bluuebunny/crossref_metadata_2025 huggingface dataset:
Ring‐Opening Metathesis Polymerization of 1,2‐Dihydroazete Derivatives
Authors: Xiong Wei , Gutekunst Will R.
Published: November 2024

Fischer carbenes have recently found great utility in the construction of degradable metathesis materials, but investigations have been limited to oxygen‐containing enol ether monomers. Here, the ring‐opening metathesis polymerization of 1,2‐dihydroazetes is reported. The polymerization proceeds regioselectively, and the resulting molecular weights are targetable by adjusting the Grubbs initiator loading. Under acidic conditions, the resulting polymers degrade into 3‐aminopropanal derivatives through hydrolysis of the recurring enamide motifs in the polymer backbone. Additionally, the underlying kinetics and thermodynamics of the polymerization were studied through DFT calculations to elucidate the origins of metathesis regioselectivity. This work further expands the suite of monomers available to generate degradable metathesis materials and provides a flexible platform for target applications.
O−O Radical Coupling in Ultrathin Reconstructed Co6.8Se8 Nanosheets for Effective Oxygen Evolution and Zinc‐Air Batteries
Authors: He Chuansheng , Yang Linlin , Dong Chengyuan , Peng Xiaohui , Ibraheem Yousef , Usoltsev Oleg , Simonelli Laura , He Ren , Cabot Andreu , Lu Yizhong
Published: November 2024

Designing ultrathin transition metal electrocatalysts with optimal surface chemistry state is crucial for oxygen evolution reaction (OER). However, the structure‐dependent electrochemical performance and the underlying catalytic mechanisms are still not clearly distinguished. Herein, we synthesize ultrathin Co6.8Se8 nanosheets (NSs) with subnanometer thickness by incorporating catalytically inactive selenium (Se) into ultrathin Co(OH)2, thereby switching the OER reaction pathway from adsorbate evolution mechanism (AEM) to oxide path mechanism (OPM). The prepared ultrathin Co6.8Se8 NSs exhibit an overpotential of 253 mV at 10 mA/cm2, outperforming the mostly reported Co‐based electrocatalysts. Advanced operando synchrotron spectroscopies and X‐ray absorption spectroscopy reveal the ultrathin Co6.8Se8 NSs, whose surface is reconstructed into Se‐doped Co(OH)2 during the OER process, could trigger direct O*−O* radical coupling rather than OOH* intermediates within AEM pathway thus lowering the energy input. Density functional theory calculations confirm that Co6.8Se8 NSs with shorter Co−Co bond length and stable Co−Se bond could optimize the rate‐determining step barrier via OPM pathway. Besides, rechargeable zinc‐air batteries based on Co6.8Se8 NSs exhibit excellent stability for more than 500 h of continuous charge–discharge cycles at 4 mA/cm2. The present study highlights the structural‐dependent switch of OER pathways and provides valuable insights for further development of ultrathin OER catalysts.
An Interstitial Boron Inserted Metastable Hexagonal Rh Nanocrystal for Efficient Hydrogen Oxidation Electrocatalysis
Authors: Han Pengyu , Wu Liqing , Zhang Yu , Yue Jianchao , Jin Yiming , Jia Hongnan , Luo Wei
Published: November 2024

Constructing metastable phase structure plays an important role in changing the physicochemical properties and improving the catalytic performance of nanocrystals. Unfortunately, the synthesis of metastable phase metallic nanocrystals is highly challenging, mainly due to the thermodynamically unstable ground‐state. Here, we report a synthesis of unconventional metastable hexagonal rhodium nanocrystal (Bint−Rhhcp/C) via interstitial boron insertion. The insertion of boron atoms into the interstitial sites of cubic Rh lattice not only induces the atomic arrangements from face‐centered cubic (fcc) to hexagonal close‐packed (hcp), but also stabilizes the metastable hexagonal Rh structure. Benefiting from the phase transition and interstitial boron doping, the Bint−Rhhcp/C catalyst exhibits remarkable catalytic performance toward hydrogen oxidation reaction (HOR) under alkaline media, with a mass activity of 1.413 mA μgPGM−1. Experimental measurements including in situ surface‐enhanced infrared absorption spectroscopy (SEIRAS) and density functional theory (DFT) calculations indicate that the strengthened adsorption of hydroxyl species on the electrode surface of Bint−Rhhcp/C is responsible for the reconstruction of interfacial water structure and increased water proportions in the gap region in the electric double layers. As a result, the increased water connectivity and hydrogen bond network facilitate high‐efficiency hydrogen transfer across the interface, thereby boost the alkaline HOR performance.
Total Synthesis of (−)‐Cordycicadin D and 3,4‐trans‐Cordycicadins A and B: Entry to the 3,4‐trans‐Fused Cordycicadin Framework
Authors: Hunt Liam R. , Grant Phillip S. , Shimokura Grace K. , Furkert Daniel P. , Brimble Margaret A.
Published: November 2024

