optical Modulation and Logic Operation
Authors: Guo Qiangbing , Wu Kan , Shao Zhengpeng , Basore Endale T. , Jiang Peng , Qiu Jianrong 
Published: May 2019

AbstractDue to its unique trivalent electronic configuration, boron features richer properties as well as higher chemical and structural complexities compared with its right neighbor carbon. Consequently, over a decade later than the exfoliation of graphene, borophene has just been experimentally demonstrated on certain metal substrates and under ultrahigh‐vacuum conditions, which, however, limit its wide and in‐depth experimental researches. Here, for the first time, by employing liquid‐exfoliated boron nanosheets, all‐optical signal processing application is explored based on its superior photo‐thermal response. A stable all‐optical modulator is presented, which shows significantly faster response speed and higher modulation efficiency compared with other 2D materials‐based similar devices. Furthermore, boron nanosheets‐based all‐optical logic gating operations are also demonstrated. This work not only presents an excellent 2D material‐based all‐optical signal processing device, but also marks a significant step toward optical and photonic researches as well as device applications of 2D boron.
CsPbBr3‐Quantum‐Dots/Polystyrene@Silica Hybrid Microsphere Structures with Significantly Improved Stability for White LEDs
Authors: Yang Weiqiang , Gao Fei , Qiu Yue , Liu Weizhen , Xu Haiyang , Yang Lili , Liu Yichun 
Published: May 2019

AbstractCesium‐lead‐halide perovskite quantum dots (PQDs), which have superior optical and electronic properties, are regarded as excellent materials for various optoelectronic devices. However, their unstable nature greatly hinders their practical application. Herein, a simple hydrolysis encapsulation method is developed to embed PQDs into mesoporous polystyrene microspheres (MPMs) followed by a silica shell covering process, which generates luminescent PQDs/MPMs@SiO2 hybrid microspheres with significantly enhanced stability. The obtained CsPbBr3‐PQDs/MPMs@SiO2 hybrid microspheres show a high photoluminescence quantum yield of 84%. More importantly, the MPMs@silica protective shells effectively cut off direct contact between outer erosive species and the inner embedded PQDs and modify the hybrid microspheres with ultralong alkyl chains for improved resistance to solvents and heat. Hence, these CsPbBr3‐PQDs/MPMs@SiO2 hybrid microspheres exhibit good chemical/physical stabilities, even when exposed to harsh environments, such as deionized water, isopropanol, acid/alkali solution, anion‐exchange reactions, and heating. Particularly, the water stability, which produced the remaining ≈48% proportion of the initial fluorescence intensity after a quite long aqueous storage period of 30 d, is the best reported among the stability‐related studies of PQDs. Meanwhile, white light‐emitting diodes (LEDs) are achieved by mixing green CsPbBr3‐PQDs/MPMs@SiO2 microspheres with red commercial phosphors on a blue chip. High power efficiency of 81 lm W−1 and good electroluminescence stability are obtained.
Stress‐Induced 3D Chiral Fractal Metasurface for Enhanced and Stabilized Broadband Near‐Field Optical Chirality
Authors: Tseng Ming Lun , Lin Zhan‐Hong , Kuo Hsin Yu , Huang Tzu‐Ting , Huang Yi‐Teng , Chung Tsung Lin , Chu Cheng Hung , Huang Jer‐Shing , Tsai Din Ping 
Published: May 2019

