bluuebunny/crossref_metadata_2025_split huggingface dataset:
Tuning the Interfacial Chemistry of Nanoparticle Assemblies via Spin‐Coating: From Single Sensors to Monolithic Sensor Arrays
Authors: Liu Chih‐Yin , Bittinger Sophia C. , Bose Ahir , Meyer Andreas , Schlicke Hendrik , Vossmeyer Tobias 
Published: May 2024

AbstractSensor arrays based on gold nanoparticle (GNP) films are promising candidates for numerous applications, including medical diagnosis and health monitoring. Their economic fabrication, however, remains challenging. This study presents a facile route to GNP chemiresistors with tunable properties via layer‐by‐layer spin‐coating (LbL‐SC). Key steps involve the alternating deposition of dodecylamine‐stabilized GNPs and mixtures of monothiols (MTs) with 1,9‐nonanedithiol (9DT). The 9DT molecules serve to reinforce the growing film via GNP cross‐linking while the MT ligands are used to tune the interfacial chemistry of the GNP assembly. Hence, by employing differently functionalized MTs the sensors' chemical selectivity can easily be adjusted. Further, by varying the MT‐9DT ratio and adjusting the size of the MT ligands the sensitivity can be tuned along with the conductivity and optical properties of the films. In general, decreasing the 9DT fraction significantly enhances the sensitivity while the response isotherms change from Langmuir‐Henry to Henry type. Finally, the cross‐linked GNP films are robust enough to be patterned via photolithography. Hence, this study demonstrates the fabrication and application of monolithic sensor arrays. Different features of the responses to numerous analytes are used as input data for linear discriminant analyses (LDA), revealing that very similar analytes can be distinguished.
Enantioselective Friedel‐Crafts Reaction of ortho‐Alkynylnaphthols with Naphthofurans: Synthesis of Polysubstituted Axially Chiral Styrenes
Authors: Zhang Wenxuan , Sun Jiaying , Yang Daoshan , Song Ran , Si Wen , Lv Jian 
Published: May 2024

AbstractHerein, we report a chiral Brønsted acid‐catalyzed enantioselective Friedel‐Crafts reaction of ortho‐alkynylnaphthols with various naphthofurans, realizing the asymmetric synthesis of axially chiral styrenes with naphthofurans in 67 to 93% yield and with 34 to 96% ee.
Pressure‐Driven Intrinsic Quantum Confinement and Semiconducting‐to‐Metallic Transition in the Topological Flat Bands Kagome Nb3Cl8 Compounds
Authors: Bouhmouche Ayoub , Rhrissi Ilyass , Moubah Reda 
Published: May 2024

AbstractNb3Cl8 is a unique subset of 2D crystalline materials renowned for their Kagome structure and distinctive flat energy bands. These bands contribute to the distinct electronic behavior, rendering Nb3Cl8 a compelling subject for study. In this study, by employing ab initio calculations, the impact of pressure on the electronic properties of Nb3Cl8is scrutinized, yielding valuable insights. Under high pressures, Nb3Cl8 undergoes a transition from a semiconductor state (with a 1.23 eV bandgap) to a metallic one, accompanied by electronic band restructuration. Notably, the flat energy bands are suppressed with increasing pressure. Furthermore, this investigation underscores the distinctive nature of flat energy bands in Nb3Cl8, delving into quantum effects, particularly their association with the quantum confinement of electronic states. The confinement of charge carriers in Nb3Cl8 results in discrete energy levels, corresponding to specific orbitals in the density of states, indicating robust electron confinement. Pressure‐induced changes in the energy gap between these quantized levels suggest a decrease in confinement strength. Consequently, the study lays a robust foundation for future exploration, contributing to the development of innovative electronic devices grounded in quantum confinement effects.
Alkali‐Ion‐Assisted Activation of ε‐VOPO4 as a Cathode Material for Mg‐Ion Batteries
Authors: Sari Dogancan , Rutt Ann , Kim Jiyoon , Chen Qian , Hahn Nathan T. , Kim Haegyeom , Persson Kristin A. , Ceder Gerbrand 
Published: May 2024

