bluuebunny/crossref_metadata_2025_split huggingface dataset:
Iron ions embedded in hexagonal mesoporous silica via a simple method: implementation in mild oxidation catalysis
Authors: Guemati Redouane , Rebilly Jean‐Noël , Fornasieri Giulia , Dragoe Diana , Biswas Subharanjan , Banse Frédéric , Bleuzen Anne 
Published: October 2023

AbstractMesoporous silica monoliths containing dispersed FeIII sites have been prepared following a direct and simple synthetic method. The iron‐containing materials are able to catalyze the epoxidation of cyclooctene by H2O2 under mild conditions. Textural and spectrophotometric analyses reveal that, when the thermal treatment temperature of the materials increases (from 500 °C to 1000 °C), the pore diameter of the silica matrix decreases while the formation of small oxo‐iron(III) clusters is promoted. Among the five materials obtained after treatment at 500, 700, 800, 900 or 1000 °C, the one prepared at 700 °C exhibits the best catalytic performances. This indicates that a compromise must be found between several parameters, such as the pore size (which decreases with calcination temperature) and the hydrophobicity of the channel surface (which is favored at higher temperature), for an optimal reactivity.
Tailoring C─N Containing Compounds into Carbon Nanomaterials with Tunable Morphologies for Electrocatalytic Applications
Authors: Wan Wenchao , Zhao Yonggui , Meng Jie , Allen Christopher S. , Zhou Ying , Patzke Greta R. 
Published: October 2023

AbstractCarbon materials with unique sp2‐hybridization are extensively researched for catalytic applications due to their excellent conductivity and tunable physicochemical properties. However, the development of economic approaches to tailoring carbon materials into desired morphologies remains a challenge. Herein, a convenient “bottom‐up” strategy by pyrolysis of graphitic carbon nitride (g‐C3N4) (or other carbon/nitrogen (C, N)‐enriched compounds) together with selected metal salts and molecules is reported for the construction of different carbon‐based catalysts with tunable morphologies, including carbon nano‐balls, carbon nanotubes, nitrogen/sulfur (S, N) doped‐carbon nanosheets, and single‐atom catalysts, supported by carbon layers. The catalysts are systematically investigated through various microscopic, spectroscopic, and diffraction methods and they demonstrate promising and broad applications in electrocatalysis such as in the oxygen reduction reaction and water splitting. Mechanistic monitoring of the synthesis process through online thermogravimetric‐gas chromatography‐mass spectrometry measurements indicates that the release of C─N‐related moieties, such as dicyan, plays a key role in the growth of carbon products. This enables to successfully predict other widely available precursor compounds beyond g‐C3N4 such as caffeine, melamine, and urea. This work develops a novel and economic strategy to generate morphologically diverse carbon‐based catalysts and provides new, essential insights into the growth mechanism of carbon nanomaterials syntheses.
Simultaneous Detection of Citric Acid and Oxalic Acid Based on Dual Spectrum and Biomimetic Peroxidase for Urolithiasis Screening with a Fully Automatic Urine Analyzer
Authors: Sun Xianyou , Zhou Shuqi , Zhang Yanchi , Ma Chiyu , Hu Yanjie , Tian Shichao , Wang Xinyi , Kong Liubing , Huang Zhuoru , Liang Tao , Wan Hao , Wang Ping 
Published: October 2023

