bluuebunny/crossref_metadata_2025_split huggingface dataset:
Simultaneous Scanning Ion Conductance and Electrochemical Microscopy in Lithium‐Ion Battery Research
Authors: Eidenschink Johannes , Matysik Frank‐Michael 
Published: January 2024

AbstractDeeper understanding of processes involved in operation of lithium‐ion batteries (LIBs) is necessary to further optimize them for future applications. Extensive research was conducted on the formation of a solid electrolyte interphase (SEI) on negative battery electrodes, still leaving several questions unanswered. Scanning probe microscopies (SPMs) enable in situ and operando investigations and have the potential to explain some phenomena. Scanning electrochemical microscopy (SECM) and scanning ion conductance microscopy (SICM) could be employed in LIB studies. A novel SICM method based on the redox couple ferrocene/ferrocenium is introduced for applications in carbonate solvents widely used in LIBs. Proof of concept measurements were conducted with a micro milled copper circuit board as model substrate. Furthermore, the proposed SICM approach was hyphenated with feedback mode SECM resulting in the simultaneous mapping of morphology and electrochemical activity. A flexible dual‐probe arrangement was developed enabling usage of both SPM techniques at the same time, and furthermore, an easy replacement of both individual probes if needed. The setup was applied in the characterisation of commercial graphite electrodes for LIBs before and after conducting a pre‐charging protocol. Changes in electrochemical activity and topography of the graphite electrode were resolved in simultaneously generated SECM/SICM recordings.
Effect of Polytetrafluorethylene Content in Fe‐N‐C‐Based Catalyst Layers of Gas Diffusion Electrodes for HT‐PEM Fuel Cell Applications
Authors: Zierdt Tanja , Müller‐Hülstede Julia , Schmies Henrike , Schonvogel Dana , Wagner Peter , Friedrich K. Andreas 
Published: January 2024

AbstractFe‐N‐C catalysts are a promising alternative to replace cost‐intensive Pt‐based catalysts in high temperature polymer electrolyte membrane fuel cell (HT‐PEMFC) electrodes. However, the electrode fabrication needs to be adapted for this new class of catalysts. In this study, gas diffusion electrodes (GDEs) are fabricated using a commercial Fe‐N‐C catalyst and different polytetrafluorethylene (PTFE) binder ratios, varying from 10 to 50 wt % in the catalyst layer (CL). The oxygen reduction reaction performance is investigated under HT‐PEMFC conditions (160 °C, conc. H3PO4 electrolyte) in a half‐cell setup. The acidophilic character of the Fe‐N‐C catalyst leads to intrusion of phosphoric acid electrolyte into the CL. The strength of the acid penetration depends on the PTFE content, which is visible via the contact angles. The 10 wt % PTFE GDE is less capable to withdraw product water and electrolyte and results into the lowest half‐cell performance. Higher PTFE contents counterbalance the acid drag into the CL and impede flooding. The power density at around 130 mA mgCatalyst−2 increases by 34 % from 10 to 50 wt % PTFE.
Nucleobase Stacking Sustained by Pt−Pt Interactions
Authors: Lorenzo‐Aparicio Carmen , García‐Álvarez Pablo , Cabeza Javier A. , Gómez‐Gallego Mar , Sierra Miguel A. 
Published: January 2024

AbstractThis article reports the use of metal–metal interactions as a way to induce nucleobase stacking in a dinucleotide chain. We synthetized and study a series of C,N‐cyclometallated platinum(II) binuclear complexes derived from 6‐phenylpurine dinucleotide 1 as proligand, and β‐diketonates, 2,2'‐bipyridines and 1,10‐phenanthroline as ancillary ligands. The X‐ray diffraction analysis revealed that the diketonate derivatives 7 and 8 are chiral helixes sustained by Pt−Pt intramolecular interactions that allow the nucleobase stacking. The folded helical structures are maintained in solution, as demonstrated by the appearance of metal–metal‐to‐ligand charge‐transfer (MMLCT) transitions in the UV‐vis spectra. The influence of the ancillary ligand in the molecular structure was evidenced by the absence of bands derived from M−M interactions in the absorption spectra of 2,2’‐bipyridine and and 1,10‐phenanthroline derivatives 12–14. The existence of Pt−Pt in the complexes of this study can be also detected by electrochemistry.
“Photo‐Adrenalines”: Photoswitchable β2‐Adrenergic Receptor Agonists as Molecular Probes for the Study of Spatiotemporal Adrenergic Signaling
Authors: Sink Alexandra , Gerwe Hubert , Hübner Harald , Boivin‐Jahns Valerie , Fender Julia , Lorenz Kristina , Gmeiner Peter , Decker Michael 
Published: January 2024

