bluuebunny/crossref_metadata_2025_split huggingface dataset:
A TLR7 Agonist Conjugated to a Nanofibrous Peptide Hydrogel as a Potent Vaccine Adjuvant
Authors: Euliano Erin M. , Pogostin Brett H. , Agrawal Anushka , Yu Marina H. , Baryakova Tsvetelina H. , Graf Tyler P. , Kunkel Alyssa A. , Cahue Kiana A. , Hartgerink Jeffrey D. , McHugh Kevin J. 
Published: October 2024

AbstractToll‐like receptors (TLRs) recognize pathogen‐ and damage‐associated molecular patterns and, in turn, trigger the release of cytokines and other immunostimulatory molecules. As a result, TLR agonists are increasingly being investigated as vaccine adjuvants. Many of these agonists are small molecules that quickly diffuse away from the vaccination site, limiting their co‐localization with antigens and, thus, their effect. Here, the small‐molecule TLR7 agonist 1V209 is conjugated to a positively‐charged multidomain peptide (MDP) hydrogel, K2, which was previously shown to act as an adjuvant promoting humoral immunity. Mixing the 1V209‐conjugated K2 50:50 with the unfunctionalized K2 produces hydrogels that retain the shear‐thinning and self‐healing physical properties of the original MDP while improving the solubility of 1V209 more than 200‐fold compared to the unconjugated molecule. When co‐delivered with ovalbumin as a model antigen, 1V209‐functionalized K2 produces a robust Th2 immune response and an antigen‐specific Th1 immune response superior to alum, a widely used vaccine adjuvant. Together, these results suggest that K2 MDP hydrogels functionalized with 1V209 are a promising adjuvant for vaccines against infectious diseases, especially those benefiting from a combined Th1 and Th2 immune response.
A Versatile Microporous Design toward Toughened yet Softened Self‐Healing Materials
Authors: Sun FuYao , Zhang JingYi , Liu Tong , Yao Hai , Wang Lin , Meng HengYu , Gao YunLong , Cao YanFeng , Yao BoWen , Xu JianHua , Fu JiaJun 
Published: October 2024

AbstractRealizing the full potential of self‐healing materials in stretchable electronics necessitates not only low modulus to enable high adaptivity, but also high toughness to resist crack propagation. However, existing toughening strategies for soft self‐healing materials have only modestly improves mechanical dissipation near the crack tip (ГD), and invariably compromise the material's inherent softness and autonomous healing capabilities. Here, a synthetic microporous architecture is demonstrated that unprecedently toughens and softens self‐healing materials without impacting their intrinsic self‐healing kinetics. This microporous structure spreads energy dissipation across the entire material through a bran‐new dissipative mode of adaptable crack movement (ГA), which substantially increases the fracture toughness by 31.6 times, from 3.19 to 100.86 kJ m−2, and the fractocohesive length by 20.7 times, from 0.59 mm to 12.24 mm. This combination of unprecedented fracture toughness (100.86 kJ m−2) and centimeter‐scale fractocohesive length (1.23 cm) surpasses all previous records for synthetic soft self‐healing materials and even exceeds those of light alloys. Coupled with significantly enhanced softness (0.43 MPa) and nearly perfect autonomous self‐healing efficiency (≈100%), this robust material is ideal for constructing durable kirigami electronics for wearable devices.
Air‐Processed Efficient Perovskite Solar Cells With Full Lifecycle Management
Authors: Tian Chuanming , Wu Tianhao , Zhou Xinliang , Zhao Yu , Li Bin , Han Xuefei , Li Kerui , Hou Chengyi , Li Yaogang , Wang Hongzhi , Zhang Qinghong 
Published: October 2024

AbstractDespite the outstanding power conversion efficiency of perovskite solar cells (PSCs) realized over the years, the entire lifecycle from preparation and operation to discarding of PSCs still needs to be carefully considered when it faces the upcoming large‐scale production and deployment. In this study, bio‐derived chitin‐based polymers are employed to realize the full lifecycle regulation of air‐processed PSCs by forming multiple coordinated and hydrogen bonds to stabilize the lead iodide and organic salt precursor inks, accelerating the solid–liquid reaction and crystallization of two‐step deposition process, then achieving the high crystalline and oriented perovskites with less notorious charge defects in the open air. The air‐prepared PSCs exhibit a decent efficiency of 25.18% with high preparation reproducibility and improved operational stability toward the harsh environment and mechanical stress stimuli. The modified PSCs display negligible fatigue behavior with keeping 92% of its initial efficiency after operating for 32 diurnal cycles (ISOS‐LC‐1 protocol). Meanwhile, closed‐loop lead management of end‐of‐life PSCs including suppression of lead leakage, toxicity evaluation of broken devices, and recycling of lead iodide components are comprehensively investigated. This work sheds light on a promising avenue to realize the entire lifecycle regulation of air‐processed efficient and stable PSCs.
Bifunctional Fluorocarbon Electrode Additive Lowers the Salt Dependence of Aqueous Electrolytes
Authors: Liu Binghang , Ma Jintao , Feng Jingnan , Lin Ting , Suo Liumin 
Published: October 2024

