bluuebunny/crossref_metadata_2025_split huggingface dataset:
TMEM106B C‐terminal fragments aggregate and drive neurodegenerative proteinopathy in transgenic Caenorhabditis elegans
Authors: Riordan Ruben , Saxton Aleen , Han Marina , McMillan Pamela J. , Kow Rebecca L. , Liachko Nicole F. , Kraemer Brian C. 
Published: December 2024

AbstractINTRODUCTIONGenetic variation in the lysosomal and transmembrane protein 106B (TMEM106B) modifies risk for several neurodegenerative disorders, especially frontotemporal lobar degeneration (FTLD). The C‐terminal (CT) domain of TMEM106B occurs as fibrillar protein deposits in the brains of dementia patients.METHODSTo determine the TMEM CT aggregation propensity and neurodegenerative potential, we generated transgenic Caenorhabditis elegans expressing the human TMEM CT fragment aggregating in FTLD cases.RESULTSPan‐neuronal expression of human TMEM CT in C. elegans causes severe neuronal dysfunction driving neurodegeneration. Cytosolic aggregation of TMEM CT proteins accompanied by behavioral dysfunction and neurodegeneration. Loss of pgrn‐1 did not modify TMEM CT phenotypes suggesting TMEM CT aggregation occurs downstream of PGRN loss of function. The mechanistic drivers of TMEM106B proteinopathy appear distinct from known modifiers of tauopathy.DISCUSSIONOur data demonstrate that TMEM CT aggregation can kill neurons. TMEM106B transgenic C.elegans provide a useful model for characterizing TMEM106B proteinopathy‐mediated neurodegeneration in FTLD.Highlights
Pan‐neuronal expression of human TMEM106B C‐terminal fragments (TMEM CT) in C. elegans neurons drives a suite of disease‐related phenotypes useful for modeling the molecular and cellular features of TMEM106B neuropathology.
TMEM CT expression results in extensive TMEM aggregation and accumulation of highly detergent insoluble protein species.
TMEM CT expression causes moderate to severe neuronal dysfunction dependent on TMEM CT abundance as measured by stereotypical behavioral readouts.
TMEM CT expression drives significant neurodegenerative changes.
Dendra2 tagged TMEM exhibits similar properties to untagged TMEM allowing ready visualization of the protein.
TMEM CT aggregates accumulate adjacent to but not within lysosomes.
PGRN loss of function does not impact TMEM CT toxicity.
Modifiers of tau and TDP‐43 proteinopathies have little impact on TMEM CT‐related neurodegenerative phenotypes.
The Influence of Alkyl Spacers and Molecular Weight on the Charge Transport and Storage Properties of Oxy‐Bithiophene‐Based Conjugated Polymers
Authors: Yu Hang , Marks Adam , Tuladhar Sachetan M. , Siemons Nicholas , Anderson Iona , Bidinger Sophia , Keene Scott T. , Quill Tyler J. , Wu Ruiheng , Gough Olivia , Wu Guanchen , Eisner Flurin , Salleo Alberto , Rivnay Jonathan , Malliaras George G. , Barnes Piers R. F. , McCulloch Iain , Nelson Jenny 
Published: December 2024