Cordycicadins A−D are four C20 polyketides, all containing a γ‐lactone fused to a 10‐membered lactone. The proposed biosynthetic pathway for the cordycicadins anticipates the formation of two more natural products which are unknown. We report the total synthesis of (–)‐cordycicadin D and the two anticipated natural products 3,4‐trans‐cordycicadins A and B. The targets were convergently assembled, in a biomimetic fashion, via an efficient ketene trapping‐intramolecular Michael addition sequence that delivered the requisite 3,4‐trans‐fused framework with high diastereoselectivity, enabled by the synthesis of complex dioxenones that serve as in situ ketene precursors. Recognition of the embedded polyketide symmetry enabled the use of a divergent‐convergent synthetic strategy, based on the use of two products from an early‐stage enzymatic resolution. The synthetic routes afforded (–)‐cordycicadin D in 14 steps and 3,4‐trans‐cordycicadins A and B in 13 steps (longest linear sequence). This work confirms the structure of (−)‐cordycicadin D and the observed instability of the anticipated natural product 3,4‐trans‐cordycicadin B during purification may explain why it is yet to be isolated.
Preparation and Properties of Basalt Fiber‐Reinforced Aqueous Polybenzoxazine Composite Aerogels Based on One‐Step Freeze‐Drying Method
Authors: Long Peijiang , Hou Zhaorun , Cheng Jinbo , Li Hui , Zhao Chunxia , Liao Jialin , Wu Yuanpeng , Zhao Haibo , Huang Haoran , Li Yuxing
Published: November 2024

Polybenzoxazine (PBa) aerogels have gained much attention as a fire‐retardant material because of their flexible molecular design and excellent mechanical properties. Incorporation of inorganic fibers into PBa aerogels using a simple and effective method seems attractive yet challenging. Herein, we report a unique method for the one‐step preparation of basalt fiber (BF) reinforced PBa composite aerogels by freeze‐drying using carboxymethyl cellulose (CMC) as a dispersion carrier. Aqueous benzoxazine (Ba) monomer was used as the matrix and phosphoric acid was used as the polymerization catalyst, while the uniform dispersion of BF was achieved by blending with CMC. The results indicate that the PBa/CMC/BF composite aerogel reveals a layered microstructure with BF dispersed between the layers. And the composite aerogel achieves a low volume shrinkage (1.11%), and strong mechanical strength (compressive stress of 1.73 MPa at 60% compressive strain). Additionally, TGA analysis reveals that the composite aerogel achieves a higher initial decomposition temperature (> 200°C) and residual mass (> 48 wt%) in a nitrogen atmosphere. Excellent flame retardancy of PBa/CMC/BF composite aerogel is achieved due to the introduction of nonflammable BF: as BF content rises, its peak heat release rate decreases by 92.5%, average heat release by 86.6%, and total smoke release by 76.7%. In combustion tests, the composite aerogel self‐extinguishes within 0.5 s. After hydrophobic modification, the composite aerogel achieves a water contact angle greater than 135°, while PBa/CMC/BF3 exhibits the typical “silver mirror phenomenon” in water. This study presents a straightforward and rapid method for constructing a lightweight, flame retardant, hydrophobic, and high‐strength fiber‐reinforced PBa composite aerogel, with promising applications in the aerospace sector.
Faunal Composition of the Sumisu Caldera Hydrothermal Vent Field as a Key Baseline for Conservation in Light of Deep‐Sea Mining
Authors: Chen Chong , Hookabe Natsumi , Hashimoto Rina , Shimooka Satoshi , Shiraki Shoki , Uyeno Daisuke , Kawagucci Shinsuke
Published: November 2024

Hydrothermal vents are biodiversity hotspots on the deep seafloor powered by chemosynthetic primary production, inhabited by a specially adapted fauna whose composition varies between regions. Sumisu Caldera, located approximately 500 km south of Tokyo, hosts a hot vent with an unusual species composition among the Izu–Ogasawara Arc sites and has been suggested as a priority site for conservation in light of upcoming deep‐sea mining for massive sulfides. However, this was based on just five species serendipitously recorded from geological surveys. Here, we carried out the first comprehensive biological sampling of Sumisu using two dives of the human‐occupied vehicle Shinkai 6500. Together with literature records, we count a total of 54 animal species of which at least 25 are endemic to chemosynthetic ecosystems, drastically increasing the known faunal diversity—including three sponges, one cnidarian, 12 molluscs, 23 annelids, 13 arthropods, one echinoderm, and one fish. The presence of sediments facilitating the occurrence of burrowing species and three non‐endemic predators contribute to the high species richness. Our findings make Sumisu the most species‐rich vent community in the entire northwestern Pacific and our work serves as a prime example for detailed faunal surveys to obtain key piece of baseline data for future environmental assessments. Although the apparent lack of massive sulfide deposits means Sumisu is unlikely to be an immediate target of mining, its close distance to Bayonnaise Knoll with a major deposit and the possibility that it acts as a critical stepping‐stone population for many species, as well as the presence of several endangered ones, presents a case for its protection.
Essential work, invisible workers: The role of digital curation in COVID‐19 Open Science
Authors: Pasquetto Irene V. , Abdu Amina A. , Chtena Natascha
Published: November 2024

In this paper, we examine the role digital curation practices and practitioners played in facilitating open science (OS) initiatives amid the COVID‐19 pandemic. In Summer 2023, we conducted a content analysis of available information regarding 50 OS initiatives that emerged—or substantially shifted their focus—between 2020 and 2022 to address COVID‐19 related challenges. Despite growing recognition of the value of digital curation for the organization, dissemination, and preservation of scientific knowledge, our study reveals that digital curatorial work often remains invisible in pandemic OS initiatives. In particular, we find that, even among those initiatives that greatly invested in digital curation work, digital curation is seldom mentioned in mission statements, and little is known about the rationales behind curatorial choices and the individuals responsible for the implementation of curatorial strategies. Given the important yet persistent invisibility of digital curatorial work, we propose a shift in how we conceptualize digital curation from a practice that merely “adds value” to research outputs to a practice of knowledge production. We conclude with reflections on how iSchools can lead in professionalizing the field and offer suggestions for initial steps in that direction.
Who, when, where, and why: A systematic review of “late diagnosis” in autism
Authors: Russell Alison S. , McFayden Tyler C. , McAllister Margaret , Liles Kimberly , Bittner Sophie , Strang John F. , Harrop Clare
Published: November 2024

