bluuebunny/crossref_metadata_2025_split huggingface dataset:
Additive‐Controlled Switchable Selectivity from Cyanobenzenes to 2‐Alkynylpyridines: Ruthenium(II)‐Catalyzed [2+2+2] Cycloadditions of Diynes and Alkynylnitriles
Authors: Bhatt Divya , Patel Neha , Chowdhury Hrishikesh , Bharatam Prasad V. , Goswami Avijit 
Published: March 2018

AbstractA highly efficient additive‐dependent chemoselective protocol for the synthesis of fused cyanoarenes and 2‐alkynylpyridines has been developed by the reaction of 1,6‐diynes with alkynylnitriles using chloro(pentamethylcyclopentadienyl) (cyclooctadiyne)ruthenium(II) as catalyst in dimethoxyethane (DME). The course of the reaction can be drastically altered simply by adding a catalytic amount of AgOTf as an additive resulting in a comprehensive shift in product formation from cyanoarenes to 2‐alkynylpyridines. Theoretical studies clearly indicate that the neutral Ru‐complex is responsible for the formation of cyanobenzenes, whereas the in situ generated cationic Ru‐complex plays a crucial role in the 2‐alkynylpyridines formation.magnified image
Trojan‐Horse‐Like Stimuli‐Responsive Microcapsules
Authors: Mou Chuan‐Lin , Wang Wei , Li Zhi‐Lu , Ju Xiao‐Jie , Xie Rui , Deng Nan‐Nan , Wei Jie , Liu Zhuang , Chu Liang‐Yin 
Published: March 2018

AbstractMulticompartment microcapsules, with each compartment protected by a distinct stimuli‐responsive shell for versatile controlled release, are highly desired for developing new‐generation microcarriers. Although many multicompartmental microcapsules have been created, most cannot combine different release styles to achieve flexible programmed sequential release. Here, one‐step template synthesis of controllable Trojan‐horse‐like stimuli‐responsive microcapsules is reported with capsule‐in‐capsule structures from microfluidic quadruple emulsions for diverse programmed sequential release. The nested inner and outer capsule compartments can separately encapsulate different contents, while their two stimuli‐responsive hydrogel shells can individually control the content release from each capsule compartment for versatile sequential release. This is demonstrated by using three types of Trojan‐horse‐like stimuli‐responsive microcapsules, with different combinations of release styles for flexible programmed sequential release. The proposed microcapsules provide novel advanced candidates for developing new‐generation microcarriers for diverse, efficient applications.
A High‐Speed and Low‐Power Multistate Memory Based on Multiferroic Tunnel Junctions
Authors: Huang Weichuan , Zhao Wenbo , Luo Zhen , Yin Yuewei , Lin Yue , Hou Chuangming , Tian Bobo , Duan Chun‐Gang , Li Xiao‐Guang 
Published: March 2018

AbstractFerroic‐order‐based devices are emerging as alternatives to high density, high switching speed, and low‐power memories. Here, multi‐nonvolatile resistive states with a switching speed of 6 ns and a write current density of about 3 × 103 A cm−2 are demonstrated in crossbar‐structured memories based on all‐oxide La0.7Sr0.3MnO3/BaTiO3/La0.7Sr0.3MnO3 multiferroic tunnel junctions. The tunneling resistive switching as a function of voltage pulse duration time, associated with the ferroelectric domain reversal dynamics, is ruled by the Kolmogorov–Avrami–Ishibashi switching model with a Lorentzian distribution of characteristic switching time. It is found that the characteristic resistance switching time decreases with increasing voltage pulse amplitude following Merz's law and the estimated write speed can be less than 6 ns at a relatively higher voltage. These findings highlight the potential application of multiferroic devices in high speed, low power, and high‐density memories.
A Graphene‐Based Filament Transistor with Sub‐10 mVdec−1 Subthreshold Swing
Authors: Tian He , Wang Xuefeng , Zhao Haiming , Mi Wentian , Yang Yi , Chiu Po‐Wen , Ren Tian‐Ling 
Published: March 2018