Abstractβ2‐adrenergic receptor (β2‐AR) agonists are used for the treatment of asthma and chronic obstructive pulmonary disease, but also play a role in other complex disorders including cancer, diabetes and heart diseases. As the cellular and molecular mechanisms in various cells and tissues of the β2‐AR remain vastly elusive, we developed tools for this investigation with high temporal and spatial resolution. Several photoswitchable β2‐AR agonists with nanomolar activity were synthesized. The most potent agonist for β2‐AR with reasonable switching is a one‐digit nanomolar active, trans‐on arylazopyrazole‐based adrenaline derivative and comprises valuable photopharmacological properties for further biological studies with high structural accordance to the native ligand adrenaline.
Boosting Hydrogen Production of a MOF‐based Multicomponent Photocatalyst with Clean Interface via Facile One‐pot Electrosynthesis
Authors: Cheng Wen‐Wen , Zhang Sheng‐Nan , Wang Jun , Yang Jia , Yang Zhengkun , Chen Xi‐Fan , Xiao Juan‐Ding , Wang Junzhong 
Published: January 2024

AbstractHydrogen production from photocatalysis via the usage of multicomponent photocatalysts represents a promising pathway for carbon peaking and carbon neutrality, owing to their structural advantages in dealing with the three crucial processes in photocatalysis, namely, light harvesting, charge transfer, and surface redox reactions. We demonstrate the fabrication of a MOF‐based multicomponent photocatalyst, denoted as semiconductor/MOF/cocatalyst, by a one‐pot electrochemical synthetic route. The as‐fabricated multicomponent photocatalyst has a clean interface among the components, leading to close connections that contribute to high‐quality heterojunction and facilitate photogenerated charge transfer and separation, thereby the efficient hydrogen evolution. The hydrogen production rate of the resultant ZrO2/Zr‐MOF/Pt is 1327 μmol ⋅ g−1 ⋅ h−1, which is much higher than that of ZrO2/Zr‐MOF (15 μmol ⋅ g−1 ⋅ h−1) and pure Zr‐MOF (10.1 μmol ⋅ g−1 ⋅ h−1), as well as the photodeposited‐Pt products ZrO2/Zr‐MOF/PtPD (287 μmol ⋅ g−1 ⋅ h−1) and Zr‐MOF/PtPD (192 μmol ⋅ g−1 ⋅ h−1) obtained by the step‐wise synthetic approach. The work gives a good inspiration for the rational design and construction of MOF‐based multicomponent photocatalysts through the one‐pot electrosynthesis.
Characterization by Gel Permeation Chromatography of the Molecular Weight of Supramolecular Polymers Generated by Forming Polyrotaxanes through the Introduction of External Stoppers
Authors: Liu Hui , Hu Ziqing , Ji Xiaofan 
Published: January 2024

AbstractSupramolecular polymers find wide applications across diverse domains, and the molecular weight exerts a critical influence on their applicability. Consequently, the measurement of molecular weight for supramolecular polymers assumes paramount significance. Gel Permeation Chromatography (GPC) requiring low‐concentration condition is a common characterization employed for molecular weight determination, which is not suitable for supramolecular polymers possessing concentration‐independence property. Here, to break this threshold, we synthesized M1 embodying dibenzo‐24‐crown‐8 (DB24C8) moiety as well as dibenzylammonium salt (DBA) group, which was capable of self‐assembling into supramolecular polymers terminated with aldehyde groups at its end. Upon the addition of (4‐ (1,2,2‐Triphenylvinyl) phenyl) methylamine (TPE‐NH2), supramolecular polymers underwent a transition into polyrotaxanes, for which it was led by the generation of imine bonds. By virtue of GPC, the molecular weight of polyrotaxanes was obtained, then it was available to gain the molecular weight of supramolecular polymers with the help of transformation efficiency.
Application and reduction of a nonlinear hyperelastic wall model capturing ex vivo relationships between fluid pressure, area, and wall thickness in normal and hypertensive murine left pulmonary arteries
Authors: Haider Mansoor A. , Pearce Katherine J. , Chesler Naomi C. , Hill Nicholas A. , Olufsen Mette S. 
Published: January 2024