An autism diagnosis can be a critical milestone toward effective and affirming support. Despite the sharp increase in the number of studies focused on late diagnosis over the last 15 years, there remains no consensus as to what constitutes a late diagnosis of autism, with cutoffs ranging from infancy to middle adulthood. This preregistered systematic review evaluated (a) the field's current quantification of late diagnosis in autism, (b) how the threshold for late diagnosis varies as a function of demographic and population factors, and (c) trends over time. Of the 11,697 records retrieved, N = 420 articles met inclusion criteria and were extracted. Articles spanned 35 years (1989–2024) and included participants from every continent except Antarctica. Only 34.7% of included studies provided a clear threshold for “late diagnosis” (n = 146/420). Late diagnosis cutoffs averaged 11.53 years (range = 2–55 years; median = 6.5 years) with a bimodal distribution (3 and 18 years). The threshold for late diagnosis varied by participant location, F(5,140) = 10.4, p < 0.0001, and sample age, F(5,140) = 20.1, p < 0.0001. Several key rationales for age determinations emerged, including access to services, considerations for adult diagnoses, and data driven approaches. What authors consider to be a “late” diagnosis of autism varies greatly according to research context. Justifications for a specific late‐diagnosis age cutoff varied, underscoring the need for authors to contextualize their conceptualizations.
Simulating Data From Marginal Structural Models for a Survival Time Outcome
Authors: Seaman Shaun R. , Keogh Ruth H.
Published: November 2024

Marginal structural models (MSMs) are often used to estimate causal effects of treatments on survival time outcomes from observational data when time‐dependent confounding may be present. They can be fitted using, for example, inverse probability of treatment weighting (IPTW). It is important to evaluate the performance of statistical methods in different scenarios, and simulation studies are a key tool for such evaluations. In such simulation studies, it is common to generate data in such a way that the model of interest is correctly specified, but this is not always straightforward when the model of interest is for potential outcomes, as is an MSM. Methods have been proposed for simulating from MSMs for a survival outcome, but these methods impose restrictions on the data‐generating mechanism. Here, we propose a method that overcomes these restrictions. The MSM can be, for example, a marginal structural logistic model for a discrete survival time or a Cox or additive hazards MSM for a continuous survival time. The hazard of the potential survival time can be conditional on baseline covariates, and the treatment variable can be discrete or continuous. We illustrate the use of the proposed simulation algorithm by carrying out a brief simulation study. This study compares the coverage of confidence intervals calculated in two different ways for causal effect estimates obtained by fitting an MSM via IPTW.
Diverse Motions and Responses in Crowd Simulation
Authors: Ma Yiwen , Liu Tingting , Liu Zhen
Published: November 2024

A challenge in crowd simulation is to generate diverse pedestrian motions in virtual environments. Nowadays, there is a greater emphasis on the diversity and authenticity of pedestrian movements in crowd simulation, while most traditional models primarily focus on collision avoidance and motion continuity. Recent studies have enhanced realism through data‐driven approaches that exploit the movement patterns of pedestrians from real data for trajectory prediction. However, they have not taken into account the body‐part motions of pedestrians. Differing from these approaches, we innovatively utilize learning‐based character motion and physics animation to enhance the diversity of pedestrian motions in crowd simulation. The proposed method can provide a promising avenue for more diverse crowds and is realized by a novel framework that deeply integrates motion synthesis and physics animation with crowd simulation. The framework consists of three main components: the learning‐based motion generator, which is responsible for generating diverse character motions; the hybrid simulation, which ensures the physical realism of pedestrian motions; and the velocity‐based interface, which assists in integrating navigation algorithms with the motion generator. Experiments have been conducted to verify the effectiveness of the proposed method in different aspects. The visual results demonstrate the feasibility of our approach.
Neolignan Kadsurenin F Modulates Proteostatic Pathways and Possesses Potent Anti‐Inflammatory Properties
Authors: Evangelakou Zoi , Schwaiger Stefan , Gianniou Despoina D. , Trougakos Ioannis P. , Stuppner Hermann
Published: November 2024

Kadsurenin F, a natural neolignan‐type compound, has been described as a constituent of various members of the Lauraceae family such as Aniba spp. or Nectandra spp., but can also be found in various Piper species such as Piper kadsura Ohwi (Piperaceae). This species is traditionally used to treat asthma, rheumatic pain, arthritis, and digestive problems. Recently, several studies have highlighted the significant anti‐inflammatory potential of P. kadsura extracts and secondary metabolites. Here, we report the isolation of kadsurenin F as an active component of P. kadsura. We found that kadsurenin F increases oxidative load and suppresses proteasome functionality in normal diploid human fibroblasts, and after administration in Drosophila flies. Moreover, kadsurenin F likely possesses anti‐inflammatory properties, as apart from suppressing proteasome activity, it reversed inflammatory phenotypes and inhibited NO production in RAW 264.7 macrophage cells when administered in parallel with LPS. Our findings suggest that the kadsurenin F scaffold can be used for the development of novel highly bioactive proteasome inhibitors and/or anti‐inflammatory compounds.
Craniosynostosis in Siblings, an Extremely Rare Occurrence: A Case Report
Authors: Bhavsar Tirth , Chaudhary Sachin Mahendrakumar , Singh Sumesh
Published: November 2024