AbstractThere is a growing trend of developing steep slope transistors with subthreshold swing (SS) below 60 mV dec−1. At present, there are mainly three kinds of steep slope transistors: tunneling transistor, negative capacitance transistor, and nano‐electromechanical relay. Here, a new kind of steep slope transistor named “filament transistor” is proposed with SS down to sub‐10 mV dec−1. Due to the gate E‐filed can penetrate through the graphene, the gate can effectively control the filament formation/rupture inside the 5 nm AlOx with very steep slope. In reverse sweep, the gate can induce the filament formation with SS down to 4.6 mV dec−1. In forward sweep, the gate can break the filament with SS down to 12.2 mV dec−1. Taking the advantages of nanofilament, the filament transistor holds a great potential to scaling down to 5 nm without performance changing.
Interphases in Sodium‐Ion Batteries
Authors: Song Junhua , Xiao Biwei , Lin Yuehe , Xu Kang , Li Xiaolin 
Published: March 2018

AbstractSodium‐ion batteries (SIBs) as economical, high energy alternatives to lithium‐ion batteries (LIBs) have received significant attention for large‐scale energy storage in the last few years. While the efforts of developing SIBs have benefited from the knowledge learned in LIBs, thanks to the apparent proximity between Na‐ions and Li‐ions, the unique physical and chemical properties of Na‐ions also distinctly differ themselves from Li‐ions. It is expected that SIBs have drastically different electrode material structure, solvation–desolvation behavior, electrode–electrolyte interphase stabilities, ion transfer properties, and hence electrochemical performance of batteries. In this review, the authors comprehensively summarize the current understanding of the anode solid electrolyte interphase and cathode electrolyte interphase in SIBs, with an emphasis on how the tuning of the stability and ion transfer properties of interphases fundamentally determines the reversibility and efficiency of electrochemical reactions. Through these carefully screened references, the authors intend to reveal the intrinsic correlation between the properties/functionalities of the interphases and the electrochemical performance of batteries.
Thermodynamically Self‐Healing 1D–3D Hybrid Perovskite Solar Cells
Authors: Fan Jiandong , Ma Yunping , Zhang Cuiling , Liu Chong , Li Wenzhe , Schropp Ruud E. I. , Mai Yaohua 
Published: March 2018

AbstractThermal degradation in perovskite solar cells is still an unsettled issue that limits its further development. In this study, 2‐(1H‐pyrazol‐1‐yl)pyridine is introduced into lead halide 3D perovskites, which allows 1D–3D hybrid perovskite materials to be obtained. The heterostructural 1D–3D perovskites are proved to be capable of remarkably prolonging the photoluminescence decay lifetime and suppressing charge carrier recombination in comparison to conventional 3D perovskites. The intrinsic properties of thermodynamically stable yet kinetically labile 1D materials allow the system to alleviate the lattice mismatch and passivate the interface traps of heterojunction region of 1D–3D hybrid perovskites that may occur during the crystal growth process. Importantly, the as‐fabricated 1D–3D perovskite solar cells display a thermodynamic self‐healing ability, which is induced through blocking the ion‐migration channels of A‐site ions by the flexible 1D perovskite with less densely close‐packed structure. Particularly, the power conversion efficiency of as‐fabricated unencapsulated 1D–3D perovskite solar cells is demonstrated to be reversible under temperature cycling (25–85 °C) at 55% relative humidity, which largely outperforms the pure 3D perovskite solar cell. The present study provides a facile approach to fabricate 1D–3D perovskite solar cells with high efficiency and long‐term stability.
Exceptionally Enhanced Electrode Activity of (Pr,Ce)O2−δ‐Based Cathodes for Thin‐Film Solid Oxide Fuel Cells
Authors: Seo Han Gil , Choi Yoonseok , Jung WooChul 
Published: March 2018