AbstractThe solid electrolyte interphase (SEI) plays a crucial role in extending the life of aqueous batteries. The traditional anion‐derived SEI formation in aqueous electrolytes highly depends on high‐concentrated organic fluorinating salts, resulting in low forming efficiency and long‐term consumption. In response, this study proposes a bifunctional fluorocarbon electrode additive (BFEA) that enables electrochemical pre‐reduction instead of TFSI anion to form the LiF‐rich SEI and in situ produce conductive graphite inside the anode before the lithiation. The BFEA lowers the salt dependence of aqueous electrolytes, enabling the inorganic LiCl electrolyte to work first, but also successfully achieves a high SEI formation efficiency in the relatively low 10 m LiTFSI without mass transfer concerns, suppressing the parasitic hydrogen evolution from 11.24 to 4.35 nmol min−1. Besides, BFEA strengthens the intrinsic superiority of Li storage reaction by lowering battery polarization resulting from the in situ production of graphite, promoting charge transfer of electrode kinetics. Compared with the control group, the demonstrated Ah‐level pouch cell employing BFEA exhibits better cycle stability above 300 cycles with higher capacity retention of 78.2% and the lower decay of the round‐trip efficiency (△RTE = 2%), benefiting for maintaining the high efficiency and reducing heat accumulation in large‐scale electric energy storage.
Free‐Standing, Multifunctional Thermoelectric and Acoustic Absorbing Nanocomposite Foams
Authors: Liu Rui Yang , Sun Yu‐Chen , Liu Szu‐Ling , Fang Weiqing , Li Terek , Martinez‐Rubi Yadienka , Jakubinek Michael , Ashrafi Behnam , Kingston Christopher , Naguib Hani E. 
Published: October 2024

AbstractThermoelectric materials are potential energy harvesting technologies that enable direct, clean conversion between thermal and electrical energy. The efficacy of thermoelectric energy conversion is influenced by the electrical conductivity, thermal conductivity, and Seebeck coefficient. Flexibility, manufacturability, and cost‐effectiveness are also important factors. Polymeric nanocomposites offer advantages in these respects. However, the development of conductive‐polymer thermoelectric materials is limited to an in‐plane architecture, which does not resemble common real‐world scenarios. Moreover, existing works have low thermoelectric properties or rely on additives for performance improvement. In this work, a free‐standing thermoelectric nanocomposite foam is fabricated via the integration of thermally activated microspheres. Due to the microstructure, a thermal conductivity as low as 0.03 W m−1 K−1 is achieved, which is lower than reported for aerogels fabricated via freeze‐drying methods. Additionally, the nanocomposite foam can reach a maximum electrical conductivity of 1.13 S cm−1, power factor of 0.12 µW m−1 K−2, and thermoelectric figure of merit of 3.0 × 10−4. The study also evaluated the compressive stiffness and demonstrated the potential for sound absorption. With the unique combination of the thermoelectric, sound absorption, and mechanical behavior, these nanocomposite foams would offer versatile solutions to address the next generation energy harvesting and acoustic absorption applications.
Charge Carrier Collection Losses in Lead‐Halide Perovskite Solar Cells
Authors: Akel Samah , Wang Yueming , Yan Genghua , Rau Uwe , Kirchartz Thomas 
Published: October 2024

AbstractThe collection of photogenerated charges in halide perovskite solar cells depends on the thickness of the absorber layer, with larger thicknesses leading to a reduced collection efficiency. This observation has traditionally been associated with insufficiently high electron and hole diffusion lengths in the absorber layers. However, it is shown that in the presence of low‐mobility contact layers, charge collection can be thickness‐dependent, even if the absorber layer has infinite mobility. Here, analytical equations are derived for the thickness dependence of charge collection losses in situations where recombination is bulk or interface‐limited and show how to relate these equations to voltage‐dependent photoluminescence data. The analytical equations are compared to experimental data and numerical simulations and it is observed that experimental data on triple‐cation perovskite devices with different thicknesses approximately follows the case, where bulk recombination dominates.
Decoupling the Failure Mechanism of Li‐Rich Layered Oxide Cathode During High‐Temperature Storage in Pouch‐Type Full‐Cell: A Practical Concern on Anionic Redox Reaction
Authors: Zhang Baodan , Zhang Kang , Wu Xiaohong , Zheng Qizheng , Luo Haiyan , Zhang Haitang , Chen Yilong , Zhou Shiyuan , Zhu Yuanlong , Yin Jianhua , Zou Yeguo , Liao Hong‐Gang , Jiao Wen , Liu Na , Qin Yaru , Zhang Bin‐Wei , Shen Chongheng , Qiao Yu , Sun Shi‐Gang 
Published: October 2024

