bluuebunny/crossref_metadata_2025_split huggingface dataset:
1,4-Addition of Arylsiloxanes to Enones Catalyzed by Dicationic Palladium(II) Complexes in Aqueous Media
Authors: Nishikata Takashi , Yamamoto Yasunori , Miyaura Norio 
Published: July 2003

Abstract
Catalytic 1,4-addition of arylsiloxanes to enones was carried out at 75 °C in the presence of a dicationic palladium(II) catalyst in aqueous 1,4-dioxane. A nitrile-free complex generated in situ from Pd(dba)2 and Cu(BF4)2 in the presence of dppe or dppben was recognized to be the best catalyst to achieve high yields for the representative enones and enals.
Synthesis of New Donor–Acceptor Norbornadiene Derivatives
Authors: Nagai Takabumi , Takahashi Ikuko , Nishikubo Tadatomi 
Published: July 2003

Abstract
New donor–acceptor norbornadiene derivatives (NBDs) were synthesized from Diels–Alder reaction of methoxyphenylpentamethylcyclopendadiene with acetylene derivatives containing electron-withdrawing groups. These NBD derivatives have absorption in the visible region and photoisomerized to give thermally stable quadricyclane derivatives (QCs) with fair durability.
Unusual Enhancement of Ethylene Polymerization Activity of Benzyl Zirconium Complexes by Benzylation of the Imino Moiety of 2-(N-Aryliminomethyl)pyrrolyl Ligand
Authors: Tsurugi Hayato , Yamagata Tsuneaki , Tani Kazuhide , Mashima Kazushi 
Published: July 2003

Abstract
Reaction of Zr(CH2Ph)4 (1) with one equiv. of 2-(N-aryliminomethyl)pyrrolyl ligands (2a–e) in toluene afforded two types of products, depending upon the bulkiness of the aryl moiety. The reactions of 1 with two equiv. of the most sterically bulky 2e afforded complex 5e, whose pseudo octahedral geometry around the zirconium atom and totally dissymmetric cis-dibenzyl structure were elucidated. The high catalytic activity for ethylene polymerization was obtained by using complexes 3a and 3b.
A Novel Orthogonal Joint by Hydrogen Bonding. Pybox Ligand and Secondary Dialkylammonium Cation Complexes
Authors: Sada Kazuki , Sugimoto Takahiro , Tani Takahiro , Tateishi Yuuichi , Yi Tao , Shinkai Seiji , Maeda Hiroyuki , Tohnai Norimitsu , Miyata Mikiji 
Published: July 2003

Abstract
A novel supramolecular orthogonal joint via hydrogen bonds was constructed by a molecular complex between 2,6-bis(2-oxazolyl)pyridnes (pybox) and secondary dialkylammonium tetraphenylborates.
Reverse Micelle-assisted Route to Control Diameters of ZnO Nanorods by Selecting Different Precursors
Authors: Li Zhengquan , Xie Yi , Xiong Yujie , Zhang Rong , He Wei 
Published: July 2003

Abstract
A reverse micelle-assisted route was reported to prepare ZnO nanorods from two different precursors, Zn(NH3)42+ and Zn(OH)42−, respectively. The reverse micelles were used as microreactors, which lead into anisotropic growth of ZnO crystals during a simple solvothermal process.
A Well Characterized Example of Conversion of Molecular Configuration Depending on the Existence of Intermolecular Interactions
Authors: Zhu Qin-Yu , Zhang Yong , Dai Jie , Bian Guo-Qing , Jia Ding-Xian , Zhang Jia-Sheng , Guo Lin 
Published: July 2003

Abstract
A new complex [Ag(L)2]ClO4·2CH2Cl2 (1) (L = 4′, 5′-diaza-9′-(4,5-dimethylthio-1,3-dithiole-2-ylidene)fluorene) was synthesized. It was confirmed by 1H NMR and X-ray structure determination that when the molecules crystallize out from solution, a conversion of molecular configuration occurs because of the strong intermolecular interactions.
The tendering process: flaws and all
Authors: Spurgeon Peter , Hicks Carolyn 
Published: July 2003

