bluuebunny/crossref_metadata_2025_split huggingface dataset:
Pressure‐Induced Emission Enhancement of Multi‐Resonance o‐Carborane Derivatives via Exciton‒Vibration Coupling Suppression
Authors: Li Zening , Zhang Qing , Sun Fangxiang , Lv Chunyan , Meng Xinmiao , Hu Yu , Xu Dongqian , Li Chengjian , Li Lei , Wang Kai , Zhang Yujian 
Published: January 2025

AbstractPolycyclic multiple resonance (MR) molecules reveal narrowband emission, making them very promising emitters for high color purity display. Nevertheless, they still have challenges such as aggregation‐induced emission quenching and spectral broadening. Overcoming these obstacles requires an in‐depth understanding of the correlations among the alterations in their geometries, packing structures, and molecular vibrations and their corresponding changes in their photoluminescence (PL) properties. Herein, it is demonstrated that high‐pressure infrared, UV−visible absorption, and fluorescence spectroscopies can be combined with computational results to elucidate the influence of the subtle structural variations on the exciton‒vibration couplings and their PL properties. An ortho‐carborane‐decorated MR emitter (BNC) is a piezochromic molecule and exhibits emission enhancement under high pressure. A thorough analysis of the in situ experimental measurements and calculated results reveals that the pressure‐induced changes in the exciton binding energy and exciton‒vibration couplings are responsible for the unusual piezochromism. This research provides insights into the structure‒fluorescence relationship and potential for high‐pressure techniques to optimize MR materials for advanced organic light‐emitting diodes (OLEDs) applications.
Identifying gait differences between Alzheimer's disease and dementia with Lewy bodies and their associations with regional amyloid deposition
Authors: Elasfar Salma , Hameed Hajr , Boeve Bradley F. , Fields Julie A. , Jack Clifford R. , Kantarci Kejal , St. Louis Erik K. , Lowe Val J. , Petersen Ronald C. , Ali Farwa , Ehgoetz Martens Kaylena 
Published: January 2025

AbstractINTRODUCTIONWe aimed to compare gait between individuals with Alzheimer's disease (AD), dementia with Lewy bodies (DLB), and cognitively unimpaired (CU) individuals and to evaluate the association between gait and regional amyloid beta (Aβ) burden in AD and DLB.METHODSWe included 420 participants (70 AD, 70 DLB, 280 CU) in the Mayo Clinic Study of Aging (MCSA). Gait was assessed using a pressure‐sensor walkway. Aβ deposition was analyzed with Pittsburgh compound B (PiB) positron emission topography (PET).RESULTSThe DLB group had reduced stride velocity, step length, and stride width variability, as well as increased double support percentage (%DS) and variability in step length, swing time, and step time compared to the AD and CU groups. Aβ burden was not associated with any gait outcomes.DISCUSSIONThis study provides additional evidence that gait differs between AD and DLB. Larger studies are needed to investigate associations between Aβ burden and gait outcomes in dementia.Highlights
Gait was more impaired in dementia than in cognitively unimpaired (CU) controls.
Compared with Alzheimer's disease (AD), Dementia with Lewy bodies (DLB) had more impaired pace, variability, and postural control.
Step length and double support (%) distinguished DLB and AD with moderate accuracy.
Current practices by Alzheimer's Disease Research Centers to remunerate research participants
Authors: Gabel Matthew , Bekena Semere , O'Meara Mitch , Denny Andrea , Solomon Erin D. , Moulder Krista L. , Morris John C. , Mozersky Jessica 
Published: January 2025

AbstractINTRODUCTIONRecent guidance from the National Alzheimer's Coordinating Center (NACC) recommends remuneration for all Alzheimer's disease (AD) research participants. Given AD research recruitment challenges, we assessed the remuneration practices at Alzheimer's Disease Research Centers (ADRCs).METHODSWe surveyed 37 ADRCs about remuneration for longitudinal research participants. This included type of remuneration (i.e., compensation, reimbursement) and which study procedures are remunerated. We had a 100% response rate.RESULTSMost ADRCs (32/37) provide some remuneration but amounts and types varied. Most ADRCs reimburse for travel or food (n = 29), compensate for some study procedures (n = 32), but most do not remunerate study partners (n = 12) or offer financial incentives (n = 8). Few (n = 6) ADRCs pay for all procedures.DISCUSSIONTwo areas for potential change are compensating for annual clinical and cognitive assessments that are compulsory, and for study partners. Evaluation of the impact of remuneration on recruitment and retention is needed, including for underrepresented groups.Highlights
Recent guidance recommends remuneration for Alzheimer's disease research participants.
We surveyed all Alzheimer's Disease Research Centers about their remuneration practices.
Most centers provide some form of remuneration to participants but this is variable.
Potential areas for change are remuneration for study partners and annual study visits.
Evaluating the impact of remuneration on recruitment and retention is needed.
Mediation of modifiable risk factors in two multidomain dementia prevention trials
Authors: Hoevenaar‐Blom Marieke P. , Shourik Jason , van Dalen Jan Willem , van Gool Willem A. , Andrieu Sandrine , Richard Edo , Coley Nicola , Moll van Charante Eric ,   the preDIVA study group,   MAPT/IHU HealthAge Open Science study group
Published: January 2025

