bluuebunny/crossref_metadata_2025_split huggingface dataset:
Metal Oxide Aerogels: A New Horizon for Stabilizing Anodes in Rechargeable Zinc Metal Batteries
Authors: Shi Zhenhai , Chen Suli , Xu Zijian , Liu Zhanming , Guo Junhong , Yin Jian , Xu Pengwu , Zhang Nan , Zhang Wenli , Alshareef Husam N. , Liu Tianxi 
Published: April 2023

AbstractDendritic deposition and side reactions have been long‐standing interfacial challenges of Zn anode, which have prevented the development of practical aqueous zinc‐based batteries. Herein, an oxygen vacancy‐rich CeO2 aerogel (VAG‐Ce) interface layer that simultaneously integrates Zn2+ selectivity, porosity, and is lightweight is reported as a new strategy to achieve dendrite‐free and corrosion‐free Zn anodes. The well‐defined and uniform nanochannels of VAG‐Ce can act as ion sieves that redistribute Zn2+ at the Zn anode surface by regulating Zn2+ flux, leading to uniform Zn deposition and significantly suppressing dendrite growth. Importantly, the abundant oxygen vacancies exposed on VAG‐Ce surface can strongly capture SO42−, forming a negatively charged layer that can attract Zn2+ and accelerate the Zn2+ migration kinetics, while the subsequent repulsion of additional anions can effectively suppress the generation of (Zn4SO4(OH)6·xH2O) byproducts, thereby realizing very stable Zn anodes. Consequently, VAG‐Ce modified Zn anode (VAG‐Ce@Zn) enables a long‐term lifespan over 4000 h at 4 mA cm−2 and a record‐high cycle life of 1200 h is achieved under an ultrahigh 85% Zn utilization at 8 mA cm−2, which enables excellent capacity retention and cycling performance of VAG@Zn/MnO2 cells. This work contributes an innovative design concept by introducing oxygen vacancy‐rich aerogels and provides a new horizon for stabilizing Zn anode for large‐scale energy storage.
3D‐Printed Graded Electrode with Ultrahigh MnO2 Loading for Non‐Aqueous Electrochemical Energy Storage
Authors: Lin Dun , Chandrasekaran Swetha , Forien Jean‐Baptiste , Xue Xinzhe , Pinongcos Anica , Coester Emma , Worsley Marcus A. , Li Yat 
Published: April 2023

AbstractElectrolytic manganese dioxide is one of the promising cathode candidates for electrochemical energy storage devices due to its high redox capacity and ease of synthesis. Yet, high‐loading MnO2 often suffers from sluggish reaction kinetics, especially in non‐aqueous electrolytes. The non‐uniform deposition of MnO2 on a porous current collectors also makes it difficult to fully utilize the active materials at high mass loading. Here, a 3D printed graded graphene aerogel (3D GA) that contains sparsely separated exterior ligaments is developed to create large open channels for mass transport as well as densely arranged interior ligaments providing large ion‐accessible active surface. The unique structural design homogenizes the thickness of electro deposited MnO2 even at an ultrahigh mass loading of ≈70 mg cm−2. The electrode achieves a remarkable volumetric capacity of 29.1 mA h cm−3 in the non‐aqueous electrolyte. A Li‐ion hybrid capacitor device assembled with a graded 3D GA/MnO2 cathode and graded 3D GA/VOx anode exhibits a wide voltage window of 0–4 V and a superior volumetric energy density of 20.2 W h L−1. The findings offer guidance on 3D printed electrode design for supporting ultrahigh loading of active materials and developments of high energy density energy storage devices.
White matter hyperintensities in Alzheimer's disease: Beyond vascular contribution
Authors: Garnier‐Crussard Antoine , Cotton François , Krolak‐Salmon Pierre , Chételat Gaël 
Published: April 2023

AbstractWhite matter hyperintensities (WMH), frequently seen in older adults, are usually considered vascular lesions, and participate in the vascular contribution to cognitive impairment and dementia. However, emerging evidence highlights the heterogeneity of WMH pathophysiology, suggesting that non‐vascular mechanisms could also be involved, notably in Alzheimer's disease (AD). This led to the alternative hypothesis that in AD, part of WMH may be secondary to AD‐related processes. The current perspective brings together the arguments from different fields of research, including neuropathology, neuroimaging and fluid biomarkers, and genetics, in favor of this alternative hypothesis. Possible underlying mechanisms leading to AD‐related WMH, such as AD‐related neurodegeneration or neuroinflammation, are discussed, as well as implications for diagnostic criteria and management of AD. We finally discuss ways to test this hypothesis and remaining challenges. Acknowledging the heterogeneity of WMH and the existence of AD‐related WMH may improve personalized diagnosis and care of patients.
Boosting the Efficiency of Dye‐Sensitized Solar Cells by a Multifunctional Composite Photoanode to 14.13 %
Authors: Zhang Siqi , Huang Fuhua , Guo Xugeng , Xiong Ye , Huang Yafei , Ågren Hans , Wang Li , Zhang Jinglai 
Published: April 2023

