bluuebunny/crossref_metadata_2025_split huggingface dataset:
Rechargeable Zn–CO2 Electrochemical Cells Mimicking Two‐Step Photosynthesis
Authors: Wang Xueyuan , Xie Jiafang , Ghausi Muhammad Arsalan , Lv Jiangquan , Huang Yiyin , Wu Maoxiang , Wang Yaobing , Yao Jiannian 
Published: February 2019

AbstractMetal–CO2 batteries represent a promising priority for sustainable energy and the environment. However, CO2 utilization in nonaqueous electrolytes mostly involves difficult CO2 electrochemistry, leading to poor selectivity and limited cycle performance. Herein, an aqueous rechargeable Zn–CO2 electrochemical cell that tunably produced CO fuel gas (90% Faradaic efficiency) during cell discharge (cathodic reaction: CO2 + 2e− + 2H+ → CO + H2O) and O2 during cell charge at ≈2 V (cathodic reaction: H2O → 1/2O2 + 2e− + 2H+), mimicking the separate steps of CO2 fixation and water oxidation during photosynthesis while exhibiting the advantages of high efficiency, tunable products, and operation independent of sunlight is proposed and realized. The cell achieves a remarkable energy efficiency of 68% with fuel generation, providing an alternative for the green, efficient, and safe utilization of CO2 by metal–CO2 batteries.
Engineered Bacterial Bioreactor for Tumor Therapy via Fenton‐Like Reaction with Localized H2O2 Generation
Authors: Fan Jin‐Xuan , Peng Meng‐Yun , Wang He , Zheng Hao‐Ran , Liu Zong‐Lin , Li Chu‐Xin , Wang Xia‐Nan , Liu Xin‐Hua , Cheng Si‐Xue , Zhang Xian‐Zheng 
Published: February 2019

AbstractSynthetic biology based on bacteria has been displayed in antitumor therapy and shown good performance. In this study, an engineered bacterium Escherichia coli MG1655 is designed with NDH‐2 enzyme (respiratory chain enzyme II) overexpression (Ec‐pE), which can colonize in tumor regions and increase localized H2O2 generation. Following from this, magnetic Fe3O4 nanoparticles are covalently linked to bacteria to act as a catalyst for a Fenton‐like reaction, which converts H2O2 to toxic hydroxyl radicals (•OH) for tumor therapy. In this constructed bioreactor, the Fenton‐like reaction occurs with sustainably synthesized H2O2 produced by engineered bacteria, and severe tumor apoptosis is induced via the produced toxic •OH. These results show that this bioreactor can achieve effective tumor colonization, and realize a self‐supplied therapeutic Fenton‐like reaction without additional H2O2 provision.
Survival outcomes of appendiceal mucinous neoplasms by histological type and stage: Analysis of 266 cases in a multicenter collaborative retrospective clinical study
Authors: Sueda Toshinori , Murata Kohei , Takeda Takashi , Kagawa Yoshinori , Hasegawa Junichi , Komori Takamichi , Noura Shingo , Ikeda Kimimasa , Tsujie Masaki , Ohue Masayuki , Ota Hirofumi , Ikenaga Masakazu , Hata Taishi , Matsuda Chu , Mizushima Tsunekazu , Yamamoto Hirofumi , Sekimoto Mitsugu , Nezu Riichiro , Mori Masaki , Doki Yuichiro 
Published: February 2019