AbstractConjugated polymers (CPs) with polar side chains can conduct electronic and ionic charges simultaneously, making them promising for bioelectronics, electrocatalysis and energy storage. Recent work showed that adding alkyl spacers between CP backbones and polar side chains improved electronic charge carrier mobility, reduced swelling and enhanced stability, without compromising ion transport. However, how alkyl spacers impact polymer backbone conformation and, subsequently, electronic properties remain unclear. In this work, we design two oxy‐bithiophene‐based CP series, each featuring progressively extended alkyl spacer lengths and two distinct molecular weight (MW) distributions. Using operando characterisations, we evaluate the (spectro)electrochemical and swelling properties of the polymer thin films, and their performance in organic field‐effect transistors and organic electrochemical transistors. Surprisingly, alkyl spacers negatively impact the hole mobility of our polymers, with higher MW amplifying this effect. Using molecular dynamics simulations, we show that it is thermodynamically favourable for adjacent non‐polar alkyl spacers to aggregate in polar electrolytes, leading to backbone twisting. Further spectroscopic measurements corroborate this prediction. Our findings demonstrate the active interactions between side chain structure, MW and electrolyte/solvent polarity in influencing polymer performance, underscoring the importance of considering solvation environment effects on polymer conformation when designing new mixed conducting CPs for electrochemical applications.
Adjacent‐Ligand Tuning of Atomically Precise Cu−Pd Sites Enables Efficient Methanol Electrooxidation with a CO‐Free Pathway
Authors: Qin Yuanlong , Yu Kedi , Wang Guo , Zhuang Zechao , Dou Yuhai , Wang Dingsheng , Chen Zhengbo 
Published: December 2024

AbstractWhether the catalyst can realize the non‐CO pathway is the key to greatly improve the catalytic activity and stability of methanol oxidation reaction (MOR). It is feasible to optimize the reaction path selectivity by modifying organic ligands and constructing single‐atom systems. At the same time, heterogeneous metal nanosheets with atomic thickness have been shown to significantly enhance the catalytic activity of materials due to their ultra‐high exposure of active sites and synergistic effects. Herein, we synthesize an ultra‐thin heterogeneous alloy metallene with organic ligand‐modified surface Cu single atom by one‐pot wet chemical method, and further construct an efficient Cu−Pd active sites. The prepared octanoic acid ligand modified PdCu single‐atom alloys metallene (SAA OA−Cu‐Pdene) shows excellent catalytic activity and stability, with mass activity up to 5.64 A mgPd−1 and electrochemical active surface area (ECSA) up to 160.39 m2 gPd−1. Structural characterization and in situ experiment jointly indicate that ligand modulation brings about charge transfer, and the accompanying rapid migration of OH− greatly improves the selectivity of non‐CO pathways while improving the catalytic activity. The results highlight the importance of adjacent‐ligand regulation and provide a new strategy for the design of MOR catalysts with high selectivity of non‐CO pathway.
Charge Manipulation of Porous Coordination Cages Tunes the Efficiency and Selectivity in Electrochemical Synthesis
Authors: Su Zhifang , Liu Kang‐Kai , Xu Yu‐Qi , Yan Bing , Wang Shuangyin , Guan Zong‐Jie , Zou Yuqin , Fang Yu 
Published: December 2024

AbstractElectrocatalytic synthesis of high‐value chemicals has been attracting growing interest owing to its environmentally benign reaction pathways. Among these processes, the electrocatalytic reduction of nitrate (NO3−) to ammonia (NH3), known as NO3RR, and the oxidation of 5‐hydroxymethylfurfural (HMFOR) stand out as two cornerstone reactions; yet, their efficiency and selectivity pose ongoing challenges. In this study, we introduce a charge manipulation approach for the design of highly efficient electrocatalysts tailored for the simultaneous coupling of NO3RR and HMFOR. We have synthesized a range of porous coordination cages (PCCs) that share the same topology and Co/Ni metal centers but incorporate different charged moieties, imparting them with distinct surface net charges. Electrocatalytic evaluations revealed that PCC‐Co demonstrated a voltage‐dependent activity in NO3RR. Conversely, PCC‐Ni exhibited a precisely adjustable product selectivity in HMFOR, contingent upon the cage‘s charge state. In situ analysis and Density functional theory (DFT) calculations underscored the profound impact of catalyst charge on the differential adsorption of reaction intermediates and the lowest free energy change (ΔG) during the pivotal reaction step, resulting in alterations to both activity and selectivity. These discoveries provide invaluable insights into the “structure‐performance relationship” of NO3RR/HMFOR catalysts, highlighting PCCs as promising contenders for advanced electrocatalysts.
Towards the Use of Low‐Concentration CO2 Sources by Direct Selective Electrocatalytic Reduction
Authors: Mahbub Muhammad Adib Abdillah , Das Debanjan , Wang Xin , Lu Guilong , Muhler Martin , Schuhmann Wolfgang 
Published: December 2024

