bluuebunny/crossref_metadata_2025_split huggingface dataset:
Self‐Growth of MoS2 Sponge for Highly Efficient Photothermal Cleanup of High‐Viscosity Crude Oil Spills
Authors: Yu Miao , Xu Peng , Yang Jin , Ji Lai , Li Changsheng 
Published: January 2020

AbstractFor dealing with crude oil spills, the high viscosity of crude oil greatly limits the absorption capacity of the absorbent materials, making crude oil a major obstacle in the cleaning process. Herein, a MoS2‐rubber sponge (MoS2‐RS), as a photothermal sorbent, is prepared by a one‐step in situ synthesis. The sponge exhibits excellent superhydrophobicity (the water contact angle is 151°), a high absorption capacity for oils and organic liquids (15–67 g g−1), and an outstanding compressive elasticity of 38.6 kPa. Furthermore, MoS2‐RS shows a good photothermal conversion capability. Under illumination, the viscosity of crude oil could be effectively reduced due to the rapid temperature rise in MoS2‐RS. This response allows the modified sponge to quickly absorb crude oil, which significantly reduces the adsorption time of 20 µL crude oil from 16 h to 19 s when compared to that of absorbent materials without a photothermal conversion capability. Because of the excellent mechanical performance, MoS2‐RS could be installed in a vacuum pump to continuously collect crude oil from the water surface. This setup greatly improves the crude oil collecting efficiency. The new photothermal absorbent material shows great potential for the collection of crude oil and the cleanup of spill accidents.
1,1‐Ethendiol – Das lange Zeit schwer fassbare Enol der Essigsäure
Authors: Mardyukov Artur , Eckhardt André K. , Schreiner Peter R. 
Published: January 2020

AbstractWir berichten über die erste spektroskopische Identifizierung des bisher unbekannten 1,1‐Ethendiol, dem Enol‐Tautomer der Essigsäure. Das Enol wurde durch Hochvakuumblitzpyrolyse bei 400 °C aus Malonsäure in der Gasphase dargestellt. Alle Zersetzungsprodukte wurden anschließend in kryogenen Argonmatrices bei 10 K isoliert und mittels IR‐ und UV/Vis‐Spektroskopie charakterisiert. Alle experimentell gewonnenen Spektren wurden mit berechneten AE‐CCSD(T)/cc‐pCVTZ und B3LYP/6–311++G(2d,2p) Spektren abgeglichen. Nach Belichtung mit λ=254 nm lagert das Enol zur Essigsäure um oder wird zu Keten und Wasser zersetzt.
Molecular Springs: Integration of Complex Dynamic Architectures into Functional Devices
Authors: Huang Chang‐Bo , Ciesielski Artur , Samorì Paolo 
Published: January 2020

AbstractMolecular/supramolecular springs are artificial nanoscale objects possessing well‐defined structures and tunable physicochemical properties. Like a macroscopic spring, supramolecular springs are capable of switching their nanoscale conformation as a response to external stimuli by undergoing mechanical spring‐like motions. This dynamic action offers intriguing opportunities for engineering molecular nanomachines by translating the stimuli‐responsive nanoscopic motions into macroscopic work. These nanoscopic objects are reversible dynamic multifunctional architectures which can express a variety of novel properties and behave as adaptive nanoscopic systems. In this Minireview, we focus on the design and structure–property relationships of supramolecular springs and their (self‐)assembly as a prerequisite towards the generation of novel dynamic materials featuring controlled movements to be readily integrated into macroscopic devices for applications in sensing, robotics, and the internet of things.
A Room‐Temperature Verwey‐type Transition in Iron Oxide, Fe5O6
Authors: Ovsyannikov Sergey V. , Bykov Maxim , Medvedev Sergey A. , Naumov Pavel G. , Jesche Anton , Tsirlin Alexander A. , Bykova Elena , Chuvashova Irina , Karkin Alexander E. , Dyadkin Vadim , Chernyshov Dmitry , Dubrovinsky Leonid S. 
Published: January 2020