AbstractIt is shown that an electrochemically‐driven oxide overcoating substantially improves the performance of metal electrodes in high‐temperature electrochemical applications. As a case study, Pt thin films are overcoated with (Pr,Ce)O2−δ (PCO) by means of a cathodic electrochemical deposition process that produces nanostructured oxide layers with a high specific surface area and uniform metal coverage and then the coated films are examined as an O2‐electrode for thin‐film‐based solid oxide fuel cells. The combination of excellent conductivity, reactivity, and durability of PCO dramatically improves the oxygen reduction reaction rate while maintaining the nanoscale architecture of PCO layers and thus the performance of the PCO‐coated Pt thin‐film electrodes at high temperatures. As a result, with an oxide coating step lasting only 5 min, the electrode resistance is successfully reduced by more than 1000 times at 500 °C in air. These observations provide a new direction for the design of high‐performance electrodes for high‐temperature electrochemical cells.
Exceptionally High Performance Anode Material Based on Lattice Structure Decorated Double Perovskite Sr2FeMo2/3Mg1/3O6−δ for Solid Oxide Fuel Cells
Authors: Du Zhihong , Zhao Hailei , Li Shanming , Zhang Yang , Chang Xiwang , Xia Qing , Chen Ning , Gu Lin , Świerczek Konrad , Li Yan , Yang Tianrang , An Ke 
Published: March 2018

AbstractA novel double perovskite Sr2FeMo2/3Mg1/3O6−δ is prepared and characterized as an anode material for solid oxide fuel cells (SOFCs). X‐ray diffraction refinement reveals that Mg and Mo cations locate separately in two different B sites (B and B′ in A2BB′O6) while Fe occupies both B and B′ sites, forming the lattice structure with the form of Sr2(Mg1/3Fe2/3)(Mo2/3Fe1/3)O6−δ. The inactive element Mg doping not only endows the material with excellent redox structural stability but also triggers the creation of antisite defects in the crystal lattice, which provide the material with excellent electrochemical activity. The anode performance of Sr2FeMo2/3Mg1/3O6−δ is characterized in an La0.8Sr0.2Ga0.8Mg0.2O3−δ electrolyte supported cell with La0.58Sr0.4Fe0.8Co0.2O3−δ cathode. A peak power density of 531, 803, 1038, and 1316 mW cm−2 at 750, 800, 850, and 900 °C, respectively, is achieved in humidified H2. The Sr2FeMo2/3Mg1/3O6−δ shows suitable thermal expansion coefficient (16.9(2) × 10−6 K−1), high electrical conductivity, and good tolerance to carbon deposition and sulfur poisoning. First‐principle computations demonstrate that the presence of FeBOFeB′ bonds can promote the easy formation and fast migration of oxygen vacancies in the lattice, which are the key to affecting the anode reaction kinetics. The excellent overall performance of Sr2FeMo2/3Mg1/3O6−δ compound makes it a promising anode material for SOFCs.
An Ultrafast Rechargeable Hybrid Sodium‐Based Dual‐Ion Capacitor Based on Hard Carbon Cathodes
Authors: Chen Suhua , Wang Jue , Fan Ling , Ma Ruifang , Zhang Erjing , Liu Qian , Lu Bingan 
Published: March 2018

AbstractHybrid sodium‐based dual‐ion capacitors (NDICs), which integrate the advantages of supercapacitors and sodium‐ion batteries, have attracted tremendous attention recently. In this work, hybrid sodium‐based dual‐ion capacitors are successfully developed with nitrogen‐doped microporous hard carbon as the cathode and soft carbon as the anode. N‐doping is beneficial to the functional groups, porous structure, and electric conductivity of hard carbon. Hybrid NDICs possess a wide voltage range (0.01–4.7 V), high‐energy density of 245.7 W h kg−1 at a power density of 1626 W kg−1, long cycle life (1000 cycles), and outstanding rate performance.
Controllable fabrication and catalytic performance of nanosheet HZSM‐5 films by vertical secondary growth
Authors: Tian Yajie , Liu Hong , Wang Li , Zhang Xiangwen , Liu Guozhu 
Published: March 2018