AbstractAimAppendiceal mucinous neoplasms are rare, and thus the literature is sparse with regard to histological types, staging, and prognosis. In particular, it is unclear how long‐term outcome may differ between mucinous adenocarcinomas and other adenocarcinomas. In the present study, we aimed to investigate the histological types and stages of appendiceal neoplasms, and to evaluate the prognostic impacts of these factors in patients with mucinous adenocarcinomas and non‐mucinous adenocarcinomas.MethodsPatients with appendiceal tumors diagnosed between 2007 and 2016 were retrospectively identified from the databases of 19 institutions in the Clinical Study Group of Osaka University, Colorectal Group.ResultsA total of 266 patients with appendiceal tumors were identified, of whom 130 had pathologically diagnosed adenocarcinomas, including 57 with mucinous adenocarcinomas and 73 with non‐mucinous adenocarcinomas. Five‐year overall survival (OS) rates were 64.5% for mucinous adenocarcinomas, and 49.0% for non‐mucinous adenocarcinomas. OS was significantly shorter among patients with non‐mucinous adenocarcinomas compared to mucinous adenocarcinomas. Among patients with mucinous adenocarcinomas, 5‐year OS rates were 53.6% for stage 0/I, 82.6% for II/III, and 48.4% for IV. Among patients with non‐mucinous adenocarcinomas, 5‐year OS rates were 90.9% for stage 0/I, 68.8% for II/III, and 7.1% for IV. Analysis of patients with stage IV disease revealed significantly shorter OS among patients with non‐mucinous adenocarcinomas compared to mucinous adenocarcinomas.ConclusionOur present findings showed a better prognosis in patients with mucinous adenocarcinomas compared to non‐mucinous adenocarcinomas. In this setting, Union for International Cancer Control staging was associated with prognosis for non‐mucinous adenocarcinomas, but not for mucinous adenocarcinomas.
Enhancing the National Dialogue on the Prevention of Intimate Partner Violence
Authors: Estefan Lianne Fuino , Armstead Theresa L. , Rivera Moira Shaw , Kearns Megan C. , Carter Denise , Crowell Jessica , El‐Beshti Rasha , Daniels Brandy 
Published: February 2019

AbstractLittle systematic information exists about how community‐based prevention efforts at the state and local levels contribute to our knowledge of intimate partner violence (IPV) prevention. The Centers for Disease Control and Prevention's (CDC) DELTA FOCUS program funds ten state domestic violence coalitions to engage in IPV primary prevention through approaches addressing the outer layers of the social ecology. This paper explored the ways in which DELTA FOCUS recipients have contributed to a national‐level dialogue on IPV prevention. Previously undefined, the authors define national‐level dialogue and retrospectively apply the CDC Science Impact Framework (SIF) to describe contributions DELTA FOCUS recipients made to it. Authors conducted document review and qualitative content analysis of recipient semi‐annual progress reports from 2014 to 2016 (N = 40) using NVivo. A semi‐structured coding scheme was applied across the five SIF domains: Creating Awareness, Catalyzing Action, Effecting Change, Disseminating Science, and Shaping the Future. All recipients sought to promote IPV prevention by communicating and sharing with non‐CDC‐funded state coalitions, national partners, and other IPV stakeholders information and resources accumulated through practice‐based prevention efforts. Through implementing and disseminating their prevention work in myriad ways, DELTA FOCUS recipients are building practice‐based evidence on community‐based IPV prevention.
Sulfide‐Catalyzed Trifluoromethylthiolation‐Cyclization of Tryptamine Derivatives
Authors: Guo Rui , Cai Baohua , Jin Ming Yu , Mu Huaixue , Wang Jun (Joelle) 
Published: February 2019

AbstractA catalytic method for the incorporation of an SCF3group to tryptamine derivatives was developed via a sulfide‐catalyzed cascade trifluoromethylthiolation‐cyclization. A series of C(3)‐CF3S pyrrolidinoindolines were obtained in moderate to good yields under mild conditions. Furthermore, some enantioselectivity was observed when using chiral sulfide thiocineole as a catalyst.
Aggressive or funerary cannibalism? Skull‐cup and human bone manipulation in Cueva de El Toro (Early Neolithic, southern Iberia)
Authors: Santana Jonathan , Rodríguez‐Santos Francisco Javier , Camalich‐Massieu María Dolores , Martín‐Socas Dimas , Fregel Rosa 
Published: February 2019