AbstractRechargeable multivalent‐ion batteries are attractive alternatives to Li‐ion batteries to mitigate their issues with metal resources and metal anodes. However, many challenges remain before they can be practically used due to the low solid‐state mobility of multivalent ions. In this study, a promising material identified by high‐throughput computational screening is investigated, ε‐VOPO4, as a Mg cathode. The experimental and computational evaluation of ε‐VOPO4 suggests that it may provide an energy density of >200 Wh kg−1 based on the average voltage of a complete cycle, significantly more than that of well‐known Chevrel compounds. Furthermore, this study finds that Mg‐ion diffusion can be enhanced by co‐intercalation of Li or Na, pointing at interesting correlation dynamics of slow and fast ions.
The Functional Role of Disordered Metal Oxides from Active Catalysis to Biological Metabolism
Authors: Baghestani Ghazal , King Hannah J. , Hocking Rosalie K. 
Published: May 2024

AbstractIt has been observed by many authors that highly active electrocatalysts are frequently “disordered” or “amorphous” in nature. The correlation between this lack of order and functionality is highly debated, with researchers still questioning if this structural property is a simple coincidence of the material preparation method, or if this lack of order has an important functional role for these catalysts. Using metal oxides as an example, how amorphous and disordered metal oxides can react by fundamentally different pathways are explored from more ordered forms with very similar bonding and redox states. The distinction between amorphous, disordered, and crystalline materials is reviewed in different characterization methods and suggests how these material characteristics fundamentally change the reactivity of these materials beyond surface area effects. How disorder can change the underlying thermodynamic stability of a material is explored, which in turn impacts redox potential, proton‐transfer, and electron‐transfer properties. It is these fundamental properties that govern the electrocatalytic activity and microbial metabolism of these materials. It is further argued that understanding the amorphous and disordered state of materials may be key to understanding a range of catalytic reactions; from clean energy reactions to the biological systems that underpin life's existence.
Boosting the Proton Intercalation via Crystal Plane Optimization of TiS2 for Cycling‐Stable Aqueous Zn‐Ion Batteries
Authors: Chen Manlin , He Xin , Zhou Min , Ning Jing , Zhang Zidong , Cao Shenglin , Wang Tianqi , Wang Kangli , Jiang Kai 
Published: May 2024

AbstractTiS2 has received significant attention as a promising anode for “Rocking‐Chair”‐type aqueous Zn‐ion batteries due to the large interlayer spacing and low discharge plateau. However, the structural distortion caused by the embedding of divalent Zn2+ as well as the undesirable hydrogen evolution reaction (HER) severely affects their cycling stability. Herein, a facet‐dependent mechanism is first deeply investigated to understand charge storage behaviors of TiS2 via differential electrochemical mass spectrometry, in situ electrochemical quartz crystal microbalance, and in situ X‐ray diffraction characterizations. By regulating the exposed crystal facets of TiS2 from (001) (TS (001)) to (011) (TS(011)), HER can be effectively inhibited, and the charge storage mechanism is transformed from Zn2+ insertion/extraction dominating to H+ insertion/extraction dominating, resulting in faster charge transfer kinetics and strong structure stability during long‐term cycling. Hence, TS(011) delivers a higher reversible capacity of 212.9 mAh g−1 at 0.1 A g−1 and a strong cycling stability of 74% capacity retention over 1000 cycles, much better than that of TS (001) with a reversible capacity of 164.7 mAh g−1 at 0.1 A g−1, a capacity retention of 17% after 1000 cycles. These new findings can provide deep insight into the rational design of high‐performance intercalation‐type electrode materials for energy storage applications.
Reconstruction of Electric Double Layer on the Anode Interface by Localized Electronic Structure Engineering for Aqueous Zn Ion Batteries
Authors: Liu Jingwen , Li Caixia , Lv Qingliang , Chen Dehong , Zhao Jinling , Xia Xiaodan , Wu Zexing , Lai Jianping , Wang Lei 
Published: May 2024