AbstractFunctional oxides whose physicochemical properties may be reversibly changed at standard conditions are potential candidates for the use in next‐generation nanoelectronic devices. To date, vanadium dioxide (VO2) is the only known simple transition‐metal oxide that demonstrates a near‐room‐temperature metal–insulator transition that may be used in such appliances. In this work, we synthesized and investigated the crystals of a novel mixed‐valent iron oxide with an unconventional Fe5O6 stoichiometry. Near 275 K, Fe5O6 undergoes a Verwey‐type charge‐ordering transition that is concurrent with a dimerization in the iron chains and a following formation of new Fe−Fe chemical bonds. This unique feature highlights Fe5O6 as a promising candidate for the use in innovative applications. We established that the minimal Fe−Fe distance in the octahedral chains is a key parameter that determines the type and temperature of charge ordering. This model provides new insights into charge‐ordering phenomena in transition‐metal oxides in general.
Genetically Encoded Activators of Small Molecules for Imaging and Drug Delivery
Authors: Thiel Zacharias , Nguyen Jade , Rivera‐Fuentes Pablo 
Published: January 2020

AbstractChemical biologists have developed many tools based on genetically encoded macromolecules and small, synthetic compounds. The two different approaches are extremely useful, but they have inherent limitations. In this Minireview, we highlight examples of strategies that combine both concepts to tackle challenging problems in chemical biology. We discuss applications in imaging, with a focus on super‐resolved techniques, and in probe and drug delivery. We propose future directions in this field, hoping to inspire chemical biologists to develop new combinations of synthetic and genetically encoded probes.
Total Synthesis of (−)‐Pepluanol B: Conformational Control of the Eight‐Membered‐Ring System
Authors: Zhang Jing , Liu Meng , Wu Chuanhua , Zhao Gaoyuan , Chen Peiqi , Zhou Lin , Xie Xingang , Fang Ran , Li Huilin , She Xuegong 
Published: January 2020

AbstractThe first total synthesis of the Euphorbia diterpenoid pepluanol B in both racemic and enantioenriched form involves 20 steps from a known bicyclic diol. This synthesis features an unprecedented bromo‐epoxidation to control the eight‐membered‐ring conformation. In addition, salient reactions for the construction of the tetracyclic backbone include a sterically challenging aldol reaction to establish the quaternary center, a ring closing metathesis (RCM) to forge the eight‐membered ring, and a diastereoselective cyclopropanation to assemble the embedded cyclopropane motif.
Ion‐Pairing Assemblies of Porphyrin–AuIII Complexes in Combination with π‐Electronic Receptor–Anion Complexes
Authors: Tanaka Hiroki , Haketa Yohei , Bando Yuya , Yamakado Ryohei , Yasuda Nobuhiro , Maeda Hiromitsu 
Published: January 2020

AbstractAnion complexes of anion‐responsive π‐electronic molecules can behave as pseudo π‐electronic anions providing various ion pairs in combination with countercations. In this study, single crystals of ion‐pairing assemblies comprising porphyrin–AuIII complexes and Cl− complexes of dipyrrolyldiketone BF2 complexes were prepared from 1:1 mixtures of anion receptors and the Cl− salts of cationic porphyrins in solution. In the solid state, the ion pairs formed characteristic assemblies, depending on the substituents of the anion receptors and porphyrin–AuIII complexes. Theoretical calculations on the ion pairs revealed that the stacking structures are stabilized by compensating positive and negative charges as well as π–π interactions.
Exponential quasi‐(Q,S,R)‐dissipativity and practical stability for switched nonlinear systems
Authors: Liu Shuo , Pang Hongbo 
Published: January 2020

