bluuebunny/crossref_metadata_2025_split huggingface dataset:
N‐P Type Charge Compensatory Synergistic Effect for Schottky and Efficient Photoelectrocatalysis Applications: Doping Mechanism in (Nb/Re)@WS2/Graphene Heterojunctions
Authors: Zhou Zhonghao , Qi Wei , Li Zhi , Yang Li , Lin Zhichao , Guan Renguo 
Published: November 2024

AbstractBand gap engineering based on doped two‐dimensional (2D) transition metal dichalcogenides (TMDs) has shown great potential in the design and development of new nano photoelectronic devices and their application in photoelectrocatalysis. However, there are two key issues that are difficult to take into account, namely the impurity levels induced by dopant atoms appear in the forbidden band of the doping system, which can become the recombination center of photogenerated carriers, thereby reducing the photocatalytic efficiency. Compared with the carrier mobility of the corresponding doped systems, that of intrinsic 2D TMDs is too low. Understanding the doping mechanism of heteroatoms in these systems and designing corresponding crystal structures rationally is important for solving these problems. In this study, the crystal structures of co‐doped monolayer WS2 with Nb and Re atoms were designed using density functional theory, and doping systems with graphene (high carrier mobility) were assembled into a heterostructure using the concept of heterorecombination. The N‐P type co‐doping of Nb and Re atoms retained the continuous band characteristics of the original monolayer WS2 while also providing the high carrier mobility of graphene, yielding an excellent multipurpose material for manufacturing high‐speed Schottky devices and efficient water‐splitting H evolution catalysts.
Origins of Catalysis in Non‐Heme Fe(II)/2‐Oxoglutarate‐Dependent Histone Lysine Demethylase KDM4A with Differently Methylated Histone H3 Peptides
Authors: Devadas Sudheesh , Thomas Midhun George , Rifayee Simahudeen Bathir Jaber Sathik , Varada Bhargav , White Walter , Sommer Ethan , Campbell Kylin , Schofield Christopher J. , Christov Christo Z. 
Published: November 2024

AbstractHistone lysine demethylase 4 A (KDM4A), a non‐heme Fe(II)/2‐oxoglutarate (2OG) dependent oxygenase that catalyzes the demethylation of tri‐methylated lysine residues at the 9, 27, and 36 positions of histone H3 (H3 K9me3, H3 K27me3, and H3 K36me3). These methylated residues show contrasting transcriptional roles; therefore, understanding KDM4A's catalytic mechanisms with these substrates is essential to explain the factors that control the different sequence‐dependent demethylations. In this study, we use molecular dynamics (MD)‐based combined quantum mechanics/molecular mechanics (QM/MM) methods to investigate determinants of KDM4A catalysis with H3 K9me3, H3 K27me3 and H3 K36me3 substrates. In KDM4A‐H3(5–14)K9me3 and KDM4A‐H3(23–32)K27me3 ferryl complexes, the O−H distance positively correlates with the activation barrier of the rate‐limiting step, however in the KDM4A‐H3(32–41)K36me3, no direct one‐to‐one relationship was found implying that the synergistic effects between the geometric parameters, second sphere interactions and the intrinsic electric field contribute for the effective catalysis for this substrate. The intrinsic electric field along the Fe−O bond changes between the three complexes and shows a positive correlation with the HAT activation barrier, suggesting that modulating electric field can be used for fine engineering KDM catalysis with a specific substrate. The results reveal how KDM4A uses a combination of strategies to enable near equally efficient demethylation of different H3Kme3 residues.
Synthesis of 1,10‐Phenanthroline‐2,9‐bistriazoles: Evaluation as G‐Quadruplex Binders and Anti‐Tumor Activity
Authors: Figueiredo Joana , Carreira‐Barral Israel , Lourenço Pedro , Miranda André , Lopes‐Nunes Jéssica , Quesada Roberto , Laranjo Mafalda , Mergny Jean‐Louis , Cruz Carla 
Published: November 2024

