bluuebunny/crossref_metadata_2025_split huggingface dataset:
High‐Performance Protonic Ceramic Fuel Cells with 1 µm Thick Y:Ba(Ce, Zr)O3 Electrolytes
Authors: Bae Kiho , Kim Dong Hwan , Choi Hyung Jong , Son Ji‐Won , Shim Joon Hyung 
Published: July 2018

AbstractThis study demonstrates the effectiveness of using thin‐film electrolytes to enhance protonic ceramic fuel cells (PCFCs). The material tested in this study is yttrium‐doped barium cerate‐zirconate (BCZY), which is a representative electrolyte material of PCFCs. The thickness of the electrolyte membrane is as small as 1 µm and designed to minimize ohmic loss in proton transport pathways. Integration of this thin BCZY electrolyte is attempted on a multilayered anode comprised of two‐step supports with bulk nickel‐yttria stabilized zirconia cermet as a base and thin nickel‐BCZY as an anode functional layer atop the base. The compatibility of this support with the deposited thin electrolyte is able to be confirmed from the results of iterated tests. The power of the fabricated cell is greater than 1.1 W cm−2 at 600 °C, which is a record high for PCFCs and is reproducible. In this paper, the origin of this high power is discussed and improvements that could be made to cell performance are further suggested.
Ultrastable In‐Plane 1T–2H MoS2 Heterostructures for Enhanced Hydrogen Evolution Reaction
Authors: Wang Shuai , Zhang Di , Li Bin , Zhang Chao , Du Zhiguo , Yin Haoming , Bi Xiaofang , Yang Shubin 
Published: July 2018

AbstractMetallic 1T MoS2 is highly desirable for catalyzing electrochemical hydrogen production from water owing to its high electrical conductivity. However, stable 1T MoS2 is difficult to be produced in large‐scale by either common chemical or physical approaches. Here, ultrastable in‐plane 1T–2H MoS2 heterostructures are achieved via a simple one‐pot annealing treatment of 2H MoS2 bulk under a mixture gas of Ar and phosphorous vapor, where phosphorus cannot only occupy the interspace of MoS2 bulk, resulting in the expansion of MoS2, but also embed into the lattice of MoS2, inducing the partial phase transition from 2H to 1T phases of MoS2. Benefiting from its significantly improved electrical conductivity, highly exposed active sites, and hydrophily property, in‐plane 1T–2H MoS2 heterostructures exhibit largely improved electrocatalytic properties for hydrogen evolution reaction (HER) in alkaline electrolytes.
cPCET versus HAT: A Direct Theoretical Method for Distinguishing X–H Bond‐Activation Mechanisms
Authors: Klein Johannes E. M. N. , Knizia Gerald 
Published: July 2018

AbstractProton‐coupled electron transfer (PCET) events play a key role in countless chemical transformations, but they come in many physical variants which are hard to distinguish experimentally. While present theoretical approaches to treat these events are mostly based on physical rate coefficient models of various complexity, it is now argued that it is both feasible and fruitful to directly analyze the electronic N‐electron wavefunctions of these processes along their intrinsic reaction coordinate (IRC). In particular, for model systems of lipoxygenase and the high‐valent oxoiron(IV) intermediate TauD‐J it is shown that by invoking the intrinsic bond orbital (IBO) representation of the wavefunction, the common boundary cases of hydrogen atom transfer (HAT) and concerted PCET (cPCET) can be directly and unambiguously distinguished in a straightforward manner.
Kohlenstoffnitridmaterialien für photochemische Zellen zur Wasserspaltung
Authors: Volokh Michael , Peng Guiming , Barrio Jesús , Shalom Menny 
Published: July 2018