AbstractINTRODUCTIONWe explored which dementia risk factors in two multidomain prevention trials mediate beneficial, neutral, or counteracting effects on dementia incidence.METHODSWe pooled data from the multidomain MAPT (Multidomain Alzheimer Preventive Trial; n = 1679, up to 5‐year follow‐up) and preDIVA trials (Prevention of Dementia by Intensive Vascular Care; n = 3526, up to 12‐year follow‐up) in adults aged 70+. We used multiple mediation analysis to quantify the role of 2‐year changes in body mass index, systolic blood pressure, total cholesterol, and physical activity in the intervention effects on dementia incidence. Mixed linear and Cox proportional hazard models were used to explore pathways.RESULTSWe observed no mediation of individual risk factors in the effect of the interventions on dementia incidence. The interventions slightly lowered only blood pressure, but this did not translate into an effect on dementia incidence.DISCUSSIONIn older populations, multidomain interventions may not sufficiently affect dementia risk factors to lower dementia incidence, particularly in settings where cardiovascular risk factor management is well implemented.Highlights
There is no mediating role of risk factor change in the effects of multidomain interventions on dementia incidence in two large dementia prevention randomized controlled trials.
The lack of effect of the interventions on risk factors explains the absence of impact on dementia.
Counteracting mediators do not explain the lack of effect of the interventions on dementia.
A small effect of the interventions on blood pressure did not translate into a lower dementia incidence.
Non‐Monotonic Variation of Potential‐Dependent Surface Diffusion at Electrochemical Interfaces in the Presence of Coadsorbates
Authors: Yang Chaolong , Amirbeigiarab Reihaneh , Buttenschön Sönke , Pehlke Eckhard , Magnussen Olaf M. 
Published: January 2025

AbstractThe influence of coadsorbed ions on adsorbate diffusion, an inherent effect at solid–liquid interfaces, was studied for adsorbed sulfur on Ag(100) electrodes in the presence of bromide or iodide. Quantitative in situ high‐speed scanning tunnelling microscopy (video‐STM) measurements were performed both in the potential regime of the c(2×2) halide adlayer at its saturation coverage and in the regime of a disordered adlayer where the halide coverage increases with potential. These studies reveal a surprising non‐monotonic potential dependence of Sad diffusion with an initial increase with halide coverage, followed by a decrease upon halide adlayer ordering into the c(2×2) structure. Density functional theory (DFT) and Monte Carlo (MC) simulations only qualitatively reproduce the rise in Sad mobility with halide coverage, suggesting that many‐adsorbate interactions and the presence of the electrolyte need to be considered.
Leicht zugänglich: Borirene aus Borolen und Dialkinen
Authors: Oliveira Pedro H. R. , Rodrigues Marieli O. , da Silva Caren D. G. , Bohlen Josina L. , Arrowsmith Merle , Jayaraman Arumugam , Lubczyk Lukas , Fantuzzi Felipe , da Silva Júnior Eufrânio N. , Braunschweig Holger 
Published: January 2025

AbstractPerarylierte Borirene werden in einer selektiven einstufigen Synthese aus antiaromatischen Borolen durch Umsetzung mit 1,4‐Diaryl‐1,3‐diinen hergestellt. Experimentelle und theoretische mechanistische Untersuchen zeigen, dass die Reaktion über einige Schlüsselintermediate, wie Boranorbornadiene und 7‐Borabicyclo[4.1.0]heptadiene, abläuft, welche in einem dynamischen Gleichgewicht miteinander vorliegen. Schließlich erfolgt die Boriren‐Bildung durch eine Migration der Borandiyl‐Brücke vom Cyclohexadien‐Ring zu dem verbleibenden exocyclischen Alkinrest.
Cyano‐Modified Multi‐Resonance Thermally Activated Delayed Fluorescent Emitters Towards Pure‐Green OLEDs with a CIEy Value of 0.74
Authors: Xue Zhuixing , Hu Yuxuan , Xiao Shengbing , Liu Jiahui , Miao Jingsheng , Yang Chuluo 
Published: January 2025

