bluuebunny/crossref_metadata_2025_split huggingface dataset:
Unveiling Highly Sensitive Active Site in Atomically Dispersed Gold Catalysts for Enhanced Ethanol Dehydrogenation
Authors: Yang Ji , Zheng Juan , Dun Chaochao , Falling Lorenz J. , Zheng Qi , Chen Jeng‐Lung , Zhang Miao , Jaegers Nicholas R. , Asokan Chithra , Guo Jinghua , Salmeron Miquel , Prendergast David , Urban Jeffrey J. , Somorjai Gabor A. , Guo Yanbing , Su Ji 
Published: June 2024

AbstractDeveloping a desirable ethanol dehydrogenation process necessitates a highly efficient and selective catalyst with low cost. Herein, we show that the “complex active site” consisting of atomically dispersed Au atoms with the neighboring oxygen vacancies (Vo) and undercoordinated cation on oxide supports can be prepared and display unique catalytic properties for ethanol dehydrogenation. The “complex active site” Au−Vo−Zr3+ on Au1/ZrO2 exhibits the highest H2 production rate, with above 37,964 mol H2 per mol Au per hour (385 g H2
h−1) at 350 °C, which is 3.32, 2.94 and 15.0 times higher than Au1/CeO2, Au1/TiO2, and Au1/Al2O3, respectively. Combining experimental and theoretical studies, we demonstrate the structural sensitivity of these complex sites by assessing their selectivity and activity in ethanol dehydrogenation. Our study sheds new light on the design and development of cost‐effective and highly efficient catalysts for ethanol dehydrogenation. Fundamentally, atomic‐level catalyst design by colocalizing catalytically active metal atoms forming a structure‐sensitive “complex site”, is a crucial way to advance from heterogeneous catalysis to molecular catalysis. Our study advanced the understanding of the structure sensitivity of the active site in atomically dispersed catalysts.
Construction of Benzoxazine‐linked One‐Dimensional Covalent Organic Frameworks Using the Mannich Reaction
Authors: Cheng Cheng , Liu Yikuan , Sheng Guan , Jiang Xinru , Kang Xing , Jiang Chao , Liu Yan , Zhu Yihan , Cui Yong 
Published: June 2024

AbstractCovalent polymerization of organic molecules into crystalline one‐dimensional (1D) polymers is effective for achieving desired thermal, optical, and electrical properties, yet it remains a persistent synthetic challenge for their inherent tendency to adopt amorphous or semicrystalline phases. Here we report a strategy to synthesize crystalline 1D covalent organic frameworks (COFs) composing quasi‐conjugated chains with benzoxazine linkages via the one‐pot Mannich reaction. Through [4+2] and [2+2] type Mannich condensation reactions, we fabricated stoichiometric and sub‐stoichiometric 1D covalent polymeric chains, respectively, using doubly and singly linked benzoxazine rings. The validity of their crystal structures has been directly visualized through state‐of‐the‐art cryogenic low‐dose electron microscopy techniques. Post‐synthetic functionalizations of them with a chiral MacMillan catalyst produce crystalline organic photocatalysts that demonstrated excellent catalytic and recyclable performance in light‐driven asymmetric alkylation of aldehydes, affording up to 94 % enantiomeric excess
Aluminum in Frustrated Lewis Pair Chemistry
Authors: Krämer Felix 
Published: June 2024

AbstractThis review article describes the development of the use of aluminum compounds in the chemistry of frustrated Lewis pairs (FLPs) over the last 14 years. It also discusses the synthesis, reactivity and catalytic applications of intermolecular, intramolecular and so‐called hidden FLPs with phosphorus, nitrogen and carbon Lewis bases. The intrinsically higher acidity of aluminum compounds compared to their boron analogs opens up different reaction pathways. The results are presented in a more or less chronological order. It is shown that Al FLPs react with a variety of polar and non‐polar substrates and form both stable adducts and reversibly activate bonds. Consequently, some catalytic applications of the title compounds were presented such as dimerization of alkynes, hydrogenation of tert‐butyl ethylene and imines, C−F bond activation, reduction of CO2, dehydrogenation of amine borane and transfer of ammonia. In addition, various Al FLPs were used as initiators in polymerization reactions.
Catalyst‐Free Dynamic Covalent C=C/C=N Metathesis Reaction for Associative Covalent Adaptable Networks
Authors: Li Pengyun , Jiang Xin , Gu Ruirui , Tian He , Qu Da‐Hui 
Published: June 2024