AbstractIn addressing the global climate crisis, the energy storage performance of Li‐ion batteries (LIBs) under extreme conditions, particularly for high‐energy‐density Li‐rich layered oxide (LRLO) cathode, is of the essence. Despite numerous researches into the mechanisms and optimization of LRLO cathodes under ideal moderate environment, there is a dearth of case studies on their practical/harsh working environments (e.g., pouch‐type full‐cell, high‐temperature storage), which is a critical aspect for the safety and commercial application. In this study, using pouch‐type full‐cells as prototype investigation target, the study finds the cell assembled with LRLO cathode present severer voltage decay than typical NCM layered cathode after high‐temperature storage. Further decoupling elucidates the primary failure mechanism is the over‐activation of lattice oxidized oxygen (aggravate by high‐temperature storage) and subsequent escape of oxidized oxygen species (On−), which disrupts transition metal (TM) coordination and exacerbates electrolyte decomposition, leading to severe TM dissolution, interfacial film reconstruction, and harmful shuttle effects. These chain behaviors upon high‐temperature storage significantly influence the stability of both electrodes, causing substantial voltage decay and lithium loss, which accelerates full‐cell failure. Although the anionic redox reaction can bring additional energy, but the escape of metastable On− species would introduce new concerns in practical cell working conditions.
Association Between Early‐Life and Premorbid Measurements of Body Composition and Risk of Motor Neuron Disease: A Prospective Cohort Study in the UK Biobank
Authors: Joyce Emily E. , Xu Shishi , Ingre Caroline , Potenza Rosa Luisa , Seitz Christina , Yang Huazhen , Zeng Yu , Song Huan , Fang Fang 
Published: October 2024

ObjectiveThe objective of this study was to investigate the association between developmental and premorbid body composition measurements and the risk of motor neuron disease (MND).MethodsWe performed a cohort study in the UK Biobank to assess the association of developmental body metrics and premorbid body composition measures (using 28 measurements and 7 patterns of body composition) with the risk of MND. Among participants with longitudinal measures, we compared the changes in body composition over time between individuals who later developed MND and those who remained free of MND.ResultsAmong the 412,691 individuals included in this study, 549 people received an MND diagnosis during the follow‐up visit. Higher birth weight was associated with an increased risk of MND among individuals born over 4 kg (hazard ratio [HR] per kg increase = 2.21, 95% confidence interval [CI] = 1.38–3.55), and taller adult height was associated with an increased risk of MND (HR per 5 cm increase = 1.10, 95% CI = 1.03–1.17). We observed that measures of elevated fat mass were associated with a lower risk of MND more than 5 years before diagnosis. A higher “leg‐dominant fat distribution” pattern was associated with an increased risk whereas higher “muscle strength” was associated with a reduced risk of MND 5 years before diagnosis. Longitudinal analyses indicated a faster decline in measures of fat mass and muscle strength, as well as a shift in fat distribution from arm to leg dominant, among individuals who later developed MND, compared with others.InterpretationBody composition at early and middle age may be indicative of the risk of MND development. ANN NEUROL 2025;97:259–269
Electrothermal Conversion of Methane to Methanol at Room Temperature with Phosphotungstic Acid
Authors: Chang Jinquan , Wang Sikai , Hülsey Max J. , Zhang Sheng , Nee Lou Shi , Ma Xinbin , Yan Ning 
Published: October 2024