AbstractThe development of pure‐green organic emitters with ideal emission peaks and ultra‐narrow full‐widths at half‐maximum (FWHMs) remains a formidable challenge. Herein, we report two new green emitters, CNBN and MCNBN, which achieve extremely narrow FWHMs by synergistic rigid π‐extension and cyano‐substitution of a sky‐blue multi‐resonance thermally activated delayed fluorescence (MR‐TADF) core. The introduction of cyano groups induces red‐shifts in the emission to the green region and dramatically minimizes the FWHMs. In toluene solution, CNBN and MCNBN exhibit narrowband emission with a maximum at 501 nm and 510 nm with ultra‐narrow FWHMs of 14 nm/0.066 eV and 15 nm/0.071 eV, respectively. Given the near‐unity photoluminescence quantum yields and almost 100 % horizontal dipole orientation, the electroluminescent (EL) devices based on CNBN and MCNBN deliver external quantum efficiencies (EQEs) exceeding 30 % with FWHMs of 16 nm/0.072 eV and 17 nm/0.080 eV, respectively. Notably, the MCNBN‐based device achieves pure‐green emission with a maximum at 517 nm with Commission Internationale de l’Éclairage coordinates of (0.17, 0.74), closely aligning with the BT.2020 green standard.
Photoelectrocatalyzed Alkylation of Phosphonites by Direct Decarboxylative C(sp3)‐P Coupling
Authors: Yuan Kang‐Ning , Xie Tian , Wang Jia‐Bao , Wang Dali , Shang Ming 
Published: January 2025

AbstractA photoelectrocatalytic method is presented that achieves direct decarboxylative C(sp3)‐P coupling, providing a modular route to alkylphosphinates and alkylphosphonates from readily available carboxylic acids. The success of this reaction hinges on the synergistic combination of electrochemical anodic oxidation and photocatalytic ligand to metal charge transfer (LMCT) decarboxylation. By employing P(III) reagents as limiting reagents, our approach enables efficient alkyl modification of medicinally important nucleosides and complex molecules derived phosphonites, which were challenging to access by existing methods. Detailed mechanistic studies elucidate the critical roles of Fe catalysts and additives, offering valuable insights into the reaction pathway and laying the foundation for future advancements in photoelectrocatalytic C(sp3)‐heteroatom bond‐forming reactions.
Force‐Trainable Liquid Crystal Elastomer Enabled by Mechanophore‐Induced Radical Polymerization
Authors: Xu Yiyi , Huang Yinliang , Wang Jinyu , Huang Shuai , Yang Hong , Li Quan 
Published: January 2025

AbstractIn nature, organisms adapt to environmental changes through training to learn new abilities, offering valuable insights for developing intelligent materials. However, replicating this “adaptive learning” in synthetic materials presents a significant challenge. This study introduces a feasible approach to train liquid crystal elastomers (LCEs) by integrating a mechanophore tetraarylsuccinonitrile into their main chain, addressing the challenge of enabling synthetic materials to exchange substances with their environment. Inspired by biological training, the LCEs can self‐strengthen and acquire new functionalities through mechanical stress‐induced radical polymerization. The research not only enhances the mechanical performance of LCEs, but also endows them with the ability to learn properties such as flexibility, light responsiveness, and fluorescence. These advancements are crucial for overcoming the limitations of current materials, paving the way for the creation of advanced intelligent soft materials with autonomous self‐improvement, akin to the adaptive skills of living organisms.
Ph3PC – A Monosubstituted C(0) Atom in Its Triplet State
Authors: Kutin Yury , Koike Taichi , Drosou Maria , Schnegg Alexander , Pantazis Dimitrios A. , Kasanmascheff Müge , Hansmann Max M. 
Published: January 2025