SignificanceNanosheet HZSM‐5 film vertically grown on the substrate with the tailorable macro‐ and meso‐pores between the layers of nanosheets is hydrothermally synthesized by seed‐assisted secondary growth method. The as‐prepared nanosheet HZSM‐5 film exhibits reaction rate enhancement up to 312% in catalytic cracking of n‐dodecane as well as twice light olefins selectivity, ascribed to the better mass transfer of reactants in the hierarchical porous structure and the ultra‐thin b‐axis pores of nanosheets. © 2018 American Institute of Chemical Engineers AIChE J, 64: 1923–1927, 2018
Haploidentical transplantation outcomes for secondary acute myeloid leukemia: Acute Leukemia Working Party (ALWP) of the European Society for Blood and Marrow Transplantation (EBMT) study
Authors: Li Zhuoyan , Labopin Myriam , Ciceri Fabio , Blaise Didier , Tischer Johanna , Ehninger Gerhard , Van Lint MT , Koc Yener , Santarone Stella , Forcade Edouard , Castagna Luca , Polge Emmanuelle , Mailhol Audrey , Ruggeri Annalisa , Mohty Mohamad , Savani Bipin N. , Nagler Arnon 
Published: March 2018

AbstractSecondary acute myeloid leukemia (sAML) traditionally has inferior outcomes compared to de novo AML. Allogeneic hematopoietic cell transplantation (HCT) is the sole potentially curative therapy. This study analyzes the outcomes for unmanipulated haploidentical HCT (haploHCT) for sAML using the Acute Leukemia Working Party (ALWP) registry of the European Society for Blood and Marrow Transplantation (EBMT). We identified 154 patients with sAML who underwent haploHCT from 2006 to 2016. Median age at HCT was 60 years with time from diagnosis to HCT 5 months. At transplantation, 69 patients were in first CR and 85 had active disease. Fifty‐seven (38.0%) patients underwent myeloablative conditioning and 97 (62.0%) reduced intensity conditioning (RIC) conditioning. Multivariate analysis showed that there was no difference in RI, nonrelapse mortality (NRM), leukemia free survival (LFS), overall survival (OS), or GVHD‐free/relapse free survival (GRFS) for conditioning intensity, age, performance status, or graft source. Active disease was associated with higher RI and inferior LFS, OS, and GRFS compared with patients in CR at time of transplant. T‐cell depletion with anti‐thymoglobulin resulted in higher NRM and inferior LFS, OS, and GRFS compared to post‐transplant cyclophosphamide (PTCy) (HR 2.25, 2.01, 2.16, and 1.73, respectively with P values <.05). Our data shows that haploHCT is a feasible alternative for sAML when matched transplantation is unavailable.
Changes in intracranial volume and cranial shape in modern Koreans over four decades
Authors: Kim Ye Sel , Park In Sung , Kim Hyun Jung , Kim Dasom , Lee Nam Joon , Rhyu Im Joo 
Published: March 2018

AbstractObjectivesThis study investigated whether there was any secular change in cranial vault morphology among Koreans born between the 1930s and 1970s, a period of dramatic shift in Korea's socioeconomic conditions.Materials and methodsUsing three‐dimensional MRI volumetry, we obtained the intracranial volume (ICV) and craniometric measurements of 115 healthy Koreans: 58 individuals (32 males and 26 females) born in the 1930s (1926–1936) and 57 (28 males and 29 females) born in the 1970s (1972–1979).ResultsThe intracranial volume of males was 1502.3 ± 110.3 cm3 for the 1930s group and 1594.1 ± 99.5 cm3 for the 1970s group, and for females, it was 1336.0 ± 53.0 cm3 for the 1930s group and 1425.9 ± 79.6 cm3 for the 1970s group. On average, ICV increased by 94 cm3 in males and by 90 cm3 in females. Cranial measurements for the 1970s group were significantly larger than the 1930s group for both sexes except in female cranial length. Each measurement was significantly correlated with ICV [cranial height (R = 0.720), breadth (R = 0.706), and length (R = 0.531)]. The cephalic index decreased from 0.846 to 0.828 in males, indicating the cranium became narrower relative to the cranial length. In females, the cephalic index increased from 0.831 to 0.850. Sex and birthyear were marginally interrelated in cephalic indices.DiscussionFrom the 1930s to 1970s, the Korean Peninsula experienced important historical shifts, and we speculate that the consequent shift in socioeconomic status is the most likely factor responsible for Koreans’ cranial vault remodeling.
A High‐Voltage Molecular‐Engineered Organic Sensitizer–Iron Redox Shuttle Pair: 1.4 V DSSC and 3.3 V SSM‐DSSC Devices
Authors: Rodrigues Roberta R. , Cheema Hammad , Delcamp Jared H. 
Published: March 2018