The tendering process has become the dominant and now traditional approach to the allocation of research and consultancy projects. This is largely built around the notion that it ensures accountability and probity within the allocative procedure, and that high quality of work and 'value for money' are the outcomes. It appears to have become an institutionalized and unchallengeable process. Yet it is rarely costed in terms of the true resource implications for all the organizations involved, nor is quality assessed in terms of alternative processes that might be employed. This paper explores the tendering process in terms of factors that may suggest that the quality of work produced via the tendering process is not always as good as it might be. Also in a hypothetical example involving the university sector and the National Health Service, data are presented indicating that the overall cost to the public sector is often actually greater than the value of the contract being allocated. An alternative preferred provider relationship-based allocative process is advocated as an improvement to the current established tendering procedure.
Early Switch From Intravenous to Oral Antibiotics for Patients With Uncomplicated Gram-Negative Bacteremia
Authors: Tingsgård Sandra , Bastrup Israelsen Simone , Jørgensen Henrik Løvendahl , Østergaard Christian , Benfield Thomas 
Published: January 2024

ImportanceGram-negative bacteremia is a global health concern, and optimizing the transition from intravenous (IV) to oral antibiotics is a critical step in improving patient treatment and resource utilization.ObjectiveTo assess the association of switching to oral antibiotics within 4 days after initial blood culture with 90-day all-cause mortality compared with prolonged IV antibiotic treatment for patients with uncomplicated gram-negative bacteremia.Design, Setting, and ParticipantsThis cohort study conducted using the target trial emulation framework included observational data from adults with uncomplicated gram-negative bacteremia in 4 hospitals in Copenhagen, Denmark, from January 1, 2018, through December 31, 2021. The duration of follow-up was 90 days. Eligibility criteria included a blood culture positive for growth of gram-negative bacteria, clinical stability within 4 days of initial blood culture, an available susceptibility report on day 4, and initiation of appropriate empirical IV antibiotic treatment within 24 hours of blood culture.ExposureSwitching to oral antibiotics within 4 days after initial blood culture compared with continuing IV antibiotic treatment for at least 5 days after initial blood culture.Main Outcomes and MeasuresThe main outcome was 90-day all-cause mortality. Inverse probability of treatment weighting was applied to adjust for confounding. Intention-to-treat and per-protocol analyses were performed using pooled logistic regression to estimate absolute risk, risk difference (RD), and risk ratio (RR); 95% CIs were computed using bootstrapping.ResultsA total of 914 individuals were included in the target trial emulation analysis (512 [56.0%] male; median age, 74.5 years [IQR, 63.3-83.2 years]); 433 (47.4%) transitioned early to oral antibiotic treatment, and 481 (52.6%) received prolonged IV treatment. Ninety-nine individuals (10.8%) died during follow-up. The proportion of individuals who died was higher in the group receiving prolonged IV treatment (69 [14.3%] vs 30 [6.9%]). In the intention-to-treat analysis, 90-day all-cause mortality risk was 9.1% (95% CI, 6.7%-11.6%) for the early-switch group and 11.7% (95% CI, 9.6%-13.8%) for the group receiving prolonged IV treatment; the RD was −2.5% (95% CI, −5.7% to 0.7%) and RR was 0.78 (95% CI, 0.60-1.10). In the per-protocol analysis, the RD was −0.1% (95% CI, −3.4% to 3.1%) and RR was 0.99 (95% CI, 0.70-1.40).Conclusions and RelevanceIn this cohort study of uncomplicated gram-negative bacteremia, early transition to oral antibiotics within 4 days of initial blood culture was associated with 90-day all-cause mortality risk comparable to that of continuing IV antibiotic treatment and may be an effective alternative to prolonged IV treatment.
Thermal‐Cascade Multifunctional Therapeutic Systems for Remotely Controlled Synergistic Treatment of Drug‐Resistant Bacterial Infections
Authors: Zeng Zenan , Li Yachao , Deng Kefurong , Zou Dongzhe , Liu Liguo , Guo Beiling , Liu Yiming , Shen Cheng , Liang Xiaoyu , Xu Xianghui 
Published: January 2024

AbstractAntimicrobial therapy remains one of the major global challenges, particularly in the absence of effective treatment strategies for drug‐resistant bacteria. In this study, a comprehensive treatment approach is proposed for drug‐resistant bacterial wound infections based on the development of thermal‐cascade multifunctional therapeutic systems (MTSs), spanning from the design of functional nanoscale materials to macroscopic smart hydrogel. Within the MTSs, functional antibiotic‐loaded hybrid nanoclusters enable targeted therapeutic delivery and synergistic mild hyperthermia‐antibiotic treatment, strongly suppressing drug‐resistant bacteria while demonstrating excellent biocompatibility with normal cells and tissues. Furthermore, near‐infrared irradiation can trigger the photothermal effects of hybrid nanoclusters to induce gelation of thermal‐sensitive hydrogel, forming MTSs to serve as highly adaptable, drug‐enriched protective dressings for infected wounds. Both in vitro and in vivo results substantiate that MTSs enhance the bioavailability of therapeutic agents (including bacterial internalization and tissue penetration), exert synergistic effects to completely eradicate drug‐resistant bacteria, promoted wound healing and revascularization, and demonstrate excellent biocompatibility. This work offers an innovative demonstration to address drug‐resistant bacterial infections through the advancement of sophisticated material systems.
Injectable Bioadhesive Photocrosslinkable Hydrogels with Sustained Release of Kartogenin to Promote Chondrogenic Differentiation and Partial‐Thickness Cartilage Defects Repair
Authors: Han Qian , He Jiahui , Bai Lang , Huang Ying , Chen Baojun , Li Zhenlong , Xu Meiguang , Liu Qiaonan , Wang Shuai , Wen Nuanyang , Zhang Jing , Guo Baolin , Yin Zhanhai 
Published: January 2024