AbstractMetasurfaces comprising 3D chiral structures have shown great potential in chiroptical applications such as chiral optical components and sensing. So far, the main challenges lie in the nanofabrication and the limited operational bandwidth. Homogeneous and localized broadband near‐field optical chirality enhancement has not been achieved. Here, an effective nanofabrication method to create a 3D chiral metasurface with far‐ and near‐field broadband chiroptical properties is demonstrated. A focused ion beam is used to cut and stretch nanowires into 3D Archimedean spirals from stacked films. The 3D Archimedean spiral is a self‐similar chiral fractal structure sensitive to the chirality of light. The spiral exhibits far‐ and near‐field broadband chiroptical responses from 2 to 8 µm. With circularly polarized light (CPL), the spiral shows superior far‐field transmission dissymmetry and handedness‐dependent near‐field localization. With linearly polarized excitation, homogeneous and highly enhanced broadband near‐field optical chirality is generated at a stably localized position inside the spiral. The effective yet straightforward fabrication strategy allows easy fabrication of 3D chiral structures with superior broadband far‐field chiroptical response as well as strongly enhanced and stably localized broadband near‐field optical chirality. The reported method and chiral metasurface may find applications in broadband chiral optics and chiral sensing.
Biocatalysis: A Pharma Perspective
Authors: Adams Joseph P. , Brown Murray J. B. , Diaz‐Rodriguez Alba , Lloyd Richard C. , Roiban Gheorghe‐Doru 
Published: May 2019

AbstractBiocatalysis over the past few years has matured into an essential tool for modern, cost effective and sustainable pharmaceutical manufacturing. While some reaction classes are well established, and may even be the option of first intent, other more recently discovered enzyme classes are being rapidly developed both in academia and industry. Notwithstanding this, there are further promising enzymes that require further investment and investigation to allow their future industrial use. We here outline GSK's perspective on the current status of biocatalysis for pharmaceutical manufacturing and provide our views on areas of significant potential.magnified image
Ambipolarity and Air Stability of Silicon Phthalocyanine Organic Thin‐Film Transistors
Authors: Melville Owen A. , Grant Trevor M. , Mirka Brendan , Boileau Nicholas T. , Park Jeongwon , Lessard Benoît H. 
Published: May 2019

AbstractSilicon phthalocyanines (SiPcs) are a class of conjugated, planar molecule that have recently been investigated for use in organic photovoltaics (OPVs), organic light‐emitting diodes (OLEDs), and organic thin‐film transistors (OTFTs) due to their variable structure and ease of synthesis. Bottom‐gate, bottom‐contact OTFTs with four SiPc derivatives used as the semiconducting layers are prepared using physical vapor deposition. Devices using bis(pentafluorophenoxy) silicon phthalocyanine (F10‐SiPc) deposited on 140 °C substrates demonstrate electron field‐effect mobilities (μ) of up to 0.54 cm2 V−1 s−1, among the best currently reported for N‐type phthalocyanine‐based transistors. All materials show dramatic changes in charge transport when characterized under vacuum (P < 0.1 Pa) compared to in air at atmospheric pressure, typically switching from electron majority charge carriers to holes, with the change dependent on material structure and energetics. F10‐SiPc is close to balanced ambipolar in air, with μ around 5 × 10−3 cm2 V−1 s−1 for both holes and electrons. These results demonstrate SiPcs' potential as N‐type semiconductors in OTFTs as well as their adjustable charge transport as affected by operation environment.
Enhanced yeast surface display of β‐glucuronidase using dual anchor motifs for high‐temperature glycyrrhizin hydrolysis
Authors: Wang Xudong , Feng Xudong , Lv Bo , Zhou Anqi , Hou Yuhui , Li Chun 
Published: May 2019

Abstractβ‐Glucuronidases (GUSs) have been widely used for the modification of natural glucuronide compounds, but the low reusability and stability of GUSs have limited their large‐scale use. In this study, PGUS (GUS from Aspergillus oryzae) and AtGUS (GUS from Aspergillus terreus) were independently displayed on the surface of Pichia pastoris via the Pir1 or Agα1 anchoring motif for the efficient preparation of glycyrrhetinic acid (GA) using glycyrrhizin (GL) hydrolysis. The PGUS displayed using Pir1 had 35‐fold increased activity than free PGUS. The displayed PGUS also exhibited 6.92‐fold higher thermostability at 70°C than free PGUS and retained 75% activity after 10 consecutive runs. Furthermore, the activity of displayed PGUS was increased by 1.44‐fold by using the dual complementary anchoring motifs Agα1 and Pir1. A new GL biotransformation process at elevated temperature (60°C) was designed with the displayed PGUS that shows considerable potential for use in the industrial production of GA.
Clinical and molecular spectrum of CHOPS syndrome
Authors: Raible Sarah E. , Mehta Devanshi , Bettale Chiara , Fiordaliso Sarah , Kaur Maninder , Medne Livija , Rio Marlene , Haan Eric , White Susan M. , Cusmano‐Ozog Kristina , Nishi Eriko , Guo Yiran , Wu Honglin , Shi Xiaoqing , Zhao Qingjie , Zhang Xueqin , Lei Qi , Lu Aimei , He Xiyu , Okamoto Nobuhiko , Miyake Noriko , Piccione Joseph , Allen Julian , Matsumoto Naomichi , Pipan Mary , Krantz Ian D. , Izumi Kosuke 
Published: May 2019