AbstractThe development of high voltage solar cells is an attractive way to use sunlight for solar‐to‐fuel devices, multijunction solar‐to‐electric systems, and to power limited‐area consumer electronics. By designing a low‐oxidation‐potential organic dye (RR9)/redox shuttle (Fe(bpy)33+/2+) pair for dye‐sensitized solar‐cell (DSSC) devices, the highest single device photovoltage (1.42 V) has been realized for a DSSC not relying on doped TiO2. Additionally, Fe(bpy)33+/2+ offers a robust, readily tunable ligand platform for redox potential tuning. RR9 can be regenerated with a low driving force (190 mV), and by utilizing the RR9/Fe(bpy)33+/2+ redox shuttle pair in a subcell for a sequential series multijunction (SSM)‐DSSC system, one of the highest known three subcell photovoltage was attained for any solar‐cell technology (3.34 V, >1.0 V per subcell).
Lithium‐Ion Endohedral Fullerene (Li+@C60) Dopants in Stable Perovskite Solar Cells Induce Instant Doping and Anti‐Oxidation
Authors: Jeon Il , Ueno Hiroshi , Seo Seungju , Aitola Kerttu , Nishikubo Ryosuke , Saeki Akinori , Okada Hiroshi , Boschloo Gerrit , Maruyama Shigeo , Matsuo Yutaka 
Published: March 2018

AbstractHerein, we report use of [Li+@C60]TFSI− as a dopant for spiro‐MeOTAD in lead halide perovskite solar cells. This approach gave an air stability nearly 10‐fold that of conventional devices using Li+TFSI−. Such high stability is attributed to the hydrophobic nature of [Li+@C60]TFSI− repelling moisture and absorbing intruding oxygen, thereby protecting the perovskite device from degradation. Furthermore, [Li+@C60]TFSI− could oxidize spiro‐MeOTAD without the need for oxygen. The encapsulated devices exhibited outstanding air stability for more than 1000 h while illuminated under ambient conditions.
Isolierbare, neutrale Analoga des [B2H5]−‐Ions als vielseitige und stark bindende η2‐Donorliganden
Authors: Wang Sunewang R. , Prieschl Dominic , Mattock James D. , Arrowsmith Merle , Pranckevicius Conor , Stennett Tom E. , Dewhurst Rian D. , Vargas Alfredo , Braunschweig Holger 
Published: March 2018

AbstractZwei isolierbare, neutrale, Basen‐stabilisierte Diborane(5) sind dazu in der Lage, ausschließlich durch ihre B‐B‐Bindung stark an mehrere Kupfer(I)‐Komplexe zu binden. Die resultierenden Komplexe repräsentieren die ersten bekannten Komplexe mit neutralen, ungeschützten σB‐B‐Diboranliganden. Die Einkristall‐Röntgenstrukturanalysen dieser Komplexe zeigen, dass die X‐Cu‐Einheit (X=Cl, OTf, C6F5) gegenüber vom verbrückenden Wasserstoffatom des Diborans liegt und annähernd senkrecht zur B‐B‐Bindung steht. Dabei wechselwirkt diese nahezu gleichermaßen mit beiden Boratomen, woraus eine Verlängerung der B‐B‐Bindung resultiert. DFT‐Studien belegen, dass sowohl σ‐Donor‐ als auch π‐Akzeptor‐Effekte der B‐B‐Bindung für die Bildung dieser Produkte verantwortlich sind. Erstaunlicherweise zeigen sich diese Kupfer‐σB‐B‐Komplexe inert gegen thermisch oder photolytisch induzierten Ligandenaustausch mit Pyridin.
Structural Basis of a Broadly Selective Acyltransferase from the Polyketide Synthase of Splenocin
Authors: Li Yuan , Zhang Wan , Zhang Hui , Tian Wenya , Wu Lian , Wang Shuwen , Zheng Mengmeng , Zhang Jinru , Sun Chenghai , Deng Zixin , Sun Yuhui , Qu Xudong , Zhou Jiahai 
Published: March 2018