AbstractIn this paper, the problems of exponential quasi‐(Q,S,R)‐dissipativity and practical stability analysis for a switched nonlinear system are addressed. First, the concept of exponential quasi‐(Q,S,R)‐dissipativity for switched nonlinear systems without requiring the exponential quasi‐(Q,S,R)‐dissipativity property of each subsystem is proposed. Then, we show that an exponentially quasi‐(Q,S,R)‐dissipative switched nonlinear system is practically stable. Second, this exponential quasi‐(Q,S,R)‐ dissipativity property for a switched nonlinear system is obtained by the design of a state‐dependent switching law. Third, a composite state‐dependent switching law is designed to render the feedback interconnection of switched nonlinear systems exponentially quasi‐(Q,S,R)‐dissipative. This switching law allows interconnected switched nonlinear systems to switch asynchronously. Finally, the effectiveness of the results is verified by a numerical example.
Heavier Alkaline‐Earth Catalyzed Dehydrocoupling of Silanes and Alcohols for the Synthesis of Metallo‐Polysilylethers
Authors: Morris Louis J. , Hill Michael S. , Mahon Mary F. , Manners Ian , S. McMenamy Fred , Whittell George R. 
Published: January 2020

AbstractThe dehydrocoupling of silanes and alcohols mediated by heavier alkaline‐earth catalysts, [Ae{N(SiMe3)2}2⋅(THF)2] (I–III) and [Ae{CH(SiMe3)2}2⋅(THF)2], (IV–VI) (Ae=Ca, Sr, Ba) is described. Primary, secondary, and tertiary alcohols were coupled to phenylsilane or diphenylsilane, whereas tertiary silanes are less tolerant towards bulky substrates. Some control over reaction selectivity towards mono‐, di‐, or tri‐substituted silylether products was achieved through alteration of reaction stoichiometry, conditions, and catalyst. The ferrocenyl silylether, FeCp(C5H4SiPh(OBn)2) (2), was prepared and fully characterized from the ferrocenylsilane, FeCp(C5H4SiPhH2) (1), and benzyl alcohol using barium catalysis. Stoichiometric experiments suggested a reaction manifold involving the formation of Ae–alkoxide and hydride species, and a series of dimeric Ae–alkoxides [(Ph3CO)Ae(μ2‐OCPh3)Ae(THF)] (3 a–c, Ae=Ca, Sr, Ba) were isolated and fully characterized. Mechanistic experiments suggested a complex reaction mechanism involving dimeric or polynuclear active species, whose kinetics are highly dependent on variables such as the identity and concentration of the precatalyst, silane, and alcohol. Turnover frequencies increase on descending Group 2 of the periodic table, with the barium precatalyst III displaying an apparent first‐order dependence in both silane and alcohol, and an optimum catalyst loading of 3 mol % Ba, above which activity decreases. With precatalyst III in THF, ferrocene‐containing poly‐ and oligosilylethers with ferrocene pendent to‐ (P1–P4) or as a constituent (P5, P6) of the main polymer chain were prepared from 1 or Fe(C5H4SiPhH2)2 (4) with diols 1,4‐(HOCH2)2‐(C6H4) and 1,4‐(CH(CH3)OH)2‐(C6H4), respectively. The resultant materials were characterized by NMR spectroscopy, gel permeation chromatography (GPC) and DOSY NMR spectroscopy, with estimated molecular weights in excess of 20,000 Da for P1 and P4. The iron centers display reversible redox behavior and thermal analysis showed P1 and P5 to be promising precursors to magnetic ceramic materials.
Dihalogenated Methylperoxy Radicals: Spectroscopic Characterization and Photodecomposition by Release of HO.
Authors: Lu Bo , Song Chao , Liu Jie , Trabelsi Tarek , Francisco Joseph S. , Wang Lina , Zeng Xiaoqing 
Published: January 2020