AbstractThe electric double layer (EDL) at the electrode/electrolyte interface plays a crucial role to the electrochemical reactions of zinc ion batteries. For Zn anode, the EDL consists of H2O dipoles, which can cause Zn corrosion and passivation. Herein, the localized electronic‐rich (LER) structure performing as soild electrolyte interphase (SEI) changes the electron distribution, leading to the rapid capture of Zn2+, thus promoting the desolvation of the cH2O shell. Moreover, the LER generates an electrostatic repulsion effect to SO42−. Consequently, a unique H2O‐poor EDL is reconstructed with the distribution of Zn2+‐H2O‐SO42−, which inhibits side reactions and improves the deposition kinetics of Zn2+. In situ Raman intuitively confirms that the zinc‐ion‐flux is uniform during the whole electroplating process. LER as regulator for EDL structure, leads to smooth and fast Zn2+ deposition. The performance enhancement is demonstrated by LER@Zn//LER@Zn cells, which exhibit exceptional lifespan for 4800 h. Furthermore, the LER@Zn///MnO2 cell shows improved cycling stability over 1500 cycles, with a high capacity of 124 mAh g−1 at 5 C.
Proteomic changes in the human cerebrovasculature in Alzheimer's disease and related tauopathies linked to peripheral biomarkers in plasma and cerebrospinal fluid
Authors: Wojtas Aleksandra M. , Dammer Eric B. , Guo Qi , Ping Lingyan , Shantaraman Ananth , Duong Duc M. , Yin Luming , Fox Edward J. , Seifar Fatemeh , Lee Edward B. , Johnson Erik C. B. , Lah James J. , Levey Allan I. , Levites Yona , Rangaraju Srikant , Golde Todd E. , Seyfried Nicholas T. 
Published: May 2024

AbstractINTRODUCTIONCerebrovascular dysfunction is a pathological hallmark of Alzheimer's disease (AD). Nevertheless, detecting cerebrovascular changes within bulk tissues has limited our ability to characterize proteomic alterations from less abundant cell types.METHODSWe conducted quantitative proteomics on bulk brain tissues and isolated cerebrovasculature from the same individuals, encompassing control (N = 28), progressive supranuclear palsy (PSP) (N = 18), and AD (N = 21) cases.RESULTSProtein co‐expression network analysis identified unique cerebrovascular modules significantly correlated with amyloid plaques, cerebrovascular amyloid angiopathy (CAA), and/or tau pathology. The protein products within AD genetic risk loci were concentrated within cerebrovascular modules. The overlap between differentially abundant proteins in AD cerebrospinal fluid (CSF) and plasma with cerebrovascular network highlighted a significant increase of matrisome proteins, SMOC1 and SMOC2, in CSF, plasma, and brain.DISCUSSIONThese findings enhance our understanding of cerebrovascular deficits in AD, shedding light on potential biomarkers associated with CAA and vascular dysfunction in neurodegenerative diseases.
Correlation analysis of peripheral platelet markers and disease phenotypes in Alzheimer's disease
Authors: Fu Jiajia , Lai Xiaohui , Zhang Chongwei , Wei Qianqian , Chen Xueping , Shang Huifang 
Published: May 2024