Craniosynostosis (CS) is the premature fusion of skull sutures, with all sutures except the metopic suture typically fusing in adulthood. Premature fusion constrains brain growth, leading to abnormal skull shape and potential neurocognitive or neurological issues, along with syndromic features in some cases. While CS is rare, its occurrence in siblings is exceptionally uncommon and holds significant academic importance. We report a case of CS in siblings: a 13‐month‐old boy and his five‐and‐a‐half‐year‐old sister. Neither parent exhibits craniofacial dysmorphism or signs of increased intracranial pressure (ICP). The younger sibling presents with dolichocephaly and normal neurological, cognitive, and motor development, while the elder sibling exhibits proptosis, midface hypoplasia, and normal developmental milestones. Neither sibling displays limb or systemic anomalies. Imaging studies, including multislice plain CT brain with 3D skull reconstruction and MRI, revealed multiple suture closures. The younger sibling has complete sagittal suture closure with partial closure of other sutures, while the elder sibling shows multisutural CS. Ophthalmologic evaluations and developmental assessments excluded increased ICP and systemic issues. Most CS cases follow an autosomal dominant inheritance pattern, making this case particularly significant. CT with 3D skull reconstruction remains the diagnostic gold standard. Management aims to preserve cosmetic appearance and prevent complications from increased ICP. Treatment options range from conservative follow‐up to surgical interventions, including endoscopic suturectomy, open craniotomy, and distraction osteogenesis, depending on the presence of neurocognitive issues or elevated ICP. Both siblings currently show normal neurological, cognitive, and motor development without increased ICP, emphasizing the need for ongoing monitoring to identify new developments or recurrence after treatment. Differential diagnoses, such as deformational plagiocephaly, must also be considered in such cases.
Electrochemical Radical Allylation Reaction of Arylphosphine Oxides
Authors: Huang Jianming , Wang Qiannan , Wang Xinyu , Song Jin , Guo Chang
Published: November 2024

Functionalized organophosphorus compounds are key structural motifs in many natural products and pharmaceutical chemicals. Herein, we describe the electrochemical radical allylation reaction for the direct and efficient construction of C(sp3)─P bonds. A wide range of arylphosphine oxides and allylsilanes were well tolerated, providing valuable organophosphorus compounds with generally good yields. Mechanistic studies indicate that a phosphoryl radical is generated through a single‐electron transfer oxidation process and plays a pivotal role in the reaction pathway.
Role of Copper Species in Copper Phyllosilicate Catalysts for the Catalytic Transfer Hydrogenation of Furfural to γ‐Valerolactone
Authors: Shoosri Tanyarat , Thongratkaew Sutarat , Rungtaweevoranit Bunyarat , Kraithong Wasawat , Faungnawakij Kajornsak , Teerawatananond Thapong , Sooknoi Tawan , Kuboon Sanchai , Panpranot Joongjai , Weerachawanasak Patcharaporn
Published: November 2024

Copper phyllosilicate (CuPS) catalysts were synthesized and evaluated for the catalytic transfer hydrogenation of furfural to γ‐valerolactone (GVL). Various copper loadings (10–30 wt.%) were studied to elucidate the impact of copper species on catalytic performance. Notably, a high dispersion of copper (%DCu ≈ 70%) and a substantial BET surface area (620 m2/g) were achieved, even at the maximum copper loading of 30 wt.%. TR‐XANEs and XPS analyses identified the two geometric structures of Cu2⁺ on the CuPS catalysts; square planar and octahedral alongside Cu⁺/Cu⁰ species were formed upon reduction at temperatures exceeding 200 °C. The reduced 30% CuPS‐R catalyst, enriched in metallic Cu⁰, achieved complete conversion of furfural, but exhibited low GVL selectivity (22%). Conversely, the as‐synthesized 30% CuPS, predominantly composed of Cu2⁺, showed a lower furfural conversion (14%) but higher selectivity for GVL (37%). The physical mixing of 30% CuPS‐R and 30% CuPS in a 50:50 ratio yielded the best catalytic performance, resulting in 100% furfural conversion and 86% GVL selectivity. The findings suggest that metallic Cu⁰ is essential for initiating the conversion of furfural, while Cu2⁺ plays a critical role in GVL formation. An optimal Lewis/Brønsted acidity (L/B) ratio of 5.7 is proposed for the mixed catalysts. The proposed reaction mechanism underscores the complex interplay between different copper species and acid sites, emphasizing the need for optimizing both metal and acid functionalities in catalyst design.
Nanostructured Ceria–Niobia Catalyst for Selective Synthesis of N‐Benzylideneanilines
Authors: Putla Suresh Babu , Swapna Bhattu , Kumar Mudavath Arun , Sudarsanam Putla , Srinivasu Pavuluri
Published: November 2024

The shape and structure engineering of metal oxide nanomaterials are the potential strategies to optimize surface‐active sites with tunable selectivity for heterogeneous catalysis. This work reports the synthesis of two types of nanostructured CeO2–Nb2O5 catalysts: (i) one‐pot hydrothermal synthesis of CeO2–Nb2O5 (CeNb2O5‐HTS, HTS stands for hydrothermal synthesis) and (ii) CeO2 impregnation on hydrothermally synthesized Nb2O5 nanorods (CeNb2O5‐WI, WI stands for wet‐impregnation) to elucidate the role of particle shape and CeO2 addition in the structure–activity efficacy of Nb2O5 nanocatalyst for the selective oxidative C–N coupling of benzyl alcohol with aniline to produce N‐benzylideneaniline (NBA). The characterization studies showed nanorod morphology of Nb2O5 and high dispersion of CeO2 on Nb2O5 nanorods in the CeNb2O5‐WI catalyst with strong acidic sites and more oxygen vacancies. Consequently, a significantly enhanced catalytic activity was achieved with CeNb2O5‐WI nanocatalyst in the coupling of benzyl alcohol and aniline with 96% yield to NBA, whereas 62% conversion of aniline with 92% selectivity to NBA was obtained with pure Nb2O5 nanorods. In contrast, the CeNb2O5‐HTS catalyst gave 37% conversion of aniline only. The versatile efficiency of the CeNb2O5‐WI nanocatalyst is showcased by synthesizing various functional NBA products. The CeNb2O5‐WI catalyst can be recycled 4 times without much variation in NBA selectivity by achieving reasonably good conversion of aniline.
First person profile: Quynh‐Thu Le, MD
Authors: Nierengarten Mary Beth
Published: November 2024