AbstractPolyketides are a large family of pharmaceutically important natural products, and the structural modification of their scaffolds is significant for drug development. Herein, we report high‐resolution X‐ray crystal structures of the broadly selective acyltransferase (AT) from the splenocin polyketide synthase (SpnD‐AT) in the apo form and in complex with benzylmalonyl and pentynylmalonyl extender unit mimics. These structures revealed the molecular basis for the stereoselectivity and substrate specificity of SpnD‐AT, and enabled the engineering of the industrially important Ery‐AT6 to broaden its substrate scope to include three new types of extender units.
Assessing Human Exposure to Organic Pollutants in the Indoor Environment
Authors: Salthammer Tunga , Zhang Yinping , Mo Jinhan , Koch Holger M. , Weschler Charles J. 
Published: March 2018

AbstractThere is an ongoing probing of the role of chemicals in the indoor environment. The majority of potential target substances are so‐called very volatile, volatile, and semi‐volatile organic compounds (VVOCs, VOCs, and SVOCs). Depending on their physical properties and the mass transfer conditions, they are distributed in or between the gas phase, particle phase, settled house dust, surface films, clothing, and other fabrics as well as the exposed skin and hair of the occupants themselves. Therefore, inhalation, ingestion, and dermal uptake all must be considered as relevant pathways for exposure assessment in human habitats. Exposure to VVOCs, VOCs, and SVOCs can be estimated by measuring their concentrations in relevant indoor compartments or by determining the amounts of the target compounds and/or their metabolites in urine and blood. Assessing the various routes of exposure often requires a combination of sophisticated and interdisciplinary theoretical background and experimental techniques. Consequently, close communication and collaboration between chemical and exposure scientists are needed to achieve a better understanding of human exposure to chemical substances in various indoor environments. Embedded in the toxicological context, this is the basis for assessing the corresponding health risks and for determining control strategies or approaches to limit such risks.
Functional Liquid Crystals towards the Next Generation of Materials
Authors: Kato Takashi , Uchida Junya , Ichikawa Takahiro , Sakamoto Takeshi 
Published: March 2018

AbstractSince the discovery of the liquid‐crystalline state in 1888, liquid crystal science has made great advances through fusion with various technologies and disciplines. Recently, new molecular design strategies and new self‐assembled structures have been developed as a result of the progress made in synthetic procedures and characterization techniques. Since these liquid crystals exhibit new functions and properties derived from their nanostructures and alignment, a variety of new functions for liquid crystals, such as transport for energy applications, separation for environmental applications, chromism, sensing, electrooptical effects, actuation, and templating have been proposed. This Review presents recent advances of liquid crystals that should contribute to the next generation of materials.
Synthesis of Branched‐Chain Sugars with a DHAP‐Dependent Aldolase: Ketones are Electrophile Substrates of Rhamnulose‐1‐phosphate Aldolases
Authors: Laurent Victor , Darii Ekaterina , Aujon Angelina , Debacker Marine , Petit Jean‐Louis , Hélaine Virgil , Liptaj Tibor , Breza Martin , Mariage Aline , Nauton Lionel , Traïkia Mounir , Salanoubat Marcel , Lemaire Marielle , Guérard‐Hélaine Christine , de Berardinis Véronique 
Published: March 2018

AbstractDihydroxyacetone phosphate (DHAP)‐dependent rhamnulose aldolases display an unprecedented versatility for ketones as electrophile substrates. We selected and characterized a rhamnulose aldolase from Bacteroides thetaiotaomicron (RhuABthet) to provide a proof of concept. DHAP was added as a nucleophile to several α‐hydroxylated ketones used as electrophiles. This aldol addition was stereoselective and produced branched‐chain monosaccharide adducts with a tertiary alcohol moiety. Several aldols were readily obtained in good to excellent yields (from 76 to 95 %). These results contradict the general view that aldehydes are the only electrophile substrates for DHAP‐dependent aldolases and provide a new C−C bond‐forming enzyme for stereoselective synthesis of tertiary alcohols.