AbstractTwo atmospherically relevant dihalogenated methylperoxy radicals CHX2OO. (X=F and Cl) have been generated through O2‐oxidation of the corresponding alkyl radicals CHX2. in the gas phase. The IR spectroscopic characterization of both radicals in cryogenic Ar‐ and N2‐matrices (15 K) is supported by 18O‐labeling and ab initio calculations at the UCCSD(T)/aug‐cc‐pVTZ level. Upon 266 nm laser irradiation, both radicals decompose mainly by releasing hydroxyl radicals (→HO.+X2CO) via the intermediacy of intriguing α‐hydroperoxyalkyl radicals (.CX2OOH), implying that the photooxidation of dihalogenated hydrocarbons might serve as important sources of HO. radicals in the atmosphere.
Multimodal psychosocial intervention for family caregivers of patients undergoing hematopoietic stem cell transplantation: A randomized clinical trial
Authors: El‐Jawahri Areej , Jacobs Jamie M. , Nelson Ashley M. , Traeger Lara , Greer Joseph A. , Nicholson Showly , Waldman Lauren P. , Fenech Alyssa L. , Jagielo Annemarie D. , D’Alotto Jennifer , Horick Nora , Spitzer Thomas , DeFilipp Zachariah , Chen Yi‐Bin A. , Temel Jennifer S. 
Published: January 2020

BackgroundCaregivers of patients undergoing hematopoietic stem cell transplantation (HCT) experience an immense caregiving burden before, during, and after HCT.MethodsWe conducted an unblinded, randomized trial of a psychosocial intervention (BMT‐CARE) for caregivers of patients undergoing autologous and allogeneic HCT at Massachusetts General Hospital. Caregivers were randomly assigned to BMT‐CARE or usual care. BMT‐CARE was tailored to the HCT trajectory and integrated treatment‐related education and self‐care with cognitive‐behavioral skills to promote coping. Caregivers assigned to BMT‐CARE met with a trained interventionist (a psychologist or a social worker) in person, via telephone, or via videoconferencing for 6 sessions starting before HCT and continuing up to day +60 after HCT. The primary endpoint was feasibility, which was defined as at least 60% of eligible caregivers enrolling and completing 50% or more of the intervention sessions. We assesed caregiver quality of life (QOL; Caregiver Oncology Quality of Life Questionnaire), caregiving burden (Caregiver Reaction Assessment), psychological distress (Hospital Anxiety and Depression Scale), self‐efficacy (Cancer Self‐Efficacy Scale–Transplant), and coping (Measures of Current Status) at baseline and 30 and 60 days after HCT. We used mixed linear effect models to assess the effect of BMT‐CARE on outcomes longitudinally.ResultsWe enrolled 72.5% of eligible caregivers (100 of 138), and 80% attended 50% or more of the intervention sessions. Caregivers randomized to BMT‐CARE reported improved QOL (B = 6.11; 95% CI, 3.50‐8.71; P < .001), reduced caregiving burden (B = –6.02; 95% CI, –8.49 to –3.55; P < .001), lower anxiety (B = –2.18; 95% CI, –3.07 to –1.28; P < .001) and depression symptoms (B = –1.23; 95% CI, –1.92 to –0.54; P < .001), and improved self‐efficacy (B = 7.22; 95% CI, 2.40‐12.03; P = .003) and coping skills (B = 4.83; 95% CI, 3.04‐6.94; P < .001) in comparison with the usual‐care group.ConclusionsA brief multimodal psychosocial intervention tailored for caregivers of HCT recipients is feasible and may improve QOL, mood, coping, and self‐efficacy while reducing the caregiving burden during the acute HCT period.
Understanding the ability, and inability, of high‐resolution ultrasound to guide thyroid nodule evaluation
Authors: Alexander Erik K. 
Published: January 2020

Ultrasound is the primary tool used to initially guide clinical decisions about newly detected thyroid nodules, and numerous ultrasound‐based risk stratification systems have been developed that allow low to high cancer risk stratification. These systems can similarly assist with risk assessment for follicular thyroid carcinoma, but with important cautionary caveats.
Simulation of the influence of voltage level and pulse spacing on the efficiency, aggressiveness and uniformity of the electroporation process in tissues using meshless techniques
Authors: Vélez Salazar Fabián M. , Patiño Arcila Iván D. , Ruiz Villa Carlos A. 
Published: January 2020