AbstractThis study introduces a novel class of carbon‐centered diradicals: a monosubstituted C atom stabilized by a phosphine. The diradical Ph3P→C was photochemically generated from a diazophosphorus ylide precursor (Ph3PCN2) and characterized by EPR and isotope‐sensitive ENDOR spectroscopy at low temperatures. Ph3P→C features an axial zero‐field splitting parameter D=0.543 cm−1 with a vanishingly small rhombicity |E|/D=0.002. Time‐ and temperature‐dependent measurements confirm a triplet ground state with a lifetime of approximately 10 min at 127 K in toluene‐d8. Multireference electronic structure calculations predict a clear triplet ground state with a singlet‐triplet gap greater than 20 kcal/mol. In contrast to divalent C(0) compounds, such as Ph3P→C←PPh3, in which carbon needs excitation into a highly‐excited closed‐shell 2s02p4 configuration, Ph3P→C can be explained by direct involvement of carbon in its natural 3P state arising from the 2s22p2 configuration.
Shifting Lithium Amide Reactivity to the Radical Domain: Regioselective Radical C−H Functionalization of 3‐Iodooxetane for the Synthesis of 1,5‐Dioxaspiro[2.3]hexanes
Authors: Natho Philipp , Colella Marco , Vicenti Annarita , Romanazzi Giuseppe , Ullah Faizan , Sheikh Nadeem S. , White Andrew J. P. , Pasca Francesco , Luisi Renzo 
Published: January 2025

AbstractStrained spiro‐heterocycles (SSHs) have gained significant attention within the medicinal chemistry community as promising sp3‐rich bioisosteres for their aromatic and non‐spirocyclic counterparts. We herein report access to an unprecedented spiro‐heterocycle—1,5‐dioxaspiro[2.3]hexane. Our synthetic approach leverages a lithium‐amide induced single‐electron transfer to benzophenones generating an N‐centered radical and a ketyl radical anion—reminiscent of a frustrated radical pair. This pair works synergistically to selectively abstract the β‐hydrogen from 3‐iodooxetane, initiating an exergonic radical‐radical coupling reaction. This process enables the formation of the desired bond between the oxetane core and benzophenone derivatives, ultimately yielding the novel 1,5‐dioxaspiro[2.3]hexane core. The stability and synthetic utility of the novel 1,5‐dioxaspiro[2.3]hexane motif are showcased. An in‐depth mechanistic investigation is presented, including cyclic voltammetry studies, as well as computational calculations and experiments to support the mechanism of this new single electron synthetic tactic.
Rational Design Two‐ or Four‐Electron Reaction Pathway Covalent Organic Frameworks for Efficient and Selective Electrocatalytic Hydrogen Peroxide Production
Authors: Liu Jiayi , Zhang Wenjing , Shen Jin , Feng Liang , Yao Yao , Peng Qiang 
Published: January 2025

AbstractCovalent organic frameworks (COFs) are often employed in oxygen reduction reactions (ORR) for hydrogen peroxide production due to their tunable structures and compositions. However, COF electrocatalysts require precise structural engineering, such as heteroatoms or metal site doping, to modulate the reaction pathway during the ORR process. In this work, we designed a tetraphenyl‐p‐phenylenediamine based COF electrocatalyst, namely TPDA‐BDA, which exhibited excellent two‐electron (2e) ORR performance with high H2O2 selectivity of 89.7 % and faraday efficiency (FE) of 86.7 %, higher than the reported COFs to date for H2O2 electrosynthesis. The theoretical and experimental results showed that the rate‐determining step energy barrier for reduction of O2 to OOH* intermediates was significantly reduced by replacing of bipyridine with biphenyl blocks, changing from 4e to 2e ORR reaction pathway. Also, the donor‐acceptor characteristic and narrower optical band gap of TPDA‐BDA COF enhanced the electronic conductivity and reduction ability, thus elevating the catalytic activity. As a result, the H2O2 selectivity was maintained above 85 % even after 50 h stability test. This work reveals the structure‐property relationship of COF electrocatalysts and provides a new strategy for rational design of high performance 2e ORR COF electrocatalysts for efficient and selective hydrogen peroxide production.
Optimization and Pyrolysis Kinetics of Waterborne Coatings Based on Saturated Polyester Resins and Totally Methyl Etherified Amino Resins
Authors: Che Zhaoxian , Niu Lidan , He Yuhan , Huang Xianliang , Shi Jiarong , Xu Shihan , Long Hang , Zheng Jie , Xu Xiao 
Published: January 2025