AbstractUrolithiasis stands as a prevalent ailment within the urinary system, with hyperoxaluria and hypocitraturia being the most frequent manifestations characterized by excessive oxalic acid (OA) and deficient citric acid (CA) levels in urine. Detecting these compounds in urine quantitatively holds paramount importance for early urolithiasis screening. Existing methodologies fall short in achieving simultaneous and on‐site identification of OA and CA, posing challenges for accurate urolithiasis screening. Addressing this concern, the study successfully accomplishes the concurrent identification of OA and CA in urine through a combination of dual‐spectral analysis and biomimetic peroxidase utilization. Bovine serum albumin and dithiothreitol‐modified copper nanoclusters (BSA‐DTT‐CuNCs) are employed as biomimetic peroxidases, effectively mitigating interference and enabling the simultaneous determination of OA and CA. The quantification range spans from 0 to 12 mm for OA and 0.5 to 2.5 mm for CA, with detection limits of 0.18 and 0.11 mm, respectively. To facilitate swift and on‐location urine analysis, a fully automated urine analyzer (FAUA) is introduced that streamlines the process of biomarker pretreatment and identification within urine samples. Validation with real urine samples from urolithiasis patients demonstrates the method's diagnostic precision, highlighting the dual‐spectral technique and analyzer's promising role in urolithiasis screening.
Bidirectional Uptake, Transfer, and Transport of Dextran‐Based Nanoparticles in Plants for Multidimensional Enhancement of Pesticide Utilization
Authors: Xiong Qiuyu , Liang Wenlong , Shang Wenxuan , Xie Zhengang , Cheng Jingli , Yu Bin , Fang Yun , Sun Li , Zhao Jinhao 
Published: October 2023

AbstractThe development of effective multifunctional nano‐delivery approaches for pesticide absorption remains a challenge. Here, a dextran‐based pesticide delivery system (MBD) is constructed to deliver tebuconazole for multidimensionally enhancing its effective utilization on tomato plants. Spherical MBD nanoparticles are obtained through two‐step esterification of dextran, followed by tebuconazole loading using the Michael addition reaction. Confocal laser scanning microscopy shows that fluorescein isothiocyanate‐labeled MBD nanoparticles can be bidirectionally transported in tomato plants and a modified quick, easy, cheap, effective, rugged, and safe‐HPLC approach demonstrates the capacity to carry tebuconazole to plant tissues after 24 h of root uptake and foliar spray, respectively. Additionally, MBD nanoparticles could increase the retention of tebuconazole on tomato leaves by up to nearly 2.1 times compared with the tebuconazole technical material by measuring the tebuconazole content retained on the leaves. In vitro antifungal and pot experiments show that MBD nanoparticles improve the inhibitory effect of tebuconazole against botrytis cinerea by 58.4% and the protection against tomato gray molds by 74.9% compared with commercial suspensions. Furthermore, the MBD nanoparticles do not affect the healthy growth of tomato plants. These results underline the potential for the delivery system to provide a strategy for multidimensional enhancement of pesticide efficacy.
Ultrastretchable E‐Skin Based on Conductive Hydrogel Microfibers for Wearable Sensors
Authors: Wang Jinpeng , Qi Yongkang , Gui Yuhan , Wang Can , Wu Yikai , Yao Jiandong , Wang Jie 
Published: October 2023

AbstractConductive microfibers play a significant role in the flexibility, stretchability, and conductivity of electronic skin (e‐skin). Currently, the fabrication of conductive microfibers suffers from either time‐consuming and complex operations or is limited in complex fabrication environments. Thus, it presents a one‐step method to prepare conductive hydrogel microfibers based on microfluidics for the construction of ultrastretchable e‐skin. The microfibers are achieved with conductive MXene cores and hydrogel shells, which are solidified with the covalent cross‐linking between sodium alginate and calcium chloride, and mechanically enhanced by the complexation reaction of poly(vinyl alcohol) and sodium hydroxide. The microfiber conductivities are tailorable by adjusting the flow rate and concentration of core and shell fluids, which is essential to more practical applications in complex scenarios. More importantly, patterned e‐skin based on conductive hydrogel microfibers can be constructed by combining microfluidics with 3D printing technology. Because of the great advantages in mechanical and electrical performance of the microfibers, the achieved e‐skin shows impressive stretching and sensitivity, which also demonstrate attractive application values in motion monitoring and gesture recognition. These characteristics indicate that the ultrastretchable e‐skin based on conductive hydrogel microfibers has great potential for applications in health monitoring, wearable devices, and smart medicine.
Reconfiguration, Welding, Reprogramming, and Complex Shape Transformation of An Optical Shape Memory Polymer Network Enabled by Patterned Secondary Crosslinking
Authors: Zhang Guoxian , Zhang Qing , Guo Zijian , Li Chunmei , Ge Feijie , Zhang Qiuyu 
Published: October 2023

