bluuebunny/crossref_metadata_2025_split huggingface dataset:
Tailoring the Tunneling‐Effect‐Boosted Interfacial Charge Trapping via Effective Conjugation Length
Authors: Prakoso Suhendro Purbo , Peng Hsun‐Xien , Chen Mei‐Nung , Hong Qi‐An , Saleh Rosari , Chiu Yu‐Cheng 
Published: October 2024

AbstractHighly efficient charge injection and charge trapping stability of the tunneling layer are of desirable and practical importance to transistor memory applications. However, both of which can be contradictory to the nature properties of its material. It is herein demonstrated that lowering the energy mismatch of the tunneling layer by employing a longer conjugation length of the polymer can improve the charge injection efficiency, albeit the trapped charges will be easily diminished and finally losing its memory characteristics, and vice versa. To further elaborate and verify this concept, both materials are blended with distinct nature of properties as the tunneling layer in pentacene‐based transistor devices. As the results, the device using 300 nm SiO2 with optimum blending ratio displays a broad memory window of ≈77.6 V which is superior to the non‐blended tunneling layer carrying appropriate energy levels and band gap energy, not to mention, revealing fast operation time (≈1 s), low driving voltage (≈20 V), long retention (>104 s), and high switching stability over 50 cycles with on–off ratio of >104. Most importantly, this finding shed insight into the design of tunneling materials for advancing organic transistor memory technologies based on tunneling‐effect‐boosted interfacial charge trapping.
Advancing Multi‐Optical Performances in Lanthanide‐Doped Fluoride Core@Shell Nanoarchitectures by Minimizing Cation Intermixing
Authors: Xu Weixin , Zhang Shuning , Wei Aoqing , Deng Degang , Zhou Su , Xu Shiqing , Lei Lei 
Published: October 2024

AbstractCore/shell structures are widely employed to enhance photoluminescence efficiency and manipulate excitation dynamics in lanthanide‐doped fluoride nanoparticles (NPs). However, prominent cation intermixing leads to significant deviations from the expected optical performances, presenting a formidable challenge in a deeper understanding of the chemical processes involved, as well as developing efficient suppression methods. Here, a reliable and facile multi‐optical reference strategy to reveal the integral cation intermixing processes is designed. This strategy analyzes the presence of Ce3+ ions in the core (or shell) and their influences on near‐infrared light‐triggered upconversion (UC), ultraviolet (UV)‐activated downshifting (DS), and X‐ray‐excited optical/persistent luminescence (XEOL/XEPL) of Tb3+ ions in the shell (or core). The results demonstrate that a thin surface layer of core NPs dissolves to reach dissolution equilibrium, which then distributes throughout the entire shell layer, rather than being confined to an interfacial region. It is further developed an improved technique to greatly inhibit cation intermixing by successive shell growth with excessive cation precursors, enabling superior multi‐optical performances, including UC, DS, XEOL/XEPL, and time‐dependent multicolor evolution. The findings significantly advance the development of lanthanide‐doped fluoride core/shell NPs with superior optical performances, broadening their potential applications in bio‐medicine, healthcare, industrial inspection, and optical information science.
Enhanced Local CO Coverage on Cu Quantum Dots for Boosting Electrocatalytic CO2 Reduction to Ethylene
Authors: Wang Yan , Wang Jiarui , Cai Rui , Zhang Jianfang , Xia Shuai , Li Zeping , Yu Cuiping , Wu Jingjie , Wang Peng , Wu Yucheng 
Published: October 2024