AbstractCovalent adaptable networks (CANs), leveraging the dynamic exchange of covalent bonds, emerge as a promising material to address the challenge of irreversible cross‐linking in thermosetting polymers. In this work, we explore the introduction of a catalyst‐free and associative C=C/C=N metathesis reaction into thermosetting polyurethanes, creating CANs with superior stability, solvent resistance, and thermal/mechanical properties. By incorporating this dynamic exchange reaction, stress‐relaxation is significantly accelerated compared to imine‐bond‐only networks, with the rate adjustable by modifying substituents in the ortho position of the dynamic double bonds. The obtained plasticity enables recycle without altering the chemical structure or mechanical properties, and is also found to be vital for achieving shape memory functions with complex spatial structures. This metathesis reaction as a new dynamic crosslinker of polymer networks has the potential to accelerate the ongoing exploration of malleable and functional thermoset polymers.
Synthesis of All‐Benzene Multi‐Macrocyclic Nanocarbons by Post‐Functionalization of meta‐Cycloparaphenylenes
Authors: Gao Jia‐Nan , Bu An , Chen Yiming , Huang Mianling , Chen Zhi , Li Xiaopeng , Tung Chen‐Ho , Wu Li‐Zhu , Cong Huan 
Published: June 2024

AbstractExpanding the diversity of multi‐macrocyclic nanocarbons, particularly those with all‐benzene scaffolds, represents intriguing yet challenging synthetic tasks. Complementary to the existing synthetic approaches, here we report an efficient and modular post‐functionalization strategy that employs iridium‐catalyzed C−H borylation of the highly strained meta‐cycloparaphenylenes (mCPPs) and an mCPP‐derived catenane. Based on the functionalized macrocyclic synthons, a number of novel all‐benzene topological structures including linear and cyclic chains, polycatenane, and pretzelane have been successfully prepared and characterized, thereby showcasing the synthetic utility and potential of the post‐functionalization strategy.
Long‐term tracking reveals the influence of body size and habitat type on the home range of Antillean manatees (Trichechus manatus manatus)
Authors: Normande Iran C. , Borges João Carlos G. , Attademo Fernanda L.N. , Deeks Emma , dos Santos Sebastião S. , Negrão Cristine P. , Silva Flávio José L. , Queiroz Nuno , Ladle Richard J. , Luna Fabia O. , Santos Robson G. 
Published: June 2024

AbstractAntillean manatees (Trichechus manatus manatus) are endangered coastal, marine, and riverine megaherbivores with high environmental plasticity, constrained by tidal and seasonal water level cycles that affect access to food and fresh water. Accurate quantification of the species' habitat requirements, typically achieved through home range (HR) estimation, is required to implement area‐based conservation initiatives. In this study, we used GPS tracking data from 38 wild and captive‐rehabilitated released manatees to estimate HR using autocorrelated kernel density estimators (AKDE) and average time speed. We investigated whether body size, habitat type, sex and behavioural group influence home range size due to energy requirements, resources availability, a scramble‐competitive polygyny mating system, and adaptation to the wild. Eighteen manatees exhibited range‐resident behaviour, with a mean 95% home range of 72.96 km2 (± 218.52) and a median of 10.69 km2. The mean daily speed was estimated to be 13.47 km/day (± 4.16). Home range and body size were positively correlated, consistent with HR allometry theory. Long‐term tracked individuals showed a trend of increasing HR over time. Only four released animals (17.4%) were range‐resident, suggesting that they may need additional time to establish a home range. Individuals using only the marine environment had larger home ranges compared to mixed (marine and estuarine) and estuarine environments, probably due to freshwater availability. Our study contributes to the understanding of the factors driving manatee movement and provides more accurate estimates of area requirements, which can inform the establishment and zoning of marine protected areas.
Evidence of the Electrochemical Ca2+ Intercalation in Anatase Nanotubes
Authors: Ceppetelli Andrea , Busato Matteo , Dilena Gabriele , Cavallo Carmen , Navarra Maria Assunta , D'Angelo Paola , Silvestri Laura , Reale Priscilla , Santoni Antonino , Stievano Lorenzo , Brutti Sergio 
Published: June 2024