AbstractTraditional methods for the aerobic oxidation of methane to methanol frequently require the use of noble metal catalysts or flammable H2‐O2 mixtures. While electrochemical methods enhance safety and may avoid the use of noble metals, these processes suffer from low yields due to limited current density and/or low selectivity. Here, we design an electrothermal process to conduct aerobic oxidation of methane to methanol at room temperature using phosphotungstic acid (PTA) as a redox mediator. When electrochemically reduced, PTA activates methane with O2 to produce methanol selectively. The optimum productivity reaches 29.45
with approximately 20.3 % overall electron yield. Under continuous operation, we achieved 19.90
catalytic activity, over 74.3 % methanol selectivity, and 10 hours durability. This approach leverages reduced PTA to initiate thermal catalysis in solution phase, addressing slow methane oxidation kinetics and preventing overoxidations on electrode surfaces. The current density towards methanol production increased over 40 times compared with direct electrochemical processes. The in situ generated hydroxyl radical, from the reaction of reduced PTA and oxygen, plays an important role in the methane conversion. This study demonstrates reduced polyoxotungstate as a viable platform to integrate thermo‐ and electrochemical methane oxidation at ambient conditions.
Topology of Gemini‐shaped Hexagonal Heterojunction for Efficient Stereoconvergent Transformation via Dynamic Kinetic Resolution
Authors: Mou Qi , Han Qingqing , Tai Hulin , Fang Yajun , Kim Young Yong , Mu Yingxiao , Chen Shuixia , Huang Liping , Zhang Yi , Jin Long Yi , Huang Zhegang , Lee Myongsoo 
Published: October 2024

AbstractDespite recent advances in the combination of kinetic resolution and racemization for efficient stereoconvergent transformation, the poor stability and limited reaction activities of the products restrict their wide application in industrial production. To overcome these problems, Gemini‐shaped hexagons with para‐heterojunctions for one‐dimensional and two‐dimensional supramolecular polymers were designed via hydrogen‐bonding adhesion by racemization catalyst 1 and kinetic resolution 2 in this work. The polymers from the assembly of Gemini‐shaped hexagons exhibit rapid catalytic behaviour with efficient selectivity for the desired configuration in the synthesis of tertiary alcohols with contiguous stereocenters through dynamic kinetic resolution for the nanoscale heterojunctions of dissimilar catalysts. Among them, the developed 2D polymers gave outstanding enantioselectivities and diastereoselectivities (>99 % ee, 20 : 1 dr) through the cooperation of adjacent dissimilar catalysts. The heterojunctions varying dimensions and distances of dissimilar catalysts provide new insight for increasing the enantioselectivity of chiral organocatalysts.
Carbon Nanocage Supported Asymmetrically Coordinated Nickle Single‐Atom for Enhanced CO2 Electroreduction in Membrane Electrode Assembly
Authors: Lin Yingxi , Xia Chenfeng , Zhu Zhaozhao , Wang Junjie , Niu Huiting , Gong Shuning , Li Zhao , Yang Na , Song Chen Jun , Wu Rui , Xia Bao Yu 
Published: October 2024

AbstractDesigning efficient catalysts for operating CO2 electroreduction in membrane electrode assembly (MEA) faces significant obstacles. Herein, we propose an asymmetrically coordinated Ni single‐atom catalyst featuring axial Br coordination at NiN4Br sites anchoring onto hollow Br/N co‐doped carbon nanocages, achieved through a NaBr‐assisted confined‐pyrolysis strategy. The Ni‐NBr‐C catalyst exhibits a high CO Faradaic efficiency (FECO>97 %) over the current density range of 50 to 350 mA cm−2 in the MEA device. Furthermore, Ni‐NBr‐C shows a stable cell voltage of 2.66±0.2 V while delivering a large current density of 350 mA cm−2 over an 85‐hour long‐term operation, demonstrating its potential for industrial‐scale applications. Advanced characterization techniques and theoretical calculations reveal that the coordination and doping of Br not only enhance the intrinsic activity but also highlight that the unique pore structure improves mass transfer efficiency.
Evaluation of Antimicrobial, Antitumor, Antioxidant Activities, and Molecular Docking Studies of Some Co(II), Cu(II), Mn(II), Ni(II), Pd(II), and Pt(II) Complexes With a Schiff Base Derived From 2‐Chloro‐5‐(trifluoromethyl)aniline
Authors: Pahonțu Elena , Dinu Pîrvu Cristina Elena , Vișan Diana Carolina , Socea Laura Ileana , Apostol Teodora Venera , Oprean Camelia , Păunescu Virgil , Ungurianu Anca , Margină Denisa Marilena , Codiță Irina , Dumitrescu Silviu , Drăgănescu Doina , Lupașcu Gina 
Published: October 2024