This news section offers Cancer readers timely information on events, public policy analysis, topical issues, and personalities. This issue features Dr Quynh‐Thu Le, who confronts the difficult challenges of improving the efficacy and safety of radiation therapy in the treatment of head and neck cancers. In addition, molecularly guided therapy improves survival outcomes for patients with a cancer of unknown primary, and annual screening mammography lowers the risk of late‐stage cancer.
Design and Construction of an Artificial Light‐Harvesting System Based on Polyacrylic Acid and a Cyanostilbene Derivative
Authors: Duan Qunpeng , Chen Dengli , Zhang Qiaona , Lin Shihao , Zeng Rong , Xiao Tangxin
Published: November 2024

The development of materials with tunable fluorescence properties is critical for advancing applications in sensing, imaging, and information encryption. In this study, we synthesized a cyanostilbene derivative (CSA) that combines the benefits of aggregation‐induced emission (AIE) and self‐assembly in water. CSA, featuring a cyanostilbene core and hydrophilic carboxylate groups, exhibits weak fluorescence in solution but forms highly fluorescent nanoaggregates (CSA‐PAA) upon self‐assembly with polyacrylic acid (PAA). By integrating rhodamine 6G (Rh6G) as an energy acceptor, we constructed a light‐harvesting system (CSA‐PAA‐Rh6G) with high Förster resonance energy transfer (FRET) efficiency and tunable emission from green to yellow. This work presents a facile approach for the development of aqueous light‐harvesting systems and shows promise for future applications in tunable luminescent materials.
Biomass Valorization via Paired Electrocatalysis
Authors: Huddleston Morgan , Sun Yujie
Published: November 2024

Electrochemical valorization of biomass represents an emerging research frontier, capitalizing on renewable feedstocks to mitigate carbon emissions. Traditional electrochemical approaches often suffer from energy inefficiencies due to the requirement of a second electrochemical conversion at the counter electrode which might generate non‐value‐added byproducts. This review article presents the advancement of paired electrocatalysis as an alternative strategy, wherein both half‐reactions in an electrochemical cell are harnessed to concurrently produce value‐added chemicals from biomass‐derived feedstocks, potentially doubling the Faradaic efficiency of the whole process. The operational principles and advantages of different cell configurations, including 1‐compartment undivided cells, H‐type cells, and flow cells, in the context of paired electrolysis are introduced and compared, followed by the analysis of various catalytic strategies, from catalyst‐free systems to sophisticated homogeneous and heterogeneous electrocatalysts, tailored for optimized performance. Key substrates, such as CO2, 5‐hydroxymethylfurfural (HMF), furfural, glycerol, and lignin are highlighted to demonstrate the versatility and efficacy of paired electrocatalysis. This work aims to provide a clear understanding of why and how both cathode and anode reactions can be effectively utilized in electrocatalytic biomass valorization leading to innovative industrial scalability.
Covalent Organic Frameworks with Regulated Water Adsorption Sites for Efficient Cooling of Electronics
Authors: Zhang Jun , Liu Yong , Hu Yu , Han Wang‐Kang , Fu Jia‐Xing , Zhu Ruo‐Meng , Pang Huan , Zhang Jiangwei , Gu Zhi‐Guo
Published: November 2024

The excessive heat accumulation has been the greatest danger for chips to maintain the computing power. In this paper, a passive thermal management strategy for electronics cooling was developed based on the water vapor desorption process of the covalent organic frameworks (COFs). The precise regulation for the number of carbonyl group and the ratio of hydrophilicity and hydrophobicity within pore channels was achieved by water adsorption sites engineering. In particular, COF‐THTA with abundant water adsorption sites exhibited highest water uptake and desorption energy, which facilitate efficient cooling of electronics. In proof‐of‐concept testing, COF‐THTA coating (40×40 mm) provided a temperature drop of 7.5 °C in 25 minutes at a heating power of 937.5 W/m2, and remained stable after 10 intermittent heat cycles. Furthermore, the equivalent enthalpy of COF‐THTA coating can reach up to 1136 J/gcoating. In real application scenarios, COF‐THTA coating improved the performance of two real computing devices by 26.73 % and 22.61 %, respectively. This strategy based on COFs provides a new thinking for passive thermal management, exhibiting great potential in efficient cooling of electronics.
Wireless Power Transfer System for Cardiac Pacemakers Based on Spiral Ring mu‐Negative Materials
Authors: Guirreh Souleiman Hassan , Zhu Feiyu , Chen Weihua , Peng Jishen
Published: November 2024