AbstractThe direct CO2 reduction reaction (CO2RR) from simulated flue gas of various CO2 concentrations could minimize extra energy for pre‐concentration processes to highly concentrated CO2 as a feedstock. We investigate the challenges for CO2RR caused by low CO2 concentrations and provide strategies concerning the impact of the chosen electrocatalyst material and the selection of the electrolyte to attain high CO selectivity. We continuously feed CO2 mixed with N2 (the typical dilutant in flue gas) in various ratios to gas diffusion electrodes in a model flow‐through electrolyzer. Operating the CO2RR at lower CO2 concentrations results in an overpotential shift to more cathodic values. We show that higher active catalysts can maintain high CO selectivity down to 5 % CO2 by using NiCu‐based catalysts. NiCu reached its limit when the CO2 concentration was lowered to 2 %, due to low CO2 availability and competition of carbonate formation. Employing near‐neutral electrolytes with buffering capacity, we maintained high Faradaic efficiency at low overpotentials and higher CO2 utilization at low CO2 concentration.
The Influence of Air Gap Length on the Characteristics and Performance of Hybrid Polyethersulfone/Cellulose Nanocrystal/Multiwalled Carbon Nanotubes Hollow Fiber Membrane for Humic Acid Removal
Authors: C. Mahmud Nor Azura , Saufi Syed M. , Abu Seman Mazrul Nizam , Takriff Mohd Sobri , Ang Wei Lun , Ab Latiff Mohd Helmi 
Published: December 2024

ABSTRACTReady‐made or commercial hollow fiber (HF) membranes have limited performance for removing humic acid (HA) from water streams unless they undergo surface modification. Alternatively, a membrane can be tailor‐made specifically for HA removal by developing a new formulation and adjusting its fabrication parameters. In this study, to enhance the performance and antifouling properties of HF membranes, a hybrid membrane was developed by blending polyethersulfone (PES) with cellulose nanocrystals (CNC) and multiwalled carbon nanotubes (MWCNT). The effect of air gap length during the dry–wet spinning process was investigated, ranging from 3 cm to 12 cm, to regulate the properties of the hybrid membrane. The membranes were evaluated in terms of morphology (FESEM and AFM), porosity, and hydrophilicity (contact angle). Water flux, HA rejection, and flux recovery ratio (FRR) were also measured. The air gap length significantly influenced the fiber structure, with the finger‐like structure expanding from the outer surface to the center of the fiber as the air gap extended up to 9 cm. This increase in air gap length resulted in a significant reduction in porosity, decreasing from 75.59% to 43.45%, while simultaneously enhancing the contact angle from 78° to 89.60°. The membrane produced at a 9 cm air gap length exhibited the best performance, with a pure water flux of 15.83 LMH, HA rejection over 95%, and a high FRR of 98.78%. The synergistic effect of combining CNC with MWCNT and simply adjusting the air gap distance proves to be an effective approach for preparing custom‐made HF membranes for HA removal.
Subsurface AFM Study of Inhomogeneous Polymeric Materials
Authors: Morozov I. A. 
Published: December 2024

ABSTRACTFast indentation by atomic force microscopy allows the study of structural and physico‐mechanical properties of polymer surfaces. However, the applied load and the choice of the contact point affect the measured surface properties of the inhomogeneous material. The method of tracing the evolution of the surface structure under the load is presented. The stages of loading (tip‐surface contact, penetration into the outer surface layer revealing the internal structure) and unloading (viscoelastic recovery of the surface) are studied. Three polymers (epoxy, polyethylene, and filled rubber), whose internal heterogeneous structure is covered by a soft layer, have been analyzed. The importance of accurate determination of the contact point and the related limitations of static contact models at shallow indentation depths are shown. A dynamic model of nonequilibrium tip‐surface interaction is used to determine the surface energy and elastic modulus of the upper surface layer. The elastic moduli obtained at shallow and deep indentation depths allowed the estimation of the thickness of the layer covering the subsurface structures of the epoxy and the polyethylene. Analysis of the evolution of the filled rubber surface under the load showed the filler distribution in the matrix.
Miniaturized Mechanical Antennas: Advances, Challenges, and Future Directions
Authors: Ren Hao 
Published: December 2024