AbstractGraphitische Kohlenstoffnitridmaterialien (CN) sind aufgrund ihrer einstellbaren Bandlücke, geeigneten Energiebandposition, hohen Stabilität unter harschen chemischen Bedingungen und geringen Kosten interessante Photokatalysatoren und heterogene Katalysatoren für zahlreiche Reaktionen. Allerdings befindet sich die Nutzung von CN in photoelektrochemischen (PEC) und photoelektronischen Bauelementen noch in einem frühen Stadium, da die Abscheidung einer hochwertigen und homogenen CN‐Schicht auf Substraten, die breite Bandlücke, die schlechte Ladungstrennungseffizienz sowie die geringe elektronische Leitfähigkeit noch Schwierigkeiten bereiten. In diesem Kurzaufsatz diskutieren wir Synthesewege zur Herstellung verschiedener Strukturen von CN auf Substraten und deren grundlegende photophysikalische Eigenschaften und photoelektrochemische Aktivität. Wir beschreiben die wesentlichsten Herausforderungen bei der Einbindung von CN in PEC‐Zellen sowie mögliche Wege zur Überwindung der bestehenden Beschränkungen zur Integration von CN‐Materialien in PEC und andere photoelektronische Bauelemente.
A Stable Crystalline Copper(I)–N2O Complex Stabilized as the Salt of a Weakly Coordinating Anion
Authors: Zhuravlev Vadim , Malinowski Przemysław J. 
Published: July 2018

AbstractNitrous oxide is considered a poor ligand, and therefore only a handful of well‐defined metal–N2O complexes are known. Oxidation of copper powder with an extreme oxidant, [Ag2I2][An]2 ([An]−=[Al(OC(CF3)3)4]−) in perfluorinated hexane leads to CuI[An], the first auxiliary ligand‐free CuI salt of the perfluorinated alkoxyaluminate anion. The compound is capable of forming a stable and crystalline complex with nitrous oxide, Cu(N2O)[An], where the Cu−N2O bond is by far the strongest among all other molecular metal–N2O complexes known. Thorough characterization of the compounds together with the crystal structure of Cu(N2O)[An] complex supported with DFT calculations are presented. These give insight into the bonding in the Cu+–N2O system and confirm N‐end coordination of the ligand.
Rational Design of MOF/COF Hybrid Materials for Photocatalytic H2 Evolution in the Presence of Sacrificial Electron Donors
Authors: Zhang Feng‐Ming , Sheng Jing‐Li , Yang Zhao‐Di , Sun Xiao‐Jun , Tang Hong‐Liang , Lu Meng , Dong Hong , Shen Feng‐Cui , Liu Jiang , Lan Ya‐Qian 
Published: July 2018

AbstractCrystalline and porous covalent organic frameworks (COFs) and metal‐organic frameworks (MOFs) materials have attracted enormous attention in the field of photocatalytic H2 evolution due to their long‐range order structures, large surface areas, outstanding visible light absorbance, and tunable band gaps. In this work, we successfully integrated two‐dimensional (2D) COF with stable MOF. By covalently anchoring NH2‐UiO‐66 onto the surface of TpPa‐1‐COF, a new type of MOF/COF hybrid materials with high surface area, porous framework, and high crystallinity was synthesized. The resulting hierarchical porous hybrid materials show efficient photocatalytic H2 evolution under visible light irradiation. Especially, NH2‐UiO‐66/TpPa‐1‐COF (4:6) exhibits the maximum photocatalytic H2 evolution rate of 23.41 mmol g−1 h−1 (with the TOF of 402.36 h−1), which is approximately 20 times higher than that of the parent TpPa‐1‐COF and the best performance photocatalyst for H2 evolution among various MOF‐ and COF‐based photocatalysts.
An Environmentally Friendly and Flexible Aqueous Zinc Battery Using an Organic Cathode
Authors: Guo Zhaowei , Ma Yuanyuan , Dong Xiaoli , Huang Jianhang , Wang Yonggang , Xia Yongyao 
Published: July 2018