AbstractObjectiveWe analyze the processing sequence involved in the manufacture of a skull‐cup and the manipulation of human bones from the Early Neolithic of Cueva de El Toro (Málaga, Spain).Materials and methodsThe Early Neolithic material studied includes human remains found in two separate assemblages. Assemblage A consists of one skull‐cup, a non‐manipulated adult human mandible, and four ceramic vessels. Assemblage B contains manipulated and non‐manipulated human remains that appeared mingled with domestic waste. Using a taphonomic approach, we evaluate the skull‐cup processing and the anthropogenic alteration of human bones.ResultsThe skull‐cup was processed by careful paring away of skin, fragmentation of the facial skeleton and base of the skull, and controlled percussion of the edges of the calotte to achieve a regular shape. It was later boiled for some time in a container that caused pot polish in a specific area. The other human bones appeared scattered throughout the living area, mixed with other remains of domestic activity. Some of these bones show cut marks, percussion damage for marrow extraction, and tooth/chewing marks.DiscussionEvidence from Cueva de El Toro suggests that cannibalism was conducted in the domestic sphere, likely following ritualized practices where the skull‐cup could have played a part. Interpretation of this evidence suggests two hypotheses: (a) aggressive cannibalism relates to extreme inter‐group violence; and (b) funerary cannibalism is a facet of multi‐stage burial practices. Similar evidence has been found in other Neolithic sites of this region and suggests that cannibalism and skull‐cups were elements widespread in these communities. These practices may be linked to significant transformations associated with the end of the Early Neolithic in southern Iberia.
Distractors in obstetric ultrasound: Do sonographers have safety concerns?
Authors: Najafzadeh Afrooz , Woodrow Nicole , Thoirs Kerry 
Published: February 2019

AbstractIntroductionObstetric sonography is a highly skilled diagnostic medical examination. Pregnant women like to socialise their ultrasound experience with family, introducing distractions for the sonographer. Our objective was to survey ultrasound practitioners to identify concerns regarding interruptions and their opinions about socialisation during the examination.MethodsAn online questionnaire was disseminated to study the views of Australian and New Zealand obstetric sonographers/sonologists. It was informed by a pilot study of possible distractors with quality and safety concerns and operator opinions regarding family bonding.ResultsThe opinions of 393 obstetric sonographers/sonologists informed our results. Distractors with the most negative aspects included disruptive children (93.3%) and mobile phone conversations (84.3%). Most respondents (62%) believed that a distractor only had to be present for 5 min or less to have an impact. Small children were identified by 87.5% of respondents as safety risks to themselves, to the patient and to sonographers. Sonographers were concerned that distractors caused a loss of concentration, interruption to a systematic scanning approach and increased false negatives in screening, missing important diagnoses. Sonographers strongly agreed that obstetric sonography facilitated maternal–fetal bonding, but only 15% thought that siblings bond with the fetus during the scan.ConclusionObstetric sonographers in our study are concerned that distractors pose a negative impact on the quality and safety of ultrasound. They also recognise the importance of family bonding. Strategies to bridge the medical and social components of obstetric sonography should be developed to reduce quality and safety threats.
Magnetic resonance imaging–guided phase 1 trial of putaminal AADC gene therapy for Parkinson's disease
Authors: Christine Chadwick W. , Bankiewicz Krystof S. , Van Laar Amber D. , Richardson R. Mark , Ravina Bernard , Kells Adrian P. , Boot Brendon , Martin Alastair J. , Nutt John , Thompson Marin E. , Larson Paul S. 
Published: February 2019