AbstractPulmonary hypertension is a cardiovascular disorder manifested by elevated mean arterial blood pressure (>20 mmHg) together with vessel wall stiffening and thickening due to alterations in collagen, elastin, and smooth muscle cells. Hypoxia‐induced (type 3) pulmonary hypertension can be studied in animals exposed to a low oxygen environment for prolonged time periods leading to biomechanical alterations in vessel wall structure. This study introduces a novel approach to formulating a reduced order nonlinear elastic structural wall model for a large pulmonary artery. The model relating blood pressure and area is calibrated using ex vivo measurements of vessel diameter and wall thickness changes, under controlled pressure conditions, in left pulmonary arteries isolated from control and hypertensive mice. A two‐layer, hyperelastic, and anisotropic model incorporating residual stresses is formulated using the Holzapfel–Gasser–Ogden model. Complex relations predicting vessel area and wall thickness with increasing blood pressure are derived and calibrated using the data. Sensitivity analysis, parameter estimation, subset selection, and physical plausibility arguments are used to systematically reduce the 16‐parameter model to one in which a much smaller subset of identifiable parameters is estimated via solution of an inverse problem. Our final reduced one layer model includes a single set of three elastic moduli. Estimated ranges of these parameters demonstrate that nonlinear stiffening is dominated by elastin in the control animals and by collagen in the hypertensive animals. The pressure–area relation developed in this novel manner has potential impact on one‐dimensional fluids network models of vessel wall remodeling in the presence of cardiovascular disease.
(Pyridin‐2‐ylmethyl)triel Derivatives as Masked Frustrated Lewis Pairs. Interactions and CO2‐Sequestration
Authors: Ferrer Maxime , Alkorta Ibon , Elguero Jose , Oliva‐Enrich Josep M. 
Published: January 2024

AbstractThe isolated (pyridin‐2‐ylmethyl)triel derivatives (triel=B, Al and Ga) show an intramolecular N⋅⋅⋅Tr triel bond as shown by compounds found in the Cambridge Structural Database and DFT calculations. The possibility to use them as masked frustrated Lewis pairs (mFLP) has been explored theoretically concerning their reaction with CO2. The adduct formation proceeds in two steps. In the first one, the (pyridin‐2‐ylmethyl)triel derivatives break the intramolecular N⋅⋅⋅Tr bond assisted by CO2 and in the second step the adduct is formed with Tr−O and N−C covalent bonds. The corresponding energy minima and transition states (TS) of the reaction have been characterized and analyzed. The distortion/interaction model analysis of the stationary points indicates that the whole process can be divided in two parts: reorganization of the mFLP in the first steps of the reaction while the reaction with CO2 (associated to the distortion of this molecule) is more important in the formation of the final adduct. In all cases studied, the final products are more stable than the starting molecules that combine with reasonable TS energies indicating that these reactions can occur.
Through‐space scalar spin‐spin coupling: from rigid intramolecular cases to short‐lived van der Waals complexes
Authors: Saielli Giacomo 
Published: January 2024

AbstractWe will discuss, with the help of few selected examples, how the concept of through‐space scalar spin‐spin coupling between non covalently bonded nuclei has evolved in recent years. We will first present systems where ‘no covalent bond’ actually means that the two atoms are separated by a large number of bonds; then we will see cases where it is referred to true van der Waals dimers, but with the two atoms somehow constrained in their positions; we will finish with the most recent examples of liquids and even gaseous mixtures with full translational degrees of freedom in a regime of intermolecular/interatomic fast exchange.
The associations of grief‐related rumination with prolonged grief and posttraumatic stress symptoms: A longitudinal study of bereaved after the 2011 terror attack in Norway
Authors: Thimm Jens C. , Kristensen Pål , Aulie Ingebjørg Fossberg , Larsen Ida Marie , Johnsen Iren 
Published: January 2024