AbstractRechargeable batteries have been used to power various electric devices and store energy from renewables, but their toxic components (namely, electrode materials, electrolyte, and separator) generally cause serious environment issues when disused. Such toxicity characteristic makes them difficult to power future wearable electronic devices. Now an environmentally friendly and highly safe rechargeable battery, based on a pyrene‐4,5,9,10‐tetraone (PTO) cathode and zinc anode in mild aqueous electrolyte is presented. The PTO‐cathode shows a high specific capacity (336 mAh g−1) for Zn2+ storage with fast kinetics and high reversibility. Thus, the PTO//Zn full cell exhibits a high energy density (186.7 Wh kg−1), supercapacitor‐like power behavior and long‐term lifespan (over 1000 cycles). Moreover, a belt‐shaped PTO//Zn battery with robust mechanical durability and remarkable flexibility is first fabricated to clarify its potential application in wearable electronic devices.
Leveraging γ‐Glutamyl Transferase To Direct Cytotoxicity of Copper Dithiocarbamates against Prostate Cancer Cells
Authors: Bakthavatsalam Subha , Sleeper Mark L. , Dharani Azim , George Daniel J. , Zhang Tian , Franz Katherine J. 
Published: July 2018

AbstractA prodrug approach is presented to direct copper‐dependent cytotoxicity to prostate cancer cells. The prochelator GGTDTC requires activation by γ‐glutamyl transferase (GGT) to release the metal chelator diethyldithiocarbamate from a linker that masks its thiol reactivity and metal binding properties. In vitro studies demonstrated successful masking of copper binding as well as clean liberation of the chelator by GGT. GGTDTC was stable to non‐specific degradation when incubated with a series of prostate cancer and normal cell lines, with selective release of diethyldithiocarbamate only occurring in cells with measurable GGT activity. The antiproliferative efficacy of the prochelator correlated with cellular GGT activity, with 24 h inhibitory concentrations ranging from 800 nm in prostate cancer lines 22Rv1 and LNCaP to over 15 μm in normal prostate PWR‐1E cells. These findings underscore a new strategy to leverage the amplified copper metabolism of prostate cancer by conditional activation of a metal‐binding pharmacophore.
Functionalization in solution of polypropylene with a maleinized hyperbranched polyol polyester: Structural, thermal, rheological, and mechanical properties
Authors: Nova María , Arévalo Yaritza , Murillo Edwin A. 
Published: July 2018

AbstractThe functionalization of polypropylene (PP) with a maleinized hyperbranched polyester polyol (MHBP) was performed in solution to obtain PP‐g‐MHBPs. The degree of functionalization (FD) increased with MHBP and dicumyl peroxide (DCP) contents, but the contact angle followed an opposite behavior. The sample obtained with the proportion of 9.0 wt % MHBP and 2.0 wt % DCP and presented the highest FD value. An FD value of 2.4 wt %, produced a reduction of 19° on the contact angle. It was observed by differential scanning calorimetry (DSC) that the PP‐g‐MHBPs obtained by employing 3.0 wt % of MHBP, exhibited a slight reduction of the melting temperature (Tm) with the increase in the amounts of FD and DCP. Some FD values obtained in this study are higher than those obtained both commercial and noncommercial grades of PP functionalized with maleic anhydride. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 46932.
Revealing early villages – Pseudo‐3D ERT geophysical survey at the pre‐pottery Neolithic site of Kharaysin, Jordan
Authors: Moník Martin , Lenďáková Zuzana , Ibáñez Juan José , Muñiz Juan , Borell Ferrán , Iriarte Eneko , Teira Luis , Kuda František 
Published: July 2018

AbstractElectric resistivity tomography (ERT) prospection conducted at the Pre‐Pottery Neolithic site at Kharaysin, Jordan, building on previous surface prospection and excavation, found a number of new sub‐surface anomalies. Subsequent excavations determined that the anomalies corresponded with the stone walls of habitation structures and possibly terrace walls. These features covered large areas of the site slope, inclusive of clustered settlement structures and frequent building superpositions indicative of multi‐phase occupation. Despite the generally arid conditions, the moist soil matrix allowed for the effective use of ERT. This article presents the integrated data of the archaeological excavation and the geophysical survey. As a test case it proves the utility of ERT in the identification of Pre‐Pottery Neolithic A (PPNA) and Pre‐Pottery Neolithic B (PPNB) sub‐surface anthropogenic features.
Aggregation‐Induced Emission with Long‐Lived Room‐Temperature Phosphorescence from Methylene‐Linked Organic Donor–Acceptor Structures
Authors: Chen Biao , Zhang Xuepeng , Wang Yucai , Miao Hui , Zhang Guoqing 
Published: July 2018