AbstractHere, we demonstrate the electrochemical intercalation of Ca2+ ions within the lattice of anatase nanotubes (a‐NTs) synthesized by hydrothermal treatment of TiO2/NaOH precursors followed by Na+/H+ ion exchange and H2O‐loss at high temperature in air. Scanning electron microscopy, X‐ray diffraction, and Raman spectroscopy confirm the formation of nanosized anatase, whereas transmission electron microscopy highlights the formation of nanotubular morphologies with an average diameter of 10 nm. TiO2 electrodes are able to deliver reversible specific capacities in aprotic batteries vs. calcium metal or in hybrid configurations vs. capacitive activated carbon using aprotic electrolytes (i. e., Ca(BH4)2 in tetrahydrofuran or Ca(TFSI)2 in dimethoxyethane, respectively). The electrochemical intercalation of Ca2+ ions into the anatase lattice is confirmed by X‐ray absorption spectroscopy in close comparison with Na+ and Li+ intercalations. Ca2+ incorporation leads to the partial amorphization of the TiO2 lattice despite the limited Ca/Ti ratio (i. e., 0.09) obtained in discharge. The analysis of the extended X‐ray absorption fine structure region allows the determination of the local structure of the incorporated Ca2+ ions and confirms that a disordered environment is obtained after the electrochemical reaction.
Nucleation Mechanisms of Electrodeposited Magnesium on Metal Substrates
Authors: Löw Mario , Maroni Fabio , Zaubitzer Steve , Dongmo Saustin , Marinaro Mario 
Published: June 2024

AbstractMagnesium rechargeable batteries (RMBs) are a promising alternative to lithium‐based ones. However, a major challenge in their advance concerns the development of aprotic electrolytes from which magnesium can be electrodeposited with high efficiency and without the formation of dendrites. Of note, the mechanism of the magnesium electrodeposition from aprotic electrolytes remains largely unexplored. In this study, we propose a combined experimental and theoretical approach based on the Scharifker‐Hills (S−H) mathematical model for the potentiostatic transients to analyse the nucleation and growth of magnesium during electrodeposition in order to shed light on the nucleation process and increase battery safety and cycle lifetime. The model is used to investigate the electrodeposition of magnesium from a Magnesocene (MgCp2)‐based electrolyte onto metal current substrates such as copper, nickel, aluminium and stainless steel.
Understanding the impact of artificial intelligence on the justice of charitable giving: The moderating role of trust and regulatory orientation
Authors: Yang Chen , Yang Yi , Zhang Yuezi 
Published: June 2024

AbstractThe issue of distributive justice in charitable donations has become increasingly prominent. It not only weakens people's confidence in philanthropy but also their enthusiasm for participation. With the widespread use of artificial intelligence technology in donations, a key question arises: Can artificial intelligence inspire people to be more willing to donate by improving their perception of justice in donation distribution? This question is vital for charities but has yet to be answered. To address this gap, this research conducted five comprehensive studies to investigate the impact of AI decision‐makers on consumers' willingness to donate. The findings of Studies 1 and 2 consistently revealed that consumers perceive higher distributive justice in AI decision‐makers compared with humans, motivating increased participation in charitable donations. Study 3 examined two different experimental scenarios and found that this effect only occurs among consumers with lower trust in nonprofit organizations. Study 4 further explored the effect that is only present among prevention‐oriented consumers. These findings reveal how perceptions of distributive justice toward AI decision‐makers can facilitate public charitable giving and highlight the significance of this effect across different groups of consumers, providing invaluable insights for charitable organizations. This research not only fills the theoretical gap in the philanthropic field about the impact of artificial intelligence decision‐makers on donation distribution justice but also provides charitable organizations with artificial intelligence‐based donation promotion strategies.
Phytochemical Profiling and Biological Activity of the Methanolic Extracts of Cirsium Monspessulanum (L.) Hill.
Authors: Kozyra Małgorzata , Biernasiuk Anna , Gryta Elżbieta , Kozyra Paweł , Malm Anna 
Published: June 2024

AbstractThe study of new plant species and the identification of their chemical composition may contribute to the discovery of a new breakthrough substances for pharmacotherapeutical applications. For the first time, we examined antioxidant and antimicrobial activity of 70 % v/v methanolic extracts from inflorescences and roots of Cirsium monspessulanum (L.) Hill. obtained by the ASE method. In the (2,2‐diphenyl‐1‐picrylhydrazyl) DPPH analysis, tested extract of inflorescences showed antioxidant activity with an EC50=0.223±0.0479 mg/mL, and (Cupric Ion Reducting Antioxidant Capacity) CUPRAC test assessed the antiradical activity on 14.95±0.13 mgTE/g and for roots the values were EC50=0.307±0.0554 mg/mL and 11.18±0.49 mgTE/g, respectively. Furthermore, extract from the inflorescences possessed the highest antimicrobial activity against Staphylococcus aureus, Staphylococcus epidermidis and Micrococcus luteus with MIC=1.25 mg/mL for each. HPLC/ESI‐QTOF‐MS/MS method identified 7 phenolic acids and 14 flavonoids in inflorescences extract and only 7 phenolic acids in roots extract. To the best of our knowledge, this is the first qualitative analysis of Cirsium monspessulanum (L.) Hill. and all substances were described for the first time.
Recent Advances in DNA Nanotechnology‐Based Sensing Platforms for Rapid Virus Detection
Authors: Dong Yuxiang , Guo Cheng , Wang Jialing , Ye Changqing , Min Qianhao 
Published: June 2024