AbstractWe report a new strategy to fabricate a multifunctional composite photoanode containing TiO2 hollow spheres (TiO2‐HSs), Au nanoparticles (AuNPs) and novel NaYF4 : Yb,Er@NaLuF4 : Eu@SiO2 upconversion nanoparticles (UCNPs). The AuNPs are grown on the photoanode film including TiO2‐HSs and UCNPs by a simple in situ plasmonic treatment. As a result, an impressive power conversion efficiency of 14.13 % is obtained, which is a record for N719 dye‐based dye‐sensitized solar cells, demonstrating great potential for the solar cells toward commercialization. This obvious enhancement is ascribed to a collaborative mechanism of the TiO2‐HSs exhibiting excellent light‐scattering ability, of the UCNPs converting near‐infrared photons into visible photons and of the AuNPs presenting outstanding surface plasmon resonance effect. Notably, a steady‐state experiment further reveals that the champion cell exhibits 95.33 % retainment in efficiency even after 180 h of measurements, showing good device stability.
Rational Design in Photopharmacology with Molecular Photoswitches
Authors: Kobauri Piermichele , Dekker Frank J. , Szymanski Wiktor , Feringa Ben L. 
Published: April 2023

AbstractPhotopharmacology is an attractive approach for achieving targeted drug action with the use of light. In photopharmacology, molecular photoswitches are introduced into the structure of biologically active small molecules to allow for the optical control of their potency. Going beyond trial and error, photopharmacology has progressively applied rational drug design methodologies to devise light‐controlled bioactive ligands. In this review, we categorize photopharmacological efforts from the standpoint of medicinal chemistry strategies, focusing on diffusible photochromic ligands modified with photoswitches that operate through E‐Z bond isomerization. In the vast majority of cases, photoswitchable ligands are designed as analogs of existing compounds, through a variety of approaches. By analyzing in detail a comprehensive list of instructive examples, we describe the state of the art and discuss future opportunities for rational design in photopharmacology.
Tailoring *H Intermediate Coverage on the CuAl2O4/CuO Catalyst for Enhanced Electrocatalytic CO2 Reduction to Ethanol
Authors: Zhang Tingting , Yuan Bowen , Wang Wenlong , He Jing , Xiang Xu 
Published: April 2023

AbstractThe direct electrochemical conversion of CO2 to multi‐carbon products offers a promising pathway for producing value‐added chemicals using renewable electricity. However, producing ethanol remains a challenge because of the competitive ethylene formation and hydrogen evolution reactions. Herein, we propose an active hydrogen (*H)‐intermediate‐mediating strategy for ethanol electroproduction on a layered precursor‐derived CuAl2O4/CuO catalyst. The catalyst delivered a Faradaic efficiency of 70 % for multi‐carbon products and 41 % for ethanol at current density of 200 mA cm−2 and exhibited a continuous 150 h durability in a flow cell. The intensive spectroscopic studies combined with theoretical calculations revealed that the in situ generated CuAl2O4 could tailor *H intermediate coverage and the elevated *H coverage favors the hydrogenation of the *HCCOH intermediate, accounting for the increased yield of ethanol. This work directs a pathway for enhancing ethanol electroproduction from CO2 reduction by tailoring *H intermediate coverage.
Einfluss der Luftdichtheit auf den Heizwärme‐ und Klimakältebedarf bei neuen Einfamilienhäusern
Authors: Hall Monika 
Published: April 2023