AbstractAggregation‐caused quenching (ACQ), where excited‐state and/or ground‐state electronic structures are altered to exhibit an increased proclivity for non‐radiative decay for the aggregates, is largely responsible for the lack of fluorescence and phosphorescence in molecular solids in general. Here we show that ACQ could be effectively circumvented by constructing an aromatic system with a methylene‐linker, where the system exhibits typical aggregation‐induced emission (AIE) with long‐lived room‐temperature phosphorescence, since the tetrahedral structure in the solid state may significantly reduce strong intermolecular interactions contributing to ACQ.
Financial burden among older, long‐term cancer survivors: Results from the LILAC study
Authors: Hastert Theresa A. , Young Gregory S. , Pennell Michael L. , Padamsee Tasleem , Zafar S. Yousuf , DeGraffinreid Cecilia , Naughton Michelle , Simon Michael , Paskett Electra D. 
Published: July 2018

AbstractBackgroundIncreasing attention is being paid to financial burdens of cancer survivorship, but little is known about the prevalence and predictors of these burdens in older, long‐term survivors.MethodsWe used data from 6012 participants diagnosed with cancer since enrolling in the Women's Health Initiative, and who participated in the Life and Longevity After Cancer (LILAC) ancillary study to estimate prevalence and identify predictors of financial burden. We used logistic regression to identify sociodemographic, socioeconomic, health‐ and cancer‐related factors associated with financial burden and backward selection to build a final multivariable model.ResultsAverage age at LILAC participation was 79 and 9.2 years had elapsed since cancer diagnosis. Overall, 6% experienced some form of financial burden, including having an insurance company refuse a claim (2.6%), being denied loans or insurance due to cancer history (2.2%), or experiencing significant indebtedness (1.8%, including facing large debts or bills or declaring bankruptcy). Eight predictors remained associated (P < 0.05) with financial burden in the fully‐adjusted model: younger age, shorter time since diagnosis, African‐American race, household income <$20 000/year, modified Charlson comorbidity score ≥2, receipt of chemotherapy, regional stage at diagnosis, and no private health insurance. Education, cancer site, social support, receipt of radiation, and receipt of hormone therapy were not associated with financial burden. Predictors differed between types of financial burden experienced and age at diagnosis (<65 vs 65+).ConclusionCancer‐related financial burden was rare in this population of older, female long‐term cancer survivors. The identification of several socioeconomic, health‐related and demographic predictors of financial burden may suggest targets of intervention to reduce financial burdens.PrecisFinancial burden was uncommon in older, female, long‐term survivors. Predictors of financial burden included age, race, income, comorbidities, time since diagnosis, stage, insurance, and receipt of chemotherapy.
Extracellular calcium regulates the adhesion and migration of osteoclasts via integrin αvβ3/Rho A/Cytoskeleton signaling
Authors: Xiang Bilu , Liu Yang , Zhao Wei , Zhao Hanchi , Yu Haiyang 
Published: July 2018