Considering the impact of metamaterials on the magnetic coupling effect and electromagnetic response characteristics in wireless power transfer systems for implantable cardiac pacemakers, this paper proposes a wireless power transfer system operating at the 300‐kHz frequency band, enhanced by spiral ring mu‐negative materials (SR‐MNG) to improve magnetic coupling efficiency. First, based on the resonance principle, the SR‐MNG is designed, and the system's mutual inductance coupling is analyzed using the magnetic dipole coupling model theory. Second, the impact of metamaterial thickness and loss on the system's coupling strength is investigated, and the performance of the system is analyzed when using FR4, polyimide, and aluminum nitride as dielectric substrate. The system's tolerance to misalignment is discussed bearing in mind the special implantation environment of the peacemaker. The experimental results indicate that, at a transmission distance of 20 mm, the system achieves optimal magnetic coupling strength with a thickness of 1.6 mm, resulting in a minimum power transmission efficiency of 71%. Increasing the thickness to 2 mm disrupts the trend of increasing efficiency, causing it to drop by at least 23.3%. The SR‐MNG with polyimide as the dielectric plate performs exceptionally well, maintaining an efficiency range of 17.3%–73.1% for lateral displacements between 0 and 30 mm and achieving a minimum efficiency of 39.2% for angular misalignment of 15°.
Performance of plasma p‐tau217 and NfL in an unselected memory clinic setting
Authors: Rousset Rebecca Z. , Claessen Thomas , van Harten Argonde C. , Lemstra Afina W. , Pijnenburg Yolande A. L. , van der Flier Wiesje M. , Braber Anouk den , Jeromin Andreas , Verberk Inge M. W. , Teunissen Charlotte E.
Published: November 2024

INTRODUCTION

Plasma phosphorylated tau‐217 (p‐tau217) and neurofilament light (NfL) can differentiate between different dementias in selected cohorts. We aim to test the discrimination potential of these markers in a real‐world cohort.

METHODS

We measured p‐tau217 (ALZpath) and NfL (Quanterix) in 415 (unselected) consecutive memory clinic patients. Biomarker levels were dichotomized as low/high to create four biomarker profiles based on p‐tau217 and NfL levels.

RESULTS

p‐Tau217 levels were highest in patients with Alzheimer's disease (AD) dementia, whereas NfL levels were highest in patients with frontotemporal dementia (FTD). Low p‐tau217/low NfL was associated mostly with non‐neurological diagnoses (79%), and high p‐tau217/low NfL indicated AD pathology at any stage (84%). Low p‐tau217/high NfL indicated FTD (38%) and high p‐tau217/high NfL indicated AD dementia (87%).

DISCUSSION

p‐Tau217 can identify AD pathology at any disease stage. NfL can differentiate FTD from other diagnoses (e.g., AD dementia). Plasma p‐tau217 and NfL can support clinical decision‐making, and we suggest using them as complements to standard clinical assessment.

Highlights

Phosphorylated tau‐2017 (p‐tau217) can detect Alzheimer's disease (AD) across the clinical continuum.

Neurofilament light (NfL) can differentiate frontotemporal dementia (FTD) from other diagnoses (AD dementia, dementia with Lewy bodies [DLB], and Psychiatry).

p‐Tau217 may detect AD co‐pathology in other diseases or dementia types (e.g., DLB).

p‐Tau217 and NfL show potential for clinical implementation.
Input of exome sequencing in early‐onset cerebral amyloid angiopathy
Authors: Grangeon Lou , Charbonnier Camille , Rousseau Stéphane , Richard Anne Claire , Quenez Olivier , Zarea Aline , Boland Anne , Olaso Robert , Deleuze Jean‐François ,   CAA study group, Tournier‐Lasserve Elisabeth , Nicolas Gael , Wallon David
Published: November 2024

INTRODUCTION

Genetics of cerebral amyloid angiopathy (CAA) remains understudied.

METHODS

We assessed variants in Alzheimer's disease (AD) risk factor genes and differential diagnosis genes by performing exome sequencing among 78 patients with early‐onset definite or probable CAA, after negative screening for APP mutation or duplication.

RESULTS

Among 14 genes involved in non‐Aβ CAA, or vascular leukoencephalopathies, we detected pathogenic NOTCH3 variants in two patients, who exhibited lobar hematomas at the ages of 58 and 65, leading to a diagnosis redirection toward CADASIL. Of the remaining 76 patients, 23.1% carried at least one apolipoprotein E (APOE) ε2 allele and 43.6% carried at least one APOE ε4 allele, known as CAA risk factors. A total of 15 out of 76 (19.7%) carried either a loss‐of‐function or a rare predicted damaging missense or known AD risk variant in SORL1, TREM2, ABCA7, ABCA1, and ATP8B4.

DISCUSSION

Exome sequencing allowed the redirection toward CADASIL in two patients and suggested shared genetic factors between AD and CAA, beyond the APOE gene.

Highlights

The genetic component of cerebral amyloid angiopathy (CAA) remains understudied.

Rare differential diagnoses such as CADASIL should be considered, even in cases of cerebral hemorrhage.

Our study suggests shared genetic factors between AD and CAA, beyond the APOE gene.

Rare variants in SORL1, TREM2, ABCA7, ABCA1 and ATP8B4 might be susceptibility factors in early‐onset CAA.,
Association of circulating ketone bodies with cognitive performance and dementia in the Multi‐Ethnic Study of Atherosclerosis (MESA)
Authors: Chevli Parag Anilkumar , Schaich Christopher L. , Wood Alexis C. , TK Luqman A. , Mehta Anurag , Jain Vardhmaan , Connelly Margery , Craft Suzanne , Shemesh Elad , Luchsinger José A. , Hayden Kathleen M. , Sachs Bonnie Colleen , Hughes Timothy M. , Shapiro Michael D.
Published: November 2024

Introduction

Growing interest centers on the association between circulating ketone bodies (KB) and cognitive function, notably in aging and neurodegenerative diseases.