AbstractDie Luftdichtheit von Gebäuden hat einen Einfluss auf den Lüftungswärmestrom und damit auf den Heizwärme‐ und Klimakältebedarf. Der unkontrollierte Luftstrom durch Leckagen gewinnt mit zunehmendem Dämmniveau an Bedeutung. Um den Einfluss der Luftdichtheit bei hohem Dämmstandard auf den Heizwärme‐ und Klimakältebedarf zu untersuchen, werden verschiedene Szenarien mit einer thermischen Gebäudesimulation betrachtet. Zusätzlich werden an 28 neuen Einfamilienhäusern Luftdichtheitstests durchgeführt, um die Luftdichtheit von Standardneubauten zu bestimmen.Die Simulationen bestätigen, dass der Heizwärme‐ und Klimakältebedarf mit zunehmender Undichtheit zunimmt. Infolge der großen Temperaturdifferenz zwischen innen und außen sowie höheren Windgeschwindigkeiten im Winter ist der Einfluss der Luftdichtheit auf den Heizwärmebedarf größer als auf den Klimakältebedarf im Sommer. Die ermittelte Luftdichtheit der gemessenen Gebäude weist im Mittel ein q50 = 0,8 m3/(h · m2) auf, was ein sehr guter Luftdichtheitswert ist. Ihr Heizwärmebedarf wird sich durch die Undichtheiten voraussichtlich um ca. 3 % bis 6 % gegenüber einem dichten Gebäude mit q50 = 0,6 m3/(h · m2) erhöhen. Der Klimakältebedarf wird sich um ca. 1 % bis 2 % reduzieren.
Ökobilanzierung adaptiver Hüllen und Strukturen
Authors: Borschewski David , Albrecht Stefan , Bischoff Manfred , Blandini Lucio , Bosch Matthias , Dazer Martin , Efinger Dshamil , Eisenbarth Christina , Haase Walter , Kreimeyer Matthias , Leistner Philip , Nitzlader Markus , Roth Daniel , Sawodny Oliver , van den Adel Friederike , Voigt Michael , Weber Simon 
Published: April 2023

AbstractDie Bilanzierung von Umweltwirkungen spielt eine entscheidende Rolle bei der Entwicklung nachhaltiger und umweltfreundlicher Technologien und Konzepte. Dies gilt auch in der Entwicklung von Gebäuden mit adaptiven Hüllen und Strukturen und stellt darüber hinaus weitreichende Anforderungen an alle beteiligten Disziplinen. Die vollständige Integration der Ökobilanzierung in den Planungs‐ und Auslegungsprozess ermöglicht, Umweltwirkungen als Optimierungsgrößen in den komplexen, dynamischen Berechnungswerkzeugen einzusetzen. Die bisherigen Ergebnisse des SFB 1244 bescheinigen adaptiven Tragwerken und Fassaden großes Potenzial zur Einsparung von Ressourcen und Umweltwirkungen. Die ganzheitliche Betrachtungsweise, sowohl in Bezug auf den Lebenszyklus als auch auf die interdisziplinären Wechselwirkungen, stellt sicher, dass die relevanten Effekte und Einflüsse in der Bilanzierung berücksichtigt werden. Das stellt die Methode der Ökobilanzierung selbst jedoch vor neue Herausforderungen im Umgang mit einer Vielzahl an Varianten und den umfangreichen Wechselwirkungen zwischen Auslegung und Einflüssen auf Parameter in der Nutzungsphase, wie z. B. den Energieverbrauch oder die Lebensdauer.
Living (dys)regulated and alienated young masculinity—Young men's embodied experiences of mental disorders and suicidality
Authors: Åhlander Anna , Strömbäck Maria , Sandlund Jonas , Wiklund Maria 
Published: April 2023

AbstractIntroductionMental disorders, such as depression and anxiety with interlinked suicidality, are the leading cause of health‐related disability among young men. Knowledge of the interaction between emotional, bodily, social and gendered mental health processes in young men is limited and therefore needed.AimThis study aimed to explore young men's lived embodied experiences of mental disorders and suicidality, and to conceptualise these by integrating affective–emotional, physiological, social and gendered processes.MethodsSemistructured individual interviews were conducted with 13 young men who had sought professional help for mental disorders and suicidality. Grounded theory (GT) was used with a social constructivist perspective.ResultsThe results comprise one core category—Living (dys)regulated and alienated young masculinity—with related categories “battling with the emotional body,” “suffering in social silence” and “balancing embodied darkness and distress.” The GT illustrates how young men navigate and manage their embodied and emotional suffering in a context of “regulative” masculine and social norms alongside insufficient social support.ConclusionOur results suggest that young men's lived embodied experiences of mental disorders and suicidality can be understood as a dynamic process of internal and external “(dys)regulation and alienation.” The generated GT provides a broad tentative explanation model, contributing to theory development, and serves as a basis for gender‐sensitive interventions—in both psychotherapy and physiotherapy—integrating body, mind and the social context.
Au Nanozyme Driven Cascading Catalysis in Tollens′ Reaction: An Insight of Glucose Oxidase‐Like Mechanism
Authors: Xiang Henglong , Huang Sijun , Zhu Dongwei , Yu Liqiang , Liu Rui , Guo Yi , Xu Li 
Published: April 2023