AbstractIntegrin αvβ3 is a transmembrane integrin, which can initiate osteoclasts’ attachment on bones, leading to downward signaling pathways and subsequent bone resorption. Different calcium concentrations have been reported to have an influence on the activation of integrin αvβ3. To elucidate the regulatory mechanism of extracellular calcium concentrations on osteoclasts, a controlled micro flow plate (M04S) was utilized in the ONIX flow control system to observe the osteoclasts’ adhesion and migration in different calcium concentration media. Fluorescent staining is conducted to show the distribution of integrin αvβ3 and cytoskeleton reorganization. In addition, western blots were performed to detect the expression of integrin αvβ3 and its downstream signaling pathways related to bone resorption. Also, real‐time reverse‐transcription polymerase chain reaction data of transcription co‐activator (YAP/TAZ) and hydrolytic enzymes (the matrix metalloproteinase 9 and cathepsin K) are evaluated. Our findings suggest that osteoclasts’ migration and adhesion is better promoted at 0.5 mM than 1.2 mM, which can be partly explained by the induced cytoskeleton organization via integrin αvβ3/Rho GTPase. But the activation and nuclear localization of YAP/TAZ, and the secretion of hydrolytic enzymes were upregulated when the calcium concentration is at a higher level (1.2 mM). According to our study, there is a high possibility that the migration and attachment of osteoclasts and subsequent osteoclastic bone resorption are regulated over a specific range of extracellular calcium concentration.
Impella‐assisted chronic total occlusion percutaneous coronary interventions: A multicenter retrospective analysis
Authors: Riley Robert F. , McCabe James M. , Kalra Sanjog , Lazkani Mohamad , Pershad Ashish , Doshi Darshan , Kirtane Ajay J. , Nicholson William , Kearney Katherine , Demartini Tony , Aaron Grantham J. , Moses Jeffrey , Lombardi William , Karmpaliotis Dimitri 
Published: July 2018

AbstractIntroductionPatients with coronary chronic total occlusions (CTO) often have concurrent higher‐risk anatomy and physiology (significant calcium, left ventricular dysfunction, multivessel disease) that increase their procedural risk. We present a retrospective multicenter case series describing use of the Impella percutaneous ventricular assist device (p‐VAD) during CTO PCI.MethodsWe performed a retrospective analysis of self‐reported data from five large referral centers from 2013 to 2017 and identified patients that underwent elective, hemodynamically supported CTO PCI with the Impella p‐VAD device (2.5 or CP). Preprocedural demographics, procedural invasive hemodynamics and characteristics, and in‐hospital outcomes were reported.ResultsAbout 57 patients (2% of the overall CTO volume of these centers) were included in this retrospective cohort. The primary indication in the majority (78.9%) of cases was chronic angina; in 21.1% the primary indication was for chronic congestive heart failure because of an ischemic cardiomyopathy. The median LVEF was 20% (15%, 30%) and 63.2% were surgical turndowns. Significant proportions of the group underwent multivessel PCI (91.2%), intervention on an unprotected left main or last remaining conduit vessel (35.1%), and/or atherectomy (17.5%). Technical success was 87.7%. In‐hospital procedural complications included: vascular injury (5.3%), all‐cause death (5.3%), major bleeding (3.5%), stroke (1.8%), and coronary perforation resulting in tamponade (1.8%).ConclusionImpella‐assisted CTO PCI can be performed with high technical success rates. However, assiduous attention to appropriate case selection is critical, given the periprocedural complication rates reported in this patient population.
Copper‐Catalyzed Monoorganylation of Trialkyl Borates with Functionalized Organozinc Pivalates
Authors: Fu Ying , Gou Bei‐Lei , Shi Chun‐Zhao , Du Zhengyin , Shen Tong 
Published: July 2018

AbstractOrganozinc pivalates, a recently developed air‐ and moisture‐stable organozinc species, were found for the first time as excellent organometallic species in the monoorganylation of trialkyl borates whereby boronic acids were prepared in high yields. The significant advantage of organozinc pivalates over another previously employed organometallic reagents, e. g., organolithium reagents, Grignard reagents and organozinc halides, is that the generation of multiorganylation byproducts such as borinic acids and trialkylboranes were completely suppressed. Additionally, the in situ generated boronates could be directly arranged into Suzuki‐Miyaura type cross‐coupling reactions to produce biaryls in high yields.
Yttrium‐Catalyzed Synthesis of Bipyridine‐Functionalized AB‐Block Copolymers: Micellar Support for Photocatalytic Active Rhenium‐Complexes
Authors: Adams F. , Pschenitza M. , Rieger B. 
Published: July 2018