AbstractPartial‐thickness cartilage defect (PTCD) is a common and formidable clinical challenge without effective therapeutic approaches. The inherent anti‐adhesive characteristics of the extracellular matrix within cartilage pose a significant impediment to the integration of cells or biomaterials with the native cartilage during cartilage repair. Here, an injectable photocrosslinked bioadhesive hydrogel, consisting of gelatin methacryloyl (GM), acryloyl‐6‐aminocaproic acid‐g‐N‐hydroxysuccinimide (AN), and poly(lactic‐co‐glycolic acid) microspheres loaded with kartogenin (KGN) (abbreviated as GM/AN/KGN hydrogel), is designed to enhance interfacial integration and repair of PTCD. After injected in situ at the irregular defect, a stable and robust hydrogel network is rapidly formed by ultraviolet irradiation, and it can be quickly and tightly adhered to native cartilage through amide bonds. The hydrogel exhibits good adhesion strength up to 27.25 ± 1.22 kPa by lap shear strength experiments. The GM/AN/KGN hydrogel demonstrates good adhesion, low swelling, resistance to fatigue, biocompatibility, and chondrogenesis properties in vitro. A rat model with PTCD exhibits restoration of a smoother surface, stable seamless integration, and abundant aggrecan and type II collagen production. The injectable stable adhesive hydrogel with long‐term chondrogenic differentiation capacity shows great potential to facilitate repair of PTCD.
Leveraging Oriented Lateral Walls of Nerve Guidance Conduit with Core–Shell MWCNTs Fibers for Peripheral Nerve Regeneration
Authors: Sun Renyuan , Lang Yuna , Chang Ming‐Wei , Zhao Mingkang , Li Chao , Liu Shiheng , Wang Baolin 
Published: January 2024

AbstractPeripheral nerve regeneration and functional recovery rely on the chemical, physical, and structural properties of nerve guidance conduits (NGCs). However, the limited support for long‐distance nerve regeneration and axonal guidance has hindered the widespread use of NGCs. This study introduces a novel nerve guidance conduit with oriented lateral walls, incorporating multi‐walled carbon nanotubes (MWCNTs) within core‐shell fibers prepared in a single step using a modified electrohydrodynamic (EHD) printing technique to promote peripheral nerve regeneration. The structured conduit demonstrated exceptional stability, mechanical properties, and biocompatibility, significantly enhancing the functionality of NGCs. In vitro cell studies revealed that RSC96 cells adhered and proliferated effectively along the oriented fibers, demonstrating a favorable response to the distinctive architectures and properties. Subsequently, a rat sciatic nerve injury model demonstrated effective efficacy in promoting peripheral nerve regeneration and functional recovery. Tissue analysis and functional testing highlighted the significant impact of MWCNT concentration in enhancing peripheral nerve regeneration and confirming well‐matured aligned axonal growth, muscle recovery, and higher densities of myelinated axons. These findings demonstrate the potential of oriented lateral architectures with coaxial MWCNT fibers as a promising approach to support long‐distance regeneration and encourage directional nerve growth for peripheral nerve repair in clinical applications.
Self‐Propelled Nanomotor for Cancer Precision Combination Therapy
Authors: Lu Yijie , Liu Shikang , Liang Jiarong , Wang Zhiyi , Hou Yanglong 
Published: January 2024