AbstractAu nanoparticles (NPs) have been proven to be excellent glucose oxidase (GOx) mimics, which can catalyze the electrons transform pathway from glucose to oxygen. This study confirmed AuNPs can accelerate the reaction between [Ag(NH3)2]+ and glucose under alkaline conditions, which is also known as the Tollens′ reaction, and the possible mechanism was proposed. Here, [Ag(NH3)2]+ instead of O2 acted directedly as an electron acceptor during glucose oxidation catalyzed by AuNPs, accompanied by hydrogen transfer. The as‐synthesized Ag nanoparticles can also catalyze this process, similar to AuNPs, via a unique cascading catalysis mechanism in the Tollens′ reaction. A simple and heatless glucose colorimetric assay can be established based on the plasmonic band of AgNPs with a liner range of 0.6–22.2 μM, and the limit of detection is 0.32 μM.
Pyridone‐Doped Acenes with Improved Stability
Authors: Yan Chengguo , Ding Weiwei , Zhang Gang 
Published: April 2023

AbstractBesides the peripheral modification, the introduction of heteroatoms to modulate the property of longer acenes with improved chemical stability has been extensively studied for their potential applications in organic electronics. However, the utilization of 4‐pyridone, a common unit in the air‐ and photo‐stable acridone and quinacridone, to decorate higher acenes with increased stability has not been realized yet. Here we present the synthesis of a series of monopyridone‐doped acenes up to heptacene via the palladium‐catalyzed Buchwald‐Hartwig amination of aniline and dibromo‐ketone. The effect of pyridone on the property of doped acenes were investigated experimentally and computationally. With the π‐extension of doped acenes, the pyridone ring shows the weakened conjugation and gradual loss of aromaticity. The doped acenes demonstrate enhanced stability in solution and maintain the electronic communication between the acene planes.
Template Based Synthesis of Porous Graphdiyne Nanosheet for Reversible and Fast NO2 Detection by UV Irradiation
Authors: Li Senlin , Yu Lingmin , Zhang Chuantao , Wang Siyi , Li Ruijun , Zhao Fan , Yin Mingli , Du Hongbo , Jia Yu , Fan Xinhui 
Published: April 2023

AbstractTwo‐dimensional graphdiyne (GDY) formed by sp and sp2 hybridized carbon has been found to be an efficient toxic gas sensing material by density functional theory (DFT). However, little experimental research concerning its gas sensing capability has been reported owing to the complex preparation process and harsh experimental conditions. Herein, porous GDY nanosheets are successfully synthesized through a facile solvothermal synthesis technique by using CuO microspheres (MSs) as both template and source of catalyst. The porous GDY nanosheets exhibit a broadband optical absorption, rendering it suitable for the light‐driven optoelectronic gas sensing applications. The GDY‐based gas sensor was demonstrated to have excellent reversible to NO2 behaviors at 25 °C for the first time. More importantly, higher response value and faster response‐recovery time once exposed to NO2 gas molecules are achieved by the illumination of UV light. In this way, our work paves the way for the exploration of GDY‐based gas detection experimentally.
A broad range: From simple and brief to intensive single‐session interventions: Commentary on Schleider et al. (2023)
Authors: Ghaderi Ata , Welch Elisabeth 
Published: April 2023

AbstractTo push research and treatment in the field of eating disorders (EDs) forward, we need to not only systematically develop our current knowledge and skills through established procedures for research and clinical practice, but also make room for disruptive innovations and thinking out of the box. The paper by Schleider et al. (2023, International Journal of Eating Disorders) provides a thoughtful invitation to think differently by considering single‐session interventions (SSI) for prevention and treatment of EDs. Beyond expanding our intervention tools, SSI may force us to think more mechanistically about the processes of change, and about the format and delivery of our interventions, both for EDs and from a transdiagnostic perspective. In this commentary, we reflect on the possible benefits and implications of SSI, and the necessity of mechanistically driven and rigorous empirical research for developing efficacious SSI.
High dimensional analysis reveals distinct NK cell subsets but conserved response to stimulation in umbilical cord blood and adult peripheral blood
Authors: Buckle Irina , Johnson Anthony , Rojas Ingrid Leal , Weinert Vicky , Sester David P. , Radford Kristen , Guillerey Camille 
Published: April 2023