ABSTRACTThe antimicrobial, antitumor and antioxidant potential of Co(II), Cu(II), Mn(II), Ni(II), Pd(II), and Pt(II) complexes with 2‐(((2‐chloro‐5‐(trifluoromethyl)phenyl)imino)methyl)phenol HL ligand was investigated. A molecular docking study was carried out to estimate the predicted binding affinity of the compounds to protein targets involved in proliferative and bacterial activities. Fluorescence quenching studies and synchronous spectra were used to examine the metal complexes interactions with CT‐DNA and BSA protein. The DNA binding study have revealed that the complexes are capable of binding with DNA via intercalative mode. The antimicrobial activity of the ligand and metal complexes was studied against three Gram‐positive bacteria, two Gram‐negative bacteria, and three strains of fungi. The best antibacterial effect was demonstrated by the Pt(II) complex on the Staphylococcus aureus strain, and as for the inhibitory effect on fungi, it was stronger on the Candida albicans strain after treatment with the Co(II) complex. The in vitro antiproliferative activity of ligand and complexes was analyzed using MTT, Annexin V/PI, and cell cycle assays. The in vitro results showed that, except for Pd(II) complex, where slight effects were observed, the MCF‐7 line was resistant to the activity of the complexes. In the case of A549 cells, Cu(II) and Pd(II) complexes showed a dose‐dependent antitumor activity, confirmed by both the Alamar blue and the Annexin V/PI analysis. Finally, the antioxidant activity of the compounds was examined by ABTS and DPPH methods. Antioxidant investigation showed that the Ni(II) complex possesses a remarkable ability to trap the cation of the ABTS+ radical (IC50 value 9.35 μM).
Effect of the Introduction of ZnII and CdII Ions on EuIII and TbIII Emission in M2Ln2 Heterometallic Molecules With 2‐Furoic Acid Anions
Authors: Shmelev Maxim A. , Melnikov Stanislav N. , Nikolaevskii Stanislav A. , Kiraev Salauat R. , Ananyev Ivan V. , Nelyubina Yulia V. , Varaksina Evgenia A. , Korshunov Vladislav M. , Taydakov Ilya V. , Goloveshkin Alexander S. , Gogoleva Natalia V. , Sidorov Alexey A. , Eremenko Igor L. , Kiskin Mikhail A. 
Published: October 2024

ABSTRACTHeterometallic d‐4f coordination complexes are of paramount interest in modern coordination chemistry because of their potential applications in organic light‐emitting devices and spintronic materials. Here we report the synthesis and thorough investigation of Ln and MLn (M = Zn, Cd; Ln = Sm, Eu, Gd, Tb) molecular complexes based on 2‐furancarboxylic acid anion (Hfur): [Ln2(NO3)2(fur)4(DME)2] (Ln = Eu, Gd, Tb; DME is dimethoxyethane) and [M2Ln2(NO3)2(fur)8(bpy)2] (M = Zn, Cd; Ln = Eu, Gd, Tb, Sm; bpy is 2,2′‐bipyridyl). The structure and isostructural nature of compounds were determined based on the single‐crystal and powder X‐ray diffraction data. The photophysical properties of the obtained compounds were studied in detail: The energies of the triplet levels of the furoate anion and d‐blocks {M(fur)2(bpy)} (M = Zn, Cd), the relaxation times of the excited states, and the quantum yields were determined. Critical step from Ln complexes to ZnLn and CdLn (Ln = Eu, Tb) is accompanied by an increase in quantum yields, which correlates with a change in the energy of the triplet level of the aromatic part of the complexes and with the results of quantum chemical calculations indicating different schemes for the origination of triplet levels in MLn compounds.
Preparation of low‐temperature self‐crosslinking acrylic resin and its performance research
Authors: Xin Hua , Zhang Peiyi , Xu Yiyi , Gao Bo , Yuan Luoqi , Wei Minli 
Published: October 2024

AbstractAcrylic resin, as a common coating and adhesive, possesses excellent heat resistance, weather resistance, and is inexpensive, making it widely used in industries related to automotive, construction, electronics, fabrics, and other sectors essential to our daily life. Traditional acrylic resin not only pollutes the environment but also poses certain health risks. Therefore, we studied the synthesis of a low‐temperature self‐crosslinking acrylic emulsions were synthesized by free radical solution polymerization using methyl methacrylate (MMA), butyl acrylate (BA), acrylic acid (AA), diacetone acrylamide (DAAM), hydroxypropyl acrylate (HPA), epoxy resin (E‐51) as the monomers, vinyltriethoxysilane (A‐51) as the coupling agent, and adipic dihydrazide (ADH) as the cross‐linking agent. This water‐based acrylic resin undergoes a crosslinking reaction between the carbonyl group of DAAM and the hydrazide group of ADH, substantially improved the drying speed and adhesion compared to unmodified versions, and also improved the thermal stability. The contact angle of the film increased from 72.8° to 86.9° with the increase of the degree of cross‐linking, and the mechanical properties were improved by 60%. This study provides a suitable formulation for preparing water‐based acrylic resins with superior performance.