AbstractNovel 1,10‐phenanthroline‐2,9‐bistriazoles derivatives have been synthesized by copper‐catalyzed azide/alkyne cycloaddition reactions and assessed for their ability to bind and stabilize G‐quadruplex (G4) structures. Ten novel compounds were evaluated using Förster resonance energy transfer (FRET) melting, circular dichroism (CD), and fluorescence spectroscopy on several G4 sequences. Biophysical characterization led to the identification of compounds 4 a, 4 b, and 5 b as good G4 ligands of KRAS G4 sequences. The impact on cell viability of all derivatives was also assessed, revealing weak effects. However, compound 2 a exhibited cytotoxicity activity on A549 and H1299 cancer cells and low cytotoxicity towards MRC‐5 non‐malignant cells MRC‐5 not connected with its G4‐binding ability. Flow cytometry showed that 2 a induced a cell viability decrease in S and G2/M phases for A549 and H1299; thus, more studies should be performed to explore the proteins involved in cell cycle regulation.
Ac34deoGlcNAz: A Selective Probe for Identifying O‐GlcNAc‐Modified Proteins in Prostate Cancer
Authors: Xu Guoliang , Zhu Jiangtao , Wang Xihao , Liu Pengyue , Yan Yongjun , Li Xiaodong , Wang Lianqu , Wang Jiajia 
Published: November 2024

AbstractGlcNAcylation is a prevalent protein modification in eukaryotic cells and increasing evidences indicated that over‐expressed O‐GlcNAcylation are intimately linked to the development and prognosis of prostate cancer. Thus, exploring this modification in the context of prostate cancer is vital for understanding the underlying mechanisms and hopefully used for future targeted therapies. In this paper, we use our previously established metabolic probes to comprehensively compare the labeling efficiency of O‐GlcNAc modified proteins in PC3 cells. Our results demonstrated that all the tested probes were non‐toxic to PC3 cells and only Ac4GlcNAz, Ac4GalNAz and Ac34deoGlcNAz exhibited robust labeling signals amongst the probes. Further investigations by western blot and flow cytometry analysis revealed that Ac34deoGlcNAz was a specific and efficient probe for intracelluar protein labeling with negligible S‐glyco‐modification signal. In addition, proteomic analysis further confirmed that 94 % of the proteins identified by Ac34deoGlcNAz were in the form of O‐linked GlcNAc rather than S‐glyco‐modification, these enriched O‐GlcNAcylated proteins were mainly involved in the regulated processes of prostate cancer. Our results here together prove Ac34deoGlcNAz is a safe and reliable probe for metabolic labeling O‐GlcNAc modified proteins in prostate cancer, providing a mean to fully exploit the regulatory mechanism of O‐GlcNAcylation in the process of prostate cancer.
Two‐Factor Rule for Distinguishing the Covalent and Tetrel Bonds
Authors: Bartashevich Ekaterina , Tsirelson Vladimir 
Published: November 2024

AbstractUnderstanding and exploring the existence of a recognizable boundary between the noncovalent tetrel bond (TtB) and the coordination or weakened covalent bond are important for the bonding characterization. We have developed a simple methodology for analysing the type of bonds based on comparison of the electrostatic and total static potentials along the bond line. For the typical σ‐hole noncovalent bond formed by a Tt atom in a tetrahedral molecule, we have found that the space gap between positions of the maxima of the total static potential and the negative quantity of electrostatic potential is much wider than that for the coordination bonds in a trigonal bipyramid molecular system for the Cl−Tt/Cl⋅⋅⋅Tt and N−Tt/N⋅⋅⋅Tt (Tt=C, Si, Ge) bonds in molecules and molecular complexes. The distinction between the weakened covalent and strengthened noncovalent bonds is well reflected in behaviour of the Fermi hole along the bond line. Two‐factor empirical rule based on the superposition of the electrostatic and total static potentials is suggested.
High‐Performance Intermetallic Pt3Co/C Electrocatalyst for the Oxygen Reduction Reaction Synthesized by Pre‐Lithiation Method
Authors: Zhang Zhengying , Fang Dong , Li Liyang , Yang Hua , Liu Jian , Liu Feng , Gao Yong , Ruzimuradov Olim 
Published: November 2024