ObjectiveTo understand the safety, putaminal coverage, and enzyme expression of adeno‐associated viral vector serotype‐2 encoding the complementary DNA for the enzyme, aromatic L‐amino acid decarboxylase (VY‐AADC01), delivered using novel intraoperative monitoring to optimize delivery.MethodsFifteen subjects (three cohorts of 5) with moderately advanced Parkinson's disease and medically refractory motor fluctuations received VY‐AADC01 bilaterally coadministered with gadoteridol to the putamen using intraoperative magnetic resonance imaging (MRI) guidance to visualize the anatomic spread of the infusate and calculate coverage. Cohort 1 received 8.3 × 1011vg/ml and ≤450 μl per putamen (total dose, ≤7.5 × 1011vg); cohort 2 received the same concentration (8.3 × 1011vg/ml) and ≤900 μl per putamen (total dose, ≤1.5 × 1012vg); and cohort 3 received 2.6 × 1012vg/ml and ≤900 μl per putamen (total dose, ≤4.7 × 1012vg). (18)F‐fluoro‐L‐dihydroxyphenylalanine positron emission tomography (PET) at baseline and 6 months postprocedure assessed enzyme activity; standard assessments measured clinical outcomes.ResultsMRI‐guided administration of ascending VY‐AADC01 doses resulted in putaminal coverage of 21% (cohort 1), 34% (cohort 2), and 42% (cohort 3). Cohorts 1, 2, and 3 showed corresponding increases in enzyme activity assessed by PET of 13%, 56%, and 79%, and reductions in antiparkinsonian medication of –15%, –33%, and –42%, respectively, at 6 months. At 12 months, there were dose‐related improvements in clinical outcomes, including increases in patient‐reported ON‐time without troublesome dyskinesia (1.6, 3.3, and 1.5 hours, respectively) and quality of life.InterpretationNovel intraoperative monitoring of administration facilitated targeted delivery of VY‐AADC01 in this phase 1 study, which was well tolerated. Increases in enzyme expression and clinical improvements were dose dependent.
ClinicalTrials.gov Identifier: NCT01973543 Ann Neurol 2019;85:704–714
Total Synthesis of Carthamin, a Traditional Natural Red Pigment
Authors: Azami Kohei , Hayashi Taiki , Kusumi Takenori , Ohmori Ken , Suzuki Keisuke 
Published: February 2019

AbstractThe first total synthesis of carthamin (3), a historic natural red pigment, has been achieved. The molecular structure was efficiently constructed by assembling two equivalents of the in situ generated lithiated monomers and triisopropyl orthoformate. This synthesis confirms the structure proposed in 1996.
CsSbF2SO4: An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO4 (KTP)‐type Structure
Authors: Dong Xuehua , Huang Ling , Hu Cuifang , Zeng Hongmei , Lin Zhien , Wang Xin , Ok Kang Min , Zou Guohong 
Published: February 2019

AbstractA novel noncentrosymmetric (NCS) polar fluoride sulfate, CsSbF2SO4, was obtained by ionothermal synthesis. A meticulously designed co‐substitution approach was used to successfully replace the [TiO6]8− and [PO4]3− functional groups in KTiOPO4 (KTP) with [SbO4F2]7− and [SO4]2− units, respectively. The structure of CsSbF2SO4 features a pseudo‐3D framework consisting of interconnected 1D [SbF2O2SO4]5− chains of corner‐sharing [SbO4F2]7− octahedra and [SO4]2− tetrahedra. The title compound exhibits a sharply enlarged band gap compared to its parent compound, KTP, benefitting from the introduction of F− ions and the displacement of Sb3+ cations. Second harmonic generation (SHG) measurements manifested that CsSbF2SO4 is phase‐matchable and revealed a strong SHG response of about 3.0 KH2PO4 (KDP), which is the highest value reported for any metal sulfate reported to date. The reported fluoride sulfate is a promising near ultraviolet (UV) nonlinear optical (NLO) material.
Terpolymers from Borane‐Initiated Copolymerization of Triphenyl Arsonium and Sulfoxonium Ylides: An Unexpected Light Emission
Authors: Wang De , Hadjichristidis Nikos 
Published: February 2019