AbstractGrowing interest surrounds adoptive cellular therapies utilizing Natural Killer (NK) cells, which can be obtained from various sources, including umbilical cord blood (UCB) and adult peripheral blood (APB). Understanding NK cell receptor expression and diversity in such cellular sources will guide future therapeutic designs. We used a 20‐color flow cytometry panel to compare unstimulated and cytokine‐activated UCB and APB NK cells. Our analysis showed that UCB NK cells express slightly higher levels of the immune checkpoints PD‐1, TIGIT, and CD96 compared to their APB counterparts. Unsupervised hierarchical clustering and dimensionality reduction analyses revealed enrichment in CD56neg as well as mature NKp46neg and CD56+CD16+ NK cell populations in UCB whereas CD57+ terminally differentiated NK cells with variable expression of KIRs and CD16 were found in APB. These populations were conserved following stimulation with IL‐12, IL‐15, and IL‐18. Cytokine stimulation was associated with the downregulation of TIGIT and CD16 on multiple NK cell subsets in UCB and APB. Among UCB CD16− NK cell populations, TIGIT+ NK cells produced more IFN‐γ than their TIGIT− counterparts. Our data demonstrate higher immune checkpoint expression on UCB NK cells compared to APB. However, the expression of TIGIT immune checkpoint is not indicative of NK cell exhaustion.
Half‐Sandwich Manganese Complex Bearing Fused Oxazoline‐NHC Ligand: Conformational Analysis and Evaluation in Asymmetric Ketone Hydrosilylation
Authors: Cavailles Matthieu , Filippov Oleg A. , César Vincent , Lugan Noël , Valyaev Dmitry A. 
Published: April 2023

AbstractThe first manganese complex bearing a chiral N‐heterocyclic carbene (NHC) ligand was prepared and studied by spectroscopic methods and X‐ray diffraction. While IR spectroscopy revealed the existence of two isomers in solution with distinct νCO band patterns, DFT calculations indicated that these isomers correspond to rotamers around the Mn−NHC bond and their different spectroscopic properties were rationalized by the occurrence of attractive π(C=C)⋅⋅⋅π*(C≡O) or σ(C−H)⋅⋅⋅π*(C≡O) intramolecular interligand interactions. The evaluation of this complex in catalytic hydrosilylation of acetophenone using Ph2SiH2 under UV irradiation led to the formation of the corresponding (R)‐alcohol with low enantioselectivity.
Concise Synthesis, Conformational Study, and Aroma Properties of Carba‐Homologues of Helvetolide and Serenolide
Authors: Dacho Vladimír , Babjak Matej , Peťka Ján , Szolcsányi Peter 
Published: April 2023

AbstractWe have designed, prepared, and evaluated a set of racemic (un)saturated carba‐homologues of prominent musks Helvetolide and Serenolide. The short synthesis employs commercially available Artemone and/or Herbac, that are transformed in three steps to the target compounds. Their qualitative olfactory analysis revealed that incorporation of methylene bridge into the backbone chain of parent compounds completely erases the original musk scent and such new derivatives exhibit a pleasant and often intense sweet(ish) aroma of fruit with floral and herbal aspects. The results of computational modelling suggest that previously postulated horseshoe shape conformation might be necessary but not sufficient prerequisite for musk‐scented compounds. Thus, we offer an alternative hypothesis based on the structural differences between metallocomplexes of Helvetolide and/or Serenolide vs. their (un)saturated carba‐homologues with zinc‐atom as a model for the putative metal‐binding site in human olfactory receptors.
Free Carboxylic Acids: The Trend of Radical Decarboxylative Functionalization
Authors: Li Liubo , Yao Yan , Fu Niankai 
Published: April 2023

AbstractThe exceptional versatility of carboxylic acids has been extensively exploited in organic synthesis across several decades. There has been a recent upsurge of radical decarboxylative transformations. The process can be initiated under mild conditions, and the resultant radicals have orthogonal reactivities to closed‐shell species, thus providing immense opportunities for streamlining novel reactions. The use of free carboxylic acids is the most desirable owing to its high atom and step economy. Aiming to demonstrate the attractiveness of the strategy and to inspire chemists to tackle existing challenges, this review outlines the recent advances on radical decarboxylative functionalization of free carboxylic acids.