AbstractIn the past decade, miniaturized mechanical antennas have become a research focus. Several types of mechanical antennas based on different operation principles, including mechanical antennas based on magnetoelectric effect, mechanical antennas based on permanent magnets, mechanical antennas based on electrets, and mechanical antennas based on piezoelectric resonators, are presented, all with sizes significantly smaller than conventional electrical antennas operating at the same resonant frequencies. This review focuses on the advances in mechanical antennas, potential applications as well as challenges and potential future directions for further performance improvement. Although the sizes of the state‐of‐the‐art mechanical antennas are several orders of magnitude smaller than traditional electrical counterparts with the same resonant frequencies, the reported maximum operation distance of mechanical antennas is still short, which is a major challenge for it to be widely implemented. By adopting new materials for mechanical antennas, adopting array configurations, adopting receiving antennas with higher sensitivity, and building new electromagnetic‐electromechanical coupled simulation methods, the maximum operation distance may be significantly improved, making mechanical antennas widely implemented in the Internet of Things (IoT), wireless sensor networks (WSN), implantable medical devices (IMD), and portable electronics applications.
Ligand Assisted Co(II)‐Catalyzed Multicomponent Synthesis of Substituted Pyrroles and Pyridines
Authors: Chakraborty Subhajit , Singha Mohapatra Arijit , Saha Subhangi , Mandal Sutanuva , Paul Nanda D. 
Published: December 2024

AbstractHerein, we describe a sustainable Co(II)‐catalyzed synthesis of pyrroles and pyridines. Using a Co(II)‐catalyst [CoII2(La)2Cl2] (1 a) bearing redox‐active 2‐(phenyldiazenyl)‐1,10‐phenanthroline) (La) scaffold, various substituted pyrroles and pyridines were synthesized in good yields, taking alcohol as one of the primary feedstock. Pyrroles were synthesized by the equimolar reaction of 2‐amino and secondary alcohols. A series of 2,4,6‐substituted symmetrical pyridines were prepared via a three‐component reaction of NH4OAc with 1 : 2.2 molar primary and secondary alcohols, respectively. Unsymmetrically substituted 2,4,6‐trisubstituted, 2,4,5,6‐tetrasubstituted, and 2,3,4,5,6‐pentasubstituted pyridines were achieved via a multi‐component coupling reaction of alcohols and NH4OAc. Catalyst 1 a showed encouraging results during the gram‐scale synthesis of these N‐heterocycles. Mechanistic investigation revealed synergistic involvement of cobalt metal and the ligand during the catalytic reactions.
Multifunctional Fluorescent Material Based Red‐emitting Carbon Dots for Cell Imaging and Photodynamic Sterilization
Authors: Xu Jiatong , Zhao Zhonghua , Cao Yasong , Huang Haowen , Shen Richao , Zeng Cheng , Lv Jiawei , Qi Chunxuan , Lei Ziqiang , Feng Hai‐Tao , Ma Hengchang 
Published: December 2024