AbstractThe first synthesis of well‐defined poly[(phenylmethylene‐co‐methylpropenylene)‐b‐methylene, [(C1‐co‐C3)‐b‐C1], terpolymers was achieved by one‐pot borane‐initiated random copolymerization of ω‐methylallyl (C3 units, chain is growing by three carbon atoms at a time) and benzyltriphenylarsonium (C1 units, chain is growing by one carbon atom at a time) ylides, followed by polymerization of sulfoxonium methylide (C1 units). Other substituted arsonium ylides, such as prenyltriphenyl, propyltriphenyl and (4‐fluorobenzyl)triphenyl can also be used instead of benzyltriphenylarsonium. The obtained terpolymers are well‐defined, possess a predictable molecular weight and low polydispersity (Mn,NMR=1.83–9.68×103 g mol−1, Đ=1.09–1.22). An unexpected light emission phenomenon was discovered in these non‐conjugated terpolymers, as confirmed by fluorescence and NMR spectroscopy. This phenomenon can be explained by the isomerization of the double bonds of allylic monomeric units along the chain of the terpolymers (isomerization‐induced light emission).
A Nucleophilicity Scale for the Reactivity of Diazaphospholenium Hydrides: Structural Insights and Synthetic Applications
Authors: Zhang Jingjing , Yang Jin‐Dong , Cheng Jin‐Pei 
Published: February 2019

AbstractNucleophilicity parameters (N, sN) of a group of representative diazaphospholenium hydrides were derived by kinetic investigations of their hydride transfer to a series of reference electrophiles with known electrophilicity (E) values, using the Mayr equation log k2=sN(N+E). The N scale covers over ten N units, ranging from the most reactive hydride donor (N=25.5) to the least of the scale (N=13.5). This discloses the highest N value ever quantified in terms of Mayr's nucleophilicity scales reported for neutral transition‐metal‐free hydride donors and implies an exceptional reactivity of this reagent. Even the least reactive hydride donor of this series is still a better hydride donor than those of many other nucleophiles such as the C−H, B−H, Si−H and transition‐metal M−H hydride donors. Structure–reactivity analysis reveals that the outstanding hydricity of 2‐H‐1,3,2‐diazaphospholene benefits from the unsaturated skeleton.
Utilizing d–pπ Bonds for Ultralong Organic Phosphorescence
Authors: Tian Shuai , Ma Huili , Wang Xuan , Lv Anqi , Shi Huifang , Geng Yun , Li Jie , Liang Fushun , Su Zhong‐Min , An Zhongfu , Huang Wei 
Published: February 2019

AbstractDeveloping pure organic materials with ultralong lifetimes is attractive but challenging. Here we report a concise chemical approach to regulate the electronic configuration for phosphorescence enhancement. After the introduction of d–pπ bonds into a phenothiazine model system, a phosphorescence lifetime enhancement of up to 19 times was observed for DOPPMO, compared to the reference PPMO. A record phosphorescence lifetime of up to 876 ms was obtained in phosphorescent phenothiazine. Theoretical calculations and single‐crystal analysis reveal that the d–pπ bond not only reduces the (n, π*) proportion of the T1 state, but also endows the rigid molecular environment with multiple intermolecular interactions, thus enabling long‐lived phosphorescence. This finding makes a valuable contribution to the prolongation of phosphorescence lifetimes and the extension of the scope of phosphorescent materials.
A Size‐Flexible Organometallic Box for the Encapsulation of Fullerenes
Authors: Martínez‐Agramunt Victor , Eder Tobias , Darmandeh Heidar , Guisado‐Barrios Gregorio , Peris Eduardo 
Published: February 2019

AbstractA palladium‐cornered molecular square with four pyrene‐bis(imidazolylidene) bridging ligands is reported. This metallo‐polygon can encapsulate C60 and C70. The X‐ray diffraction structures of the empty cage as well as the cages complexed with both fullerenes are described. The fullerene encapsulation produces perturbations in the structural parameters of the metallo‐square, showing that it can adjust the shape of its cavity to the size of each fullerene.
Understanding the Mechanocatalytic Conversion of Biomass: A Low‐Energy One‐Step Reaction Mechanism by Applying Mechanical Force
Authors: Amirjalayer Saeed , Fuchs Harald , Marx Dominik 
Published: February 2019