AbstractThe emergence of nanomotor provides an innovative concept for tumor treatment strategies. Conventional chemotherapeutic agents for tumors exit various therapeutic constraints due to the unique microenvironment of the tumor itself. Calcium overload, the aberrant accumulation of free calcium ions in the cytoplasm, is a well‐recognized contributor to damage and even cell death in numerous cell types. Such undesired destructive processes can be a novel means applicable to cancer ion interference therapy. Herein, the chemotherapeutic drug doxorubicin (DOX) and calcium peroxide as the driving force into nanomotors through a facile and understandable experimental scheme are successfully assembled. The modification of nucleic acid aptamer and NIR‐II fluorescent molecules on its surface simultaneously strengthens both the active targeting and imaging capability of tumor loci. Therefore, by a comprehensive assessment of nanomotors both in vitro and in vivo experiments, CaO2/DOX@HPS‐IR‐1061‐AS1411 demonstrates superior killing effects on tumor cells, and the intracellular reactive oxygen species produced by nanomotors is verified by molecular biology experiments to induce apoptosis of tumor cells and further achieve tumor therapeutic effects.
Fouling Inhibition by Replenishable Plastrons on Microstructured, Superhydrophobic Carbon‐Silicone Composite Coatings
Authors: Manderfeld Emily , Vogler Louisa , Rosenhahn Axel 
Published: January 2024

AbstractSuperhydrophobic surfaces are known to resist diatom and bacteria adhesion if stable air layers are formed underwater (known as a plastron). However, most preparation techniques to obtain superhydrophobic surfaces need sophisticated chemical treatments and/or complicated chemical procedures. Here a 3D printing technique is used to create different molds for polymer casting. A conductive graphite‐carbon black‐silicone composite mixture is developed to fabricate different polymer surface casts from these molds. The obtained surfaces exhibited contact angles >145°, which led to a plastron formation on the surfaces underwater, and areas with intact plastrons protected the samples from diatom attachment. Due to the conductivity of the coatings, it is possible to replenish the plastrons by heating the surfaces.
Optimizing Wavelength for Enhanced Cycling Durability of Laser‐Induced Phase Change in Sb2S3 Films: A Survey on Optical Transmission Phase Shift
Authors: Gao Kun , Qiang Feifan , Tian Senmao , Tan Yu , Liu Siyuan , Zhang Wending , Mei Ting 
Published: January 2024

AbstractThe advancement of nonvolatile reconfigurable photonic elements has led to the development of Sb2S3 as a desirable phase change material for optical phase modulation in visible and near‐infrared wavebands. However, achieving long‐lasting cycling durability of the phase change remains a formidable challenge. Traditional characterization methods like transmittance or reflectance measurement fail to provide a quantitative assessment of the degree of phase change. To address this, the study focuses on enhancing the cycling durability of complete phase change in Sb2S3 films by manipulating the wavelength of a femtosecond laser for amorphization. To accurately measure optical transmission phase shifts during phase change experiments, a novel liquid‐crystal retardance matching technique based on the Mach–Zehnder interferometer is developed. This approach allows for a direct and quantitative assessment of the degree of phase change without relying on an optical model. The findings reveal that longer wavelengths and multi‐pulse irradiation with increasing pulse energy significantly enhance the cycling durability of the phase change. Additionally, the cost‐effective customization of nonvolatile photonic elements is demonstrated using laser direct writing, eliminating the need for lithography. It is anticipated that this work will drive advancements in Sb2S3‐based reconfigurable devices and contribute to the broader field of nonvolatile reconfigurable photonic elements.
Organocatalytic Enantioselective (4+2) Annulation of Cyclopropane Carbaldehydes with 2‐Mercapto‐1‐Arylethanones
Authors: Yadav Neeraj , Hazra Arijit , Singh Priyanka , Banerjee Prabal 
Published: January 2024

AbstractHere, we report the organocatalytic enantioselective synthesis of dihydrothiopyran derivatives from trans racemic donor–acceptor cyclopropane carbaldehydes (DACCs) and 2‐mercapto‐1‐arylethanone via formal thio (4+2) cycloaddition involving thia‐Michael aldol condensation and annulation. Mechanistic studies indicate a typical kinetic resolution (KR) is involved in this transformation, which results in moderate yields and enantiomeric ratios. Remarkably, this method is characterized by its one‐pot simplicity, mild reaction conditions, and resilience towards air and moisture interference.
Silver‐Catalyzed Decarboxylative Acylfluorination of Two Alkenes with Ketonic Acids
Authors: Liu Ren‐Xiang , Wang Wei , Yang Luo 
Published: January 2024

AbstractAn acylative fluorination of two different alkenes is developed, assisted by the interaction of silver catalyst and Selectflour. Various α‐ketonic acids can be decarboxylated to form acyl radicals at 35 °C, sequentially add to the electron‐deficient and electron‐ rich alkenes to provide the benzyl fluorinated compounds containing diversified functional groups.
Rational Design of Three Dimensional Hollow Heterojunctions for Efficient Photocatalytic Hydrogen Evolution Applications
Authors: Pan Jingwen , Wang Dongbo , Wu Donghai , Cao Jiamu , Fang Xuan , Zhao Chenchen , Zeng Zhi , Zhang Bingke , Liu Donghao , Liu Sihang , Liu Gang , Jiao Shujie , Xu Zhikun , Zhao Liancheng , Wang Jinzhong 
Published: January 2024