Methods

Associations of plasma KB with incident dementia and cognitive performances were examined among Multi‐Ethnic Study of Atherosclerosis (MESA) participants. KB were measured using plasma samples collected following an overnight fasting at Exam 1 (2000–02) and detailed cognitive testing at Exam 5 (2010–2012, N = 4392), Exam 6 (2016–2018, N = 1838), and in MESA‐MIND (2019–2021, N = 2060).

Results

Over 16.7 years, a doubling of total KB was associated with a greater risk of incident dementia (hazard ratio [HR]: 1.14 [1.04–1.29]). Higher total KB was associated with worse cognitive performance in the Digit Span test at exam 5 [β: −0.30 (−0.47, −0.14)]. We also found that a higher KB was associated with greater functional impairment and a higher Quick Dementia Rating Scale (QDRS) score.

Discussion

In a diverse, cardiovascular disease‐free population, elevated KB levels were associated with incident dementia and impaired cognitive performance in specific domains.

Highlights

A study of ketone bodies (KB) and cognitive performance and incident dementia.

Nuclear magnetic resonance (NMR) spectroscopy was used to measure plasma KB at baseline.

Doubling of baseline total KB was associated with higher incident dementia.

Higher KB was also associated with worse performance on a test of working memory.
The Impact of Family‐Based Treatment for Adolescent Anorexia Nervosa on Compulsive Exercise Attitudes and Behaviors
Authors: Datta Nandini , Matheson Brittany , Plessow Franziska , Citron Kyra , Le Grange Daniel , Schlegl Sandra , Lock James
Published: November 2024

Objective

While Family‐based treatment for anorexia nervosa (FBT‐AN) is effective for weight restoration and improvement in eating‐related cognitions, its effect on exercise attitudes and behaviors is little studied. Compulsive exercise is common in AN and often challenging to change.

Method

This secondary analysis examined changes in attitudes toward compulsive exercise (Compulsive Exercise Test‐CET) and behaviors (Eating Disorder Examination‐EDE) using data from a randomized clinical trial testing an adjunctive treatment for adolescents with AN who failed to gain 2.4 kg by Session 4—a predictor of poor outcome. The main hypothesis is that attitudes toward compulsive exercise and decreases in compulsive exercise behavior would improve over the course of treatment.

Results

Participants reported decreases in compulsive exercise attitudes by Session 4 and compulsive exercise episodes by end of treatment (EOT). There were no differences between early FBT responders (weight gain of 2.4 kg by session 4) and early non‐responders.

Discussion

These results suggest that FBT facilitates adolescents with AN to change attitudes toward compulsive exercise early in treatment (by Session 4) as well as reduction in compulsive exercise behaviors by EOT. Future studies should assess whether changes in attitudes toward compulsive exercise early in treatment is a mechanism of FBT treatment effect.
In‐Situ Pt‐Decorated, Direct Growth of Mixed Phase 2H/1T–MoSe2 on Carbon Paper for Enhanced Hydrogen Evolution Reaction
Authors: Park Jong‐Hwan , Kim Sun‐Woo , Lee So Young , Jung Yuri , Ro Jae‐Chul , Park Seong‐Ju , Kim Hyoung‐Juhn , Seo Dong Han , Suh Su‐Jeong
Published: November 2024

Metal dichalcogenide‐based 2D materials, gained considerable attention recently as a hydrogen evolution reaction (HER) electrocatalyst. In this work, we synthesized MoSe2‐based electrocatalyst via hydrothermal route with varying phase contents (1T/2H) and respective HER performances were evaluated under the acidic media (0.5 m H2SO4), where best HER performance was obtained from the sample consisting of mixed 1T/2H phases, which was directly grown on a carbon paper (167 mV at 10 mA cm−2) Furthermore, HER performance of electrocatalyst was further improved by in‐situ electrodeposition of Pt nanoparticles (0.15 wt%) on the MoSe2 surface, which lead to significant enhancement in the HER performances (133 mV at 10 mA cm−2). Finally, we conducted density functional theory calculations to reveal the origin of such enhanced performances when the mixed 1T/2H phases were present, where phase boundary region (1T/2H heterojunction) act as a low energy pathway for H2 adsorption and desorption via electron accumulation effect. Moreover, presence of the Pt nanoparticles tunes the electronic states of the MoSe2 based catalyst, resulting in the enhanced HER activity at heterointerface of 1T/2H MoSe2 while facilitating the hydrogen adsorption and desorption process providing a low energy pathway for HER. These results provide new insight on atomic level understanding of the MoSe2 based catalyst for HER application.
Insights Into the Uranium Phosphine Bonds in [UCp3(PR3)]: A Combined Molecular Orbital, QTAIM and EDA‐NOCV Study
Authors: Vondung Lisa
Published: November 2024

A series of ten uranium(III) complexes with cyclopentadienyl and monodentate phosphine ligands [UCp3(PR3)] with R=Me, Et, nPr, iPr, tBu, Ph, Cy, F and CF3 was investigated using density functional theory calculations. The ligand dissociation energies were calculated, as well as bonding analysis of the uranium‐phosphorus bond performed, using molecular orbitals, bond orders, quantum theory of atom in molecules (QTAIM) analysis and energy decomposition analysis with natural orbitals for chemical valence (EDA‐NOCV). It was found that the bond orders correlate well with the U−P bond lengths and phosphine cone angles, indicating a large influence of phosphine sterics on the bond properties. All bonding analyses show partial covalent character of the U−P bond, which is most pronounced for PF3 and least for PtBu3. π‐Backbonding was found for the most π‐acidic phosphine ligands. No good correlation was found between the ligand dissociation energies and bond metrics.
Photolabile ortho‐Nitro‐Benzyl Carbonate as an Amino Protecting Group for Stereocontrolled Synthesis of 2‐Amino‐2‐Deoxy‐β‐d‐Glycosides
Authors: Shang Jintao , Wang Yi , Chang Dongsheng , Zheng Jibin , Chen Hongyu , Yao Shuang , Yang You
Published: November 2024