AbstractElectroporation is a widely used method consisting of application of high‐voltage, short‐duration electric pulses to increase cell membrane permeability, allowing cellular internalization of medications. In this work, the influence of two primary parameters, voltage level (V) and pulse spacing (N), on electroporation efficiency, uniformity and aggressiveness, as quantified by the total mass transport to viable cells, intracellular concentration gradients and an aggressiveness factor introduced here, is studied by means of numerical simulations of drug transport in electroporated tissues. The global method of approximate particular solutions (Global MAPS) is used to solve the governing equations, together with domain scaling, singular value decomposition and smoothing algorithms, to address the ill‐conditioning of the final system and suppress small scale oscillations. The accuracy of Global MAPS is evaluated by comparing the initial extracellular concentration, Ce, and final intracellular concentration, Ci, with previous finite volume method results, obtaining similar behavior of Ce and Ci along the tissue domain, with some differences for Ci in high‐gradient zones. According to the Global MAPS results, the influence of V and N on Ci is only significant over a certain range, within which the largest drug transport to viable cells occurs. In general, both electroporation efficiency and aggressiveness change in nonuniform manner with V and decrease with N, whereas the electroporation uniformity decreases as V increases and N decreases. The contour plots obtained here can be considered useful tools to compare electroporation‐based treatments in terms of their efficiency, aggressiveness and uniformity, assisting in the selection of a suitable treatment plan for cancer.
Continuous Radio Amplification by Stimulated Emission of Radiation using Parahydrogen Induced Polarization (PHIP‐RASER) at 14 Tesla
Authors: Pravdivtsev Andrey N. , Sönnichsen Frank D. , Hövener Jan‐Bernd 
Published: January 2020

AbstractNuclear Magnetic Resonance (NMR) is an intriguing quantum‐mechanical effect that is used for routine medical diagnostics and chemical analysis alike. Numerous advancements have contributed to the success of the technique, including hyperpolarized contrast agents that enable real‐time imaging of metabolism in vivo. Herein, we report the finding of an NMR radio amplification by stimulated emission of radiation (RASER), which continuously emits 1H NMR signal for more than 10 min. Using parahydrogen induced hyperpolarization (PHIP) with 50 % para‐hydrogen, we demonstrated the effect at 600 MHz but expect that it is functional across a wide range of frequencies, e.g. 101–103 MHz. PHIP‐RASER occurs spontaneously or can be triggered with a standard NMR excitation. Full chemical shift resolution was maintained, and a linewidth of 0.6 ppb was achieved. The effect was reproduced by simulations using a weakly coupled, two spin‐
system. All devices used were standard issue, such that the effect can be reproduced by any NMR lab worldwide with access to liquid nitrogen for producing parahydrogen.
A Near‐Infrared Absorption Small Molecule Acceptor for High‐Performance Semitransparent and Colorful Binary and Ternary Organic Photovoltaics
Authors: Wang Chun‐Kai , Jiang Bing‐Huang , Lu Jong‐Hong , Cheng Ming‐Tsang , Jeng Ru‐Jong , Lu Yu‐Wei , Chen Chih‐Ping , Wong Ken‐Tsung 
Published: January 2020