AbstractIn this paper, a new carbon dot (R1‐CDs) was prepared by one‐pot hydrothermal method by using 1,8‐diaminonaphthalene and o‐phthalic acid (o‐PA) as precursors. Due to the high purity of R1‐CDs, NMR analysis was performed to identify the types of H and C atoms in their graphene sheets. From our research findings, three important information was disclosed such as (1) five types H atoms are presented in R1‐CDs; (2) 18 kinds of C atoms in the graphene sheets are observed, and 8 kinds of them are quaternary atoms, and 10 kinds of carbon atoms as tertiary one; (3) functional groups of ‐COOH and ‐NH2 from precursors cannot be inherited into the edges or defect sites of graphene sheet. Obviously, our research findings for the first time revealed the more details of chemical structures of CDs. We believe that our works can supply a general concept to fabricate CDs by selecting specific precursors, also can encourage CDs’ development in a more “chemistry” way by employing NMR as a powerful method.
Triazine‐Functionalized Nitrogen‐Rich Covalent Organic Framework as an Electrode Material for Aqueous Symmetric Supercapacitor
Authors: Ahmad Ikrar , Singh Omkar , Ahmed Jahangeer , Priyanka  , Alshehri Saad M. , Bharti Chitranjan , Vidivay  
Published: December 2024

AbstractCovalent triazine frameworks, with their ordered pores and crystalline structure that exhibit heteroatom impacts, demonstrate outstanding chemical stability, making them designable for charge storage applications. In this study, the triazine‐based covalent organic frameworks (TPT@BDA‐COF) was synthesized using 4′,4′′′,4′′′′′‐(1,3,5‐Triazine‐2,4,6‐triyl) tris (([1,1′‐biphenyl]‐4‐amine)) (TPT) and 4,4′‐Oxydibenzaldehyde (BDA) following polycondensation process. Interestingly, these resulted in the fabrication of a well‐connected, orderly porous crystalline structure, redox‐active moiety, and significantly high doping atomic percentages of N (~13.6 %). The three‐electrode electrochemical study, showed a stable electrochemical potential window of 1.8 V (−0.45 to +1.35) in 1 M NaClO4 electrolyte, it exhibited a high specific capacitance of 92.6 mF/cm2 with a high energy density 41.7 Wh/kg respectively. The symmetric supercapacitor designed using TPT@BDA‐COF as both anode and cathode exhibited high specific capacitance (F/g) and gravimetric energy density (Wh/kg): 17.8, 36.9, 43.7, 47.7 and 3.5, 16.6, 13.7, 21.6 in 1 M CH3COONa, 1 M Na2SO4, 1 M NaNO3, 1 M NaClO4 electrolyte respectively. It showed excellent cyclic stability (105.2 %), and Coulombic efficiency (97.5 %) even after 10 k GCD cycles in 1 M NaClO4 at 2 A/g. Interestingly, ClO4− anions exhibited a better chaotropic nature (water structure breaker) as compared to CH3COO−, SO4−2, and NO3−. Their energy storage competence is supported by the illumination of 1 white and 1 red LED upon charging a single SSC for 50 sec each. A Quantum Mechanics (QM) calculation and Molecular Dynamics (MD) simulation are performed to investigate and validate the stability of Covalent Organic Frameworks (COFs). DFT calculations were carried out using the SCF approach B3LYP‐631G(d) basis set to compute the HOMO and LUMO energies and their respective location in COF.
Bimetallic Cooperativity of a Ferrocene‐Based Iridium NHC Complex in Water Oxidation Catalysis: A New Frontier for Efficient Oxygen Evolution
Authors: Bora Debashree , Pratim Bhattacharyya Himangshu , Rahaman Gayen Firdaus , Baguli Sudip , Patel Pitambar , Sarma Manabendra , Saha Biswajit 
Published: December 2024