AbstractStimuli‐triggered generation of complicated 3D shapes from 2D strips or plates without using sophisticated molds is desirable and achieving such 2D‐to‐3D shape transformation in combination with shape reconfiguration, welding, and reprogramming on a single material is very challenging. Here, a convenient and facile strategy using the solution of a disulfide‐containing diamine for patterned secondary crosslinking of an optical shape‐memory polymer network is developed to integrate the above performances. The dangling thiolectones attached to the backbones react with the diamine in the solution‐deposited region so that the secondary crosslinking may not only weld individual strips into assembled 3D shapes but also suppress the relaxation of the deformed polymer chains to different extents for shape reconfiguration or heating‐induced complex 3D deformations. In addition, as the dynamic disulfide bonds can be thermally activated to erase the initial programming information and the excessive thiolectones are available for subsequent patterned crosslinking, the material also allows shape reprogramming. Combining welding with patterning treatment, it is further demonstrated that a gripper can be assembled and photothermally controlled to readily grasp an object.
N‐Terminalized Ti3C2Tx MXene for Supercapacitor with Extraordinary Pseudocapacitance Performance
Authors: Hu Xuewen , Gong Ning , Zhang Qicheng , Chen Qiming , Xie Tianzhu , Liu Huibin , Li Yan , Li Yang , Peng Wenchao , Zhang Fengbao , Fan Xiaobin 
Published: October 2023

AbstractMXenes have demonstrated significant potential in electrochemical energy storage, particularly in supercapacitors, owing to their exceptional properties. The surface terminal groups of MXene play a pivotal role in pseudocapacitive mechanism. Considering the hindered electrolyte ion transport caused by –F terminal groups and the limited ion binding sites associated with –O terminal groups, this study proposes a novel strategy of replacing –F with –N terminal groups. The modulated MXene‐N electrode, featuring a substantial number of –N terminal groups, demonstrates an exceptionally high gravimetric capacitance of 566 F g–1 (at a scan rate of 2 mV s–1) or 588 F g–1 (at a discharge rate of 1 A g–1) in 1 м H2SO4 electrolyte, and the potential window is significantly increased. Furthermore, subsequent spectra analysis and density functional theory calculations are employed to investigate the mechanism associated with –N terminal groups. This work exemplifies the significance of terminal modulation in the context of electrochemical energy storage.
Computational chemistry‐assisted design of hydrazine‐based fluorescent molecular rotor for viscosity sensors
Authors: Dong Miao , Wang Dazhuang , Yang Jinrong , Sun Pingping , Ding Weilu , Yang Jianxin , Yan Jinwu , Chi Weijie 
Published: October 2023

AbstractDeep understanding of the fluorescence quenching mechanisms of probes plays a crucial role in developing their practical applications. The fluorescence quenching mechanism of hydrazine‐based fluorescence probes needs to be clarified up to the present. Herein, we designed and synthesized a new hydrazine‐based fluorescence probe (HA‐Na) based on the naphthalimide skeleton. We clarified the molecular origin of the non‐fluorescence of this probe with the aid of computational chemistry and spectroscopic analysis. We showed that the significant rotation of the hydrazine group in the excited state potential energy surface, which caused the complete charge separation, was responsible for the fluorescence quenching of the probe in an organic solvent. Once the rotation was prevented in an aggregative state or high‐viscosity solution, the fluorescence of the probe recovered. In other words, the fluorescence quenching mechanism of hydrazine‐based fluorescence probes was attributed to the formation of a twisted intramolecular charge transfer (TICT) state. More importantly, we demonstrated that this fluorescence molecular rotor could be used to monitor the autophagy process in living cells by detecting lysosomal viscosity changes during starvation. Altogether, this work provides an essential theoretical basis for the developing potential hydrazine‐based fluorescence molecular rotors.
Enhanced evolutionary automated program repair by finer‐granularity ingredients and better search algorithms
Authors: Wang Bo , Liu Guizhuang , Lin Youfang , Ren Shuang , Li Honghui , Zhang Dalin 
Published: October 2023