AbstractEthylene (C2H4) electrosynthesis from the electrocatalytic CO2 reduction process holds enormous potential applications in industrial production. However, the sluggish kinetics of C─C coupling often result in low yield and poor selectivity for C2H4 production. Herein, the performance of Cu catalysts of varying sizes is investigated, prepared via a cryo‐mediated liquid phase exfoliation technique, for the electrochemical CO2 reduction to C2H4. The activity and selectivity of C2H4 gradually increase as the size of the Cu catalysts decreases from tens of nanometers to a few nanometers. Impressively, the 5 nm Cu quantum dots (Cu‐5) achieve a maximum C2H4 Faradaic efficiency (FE) of 81.5% and a half‐cell cathodic energy efficiency (CEE) of 42.2% with a large partial current density of 1.1 A cm−2 at −0.93 V versus the reversible hydrogen electrode. Structural characterization and in situ spectroscopic analysis reveal that the Cu‐5 quantum dots, dominated by the (100) facet, provide an abundance of active sites that enhance CO2 adsorption and activation, promoting the formation of *CO intermediates. The accumulation of *CO intermediates on the Cu active sites facilitates the CO‐CHO coupling reaction, thus enhancing the C2H4 production rate.
Silk Proteins: Designs from Nature with Multipurpose Utility and Infinite Future Possibilities
Authors: Numata Keiji , Kaplan David L. 
Published: October 2024

AbstractThis is a Perspective on nature as a story‐teller, where inputs of evolution drove the remarkable protein designs found in silks. This selection process has resulted in silk materials with novel chemistry and properties to support organism survival in nature, yet with newfound utility in everything from comic books and automobiles to medicine. With growing global concerns related to environmental health, silks also serve as an invaluable instructional guide to the future of sustainable material designs.
Enhanced Ornidazole Degradation via Peroxymonosulfate Activation Using Nano CoFe2O4‐Decorated Halloysite Nanotubes: A High‐Efficiency and Stable Catalyst Approach
Authors: Zhang Lihua , Dong Guowen , Yang Ye , Niu Yu , Gao Wei , Li Zaixing 
Published: October 2024

AbstractThis study proposes a novel, cost‐effective nano CoFe2O4‐decorated halloysite nanotubes (CoFe2O4/HNT) catalyst, which effectively degrades the antibiotic ornidazole (ONZ) through peroxymonosulfate (PMS) activation. By using a simple and economical preparation method, ultra‐low amounts of CoFe2O4 are uniformly loaded onto HNTs, significantly improving the activity and stability of the catalyst. The experimental results show that the CoFe2O4/HNT+PMS system can almost completely degrade ONZ within 1 h, with good pH adaptability and resistance to anion interference. The simple synthesis process and low cost of CoFe2O4/HNT make it highly practical for large‐scale applications. Mechanism studies have shown that the synergistic effect between Co and Fe greatly improves the activation efficiency of PMS, generating reactive oxygen species (such as 1O2) that play a key role in ONZ degradation. This work not only elucidates the activation mechanism, but also provides insightful information for advanced oxidation processes (AOP). The results indicate the practicality and importance of CoFe2O4/HNT catalyst in treating harmful pollutants in water, supporting effective and sustainable water purification technologies. In addition, the study emphasizes the elasticity and adaptability of this innovative catalyst system in managing various pollutants, indicating its broad potential for environmental applications.
Retrosplenial hypometabolism precedes the conversion from mild cognitive impairment to Alzheimer's disease
Authors: Terstege Dylan J. , Galea Liisa A. M. , Epp Jonathan R. ,   Alzheimer's Disease Neuroimaging Initiative
Published: October 2024