AbstractThe efficiency of photocatalytic hydrogen evolution is currently limited by poor light adsorption, rapid recombination of photogenerated carriers, and ineffective surface reaction rate. Although heterojunctions with innovative morphologies and structures can strengthen built‐in electric fields and maximize the separation of photogenerated charges. However, how to rational design of novel multidimensional structures to simultaneously improve the above three bottleneck problems is still a research imperative. Herein, a unique Cu2O─S@graphene oxide (GO)@Zn0.67Cd0.33S Three dimensional (3D) hollow heterostructure is designed and synthesized, which greatly extends the carrier lifetime and effectively promotes the separation of photogenerated charges. The H2 production rate reached 48.5 mmol g−1 h−1 under visible light after loading Ni2+ on the heterojunction surface, which is 97 times higher than that of pure Zn0.67Cd0.33S nanospheres. Furthermore, the H2 production rate can reach 77.3 mmol g−1 h−1 without cooling, verifying the effectiveness of the photothermal effect. Meanwhile, in situ characterization and density flooding theory calculations reveal the efficient charge transfer at the p‐n 3D hollow heterojunction interface. This study not only reveals the detailed mechanism of photocatalytic hydrogen evolution in depth but also rationalizes the construction of superior 3D hollow heterojunctions, thus providing a universal strategy for the materials‐by‐design of high‐performance heterojunctions.
Development of Synthetically Accessible Glycolated Polythiophenes for High‐Performance Organic Electrochemical Transistors
Authors: Ding Bowen , Le Vianna , Yu Hang , Wu Guanchen , Marsh Adam V. , Gutiérrez‐Fernández Edgar , Ramos Nicolás , Rimmele Martina , Martín Jaime , Nelson Jenny , Paterson Alexandra F. , Heeney Martin 
Published: January 2024

AbstractFour glycolated polythiophene‐based organic mixed ionic‐electronic conductors (OMIECs), PE2gTT, PE2gT, PT2gTT, and PT2gT are prepared by atom‐efficient direct arylation polymerization, avoiding the need for toxic organometallic precursors. PE2gT, PT2gTT, and PT2gT are operable in p‐type accumulation mode organic electrochemical transistors (OECTs), with PT2gT displaying the best device performance with a µC* product figure‐of‐merit of 290 F cm−1 V−1 s−1. A record volumetric capacitance among p‐type glycolated polythiophene OMIECs of 313 F cm−3 is observed for PE2gT, ascribed to the high proportionality of polar components in its materials design. The good OECT performance of PE2gT with µC* = 84.2 F cm−1 V−1 s−1, comparable with state‐of‐the‐art poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) devices, coupled with its synthetic accessibility and favorable accumulation mode operation makes PE2gT an ideal glycolated alternative to PEDOT:PSS in bioelectronics. PE2gT with the least negative threshold voltage also displays the best OECT operational cycling stability, linked to better resistance of its oxidized state against parasitic redox side reactions . Shelf life stability of OECTs stored (without bias) is observed to be better for materials with a more negative threshold voltage and higher average molecular weight (PT2gT), that are less susceptible to ambient auto‐oxidation and film delamination.
Applications of Emerging Metal and Covalent Organic Frameworks in Perovskite Photovoltaics: Materials and Devices
Authors: Cao Jiupeng , Tang Guanqi , Yan Feng 
Published: January 2024

AbstractPerovskite solar cells (PSCs) have emerged as the next generation photovoltaic technology due to their high power conversion efficiency and solution‐based fabrication process. The performance of PSCs relies on the composition of each layer and the interface properties between layers. Hence, the integration of novel materials into PSCs presents a viable strategy for enhancing device performance. Metal–organic frameworks (MOFs) and covalent organic frameworks (COFs) have recently emerged as promising materials for improving the efficiency and stability of PSCs. These materials offer a diverse range of tunable physicochemical properties and functionalities. This comprehensive review aims to provide an in‐depth summary of the progress in utilizing MOFs/COFs in PSCs. The review covers key aspects such as their electronic properties, synthesis methods, and various applications within PSCs, including their role as different components and their potential as lead absorbents. Finally, the review outlines important challenges and highlights future prospects for advancing this technology.