AbstractFuel cells are recognized as promising alternatives to existing conventional energy systems for a sustainable future. However, the synthesis of efficient and robust platinum (Pt) based catalysts remains a challenge for practical fuel cell applications. Herein, the Pt3Co/C nanoparticles with about 4.45 nm are firstly prepared by a “pre‐lithiation‐deposition” strategy on C carrier and used as efficient electrocatalysts for cathodic oxygen reduction reaction. Notably, after heat treatment at 600 °C, the obtained Pt3Co/C‐600 catalyst shows excellent mass and specific activities (MA and SA) of 0.69 A mg
and 1.01 mA cm
, respectively, which are more than one order of magnitude higher than that of Pt/C‐600. In particular, after accelerated durability testing with 20k cycles, the durability of the Pt3Co/C‐600 catalyst (98.3 % retention of MA) is much higher than that of Pt3Co/C‐600 without pre‐lithiation (42.5 % retention of MA). The alloying of Pt and Co and the use of “pre‐lithiation” to enable strong interactions between the carbon carriers and the Pt‐Co nanoparticles contributed to the increased activity and excellent stability. This work provides a new perspective for the development of high‐performance and low‐cost Pt alloy electrocatalysts.
A Simple Regeneration Process Using a CO2‐Switchable‐Polarity Solvent for Cellulose Hydrogels
Authors: Matsui Arata , Ayu Putri Deandra , Thomas Morgan L. , Takeoka Yuko , Rikukawa Masahiro , Yoshizawa‐Fujita Masahiro 
Published: November 2024

AbstractCellulose is one of the main components of plant cell walls, abundant on earth, and can be acquired at a low cost. Furthermore, there has been increasing interest in its use in environmentally friendly, carbon‐neutral, sustainable materials. It is expected that the applications of cellulose will expand with the development of a simple processing method. In this study, we dissolved cellulose in aqueous N‐butyl‐N‐methylpyrrolidinium hydroxide solution ([C4mpyr][OH]/H2O) and investigated the cellulose regeneration process based on changes in solubility upon application of CO2 gas. We investigated the effect of transformation of the anion chemical structure on cellulose solubility by flowing CO2 gas into [C4mpyr][OH]/H2O and conducted pH, FT‐IR, and 13C NMR measurements. We observed that the changes in anion structure allowed for the modulation of cellulose solubility in [C4mpyr][OH]/H2O, thus establishing a simple and safe cellulose regeneration process. This regeneration process was also applied to enable the production of cellulose hydrogels. The hydrogel formed using this method was revealed to have higher mechanical strength than an analogous hydrogel produced using the same dissolution solvent with the addition of a cross‐linker. The ability to produce cellulose‐based hydrogels of different mechanical properties is expected to expand the possible applications.
A beginner's guide to supervised analysis for mass cytometry data in cancer biology
Authors: Wlosik Julia , Granjeaud Samuel , Gorvel Laurent , Olive Daniel , Chretien Anne‐Sophie 
Published: November 2024

AbstractMass cytometry enables deep profiling of biological samples at single‐cell resolution. This technology is more than relevant in cancer research due to high cellular heterogeneity and complexity. Downstream analysis of high‐dimensional datasets increasingly relies on machine learning (ML) to extract clinically relevant information, including supervised algorithms for classification and regression purposes. In cancer research, they are used to develop predictive models that will guide clinical decision making. However, the development of supervised algorithms faces major challenges, such as sufficient validation, before being translated into the clinics. In this work, we provide a framework for the analysis of mass cytometry data with a specific focus on supervised algorithms and practical examples of their applications. We also raise awareness on key issues regarding good practices for researchers curious to implement supervised ML on their mass cytometry data. Finally, we discuss the challenges of supervised ML application to cancer research.
Generation and Characterization of a TRIM21 Overexpressing Mouse Line
Authors: Mehlmann Lisa M. , Uliasz Tracy F. , Yee Siu‐Pok , Kaback Deborah , Lowther Katie M. 
Published: November 2024

ABSTRACTSpecific removal of a protein is a key to understanding its function. “Trim‐Away” utilizes TRIM21, an antibody receptor and ubiquitin ligase, for acute and specific reduction of proteins. When TRIM21 is expressed in cells, introduction of a specific antibody causes rapid degradation of the targeted protein; however, TRIM21 is endogenously expressed in few cell types. We have generated a mouse line using CRISPR to insert a conditional overexpression cassette of TRIM21 into the safe harbor site, Rosa26. These conditionally‐expressing mice can be bred to a wide variety of Cre mice to target cell‐specific TRIM21 overexpression in different tissues. Zp3Cre mice expressed TRIM21 protein specifically in oocytes, whereas HprtCre mice expressed the protein globally. When TRIM21‐overexpressing oocytes were microinjected with specific antibodies targeting either the IP3 receptor or SNAP23, these proteins were effectively degraded. In addition, cortical neural cells from globally‐overexpressing TRIM21 mice showed a dramatic reduction in IP3 receptor protein within hours after electroporation of a specific antibody. These experiments confirm the effectiveness of the Trim‐Away method for protein reduction. These mice should make a valuable addition to the broader research community, as a wide range of proteins and cell types can be studied using this method.
Template‐Free ZSM‐5 Synthesis Using Bio‐Sourced Waste Materials
Authors: Schneider Helena , Schmitz Thaís , Gomes Flores Camila , Louis Benoît , Cristina Tessaro Isabel , Romeu Marcilio Nilson 
Published: November 2024