AbstractAn acceptor–donor–acceptor (A–D–A)‐type non‐fullerene acceptor (NFA), PTTtID‐Cl, featuring thieno[3,2‐b]thieno[2′′′,3′′′:4′′,5′′]‐pyrrolo[2′′,3′′:4′,5′]thieno[2′,3′:4,5]thieno‐[2,3‐d]pyrrole (DTPTt) as the electron‐rich core and 2‐(5,6‐dichloro‐3‐oxo‐2,3‐dihydro‐1H‐inden‐1‐ylidene)malononitrile (ID‐Cl) as the peripheral electron‐deficient terminal group was synthesized and characterized. PTTtID‐Cl exhibited strong absorption in the range of 700–850 nm in CHCl3 and redshifted absorption centered at 881 nm in a thin film. The near infrared (NIR)‐absorption of PTTtID‐Cl was combined with a low‐bandgap polymer donor (PTB7‐Th) to achieve binary and semitransparent organic photovoltaics (OPVs) with a power conversion efficiency (PCE) of 8.9 % and 7.7 % (with an average visible transmittance (AVT) of 16.7 %), respectively. A ternary device with a ratio of PM7/PTTtID‐Cl/IT‐4F=1:0.15:0.85 (w/w) achieved a short‐circuit current density of 19.46 mA cm−2, an open‐circuit voltage of 0.87 V, and a fill factor of 71.2 %, giving a PCE of 12.0 %. In addition, by employing the Ag/ITO/Ag microcavity structure, semitransparent colorful binary organic photovoltaics (OPVs) with superior transparency of 27.9 % at 427 nm and 22.7 % at 536 nm for blue and green devices, respectively, were prepared. The semitransparent colorful devices based on the optimized ternary blend gave PCEs of 8.7 %, 8.4 %, and 9.1 % for blue, green, and red devices, respectively. These results indicate the promising potential of PTTtID‐Cl as a NIR‐absorption NFA for applications in semitransparent colorful binary and ternary OPVs.
Legitimacy assessment throughout the life of collaborative water governance
Authors: Melnychuk Natalya , de Loë Robert 
Published: January 2020

AbstractCollaborative governance arrangements involving a diversity of groups (e.g., governments, civil society, industry) are increasingly being used to make decisions or give advice to decision‐makers on water issues. Legitimacy is a critical factor for the effectiveness, efficiency, stability, and popular approval of collaborative efforts. However, as a concept, legitimacy remains contested with various meanings, theoretical backgrounds, and source norms. Clarity is particularly needed around the changing sources of legitimacy as collaborative efforts mature. Drawing on case‐study research of five collaborations in British Columbia, Canada, we present a framework of legitimacy sources as collaborations evolve. Legitimacy during the establishment of a collaboration depends principally on community readiness to collaborate, a sense of need, and the perceived potential for goal achievement. As a collaboration continues to grow, its legitimacy forms mainly from normative processes—the perceived quality of factors such as accountability, transparency, consensus‐building, and representation of relevant discourses. Once a collaboration reaches maturity and faces questions of its future existence, legitimacy is largely result‐based—tangible and contextually meaningful outcomes must be easily identifiable and promoted. Increased understanding of the dynamics of legitimacy can help collaborative efforts strategically plan and work toward their goals as they evolve.
A new method for determining weathering rates in weathering pits
Authors: Wang Wei , Huang Rihui , Feng Jing 
Published: January 2020

AbstractDetermining the rates of rock weathering is difficult because, firstly, the weathering rate of rocks is usually so slow that it is difficult to measure; secondly, it is also difficult to determine the start time and duration of weathering. The Shanxi River Valley in Fujian, China dried up after a reservoir was built upstream in 1959, and became a stone quarry site. Quarrying ceased in 1977, so a large amount of quarry wastes with artificially excavated surfaces were left in the valley. The concave‐upward curved rocky surface, broken by manual excavation, easily contains rainwater in its central part, which was easily weathered into a more concave surface. Plaster mould casting was performed in situ on such a concave surface of an excavated stone rock in the valley and scanned with a high‐precision 3D scanner to obtain 3D data of the concave‐upward rock surface and its more concave middle part, which was considered as an initial weathering pit. The 3D model provided an in‐depth understanding of the initial formation process of weathering pits, indicating that: (1) the average weathering rate of a weathering pit is 10.8 ± 0.49 cm ka−1; (2) weathering pits are generally formed by standing water in depressions on a flat near‐horizontal rock surface due to weathering actions involving water; (3) the deepening rate of a weathering pit is about four times greater than that of the surrounding area; (4) the growth of a weathering pit can begin in some small concavities on the flat rock surface without pre‐existing depressions and gradually expands; (5) a weathering pit is generally wider than deep or with a flat bottom due to expansion with a lateral weathering rate that is greater than that of the vertical, and the lamination of the host rock is not necessary for the formation of flat‐floored weathering pits. © 2020 John Wiley & Sons, Ltd.