AbstractINTRODUCTIONNot all individuals who experience mild cognitive impairment (MCI) transition through progressive stages of cognitive decline at the same rate, if at all. Previous observational studies have identified the retrosplenial cortex (RSC) as an early site of hypometabolism in MCI which seems to be predictive of later transition to Alzheimer's disease (AD).METHODSWe examined N = 399 MCI subjects with baseline 18F‐fluorodeoxyglucose positron emission tomography. Subjects were classified based on whether their diagnosis converted from MCI to AD.RESULTSWhole‐brain metabolism was decreased in converters (MCI‐AD). This effect was more prominent at the RSC, where MCI‐AD subjects showed even greater hypometabolism. Observations of RSC hypometabolism and its utility in predicting transition from MCI‐AD withstood statistical analyses in a large retrospective study.DISCUSSIONThese results point to the utility of incorporating RSC hypometabolism into predictive models of AD progression risk and call for further examination of mechanisms underlying this relationship.Highlights
Not all individuals who develop MCI will progress to AD.
Individuals with MCI who progress to AD show early whole‐brain hypometabolism.
Early hypometabolism is particularly prominent at the RSC.
A short version of the Everyday Cognition scale can predict clinical progression and cognitive decline
Authors: Manjavong Manchumad , Diaz Adam , Ashford Miriam T. , Aaronson Anna , Miller Melanie J. , Kang Jae Myeong , Mackin Scott , Tank Rachana , Weiner Michael , Nosheny Rachel ,   for the Alzheimer's Disease Neuroimaging Initiative
Published: October 2024

AbstractBACKGROUNDThe Everyday Cognition scale (ECog‐39) scores are associated with future cognitive decline. We investigated whether the 12‐item ECog (ECog‐12), which is being collected in Alzheimer's Disease Neuroimaging Initiative (ADNI)4, can predict progression.METHODSBaseline self (PT)‐ and study partner (SP)‐ECog‐12 data were extracted from the 39‐item version collected in the ADNI. Weibull analysis examined the relationship between baseline ECog‐12 and future clinical progression (change in Clinical Dementia Rating Sum of Boxes [CDR‐SB] scores and diagnostic conversion).RESULTSHigher PT‐ and SP‐ECog‐12 scores were associated with faster CDR‐SB worsening, with hazard ratios in cognitively unimpaired (CU) 3.34 and 9.61, mild cognitive impairment (MCI) 1.44 and 2.82, and dementia 0.93 and 1.82. They were associated with conversion from CU to MCI 3.01 and 6.24 and MCI to dementia 1.61 and 3.07.DISCUSSIONSP‐ECog‐12 provided a higher prognostic value for predicting clinical progression, so this can help identify and monitor patients at risk in research and health‐care settings.Highlights
The 12‐item Everyday Cognition scale (ECog‐12) data obtained from both raters increased diagnostic conversion risk from cognitively unimpaired to mild cognitive impairment (MCI) and from MCI to dementia.
ECog‐12, rated by study partners, was associated with an increased risk of Clinical Dementia Rating Sum of Boxes worsening in all diagnostic groups.
Our results provide novel information about the specific scoring outputs and rater types (participant vs. study partner) of ECog‐12 that can facilitate screening, prioritization, and longitudinal monitoring of the clinical progression of participants in Alzheimer's Disease Neuroimaging Initiative 4 and other Alzheimer's disease clinical studies, clinical trials, and in health‐care settings.
Photoexcitation‐Enhanced High‐Ionic Conductivity in Polymer Electrolytes for Flexible, All‐Solid‐State Lithium‐Metal Batteries Operating at Room Temperature
Authors: Wang Rong‐Hao , Wang Weiyi , Zhang Yu‐Zhen , Hu Wei , Yue Liang , Ni Jia‐Hao , Zhang Wan‐Qun , Pei Gang , Yang Shangfeng , Chen Li‐Feng 
Published: October 2024