AbstractHydrochars synthesized from lignocellulosic waste (rice husk and exhausted black wattle bark) through hydrothermal carbonization were used as pore‐forming agents in template‐free ZSM‐5 zeolites. The influence of the amount of hydrochar added to the zeolite synthesis and the nature of the hydrochar on the zeolite features and catalytic performance were evaluated. It was observed that the hydrochar had little influence on the textural properties and Si/Al ratio of the zeolites. However, the hydrochar was able to enhance the number of Brønsted acid sites in the zeolite and led to different ZSM‐5 crystal morphologies (french‐fries and twinned crystals). The latter zeolites exhibited a higher cracking activity of n‐hexane, favoring the formation of light olefins, due to the presence of Brønsted sites and suitable shape selectivity. In contrast, they exhibited a lower conversion of methanol into hydrocarbons (MTH), favoring the formation of dimethylether due to rapid deactivation. The hydrochars acted therefore, in the synthesis of template‐free ZSM‐5 zeolite, as a mean to both raise the acidity and control the aggregation of zeolite crystals.
Atomically Precise Rhodium‐Gold Carbonyl Nanoclusters: In‐Depth Synthesis and Multivalence Investigation of [Rh16Au6(CO)36]6−, and its Correlation with [Rh10Au(CO)26]3−
Authors: Ruggieri Silvia , Bussoli Guido , Bortoluzzi Marco , Cesari Cristiana , Funaioli Tiziana , Zacchini Stefano , Iapalucci Maria Carmela , Femoni Cristina 
Published: November 2024

AbstractThe synthesis of the previously‐reported atomically‐precise [Rh16Au6(CO)36]6− (1) nanocluster has been optimized by screening different reaction variables like solvent, stoichiometric ratio, counterion and atmosphere. Its multivalence properties have also been studied by means of electrochemical and spectroelectrochemical techniques; the results pointed out a remarkable electron‐sponge behaviour, as under such experimental conditions 1 is capable to release one electron and accept up to four more, while retaining its molecular structure. This scarce structural variation has been confirmed through DFT calculations on those species whose redox processes showed the maximum reversibility, namely [Rh16Au6(CO)36]7− and [Rh16Au6(CO)36]5−. Moreover, we report herein the isolation and characterization of the new [Rh10Au(CO)26]3− (2) nanocluster, which represents one of the major fallouts of the synthetic pathway investigation of 1. Finally, we disclosed the existence of further species that, from preliminary results, appear to be new large atomically‐precise Rh−Au nanoclusters, which will be the subject of future investigations. Cluster 2 has been identified via single‐crystal X‐ray diffraction analysis, and the characterization of both clusters 1 and 2 completed by infrared (IR) spectroscopy and Electrospray Ionization Mass Spectrometry (ESI‐MS).
Direct visualization of microwires in hybrid depth electrodes using high‐resolution photon‐counting CT
Authors: Smeijers Steven , Coudyzer Walter , Keirse Elina , Bougou Vasiliki , Decramer Thomas , Theys Tom 
Published: November 2024

AbstractHybrid depth electrodes are increasingly being used for epilepsy monitoring and human neurophysiology research. Microwires extending from the tip of the Behnke‐Fried (BF) electrode into (sub)cortical areas allow to isolate single neurons and perform microstimulation. Conventional CT or MRI visualize the entire microwire bundle as an artifact extending from the BF electrode tip with low resolution, without proper identification of individual microwires. We illustrate the first direct visualization method of individual microwires using high‐resolution photon‐counting CT (PCCT). Coregistration of the PCCT scan with a preoperative MRI can visualize individual wires directly in cortex, which is an advantage as it provides feedback on the accuracy of the implantation method and can guide future implantations. This PCCT technique allows for accurately depicting individual microwires which could be relevant for neuroscientific research through improved visualization and implantation of specific cortical and subcortical brain areas.Plain Language SummaryResearchers are using hybrid depth electrodes to study epilepsy and brain activity. These electrodes, called Behnke‐Fried (BF) electrodes, have microwires at the tip that can record single neurons and stimulate brain areas. Regular CT or MRI scans do not show the individual microwires clearly. The authors use a new high‐resolution photon‐counting CT (PCCT) technique, which can show each individual microwire in the brain. By combining PCCT with MRI, the authors can precisely see where the microwires are located. This could improve future implantation surgeries and brain research.
Depression Treatment Trajectories and Associated Social Determinants: A Three‐Year Follow‐Up Study in 66,540 Older Adults Undergoing First‐Time Depression Treatment in Denmark
Authors: Ishtiak‐Ahmed Kazi , Rohde Christopher , Köhler‐Forsberg Ole , Christensen Kaj Sparle , Gasse Christiane 
Published: November 2024