AbstractINTRODUCTIONPlatelets serve as the primary peripheral reservoir of amyloid beta (Aβ). However, there is limited research on platelet markers in routine blood examinations, particularly with regard to the large platelet ratio (P‐LCR) in Alzheimer's disease (AD).METHODSThis study included 512 AD patients and 205 healthy controls (HCs). Platelet markers and apolipoprotein E (APOE) 4 status were assessed in all participants.RESULTSThe study revealed that P‐LCR was significantly elevated in AD patients compared to HCs. In AD patients carrying APOE4, P‐LCR significantly negatively correlated with Montreal Cognitive Assessment scores. There was an observed increasing trend in the rate of change in P‐LCR with disease progression. Binary logistic regression analysis indicated that P‐LCR may constitute a risk factor for AD, after adjusting for age, sex, APOE4, and body mass index.DISCUSSIONP‐LCR is associated with disease severity in AD patients carrying APOE4. P‐LCR may be a promising marker to reflect platelet activity in AD patients.Highlights
P‐LCR significantly negatively correlated with MoCA scores in AD patients with APOE4.
The rate of change in P‐LCR showed an increasing trend with disease progression.
P‐LCR may be a risk factor for AD.
Mechanical Strain Induces and Increases Vesicular Release Monitored by Microfabricated Stretchable Electrodes
Authors: Yan Jing , Zhang Fu‐Li , Jin Kai‐Qi , Li Jia‐Xin , Wang Li‐Jun , Fan Wen‐Ting , Huang Wei‐Hua , Liu Yan‐Ling 
Published: May 2024

AbstractExocytosis involving the fusion of intracellular vesicles with cell membrane, is thought to be modulated by the mechanical cues in the microenvironment. Single‐cell electrochemistry can offer unique information about the quantification and kinetics of exocytotic events; however, the effects of mechanical force on vesicular release have been poorly explored. Herein, we developed a stretchable microelectrode with excellent electrochemical stability under mechanical deformation by microfabrication of functionalized poly(3,4‐ethylenedioxythiophene) conductive ink, which achieved real‐time quantitation of strain‐induced vesicular exocytosis from a single cell for the first time. We found that mechanical strain could cause calcium influx via the activation of Piezo1 channels in chromaffin cell, initiating the vesicular exocytosis process. Interestingly, mechanical strain increases the amount of catecholamines released by accelerating the opening and prolonging the closing of fusion pore during exocytosis. This work is expected to provide revealing insights into the regulatory effects of mechanical stimuli on vesicular exocytosis.
Zwitterionic Cellulose‐Based Polymer Electrolyte Enabled by Aqueous Solution Casting for High‐Performance Solid‐State Batteries
Authors: Cheng Yong , Cai Zhichao , Xu Jinglei , Sun Zhefei , Wu Xiaoyu , Han Jiajia , Wang Yao‐Hui , Wang Ming‐Sheng 
Published: May 2024

AbstractPolyethylene oxide (PEO)‐based solid‐state batteries hold great promise as the next‐generation batteries with high energy density and high safety. However, PEO‐based electrolytes encounter certain limitations, including inferior ionic conductivity, low Li+ transference number, and poor mechanical strength. Herein, we aim to simultaneously address these issues by utilizing one‐dimensional zwitterionic cellulose nanofiber (ZCNF) as fillers for PEO‐based electrolytes using a simple aqueous solution casting method. Multiple characterizations and theoretical calculations demonstrate that the unique zwitterionic structure imparts ZCNF with various functions, such as disrupting PEO crystallization, dissociating lithium salts, anchoring anions through cationic groups, accelerating Li+ migration by anionic groups, as well as its inherent reinforcement effect. As a result, the prepared PL‐ZCNF electrolyte exhibits remarkable ionic conductivity (5.37×10−4 S cm−1) and Li+ transference number (0.62) at 60 °C without sacrificing mechanical strength (9.2 MPa), together with high critical current density of 1.1 mA cm−2. Attributed to these merits of PL‐ZCNF, the LiFePO4|PL‐ZCNF|Li solid‐state full‐cell delivers exceptional rate capability and cycling performance (900 cycles at 5 C). Notably, the assembled pouch‐cell can maintain steady operation over 1000 cycles with an impressive 93.7 % capacity retention at 0.5 C and 60 °C, highlighting the great potential of PL‐ZCNF for practical applications.
Development of Stable Water‐Soluble Supratomic Silver Clusters Utilizing A Polyoxoniobate‐Protected Strategy: Giant Core‐Shell‐Type Ag8@Nb162 Fluorescent Nanocluster
Authors: Hong Li‐Hao , Yue Sheng‐Nan , Huang Xing , Sun Cai , Cai Ping‐Wei , Sun Yan‐Qiong , Li Xin‐Xiong , Zheng Shou‐Tian 
Published: May 2024