AbstractDesigning solid polymer electrolytes (SPEs) with high ionic conductivity for room‐temperature operation is essential for advancing flexible all‐solid‐state energy storage devices. Innovative strategies are urgently required to develop SPEs that are safe, stable, and high‐performing. In this work, we introduce photoexcitation‐modulated heterojunctions as catalytically active fillers within SPEs, guided by photocatalytic design principles, and meanwhile employ natural bacterial cellulose to improve the compatibility with poly(ethylene oxide), improve the coordination environment of lithium salts, and optimize both ion transport and mechanical properties. In situ photothermal experiments and theoretical calculations reveal that the strong photogenerated electric field produced by trace heterojunctions within poly(ethylene oxide) electrolytes under photoexcitation significantly enhances lithium salt dissociation, increasing the concentration of mobile Li+. This results in a substantial increase in ionic conductivity, reaching 0.135 mS cm−1 at 25 °C, with a Li+ transference number as high as 0.46. The flexible all‐solid‐state lithium‐metal pouch cells exhibit an impressive discharge capacity of 178.8 mAh g−1 even after repeated bending and folding, and demonstrate exceptional long‐term cycling stability, retaining 86.7 % of their initial capacity after 250 cycles at 1 C (25 °C). This research offers a novel approach to developing high‐performance flexible lithium‐metal batteries.
Photooxidation of Polyolefins to Produce Materials with In‐Chain Ketones and Improved Materials Properties
Authors: Liu Xin , Hu Zhitao , Portela Brandon S. , Rettner Emma M. , Pineda Agustin , Miscall Joel , Rorrer Nicholas A. , Krummel Amber T. , Paton Robert S. , Miyake Garret M. 
Published: October 2024

AbstractHerein, we report a selective photooxidation of commodity postconsumer polyolefins to produce polymers with in‐chain ketones. The reaction does not involve the use of catalyst, metals, or expensive oxidants, and selectively introduces ketone functional groups. Under mild and operationally simple conditions, yields up to 1.23 mol % of in‐chain ketones were achieved. Installation of in‐chain ketones resulted in materials with improved adhesion of the materials and miscibility of mixed plastics relative to the unfunctionalized plastics. The introduction of ketone groups into the polymer backbone allows these materials to react with diamines, forming dynamic covalent polyolefin networks. This strategy allows for the upcycling of mixed plastic waste into reprocessable materials with enhanced performance properties compared to polyolefin blends. Mechanistic studies support the involvement of photoexcited nitroaromatics in consecutive hydrogen and oxygen atom transfer reactions.
Quasi‐Single‐Crystal Tin Halide Perovskite Films with High Structural Integrity for Near‐Infrared Imaging Array Enabling Hidden Object Recognition
Authors: Liu Tianhua , Wang Lixia , Yuan Ziquan , Wang Junfang , Huang Junjie , Wu Weitong , Meng Xiangyue 
Published: October 2024

AbstractNear‐infrared (NIR) image sensors based on solution‐processed thin film are gaining prominence in various applications, including security detection, remote sensing, medical imaging, and environmental monitoring, owing to superior penetration capabilities of NIR light. However, the reported perovskite image sensors suffer from limited resolution and performance due to poor structural integrity, bioincompatibility, and constrained response wavelength range from lead‐based perovskite materials employed. In this study, we present non‐toxic quasi‐single‐crystal (QSC) CH(NH2)2SnI3 (FASnI3) perovskite films, prepared via a simple spin‐coating technique, that demonstrate high structural integrity and effective NIR response. Through a series of in situ characterizations, we reveal that the orderly growth mode of QSC‐FASnI3 perovskite films enables a more oriented crystal growth with reduced trap and grain boundaries. Consequently, self‐powered NIR photodetector based on QSC‐FASnI3 films exhibited large detectivity over 1013 Jones in the NIR range (780–890 nm). Ultimately, due to the high structural integrity, the high‐resolution 64×64 (4096) pixels NIR imaging array, exhibiting reduced photo and dark response non‐uniformity value, was fabricated on the thin‐film transistors (TFT) backplanes, enabling ultraweak NIR light (63 nW cm−2) real‐time imaging, fingerprint imaging, and hidden object recognition. This work pioneers the application of lead‐free perovskite for high‐resolution NIR imaging arrays.
Synthesis, Characterization, and Therapeutic Potential of Novel Schiff Base Metal Complexes: Nickel(II) and Copper(II) Complexes Based 2‐[(2‐Chloroquinolin‐3‐yl)methylidene]aminobenzenethiol (CQAT)
Authors: Abd El‐Lateef Hany M. , Khalaf Mai M. , Gouda Mohamed , Amer Amer A. , Abdelhamid Antar A. , Abdou Aly 
Published: October 2024