SummaryBug repair is time consuming and tedious, which hampers software maintenance. To alleviate the burden, automated program repair (APR) is proposed and has been fruitful in the last decade. Evolutionary repair is the seminal work of this field and proliferated a family of approaches. The performance of evolutionary repair approaches is affected by two main factors: (1) search space, which defines all possible patches, and (2) search algorithms, which navigate the space. Although recent approaches have achieved remarkable progress, the main challenges of the two factors still remain. On one hand, the different kinds of search space are very coarse for containing correct patches. On the other hand, the search process guided by genetic algorithms is inefficient in finding the correct patches in an appropriate time budget. In this paper, we propose MicroRepair, a new evolutionary repair approach to address the two challenges. Rather than finding statement‐level patches like existing genetic repair approaches, MicroRepair enlarges the search space by breaking the statements into finer‐granularity ingredients that consist of AST leaves. As the search space grows exponentially, the former search algorithms may become inefficient in navigating the larger space. We utilize the best multiobjective search algorithm selected from our empirical comparison of a set of search algorithms. At last, we find redundancies search in the existing genetic process, and we further design a history‐aware search strategy to accelerate the process.We evaluated MicroRepair on 224 bugs of real‐world from the benchmark Defects4J and compared it with several state‐of‐the‐art repair approaches. The evaluation results show that MicroRepair correctly repaired 26 bugs with a precision of 62%, which significantly outperforms the state‐of‐the‐art evolutionary APR approaches in terms of precision. Moreover, the history‐aware search boosts the repair execution speed by 4% on average.
Binder‐Free Cnt Cathodes for Li‐O2 Batteries with More Than One Life
Authors: Su Zeliang , Temprano Israel , Folastre Nicolas , Vanpeene Victor , Villanova Julie , Gachot Gregory , Shevchenko Elena V. , Grey Clare P. , Franco Alejandro A. , Demortière Arnaud 
Published: October 2023

AbstractLi‐O2 batteries (LOB) performance degradation ultimately occurs through the accumulation of discharge products and irreversible clogging of the porous electrode during the cycling. Electrode binder degradation in the presence of reduced oxygen species can result in additional coating of the conductive surface, exacerbating capacity fading. Herein, a facile method to fabricate free‐standing is established, binder‐free electrodes for LOBs in which multi‐wall carbon nanotubes form cross‐linked networks exhibiting high porosity, conductivity, and flexibility. These electrodes demonstrate high reproducibility upon cycling in LOBs. After cell death, efficient and inexpensive methods to wash away the accumulated discharge products are demonstrated, as reconditioning method. The second life usage of these electrodes is validated, without noticeable loss of performance. These findings aim to assist in the development of greener high energy density batteries while reducing manufacturing and recycling costs.
An A2B2O7‐Type High‐Entropy Oxide for Efficient Photoelectrochemical Photodetector with Excellent Long‐Term Stability
Authors: Wang Dan , Xu Yiguo , Zhang Han , Zhang Ye 
Published: October 2023

AbstractOptoelectronics with excellent long‐term stability is meaningful for practical applications. Herein, for the first time, an A2B2O7 type high‐entropy oxide of (La0.2Ce0.2Nd0.2Gd0.2Bi0.2)2Ti2O7 (ATO) is synthesized and applied for photoelectrochemical photodetection. The lattice distortion, highly dispersed metal composition, and exposed active sites of ATO are beneficial for the fast separation and transmission of photogenerated electron/hole pairs, endowing ATO‐based devices with good photodetection performance. Both the density functional theory calculations and the nondegenerate transient absorption spectroscopy demonstrate the good optoelectronic properties of ATO. The systematic experimental studies reveal the tunable photodetection capability of ATO‐based photodetector (PD) in the visible region. A photocurrent of 772.00 nA cm−2 and a responsivity of 4.02 µA W−1 can be achieved as the PD in 1.0 m KOH with the bias potential of 0.6 V. Importantly, the robust and reproducible ON/OFF signals of the PD can be verified and there is only ≈5.00% attenuation in photocurrent even after 6 months, revealing the great potential of high‐ entropy oxides for practical applications.
Detection of Biomarkers through Functionalized Polymers
Authors: García‐Faustino Litzy L. , Morris Stephen M. , Elston Steve J. , Montelongo Yunuen 
Published: October 2023