AbstractCHOPS syndrome is a multisystem disorder caused by missense mutations in AFF4. Previously, we reported three individuals whose primary phenotype included cognitive impairment and coarse facies, heart defects, obesity, pulmonary involvement, and short stature. This syndrome overlaps phenotypically with Cornelia de Lange syndrome, but presents distinct differences including facial features, pulmonary involvement, and obesity. Here, we provide clinical descriptions of an additional eight individuals with CHOPS syndrome, as well as neurocognitive analysis of three individuals. All 11 individuals presented with features reminiscent of Cornelia de Lange syndrome such as synophrys, upturned nasal tip, arched eyebrows, and long eyelashes. All 11 individuals had short stature and obesity. Congenital heart disease and pulmonary involvement were common, and those were seen in about 70% of individuals with CHOPS syndrome. Skeletal abnormalities are also common, and those include abnormal shape of vertebral bodies, hypoplastic long bones, and low bone mineral density. Our observation indicates that obesity, pulmonary involvement, skeletal findings are the most notable features distinguishing CHOPS syndrome from Cornelia de Lange syndrome. In fact, two out of eight of our newly identified patients were found to have AFF4 mutations by targeted AFF4 mutational analysis rather than exome sequencing. These phenotypic findings establish CHOPS syndrome as a distinct, clinically recognizable disorder. Additionally, we report three novel missense mutations causative for CHOPS syndrome that lie within the highly conserved, 14 amino acid sequence of the ALF homology domain of the AFF4 gene, emphasizing the critical functional role of this region in human development.
SLC18A3 variants lead to fetal akinesia deformation sequence early in pregnancy
Authors: Hakonen Anna H. , Polvi Anne , Saloranta Carola , Paetau Anders , Heikkilä Päivi , Almusa Henrikki , Ellonen Pekka , Jakkula Eveliina , Saarela Janna , Aittomäki Kristiina 
Published: May 2019

AbstractFetal akinesia deformation sequence (FADS) and lethal multiple pterygium syndrome (LMPS) are clinically overlapping syndromes manifesting with reduced or absent fetal movement, arthrogryposis, and several anomalies during fetal life. The etiology of these syndromes is heterogeneous, and in many cases it remains unknown. In order to determine the genetic etiology of FADS in two fetuses with fetal akinesia, arthrogryposis, edema, and partial cleft palate, we utilized exome sequencing. Our investigations revealed a homozygous nonsense variant [c.1116C>A, p.(Cys372Ter)] in the SLC18A3 gene, which encodes for the vesicular acetylcholine transporter (VAChT) responsible for active transport of acetylcholine in the neuromuscular junction. This is the first description of a nonsense variant in the SLC18A3 gene, as only missense variants and whole gene deletions have been previously identified in patients. The previously detected SLC18A3 defects have been associated with congenital myasthenic syndromes, and therefore our findings extend the clinical spectrum of SLC18A3 defects to severe prenatal phenotypes. Our findings suggest that nonsense variants in SLC18A3 cause a more severe phenotype than missense variants and are in line with previous studies showing a lethal phenotype in VAChT knockout mice. Our results underline the importance of including SLC18A3 sequencing in the differential diagnostics of fetuses with arthrogryposis, FADS, or LMPS of unknown etiology.
Synthetische Analoga zeigen die essentiellen Strukturmotive von Lugdunin und seinen Protonentransport
Authors: Schilling Nadine A. , Berscheid Anne , Schumacher Johannes , Saur Julian S. , Konnerth Martin C. , Wirtz Sebastian N. , Beltrán‐Beleña José M. , Zipperer Alexander , Krismer Bernhard , Peschel Andreas , Kalbacher Hubert , Brötz‐Oesterhelt Heike , Steinem Claudia , Grond Stephanie 
Published: May 2019