AbstractSeveral major viral pandemics in history have significantly impacted the public health of human beings. The COVID‐19 pandemic has further underscored the critical need for early detection and screening of infected individuals. However, current detection techniques are confronted with deficiencies in sensitivity and accuracy, restricting the capability of detecting trace amounts of viruses in human bodies and in the environments. The advent of DNA nanotechnology has opened up a feasible solution for rapid and sensitive virus determination. By harnessing the designability and addressability of DNA nanostructures, a range of rapid virus sensing platforms have been proposed. This review overviewed the recent progress, application, and prospect of DNA nanotechnology‐based rapid virus detection platforms. Furthermore, the challenges and developmental prospects in this field were discussed.
Prognostic impact of vasopressor test in transcatheter edge‐to‐edge repair of secondary mitral regurgitation: The PETIT study
Authors: González‐Gutiérrez José Carlos , Benito‐González Tomas , Bosa‐Ojeda Francisco , Freixa‐Rofastes Xavier , Estevez‐Loureiro Rodrigo , Pascual Isaac , Andraka‐Ikazuriaga Leire , Díez‐Gil José Luis , Urbano‐Carrillo Cristobal , Amat‐Santos Ignacio J. 
Published: June 2024

AbstractBackgroundVasopressor test (VPT) might be useful in patients with functional mitral regurgitation (MR) and left ventricular dysfunction (MITRA‐FR‐like patients) during transcatheter edge‐to‐edge repair (TEER).AimsWe aimed to evaluate the prognostic impact of VPT.MethodsMR treated with TEER were included in a multicenter prospective registry. VPT was used intraprocedurally in patients with left ventricular dysfunction and/or hypotension. The 1‐year echocardiographic and clinical outcomes were compared according to the use of VPT. The primary endpoint was a combination of mortality + heart failure (HF) readmission at 1‐year.ResultsA total of 1115 patients were included, mean age was 72.8 ± 10.5 years and 30.4% were women. VPT was performed in 128 subjects (11.5%), more often in critically ill patients with biventricular dysfunction. Postprocedurally the VPT group had greater rate of MR ≥ 2+ (46.9% vs. 31.7%, p = 0.003) despite greater number of devices (≥2 clips, 52% vs. 40.6 p = 0.008) and device repositioning or new clip in 12.5%. At 1‐year, the primary endpoint occurred more often in the VPT group (27.3% vs. 16.9%, p = 0.002) as well as all‐cause mortality (21.9% vs. 8.1%, p ≤ 0.001) but no differences existed in HF readmission rate (14.8% vs. 13.2%, p = 0.610), cardiovascular mortality (4.4% vs. 3.9%, p = 0.713) or residual MR ≥ 2+ (51.1% vs 51.7%, p = 0.371).ConclusionsDynamic evaluation of MR during TEER procedure through VPT was performed in patients with worse baseline risk who also presented higher all‐cause mortality at 1‐year follow‐up. However, 1‐year residual MR, cardiovascular mortality and HF readmission rate remained comparable suggesting that VPT might help in the management of MITRA‐FR‐like patients.
Hydrogenation with Dissolved Pt‐Complexes Homogenously Distributed in the Ionic Liquid or Enriched at the Gas/Ionic Liquid Interface
Authors: Antara Sharmin Khan , Hemmeter Daniel , Zhai Ziwen , Kremitzl Daniel , Maier Florian , Koller Thomas M. , Steinrück Hans‐Peter , Haumann Marco 
Published: June 2024