AbstractOver the past decade, there has been a rising interest in utilizing functionalized porous polymers for sensor applications. By incorporating functional groups into nanostructured materials like hydrogels, nanosheets, and nanopores, exciting new opportunities have emerged for biomarker detection. The ability of functionalized polymers to undergo physical changes and deformations makes them perfect for modulating optical signals. This chemical mechanism enables the creation of biocompatible sensors for in situ biomarker measurement. Here a comprehensive overview of the current publication trends is provided in functionalized polymers, encompassing functional groups that can induce measurable physical deformations. It explores various materials categorized based on their detection targets, which include proteins, carbohydrates, ions, and deoxyribonucleic acid. As such, this work serves as a valuable reference for the development of functionalized polymer‐based sensors.
Improving the behavior of concentrically braced frame braces using a flexural damper: Experimental and numerical study
Authors: Jeong Seong‐Hoon , Ghamari Ali , Jawdhari Akram 
Published: October 2023

SummaryAlthough the concentrically braced frames (CBFs) systems have high lateral elastic stiffness and strength, they reflect a low seismic energy absorption capacity mainly due to their diagonal buckling under compressive loading. To overcome this problem, researchers have proposed metallic shear damper as the most popular due to its satisfactory performance and affordable cost. In this paper, an innovative metallic damper with a flexural mechanism is proposed to improve the behavior of CBF systems. It provides ease of fabrication and replacement after damage, competitive cost, and improved resistance to buckling of the CBF member. The performance of the damper was evaluated experimentally and numerically. Subsequently, two types of dampers, (a) made of rectangular flexural plates (RFP) and (b) made of I‐shaped flexural plates (IFP), were designed and evaluated. Experimental as well as numerical results indicated that both dampers provide stable and symmetrical hysteresis curves with a high energy absorption capacity. Results indicated that the IFP damper has greater stiffness (1.94–2.3 times) and ultimate strength (1.76 times) but a lower overstrength (66% less) and ductility (47% less) than the RFP damper. Moreover, design expressions were presented for the proposed damper and showed a good agreement with finite element results.
A Personal Account on Inorganic Reaction Mechanisms
Authors: Polaczek Justyna , Kieca Konrad , Oszajca Maria , Impert Olga , Katafias Anna , Chatterjee Debabrata , Ćoćić Dušan , Puchta Ralph , Stochel Grażyna , Hubbard Colin D. , van Eldik Rudi 
Published: October 2023

AbstractThe presented Review is focused on the latest research in the field of inorganic chemistry performed by the van Eldik group and his collaborators. The first part of the manuscript concentrates on the interaction of nitric oxide and its derivatives with biologically important compounds. We summarized mechanistic information on the interaction between model porphyrin systems (microperoxidase) and NO as well as the recent studies on the formation of nitrosylcobalamin (CblNO). The following sections cover the characterization of the Ru(II)/Ru(III) mixed‐valence ion‐pair complexes, including Ru(II)/Ru(III)(edta) complexes. The last part concerns the latest mechanistic information on the DFT techniques applications. Each section presents the most important results with the mechanistic interpretations.
On effective learning of English collocations: From perspectives of distributed practice and semantic restructuring
Authors: Yamagata Satoshi , Nakata Tatsuya , Rogers James 
Published: October 2023

AbstractKnowledge of collocations facilitates second language (L2) learning by enhancing accuracy and fluency. However, acquiring L2 collocations is often challenging for learners. One factor contributing to this difficulty is incongruency between first and second languages (e.g., draw distinctions in English corresponds to do distinctions in Japanese). One possible solution is to facilitate semantic restructuring, where learners develop their understanding of L2 words' semantic possibilities. For the restructuring of semantic knowledge to occur, repeated exposure to multiple collocations containing the same node word may be necessary (e.g., draw attention, draw a conclusion). However, how to facilitate semantic restructuring through repeated exposure is still unknown. Particularly, to what extent temporal distribution (i.e., spacing) of multiple collocations affects learning is an important issue to be examined. Based on recent research on collocation learning, the present article argues that a combination of massing and spacing can promote L2 collocation learning from the viewpoint of semantic restructuring. It also discusses some practical implications for effective L2 collocation learning.