ABSTRACTThis research focused on the design and comprehensive characterization of two novel transition metal complexes derived from the symmetrical Schiff base 2‐[(2‐chloroquinolin‐3‐yl)methylidene]aminobenzenethiol (CQAT), coordinated with nickel(II) (NiCQAT) and copper(II) (CuCQAT) ions. The structural elucidation of these complexes was achieved through a range of advanced analytical techniques. Thermal analysis revealed the stability and decomposition patterns of the complexes, supporting the identification of their coordination geometries. The collective data indicated that both NiCQAT and CuCQAT complexes adopt octahedral coordination, with the specific formulas [Ni(CQAT)2(H2O)2] and [Cu(CQAT)2(H2O)2], respectively. To complement the experimental findings, density functional theory (DFT) calculations were employed. These theoretical calculations confirmed the proposed molecular structures and provided detailed insights into key quantum chemical parameters, such as HOMO–LUMO energies, molecular orbitals, and electronic distributions, which are crucial for understanding the complexes' reactivity and stability. Furthermore, extensive in vitro biological evaluations were conducted to assess the anti‐inflammatory and antioxidant properties of the synthesized complexes. These assays demonstrated that both NiCQAT and CuCQAT exhibited significantly enhanced bioactivity compared to the free CQAT ligand, suggesting a synergistic effect of metal coordination on the ligand's biological efficacy. To further explore the mode of action, molecular docking studies were performed targeting two key proteins—human cyclooxygenase‐2 (PDB ID: 5IKT) and human peroxiredoxin 2 (PDB ID: 5IJT). The docking simulations provided valuable insights into the binding affinities, interaction energies, and key amino acid residues involved in the binding process, offering a molecular‐level understanding of their potential biological mechanisms. The findings from these multidisciplinary studies highlight the therapeutic potential of CQAT and its nickel and copper complexes, positioning them as promising candidates for further development in the field of medicinal chemistry.
Powering Hydrogen Evolution Reaction by Precise Control Over A Cu‐Ni Bimetallic Electrocatalyst
Authors: Liu Yaowen , Luo Zhijie , Liao Yunbin , Zheng Yuhui , Lin Yinru , Wang Qianming 
Published: October 2024

ABSTRACTPrecious metals are effective catalysts for the hydrogen evolution reaction, but their high cost with complicated operation steps drives people to search for non–noble‐metal alternatives. Building rational design concept for efficient electrocatalyst relies on the capability to control the structure and composition. Herein, a Ni/Cu bimetallic mesoporous MOFs with 4,4′,4″‐(1,3,5‐triazine‐2,4,6‐triyl)tribenzoic acid as the robust ligand has been assembled via a one‐step solvothermal method. Due to the extensive conjugate plane and high nitrogen content, the catalyst possesses large pore size of 17 nm and fast electron transfer rate, which favors hydrogen bubble overflow and exposes more active sites to solid–liquid interfaces. The bimetallic interaction between highly conductive Cu ions and Ni ions allows it to improve charge migration and realize excellent conductivity. The functionalized electrode requires an overpotential of 132 mV to achieve 10 mA current density with a small Tafel slope (87.7 mV·dec−1) and continuous electrolysis for 24 h.
The preparation of different types of reclaimed rubber and their applications in tire inner liner
Authors: Xu Yunhui , Wang Shifeng , Haq Zaheer ul , Ren Teng , Luo Zhenggang , Tu Hui , Wang Zaixue , Deng Min , Zhang Jianming , Zang Yanan , Li Peipei , Cong Houluo , Song Shuaishuai , Liu Feng 
Published: October 2024