AbstractAtomically precise low‐nuclearity (n<10) silver nanoclusters (AgNCs) have garnered significant interest due to their size‐dependent optical properties and diverse applications. However, their synthesis has remained challenging, primarily due to their inherent instability. The present study introduces a new feasible approach for clustering silver ions utilizing highly negative and redox‐inert polyoxoniobates (PONbs) as all‐inorganic ligands. This strategy not only enables the creation of novel Ag‐PONb composite nanoclusters but also facilitates the synthesis of stable low‐nuclearity AgNCs. Using this method, we have successfully synthesized a small octanuclear rhombic [Ag8]6+ AgNC stabilized by six highly negative [LiNb27O75]14− polyoxoanions. This marks the first PONb‐protected superatomic AgNC, designated as {Ag8@(LiNb27O75)6} (Ag8@Nb162), with an aesthetically spherical core–shell structure. The crystalline Ag8@Nb162 is stable under ambient conditions, What's more, it is water‐soluble and able to maintain its molecular cluster structure intact in water. Further, the stable small [Ag8]6+ AgNC has interesting temperature‐ and pH‐dependent reversible fluorescence response, based on which a multiple optical encryption mode for anti‐counterfeit technology was demonstrated. This work offers a promising avenue for the synthesis of fascinating and stable PONb‐protected AgNCs and sheds light on the development of new‐type optical functional materials.
Engineered Phenylalanine Ammonia‐Lyases for the Enantioselective Synthesis of Aspartic Acid Derivatives
Authors: Buslov Ivan , Desmons Sarah , Duhoo Yoan , Hu Xile 
Published: May 2024

AbstractBiocatalytic hydroamination of alkenes is an efficient and selective method to synthesize natural and unnatural amino acids. Phenylalanine ammonia‐lyases (PALs) have been previously engineered to access a range of substituted phenylalanines and heteroarylalanines, but their substrate scope remains limited, typically including only arylacrylic acids. Moreover, the enantioselectivity in the hydroamination of electron‐deficient substrates is often poor. Here, we report the structure‐based engineering of PAL from Planctomyces brasiliensis (PbPAL), enabling preparative‐scale enantioselective hydroaminations of previously inaccessible yet synthetically useful substrates, such as amide‐ and ester‐containing fumaric acid derivatives. Through the elucidation of cryo‐electron microscopy (cryo‐EM) PbPAL structure and screening of the structure‐based mutagenesis library, we identified the key active site residue L205 as pivotal for dramatically enhancing the enantioselectivity of hydroamination reactions involving electron‐deficient substrates. Our engineered PALs demonstrated exclusive α‐regioselectivity, high enantioselectivity, and broad substrate scope. The potential utility of the developed biocatalysts was further demonstrated by a preparative‐scale hydroamination yielding tert‐butyl protected l‐aspartic acid, widely used as intermediate in peptide solid‐phase synthesis.
A waste hemp‐based biomass carbon aerogel with high fire‐resistance
Authors: Liu Jiangtao , Yang Ke , Yang Yaru , Zhang Mingshuo , Shi Yiran , Xue Baoxia , Niu Mei , Zhang Li 
Published: May 2024