ABSTRACTObjectiveThis study aimed to describe depression treatment patterns, identify unique trajectory groups using a group‐based trajectory approach, and explore associated social determinants in older adults undergoing first‐time depression treatment during a 3‐year follow‐up.MethodsThis Danish register‐based cohort study included all adults aged ≥ 65 who initiated depression treatment by redeeming first‐time antidepressant prescriptions (no prescriptions in the last 10 years) between 2006 and 2015. The outcome of interest during the 2‐year follow‐up was depression treatment, assessed as antidepressant prescriptions redemptions and psychiatric hospital contacts for depression. Latent class growth analyses were applied to model treatment trajectories during 3 years. Multinomial logistic regression analyses were used to analyze adjusted associations between social determinates and trajectory group membership.ResultsAmong the 66,540 older adults (55.2% females, mean age: 77.3 years), we identified three distinct groups with unique patterns of depression treatment trajectories: ‘brief‐treatment’ where individuals stopped depression treatment within 6 months (33.7%); ‘gradual‐withdrawal’ (26.5%) where treatment was gradually stopped over 2 years; and ‘persistent‐treatment’ where individuals continued depression treatment for the entire 3 years (39.8%). Females, single‐person households, and residents of less‐urbanized regions were associated with higher odds of membership in the ‘persistent‐treatment’ group, while older age, widowhood or separation, and non‐Danish ethnicities were associated with lower odds.ConclusionsThree distinct patterns of depression treatment trajectories were identified in older adults, indicating differential clinical courses of depression—potentially influenced by social determinants, including sex, marital status, urban residence, and ethnicity. Early patient stratification and targeted interventions are crucial in depression care for older adults.
Language Matters: The Semantics and Politics of “Assisted Dying”
Authors: Elsner Anna M. , Frank Charlotte E. , Keller Marc , McCullough Jordan O. , Rampton Vanessa 
Published: November 2024

AbstractThis essay examines the impact of linguistic choices on the perception and regulation of assisted dying, particularly in Canada. It argues that euphemistic terms like “medical assistance in dying” and its acronym, “MAID,” serve to normalize the practice, potentially obscuring its moral gravity. This contrasts with what is seen in Belgium and the Netherlands, where terms like “euthanasia” are used, as well as in France and the United Kingdom, where terminology remains divisive and contested. By tracing the evolution of these terms and what they reveal about different cultural and legal approaches, this essay sheds light on the politics of language in end‐of‐life discourses. It suggests that the shift toward euphemistic language reflects a broader discomfort with death that can shape public attitudes and legal frameworks. It calls for a more transparent, philosophically grounded approach to terminology and suggests that continued debate about semantics is necessary to capture the complexities and ethical significance of assisted dying.
Synthetic Health Data: Real Ethical Promise and Peril
Authors: Susser Daniel , Schiff Daniel S. , Gerke Sara , Cabrera Laura Y. , Cohen I. Glenn , Doerr Megan , Harrod Jordan , Kostick‐Quenet Kristin , McNealy Jasmine , Meyer Michelle N. , Price W. Nicholson , Wagner Jennifer K. 
Published: November 2024

AbstractResearchers and practitioners are increasingly using machine‐generated synthetic data as a tool for advancing health science and practice, by expanding access to health data while—potentially—mitigating privacy and related ethical concerns around data sharing. While using synthetic data in this way holds promise, we argue that it also raises significant ethical, legal, and policy concerns, including persistent privacy and security problems, accuracy and reliability issues, worries about fairness and bias, and new regulatory challenges. The virtue of synthetic data is often understood to be its detachment from the data subjects whose measurement data is used to generate it. However, we argue that addressing the ethical issues synthetic data raises might require bringing data subjects back into the picture, finding ways that researchers and data subjects can be more meaningfully engaged in the construction and evaluation of datasets and in the creation of institutional safeguards that promote responsible use.