AbstractThe use of homogeneous catalysts dissolved in ionic liquids (ILs) is an established field of research. Thin IL films containing dissolved catalyst complexes can be immobilized on solid porous supports, thereby creating a heterogenized catalyst material. Aiming at the deliberate positioning of such supported ionic liquid phase (SILP) catalyst, we carried out investigations of two very similar Pt‐complexes: depending on the ligand periphery, the first one is homogeneously dissolved in the IL while the second one strongly enriches at the gas/IL interface. To study these different locations within thick IL films of approximately 1 mm thickness, we investigated the hydrogenation of ethene in a continuous pool‐reactor setup. The two complexes dissolved in the IL [C4C1Im][PF6] showed different activity which can be attributed to their different locations. At 313 K and 0.62 MPa total pressure, the surface‐enriched complex was approximately two times more active. However, under these conditions the formation of Pt particles could be observed, with the surface‐enriched complex exhibiting a stronger tendency for particle formation compared to the one homogeneously distributed in the IL, as derived from XPS and light‐scattering measurements.
Elucidating the Mechanism of Efficient Eu(III) and Yb(III) Sensitisation from a Re(I) Tetrazolato Triangular Assembly
Authors: Wright Phillip J. , Pfrunder Michael C. , Etchells Isaac M. , Haghighatbin Mohammad A. , Raiteri Paolo , Ogden Mark I. , Stagni Stefano , Hogan Conor F. , Cameron Lee J. , Moore Evan G. , Massi Massimiliano 
Published: June 2024

AbstractThe reaction of Re(CO)5Br with deprotonated 1H‐(5‐(2,2′:6′,2′′‐terpyridine)pyrid‐2‐yl)tetrazole yields a triangular assembly formed by tricarbonyl Re(I) vertices. Photophysical measurements reveal blue‐green emission with a maximum at 520 nm, 32 % quantum yield, and 2430 ns long‐lived excited state decay lifetime in deaerated dichloromethane solution. Coordination of lanthanoid ions to the terpyridine units red‐shifts the emission to 570 nm and also reveals efficient (90 %) and fast sensitisation of both Eu(III) and Yb(III) at room temperature, with a similar rate constant kET on the order of 107 s−1. Efficient sensitisation of Eu(III) from Re(I) is unprecedented, especially when considering the close proximity in energy between the donor and acceptor excited states. On the other hand, comparative measurements at 77 K reveal that energy transfer to Yb(III) is two orders of magnitude slower than that to Eu(III). A two‐step mechanism of sensitisation is therefore proposed, whereby the rate‐determining step is a thermally activated energy transfer step between the Re(I) centre and the terpyridine functionality, followed by rapid energy transfer to the respective Ln(III) excited states. At 77 K, the direct Re(I) to Eu(III) energy transfer seems to proceed via a ligand‐mediated superexchange Dexter‐type mechanism.
Nickel(II)‐Catalyzed Reductive Coupling of Xanthate Esters with Sulfur‐Containing and Selenium‐Containing Compounds: Synthesis of Unsymmetric Sulfides and Selenides
Authors: Han Jia‐Hui , Sheng Daopeng , Chen Yi‐Rong , Shuai Xiao‐Yue , Rao Weidong , Shen Shu‐Su , Wang Shun‐Yi 
Published: June 2024

Comprehensive SummaryUnsymmetric sulfides and selenides have great applications in the pharmaceutical field. Herein, we describe the reductive coupling reaction of xanthate esters with sulfur‐containing and selenium‐containing compounds (thio(seleno)sulfonates and disulfides(selenides)) under the nickel‐catalyzed condition. It provides a mild and effective method for the synthesis of unsymmetric sulfides and selenides which has the advantages of mild reaction conditions, high yields and a wide range of substrates.
Nickel and Molybdenum Composites Decorated Nitrogen‐Doped Carbon Catalysts from Spent Coffee Grounds for Alkaline Hydrogen Evolution
Authors: Ge Xianlong , Zhang Chuan , Meng Minfeng , Song Yankai , Hu Shaohua , Gu Yingying 
Published: June 2024

AbstractBiomass‐derived materials can help develop efficient, environmentally friendly and cost‐effective catalysts, thereby improving the sustainability of hydrogen production. Herein, we propose a simple method to produce nickel and molybdenum composites decorated spent coffee grounds (SCG) as an efficient catalyst, SCG(200)@NiMo, for electrocatalytic hydrogen production. The porous carbon supporter derived form SCG provided a larger surface, prevented aggregation during the high temperature pyrolysis, optimized the electronic structure by N and provided a reducing atmosphere for the oxides reduction to form heterojunctions. The sieved SCG showed obvious improvement of HER performance and enhanced conductivity and long‐term durability. The obtained SCG(200)@NiMo exhibits the highest electrochemical performance for the hydrogen evolution reaction process, as evidenced by the overpotential of only 127 mV at a current density of ɳ10 and 97.7 % catalytic activity retention even after 12 h of operation. This work may stimulate further exploration of efficient electrocatalysts derived from biomass.