AbstractTo enhance the efficient utilization of waste hemp rods, a kind of three‐dimensional (3D), mesh‐like lamellar structured hemp‐based biomass carbon aerogel (CA) was developed by freeze‐drying and subsequent high‐temperature carbonization method. The microstructure, flame resistance, thermal stability, and thermal conductivity of CA were investigated using several analytical techniques, including scanning electron microscopy (SEM), Fourier‐transform infrared spectroscopy (FTIR), X‐ray diffraction (XRD), simulated combustion tests, and thermogravimetric analysis (TG). Optimum formulation yielded at an alkali treatment concentration of 20% and a carbonization temperature of 700°C, CA with a 3D network of reticulated lamellae was obtained. CA exhibited minimal values for thermal conductivity (0.06 W/m K) and thermal diffusion coefficient (0.41 mm2/s), which are indicative of superior insulative properties. Moreover, the material demonstrated remarkable thermal endurance and flame resistance, achieving a char yield of 70.03% when subjected to a temperature of 700°C in an oxidative environment.
Ökobilanzen von Baustoffen für Tragwerke in Abhängigkeit von den Bewertungssystemen im DACH‐Raum
Authors: Zitterl Thomas , Bauer Peter 
Published: May 2024

AbstractAufgrund der Komplexität der Ergebnisse von Ökobilanzen bestehen Bemühungen, die Fülle an Indikatoren zu einem einzelnen aussagekräftigen Wert als Ergebnis einer Ökobilanz zusammenzuführen. Derartige vollaggregierende Bewertungsmethoden charakterisieren und gewichten einzelne Indikatoren und deren Auswirkungen und führen diese in Punktesysteme über. Die für die Berechnung herangezogenen Ökologieindikatoren basieren auf baustoffbezogenen Datensätzen, welche laut Norm zumindest die Phasen Herstellung, Entsorgung und Wiederverwendung bzw. Recycling deklarieren sollten. In der Praxis verwendete Datenbanken entsprechen derzeit jedoch nur begrenzt diesen Anforderungen. Die in Österreich verwendete Datenbank berücksichtigt etwa nur die Herstellung, in der Schweiz werden Herstellung und Entsorgung herangezogen und in Deutschland zwar alle drei Phasen, diese jedoch nicht immer vollständig. Ein Vergleich auf Baustoffebene zeigt, dass sich je nach Datengrundlage und Bewertungsmethode teilweise stark unterschiedliche Erkenntnisse und Handlungsanleitungen ergeben. Ergebnisse von Ökobilanzierungen sollten daher immer in Relation zur verwendeten Datenquelle betrachtet werden. Dieser Aufsatz zeigt auf, dass Datenbanken der KBOB und der ÖKOBAUDAT, welche Herstellung und Entsorgung der Baustoffe einbeziehen, sowie die Methode der ökologischen Knappheit empfehlenswert sind. Die Datenbank baubook sowie der Oekoindex OI3 liefern aktuell nur begrenzt verwendbare Ergebnisse.
State of Health Estimation of Lithium‐ion Batteries Based on Machine Learning with Mechanical‐Electrical Features
Authors: Gong Lili , Zhang Zhiyuan , Li Xueyan , Sun Kai , Yang Haosong , Li Bin , Ye Hong , Wang Xiaoyang , Tan Peng 
Published: May 2024

AbstractAs one of the key parameters to characterize the life of lithium‐ion batteries, the state of health (SOH) is of great importance in ensuring the reliability and safety of the battery system. Considering the complexity of practical application scenarios, a novel method based on mechanical‐electrical feature extraction and machine learning is proposed to accurately estimate the SOH. A series of degradation experiments are designed to generate battery aging datasets, including the stress and voltage changes. Health features are directly extracted from the stress‐voltage profile and the mechanical‐electrical health feature factors are obtained through correlation analysis. The long short‐term memory (LSTM) network is introduced to map the relationship between mechanical‐electrical responses and the SOH, where the health feature factors are selected as input vectors. The effectiveness of the proposed method is demonstrated by battery datasets under different conditions, from which the estimated errors are less than 1.5 %. This work demonstrates that the analysis and utilization of mechanical‐electrical parameters can not only realize accurate SOH estimation, but also provide a broader field for battery energy management.