AbstractBimetallic catalysts have gained attention as promising contenders, owing to the synergistic interaction between two distinct metal centers. In this study, we present two N‐heterocyclic carbene iridium(III) pentamethylcyclopentadienyl complexes [Cp*Ir(fcpyNHC)Cl]PF6 (1) and [Cp*Ir(pyNHC)Cl]PF6 (2) where 1 includes a ferrocene moiety making it a bimetallic complex. Using ceric ammonium nitrate as a sacrificial oxidant, both complexes were tested for water oxidation. Complex 2 achieved a maximum turnover number (TONmax) of 3240 and a turnover frequency (TOFmax) of 231 min−1. In comparison, complex 1 demonstrated nearly double the activity with a TONmax of 6047 and TOFmax of 431 min−1 compared to 2, which was attributed to the cooperative effect of the catalyst in water oxidation reaction. This bimetallic Fe Ir catalyst (1) exhibited outstanding catalytic efficiency for oxygen evolution from water at ambient conditions. We identified a proposed FeIII IrIV intermediate experimentally via UV‐Vis spectroscopy and XPS study. Theoretically, this intermediate was more stable by 7.84 kcal/mol than the traditional FeII IrV electromer intermediate. This delineates the pronounced bimetallic cooperative participation of both Fe and Ir metal centres for better activity.
Mesoporous NiFe2O4@g‐C3N4‐Based p–n Heterostructures for Boosting Solar‐Driven Photocatalytic Dye Degradation and Hydrogen Evolution
Authors: Das Suma , Pramanik Swapnamoy , Nair Ranjith G , Chowdhury Avijit 
Published: December 2024

AbstractMass‐fraction‐optimized heterojunction composites featuring precisely engineered interfaces and mesoporous structures are crucial for improving light absorption, minimizing electron‐hole recombination, and boosting overall catalytic efficiency. Herein, highly efficient mesoporous‐NiFe2O4@g‐C3N4 heterojunctions were developed by embedding p‐type NiFe2O4 nanoparticles (NPs) within n‐type porous ultrathin g‐C3N4 (p‐uCN) nanosheets. The optimized NiFe2O4@g‐C3N4, loaded with 20 wt % magnetic counterparts, exhibits exceptional photocatalytic methylene blue (MB) degradation, achieving the highest performance in both photocatalytic and photo‐Fenton processes with rate constants of 0.062 min−1 and 0.161 min−1, respectively. These performance metrics are 1.3 and 2.55 fold higher than p‐uCN (0.048 min−1 and 0.063 min−1) and 51.6 and 17.4 fold higher than NiFO (0.0012 min−1 and 0.009 min−1). Notably, mp‐NiF@uCN‐20 % with 1.0 wt % of Pt loading achieves the highest H2 evolution rate of 2294 μmolg−1h−1, which is 3.72, 1.52, and 13.49 times higher than that of pure CN, p‐uCN, and NiFO, respectively. The enhanced performance is corroborated by increased surface area, improved separation of charge carriers, and effective charge transfer, which enables simultaneous reduction and oxidation processes. Further, the magnetic nanocomposite exhibits remarkable stability even after multiple runs, indicating their reusability. The experimental findings emphasize the importance of p‐n heterojunctions, interfacial band alignment, and mesoporous architecture in enhancing the photocatalytic efficiency of NiFe2O4@g‐C3N4 nanocomposites.
Effect of Transition Metal Variability in NNN‐Pincer Complexes on Catalytic CO2 Reduction to Methanol
Authors: Vinod Parmar Saurabh , Avasare Vidya 
Published: December 2024

AbstractThe catalytic efficiency of M−H2tpda pincer complexes (M=Mn(I), Fe(II), Co(III)) in CO2 hydrogenation, emphasizing the role of transition metal variability have been discussed. The DFT analysis demonstrates that complexes with low αR values form weaker M−H bonds, enhancing catalyst reactivity with the elongation of M−H bond. The analysis further displays excellent catalytic performance for Mn−H2tpda (ΔE=20.3 kcal/mol), Fe−H2tpda (ΔE=21.0 kcal/mol) and Co−H2tpda (ΔE=23.6 kcal/mol) for CO2 to formic acid formation. The Co−H2tpda (ΔE=16.7 kcal/mol) is comparatively better than Mn−H2tpda (ΔE=20.7 kcal/mol) and Fe−H2tpda (ΔE=19.6 kcal/mol) in formaldehyde formation. All three catalysts exhibit excellent catalytic performance in the conversion of formaldehyde to methanol. The condensed Fukui function calculations of these catalyst complexes establish direct relationship between the ΔE for the rate limiting catalytic cycle and the electrophilicity of the metal centers. The TOF calculations further helped to understand the catalytic performance of the catalysts at various temperatures.