ABSTRACTAmid the urgent call for the coatings industry to increase ecological awareness, a decisive shift toward environmentally friendly coatings is imperative. In this study, the L9(34) orthogonal experimental design is used to optimize the formula of the waterborne coating made from waterborne saturated (WS) polyester resins and totally methyl etherified amino resins. The composite resin coatings exhibit excellent properties under optimized conditions (resin solid content ratio 2:1, curing time 40 min, curing temperature 433 K). FTIR confirms the successful crosslinking between WS polyester and totally methyl etherified amino resin, and TGA shows four‐stage thermal weight loss, with the most significant loss in the third stage (623–743 K). Pyrolysis kinetics at this stage, analyzed using Kissinger‐Akahira‐Sunose and Coats‐Redfern method methods, reveal a three‐dimensional diffusion mechanism with an activation energy of 215.25 kJ/mol and a pre‐exponential factor of 6.83 × 1015 min−1. This research enhances understanding and advancement of sustainable coating technologies for various industrial applications.
Bioinspired Silicone Rubber Foams With Adjustable Gradient Structures Induced via Temperature Fields
Authors: Li Donglin , Deng Wenxin , Jin Zhefeng , Hu Jiangpeng , Zhao Yujia , Cao Nuo , Wan Chao , Chen Xuhuang , Yu Peng 
Published: January 2025

ABSTRACTThe structure‐gradient silicone rubber foam (SRF) is an advanced bionic material with potential for applications in energy‐damping, triboelectric nanogenerators, and electromagnetic interference shielding. However, the production of SRFs with an adjustable gradient structure is still a significant challenge. Herein, a novel strategy combining in situ precuring of silicone rubber induced by gradient temperature fields with supercritical CO2 foaming was developed to prepare SRFs with biomimetic gradient cellular structures. By regulating the unilateral heat source temperature and precuring time, SR samples with gradient curing degrees from 16.13% to 51.21% were achieved. Finally, a prospective structure‐gradient SRF with a cell size range of 24.10–182.80 μm was successfully prepared. The energy loss coefficient of gradient SRF can be reduced by 41.65% compared with that of uniform cellular structure foam with average cell size of 31.25 μm after 50 cycles. Gradient SRFs show significantly enhanced mechanical performance, recoverability, and elasticity. Besides, the underlying mechanism for generating this gradient cellular structure was clarified.
Threats Assessment of the Endemic Idle Crayfish (Austropotamobius bihariensis Pârvulescu, 2019): Lessons From Long‐Term Monitoring
Authors: Ács Andrei‐Robert , Ion Mihaela C. , Miok Kristian , Laza Antonio V. , Pitic Alina , Robnik‐Šikonja Marko , Pârvulescu Lucian 
Published: January 2025

ABSTRACTThe idle crayfish (Austropotamobius bihariensis Pârvulescu, 2019), endemic to Romania's Apuseni Mountains, urgently requires a specific conservation plan. Due to its recent description, conservation efforts have been limited, highlighting the need for immediate and practical recommendations to ensure its protection. Over 13 years, field observations were conducted to evaluate population trends and identify threats following IUCN standards. Additionally, geospatial assessments and predictive modelling were employed to estimate both the optimal habitat and current population size under three distinct scenarios. The primary threats identified include poor forest management, extreme drought, anthropogenic development and riverbed alterations, all contributing to declines in crayfish abundance. The most severe impacts arise when these pressures converge at a single site, compounded by a chronic, low‐virulence crayfish plague infection (A‐haplogroup). The total population is estimated at 31,150 (± 449.9 SE) individuals, with 1,163,754 m2 of suitable habitat, of which only 37.9% lies within 13 protected areas under the most realistic scenario. Poor water quality was found to significantly reduce the modelled population size. In light of these findings, we propose a series of targeted conservation actions tailored for each protected area and highlight the importance of extending measures beyond their current boundaries. Additionally, we recommend implementing the ‘ark sites’ concept in regions with optimal ecological conditions, stable populations and genetic diversity, to reduce pressures and safeguard the species through effective field management.
Ultra‐Sensitive NO2 Detection at Room Temperature Enabled by ZnO@MoO3 Core‐Shell Nanocomposite
Authors: Song Zihao , Luo Junhao , Ding Shumei , Ding Jiabao , Wang Qi , Zhang Zhongxi , Li Hongpeng , Zhang Chao 
Published: January 2025

AbstractThe sensitive detection of NO2 is crucial for environmental monitoring and improving quality of life. Herein, a ZnO@MoO3 core‐shell nanocomposite was fabricated via a simple stepwise solution self‐assembly and heat‐treatment process. Remarkably, the ZnO@MoO3 sensor exhibited a high response value of 5.4 to 2 ppm NO2 at room temperature. Furthermore, it displayed excellent selectivity against interference gases such as CO2, NH3, methanol, ethylene, and trimethylamine, along with outstanding stability and repeatability under varying humidity conditions. The exceptional sensing performance of the ZnO@MoO3 sensor is attributed to the synergistic effects between ZnO and MoO3, as well as the enhanced electron transfer rate enabled by the heterostructures. This work provides an effective strategy for advancing NO2 sensing capabilities in metal oxide composite sensors.