AbstractLugdunin, ein neues Thiazolidin‐Cyclopeptid, weist gegenüber Methicillin‐resistentem Staphylococcus aureus (MRSA) antimikrobielle Wirkung im mikromolaren Bereich auf. Für die Untersuchung von Struktur‐Aktivitätsbeziehungen (SAR) wurden synthetische Alanin‐ und Stereo‐Derivate sowie Peptide mit modifiziertem Thiazolidinring auf ihre antimikrobielle Aktivität getestet. Sowohl das Thiazolidin als auch die d‐, l‐alternierende Konfiguration stellen essentielle Strukturmotive dar. Bemerkenswert ist die identische Aktivität des Enantiomers, was eine stereospezifische Wechselwirkung mit einem Zielmolekül ausschließt. Die antibakterielle Wirkung korreliert stark mit dem Einbrechen des Membranpotentials von S. aureus. Lugdunin gleicht pH‐Gradienten in künstlichen Membranvesikeln unter Erhalt der Membranintegrität aus. Der Wirkmechanismus (MoA) beruht somit auf Protonentransport. Der Einbau eines zusätzlichen Tryptophans oder einer Propargylfunktion erweitert die Diversität dieser neuen Substanzklasse der Thiazolidin‐Cyclopeptide.
Rapid Detection of Exosomal MicroRNAs Using Virus‐Mimicking Fusogenic Vesicles
Authors: Gao Xihui , Li Sha , Ding Fei , Fan Hongjia , Shi Leilei , Zhu Lijuan , Li Jing , Feng Jing , Zhu Xinyuan , Zhang Chuan 
Published: May 2019

AbstractExosomal microRNAs (miRNAs) are important biomarkers for clinical diagnosis and disease treatment monitoring. However, most approaches for exosomal miRNA detection are time‐consuming, laborious, and expensive. Herein, we report a virus‐mimicking fusogenic vesicle (Vir‐FV) that enables rapid, efficient, and high‐throughput detection of exosomal miRNAs within 2 h. Fusogenic proteins on Vir‐FVs can specifically target the sialic‐acid‐containing receptors on exosomes, inducing efficient fusion of Vir‐FVs and exosomes. Upon vesicle content mixing, the molecular beacons encapsulated in Vir‐FVs specifically hybridize with the target miRNAs in the exosomes, generating fluorescence. Combined with flow cytometry, the Vir‐FVs can not only detect exosomal miRNAs but also distinguish tumor exosomes from normal exosomes by sensing the tumor‐related miRNAs, paving the way towards the rapid and efficient detection of exosomal miRNAs for diagnosis and prognosis prediction of diseases.
π–π Interactions Between Aromatic Groups in Amphiphilic Molecules: Directing Hierarchical Growth of Porous Zeolites
Authors: Zhang Yunjuan , Che Shunai 
Published: May 2019

AbstractThe development of hierarchical macro‐ or mesoporous zeolites is essential in zeolite synthesis because the size of the micropores limits mass transport and their use as industrial catalysts for bulky molecules. Although major breakthroughs have been achieved, fabricating crystallographically ordered mesoporous zeolites using a templating strategy is still an unsolved challenge. This minireview highlights our recent efforts on the self‐assembly of amphiphilic molecules to obtain ordered hierarchical MFI zeolites by introducing aromatic groups into the hydrophobic tail of the amphiphilic molecules. Owing to the geometric matching between the self‐assembled aromatic tails and the MFI framework, a) single‐crystalline mesostructured zeolite nanosheets (SCZNs), b) SCZNs with a 90° rotational intergrowth structure, c) a hierarchical MFI zeolite with a two‐dimensional square P4mm mesostructure, and d) a single‐crystalline mesoporous ZSM‐5 with three‐dimensional pores and sheetlike mesopores layered along the a‐axis were successfully synthesized.