AbstractOn the way to establishing biomass as a renewable and environmentally friendly source to cover the ever‐increasing global demand on energy and chemicals, one great challenge is the efficient depolymerization of cellulose. Enhanced conversion rates have been discovered in ball‐milling experiments, thus opening a mechanocatalytic approach. However, an understanding of the impact of mechanical forces on the acid‐catalyzed cleavage of glycosidic bonds at the molecular level is still missing. Herein, we contribute such fundamental insight based on atomistic modeling. Mechanically stressing the macromolecular backbone radically changes the depolymerization pathway from a complex high‐barrier reaction upon thermal activation to a low‐energy single‐step mechanocatalytic process. In addition to revealing a regioselective increase in basicity under a mechanical force, our results provide molecular‐level explanations of the experimental findings and might therefore guide rational ways to improve such mechanocatalytic processes.
Instructed Assembly as Context‐Dependent Signaling for the Death and Morphogenesis of Cells
Authors: Wang Huaimin , Feng Zhaoqianqi , Xu Bing 
Published: February 2019

AbstractContext‐dependent signaling is a ubiquitous phenomenon in nature, but ways to mimic the essence of these nano‐ and microscale dynamic molecular processes by noncovalent synthesis in the cellular environment have yet to be developed. Herein we present a dynamic continuum of noncovalent filaments formed by the instructed assembly (iA) of a supramolecular phosphoglycopeptide (sPGP) as context‐dependent signals for controlling the death and morphogenesis of cells. Specifically, ectophosphatase enzymes on cancer cells catalyze the formation of sPGP filaments to result in cell death; however, damping of the enzyme activity induces the formation 3D cell spheroids. Similarly, the ratio of stromal and cancer cells in a coculture can be used to modulate the expression of the ectophosphatase, so that the iA process leads to the formation of cell spheroids. The spheroids mimic the tumor microenvironment for drug screening.
Visible‐Light‐Induced Passerini Multicomponent Polymerization
Authors: Tuten Bryan T. , De Keer Lies , Wiedbrauk Sandra , Van Steenberge Paul H. M. , D'hooge Dagmar R. , Barner‐Kowollik Christopher 
Published: February 2019

AbstractHerein, we introduce an additive‐free visible‐light‐induced Passerini multicomponent polymerization (MCP) for the generation of high molar mass chains. In place of classical aldehydes (or ketones), highly reactive, in situ photogenerated thioaldehydes are exploited along with isocyanides and carboxylic acids. Prone to side reactions, the thioaldehyde moieties create a complex reaction environment which can be tamed by optimizing the synthetic conditions utilizing stochastic reaction path analysis, highlighting the potential of semi‐batch procedures. Once the complex MCP environment is understood, step‐growth polymers can be synthesized under mild reaction conditions which—after a Mumm rearrangement—result in the incorporation of thioester moieties directly into the polymer backbone, leading to soft matter materials that can be degraded by straightforward aminolysis or chain expanded by thiirane insertion.
Poly(lactic acid) composite films reinforced with microcrystalline cellulose and keratin from chicken feather fiber in 1‐butyl‐3‐methylimidazolium chloride
Authors: Khaw Ying Ying , Chee Ching Yern , Gan Seng Neon , Singh Ramesh , Ghazali Nik Nazri Nik , Liu Nan‐Shang 
Published: February 2019

ABSTRACTAmphiphilic keratin from chicken feather fiber (CFF) and hydrophilic cellulose were incorporated as fillers into hydrophobic poly(lactic acid) (PLA) polymer blend. This study implemented ionic liquid (IL) of 1‐butyl‐3‐methylimidazolium chloride (BMIMCl) to dissolve the 1 wt % fillers. The composite films were compared with and without the addition of IL prepared from five sets of ratios of CFF to MCC using measuring mixers and compression molding. Thermal analysis showed that increase in CFF composition decreases the glass‐transition temperature (T
g), and crystallization temperature (T
c) as well as increases the degree of crystallinity. PLA composite with the 70/30 ratio of CFF to MCC was found to be the optimum composition in obtaining considerably low T
g and high crystallinity. BMIMCl enhanced the miscibility of the composites as observed in scanning electron microscope images and single T
g. Apart from creating porous structure and lowering mechanical hardness, BMIMCl also decreased the thermal stability of the PLA composites. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47642.