AbstractHerein, ortho‐methylated bipyridines are introduced as initiators in 2‐aminoalkoxy‐bis (phenolate) yttrium complexes. For this C−H bond activation (ONOO)tBuY(CH2TMS)(thf) (1) (TMS=trimethylsilyl) is reacted with the respective bipyridine to obtain complexes (ONOO)tBuY(6‐Me2bpy) (2) and (ONOO)tBuY(6‐Mebpy) (3). Both complexes were tested first in rare‐earth metal‐mediated group‐transfer polymerization of 2‐vinylpridine (2VP). Complex 3 was further tested in block copolymerizations of 2VP and diethyl vinylphosphonate. The obtained initiator‐P2VP‐PDEVP‐block copolymers can selectively react with Re(CO)5Cl at their bipyridine end‐group. The obtained rhenium functionalized block copolymers are able to self‐assemble to unimodal micelles in water, representing a possible carrier for hydrophobic metal containing complexes into cells. Furthermore, the Re‐block copolymers sustain activity in the photocatalytic homogeneous CO2 reduction and their performance exceed the catalytic activity of the analogue polymer‐free system [Re(CO)3(6‐Mebpy)Cl] (4).
Enhancing the Catalytic Performance of a CYP116B Monooxygenase by Transdomain Combination Mutagenesis
Authors: Li Ren‐Jie , Xu Jian‐He , Chen Qi , Zhao Jing , Li Ai‐Tao , Yu Hui‐Lei 
Published: July 2018

AbstractThe front cover artwork for Issue 14/2018 is provided by the Laboratory of Biocatalysis and Synthetic Biotechnology, East China University of Science and Technology (ECUST). As shown in the image, a simple transdomain combination mutation strategy (TDCM) was proposed and employed for engineering a self‐sufficient cytochrome P450 monooxygenase (P450LaMO), with significantly improved turnover frequency and electron coupling efficiency. See the Full Paper itself at https://doi.org/10.1002/cctc.201800054.
Non‐Covalently Pre‐Assembled High‐Performance Near‐Infrared Fluorescent Molecular Probes for Cancer Imaging
Authors: Shaw Scott K. , Liu Wenqi , Gómez Durán César Fernando Azael , Schreiber Cynthia L. , Betancourt Mendiola María de Lourdes , Zhai Canjia , Roland Felicia M. , Padanilam Simon J. , Smith Bradley D. 
Published: July 2018

AbstractNew fluorescent molecular probes, which can selectively target specific cell surface receptors, are needed for microscopy, in vivo imaging, and image guided surgery. The preparation of multivalent probes using standard synthetic chemistry can be a laborious process due to low reaction yields caused by steric effects. In this study, fluorescent molecular probes were prepared by a programmed non‐covalent pre‐assembly process that used a near‐infrared fluorescent squaraine dye to thread a macrocycle bearing a cyclic arginine‐glycine‐aspartate peptide antagonist (cRGDfK) as a cancer targeting unit. Cell microscopy studies using OVCAR‐4 (ovarian cancer) and A549 (lung cancer) cells that express high levels of the integrin αvβ3 or αvβ5 receptors, respectively, revealed a multivalent cell targeting effect. That is, there was comparatively more cell uptake of a pre‐assembled probe equipped with two copies of the cRGDfK antagonist than a pre‐assembled probe with only one appended cRGDfK antagonist. The remarkably high photostability and low phototoxicity of these near‐infrared probes allowed for acquisition of long‐term fluorescence movies showing endosome trafficking in living cells. In vivo near‐infrared fluorescence imaging experiments compared the biodistribution of a targeted and untargeted probe in a xenograft mouse tumor model. The average tumor‐to‐muscle ratio for the pre‐assembled targeted probe was 3.6 which matches the tumor targeting performance reported for analogous cRGDfK‐based probes that were prepared entirely by covalent synthesis. The capability to excite these pre‐assembled near‐infrared fluorescent probes with blue or deep‐red excitation light makes it possible to determine if a target site is located superficially or buried in tissue, a probe performance feature that is likely to be very helpful for eventual applications such as fluorescence guided surgery.