AbstractIn this work, the application of reclaimed ground tire rubber (RGTR) and butyl reclaimed rubber (BRR) in the inner liner rubber were investigated. Carbon black dispersion, rheological, mechanical, tear strength, dynamic compression heat build‐up, aging performance, and gas barrier properties of tire inner liner were evaluated to analyze the effects of reclaimed rubbers on the tire application. It was found that RGTR improves carbon black dispersion and tear strength of tire inner liner, while maintaining comparable tensile strength, particularly with low amount of RGTR. Furthermore, compounds containing lower amounts of RGTR exhibit reduced heat build‐up during dynamic compression tests. Additionally, RGTR with higher reclamation degree demonstrates favorable aging performance, and has superior gas barrier properties at lower amount. These findings suggest promising opportunities for the application of reclaimed rubber to enhance the performance inner liner of Radial Engineering Tires and contribute to the waste management.
Construction of epoxy resin with enhanced flame retardancy, mechanical properties, and satisfactory transparency based on a novel bi‐DOPO and hydrogen‐bonding network
Authors: Lin Xiaoling , Xiao Xingzhen , Li Dingsi , Wang Yonghui , Chen Xinrong , Zhong Wei , Lan Jiashui , Zhang Simeng , Zhang Huagui , Chen Mingfeng 
Published: October 2024

AbstractEstablishment of high‐performance epoxy resin with satisfactory fire safety, mechanical properties, and excellent transparency is urgently desirable, but still remains significant challenges. Herein, a super‐tough yet high flame retardant epoxy resin (EP/BTD) was designed and prepared by incorporating bi‐DOPO structure and hydrogen‐bonding networks. Although the phosphorus content was only 0.69 wt% (10 wt% of bi‐DOPO flame retardant [BTD]), EP/BTD‐10 showed a high limiting oxygen index value (33.4%), satisfactory UL‐94 rating (V‐0), and good heat suppression ability (total heat release [THR] and peak heat release rate [PHRR] reduced to 29.0% and 42.2%, respectively). Furthermore, the flame retardant mechanism of EP/BTD was illustrated and attributed to dual‐phase fire‐retardant effect. Additionally, EP/BTD‐7.5 featured notably mechanical properties, of which the tensile strength, elongation at break and impact strength increased by 44.6%, 40.0%, and 232.6%, respectively, due to hydrogen‐bonding network and π–π interaction. More importantly, EP/BTD maintained high visible light transmittance and excellent UV‐blocking properties. In summary, this work provided a guidance for the development of high‐performance epoxy resin and was expected to expand the practical applications.
Close‐Packed One‐Dimensional Coordination Polymer Cathode with Fast Kinetics for Sodium‐Ion Batteries
Authors: Lo Yi‐An , Yimtrakarn Trakarn , Chen Teng‐Hao , Lee Jui‐Chin , Kaveevivitchai Watchareeya 
Published: October 2024

AbstractSustainable sodium‐ion batteries (SIBs) have gained tremendous attention; however, the large‐sized Na+ poses serious challenges on the development of inorganic‐based cathodes. To overcome the issues, metal–organic electrode materials are appealing because they combine attractive characteristics of organic redox centers (e. g., flexibility, highly reversible redox properties, fast kinetics (regardless of size and charge of guest ions), structural/redox tunability, and resource abundance) with structural stability arising from metal‐ligand coordination. Herein, a one‐dimensional copper−benzoquinoid coordination polymer (CP), [CuL(Py)2]n, (LH4=1,4‐dicyano‐2,3,5,6‐tetrahydroxybenzene, Py=pyridine) is investigated as cathode for SIBs. As opposed to most CPs reported for SIBs which possess high porosity and surface area, this close‐packed CP can deliver discharge capacity as high as 277 mAh g−1 at 2C (~523 mA g−1), and at extremely high rates of 50C and 300C (~13 and 78 A g−1), reversible capacities of 131 and 74 mAh g−1 still can be delivered, respectively. The transport kinetics of Na+ in [CuL(Py)2]n is found to be even faster than that of Li+ despite the close‐packed structure. The mechanistic and kinetic studies have been performed. The findings gained in this work undoubtedly unravel a potential design strategy for high‐performance metal–organic electrode materials for emerging post‐Li‐ion batteries.