Traditional amino protecting groups are often removed under harsh conditions or incompatible with other protecting groups, rendering the synthesis of complex 2‐amino‐2‐deoxy‐β‐d‐glycosides difficult. Here, we utilize the photolabile ortho‐nitrobenzyl carbonate (oNBC) as an amino protecting group for stereocontrolled synthesis of 2‐amino‐2‐deoxy‐β‐d‐glycosides. The gold(I)‐catalyzed glycosylation with per‐O‐oNBC‐protected 2‐N‐phthaloyl (Phth)‐2‐deoxy‐, 2‐N‐trichloroacetyl (TCA)‐2‐deoxy‐, and 2‐N‐oNBC‐2‐deoxy‐glycosyl ynenoates proceeded smoothly to provide 2‐amino‐2‐deoxy glycosides with exclusive β‐selectivities via the neighboring group participation (NGP) effect. Removal of the multiple O‐ and N‐oNBC protecting groups of 2‐amino‐2‐deoxy glycosides was achieved under irradiation at 365 nm with aminomethyl polystyrene as the carbonyl scavenger.
Repeated sprint training: The effects of session volume on acute physiological, neuromuscular, perceptual and performance outcomes in athletes
Authors: Thurlow Fraser , McLaren Shaun J. , Townshend Andrew , Morrison Matthew , Cowley Nicholas , Weakley Jonathon
Published: November 2024

We examined the effects of repeated sprint training (RST) session volume on acute physiological, neuromuscular, perceptual and performance outcomes. In a randomised, counterbalanced, and crossover design, 14 healthy and trained male and female athletes (age: 23 ± 3 years) completed two sets of 10 × 40 m (10 × 40), 5 × 40 m (5 × 40), 10 × 20 m (10 × 20) and 5 × 20 m (5 × 20) sprints with 30 s rest between repetitions and 3 min rest between sets for all protocols. Average and peak heart rate, average oxygen consumption (VO2), time >90% of maximal oxygen consumption (VO2max), differential ratings of perceived exertion (RPE), session‐RPE training load (sRPE‐TL), percentage sprint decrement (Sdec), acceleration load and distance >90% of maximal sprint speed were recorded during each session. Neuromuscular performance (i.e. countermovement jump, lower‐limb stiffness and isometric hamstring strength) were measured post‐session, 24 h, and 48 h and compared to pre‐session. A univariate analysis of variance was used to compare within‐ and between‐protocol differences. To aid data interpretation, all effects were expressed as an effect size and accompanied by probability values (pMET). The 10 × 40 protocol induced the greatest training load compared to all other protocols (pMET < 0.05), including moderate to very large differences in breathlessness RPE, large differences in Sdec and time >90% VO2max and very large differences in sRPE‐TL. The 5 × 20 protocol induced the lowest training load compared to all other protocols (pMET < 0.05), including moderate to large differences in sRPE‐TL and leg muscle RPE. Heart rate, VO2, sRPE‐TL, leg muscle RPE and Sdec were similar between 5 × 40 and 10 × 20 (pMET < 0.05), but the acceleration load was greater for 10 × 20 when compared to 5 × 40 (pMET < 0.001), and this difference was large. Changes in neuromuscular performance across all timepoints and all protocols were unclear. Larger session volumes increase the demands of RST and by manipulating volume, sprint distance and the number of repetitions, practitioners can alter the internal and external training load.
Harnessing agro‐wastes for sustainable nanomaterials: The promise of biofluorescent carbon dots
Authors: Divyabharathi R. , Kalidasan B. , Sakthi Suriya Raj J. S. , Chinnasamy Subramaniyan , Pandey A. K. , Giri Jayant , Fatehmulla Amanullah
Published: November 2024

The effective utilization and high‐value bioproducts from agro‐wastes make sense for a sustainable circular economy for agriculture. The article discusses the promising potential of utilizing agro‐wastes to produce high‐value bioproducts, particularly focusing on carbon dots (C‐dots) derived from such wastes. These C‐dots exhibit remarkable fluorescence properties and excellent biocompatibility, making them valuable nanomaterials for various applications. The dual sources of these C‐dots: green precursors sourced from both edible and non‐edible plant‐based materials, and chemical precursors involving acid and non‐acid reagents are highlighted. This diversity in precursor materials underscores the versatility and sustainability of C‐dot production. Importantly, the synthesis of fluorescent C‐dots achieved quickly and directly via hydrothermal carbonization, microwave technique, thermal pyrolysis carbonization, solvothermal technique, and ultrasonic process are review concisely intended for widespread application in fields ranging from bio‐imaging to optoelectronic devices. Furthermore, the article discusses the challenges associated with synthesizing high‐quality C‐dots from agro‐residues, indicating ongoing research efforts in this area. Likewise, key energy specific characteristics like optical, photoluminestic, photosimulated electron transfer, catalytic, mechanical, and carcinogenic attributes are discussed. Despite these energy specific characteristics, various energy applications of C‐dots, including their potential use in light‐emitting diodes, supercapacitors, and photovoltaics are outlined. This highlights the multifaceted nature of C‐dots and their contribution to advancing sustainable practices in agriculture while simultaneously addressing energy needs in various sectors. Overall, the article underscores the importance of leveraging agro‐wastes for the development of innovative and environmentally friendly bioproducts, contributing to the circular economy in agriculture.