AbstractAfter the sudden and violent death of a loved one, many bereaved experience symptoms of prolonged grief (PG) and posttraumatic stress (PTS). The present study investigated the cross‐sectional and longitudinal associations of grief‐related rumination with PG and PTS symptoms among bereaved parents and siblings after the Utøya terror attack in Norway on 22 July 2011 (N = 110, Mage = 43.2 years, 59.1% female). Participants' responses on the Rumination Scale, the Inventory of Complicated Grief and the Impact of Event Scale‐Revised 28, 40 and 102 months after the loss were analysed. Cross‐sectionally and longitudinally, grief‐related rumination was positively and strongly linked with PG and PTS symptoms. When controlling for the baseline levels of PG and PTS symptoms and demographics of the sample, grief‐related rumination predicted PG symptoms after 12 months but not after 74 months. Further, grief‐related rumination predicted significantly the PTS symptoms of avoidance after 12 and 74 months and hyperarousal after 74 months beyond sample demographics and baseline symptoms. The results suggest that grief‐related rumination is an important factor in PG and PTS symptoms after traumatic bereavement.
Water droplet energy harvesting
Authors: Lin Zhiming , Yang Zhengbao 
Published: January 2024

AbstractHarnessing abundant kinetic water energy in diverse forms of river flows, ocean waves, tidal currents, raindrops, and others, is highly attractive to ease the energy crisis and satisfy the demands of scattered sensor network nodes in the Internet of things. Among them, raindrops, widely and ubiquitously distributed in nature and ambient living life, have been extensively explored and regarded as significant renewable energy carriers. Extensive efforts have been made to investigate droplet‐based electricity nanogenerators in fundamental mechanism, performance, and applications for achieving sustainable energy demands of the rapidly developing society over the past decade. In this review, we introduce the remarkable progress in this field and discuss the fundamental mechanisms of droplet energy harvesting technology for achieving high‐power generation. More significantly, a systematic review of droplet energy harvesting in different two‐phase interfaces, including liquid–solid, liquid–liquid, and liquid–gas interfaces, is provided. Finally, this survey reveals that droplet‐based electricity generators present vast potential in the power supply. At the same time, several development challenges and prospective solutions are discussed to spur future technological advancements.
Synthesis and Twin Polymerization of Si(OCH2py)4 for Nitrogen‐containing Carbon Materials
Authors: Scharf Sebastian , Notz Sebastian , Pfefferkorn Kai , Rüffer Tobias , Formánek Petr , Hübner René , Selyshchev Oleksandr , Madeira Teresa I. , Zahn Dietrich R. T. , Lang Heinrich 
Published: January 2024

AbstractThe synthesis and twin polymerization (TP) of Si(OCH2py)4 (3 a, py=2‐cC5H4N; 3 b, py=3‐cC5H4N; 3 c, py=4‐cC5H4N) is discussed. The solid state structures of 3 b, c were confirmed by single‐crystal X‐ray crystallography showing non‐conventional H‐bonding, forming 2D chains (3 b) or 3D networks (3 c). Thermally induced TP of 3 a–c and their simultaneous polymerization with 2,2‘‐spiro‐bi[4H‐1,3,2‐benzodioxasiline] (4) is described. The resulting hybrid materials were characterized by 1H, 13C{1H}, and 29Si{1H} CP MAS NMR spectroscopy confirming the transformation of the SiOCH2 moieties into CH2 groups enabling the formation of the respective polymers. These results were supported by HAADF‐STEM studies, displaying micro‐structuring. Nitrogen‐containing porous carbon materials C_1–C_3 show surface areas of 1300 and 1700 m2 g−1, large pore volumes between 0.6–1.2 cm3 g−1, and nitrogen contents of up to 3.1 at‐%. X‐ray photoemission spectroscopy reveal that pyrrolic, pyridine, and pyridone nitrogen atoms are present. If equimolar amounts of 3 a–c and 4 are simultaneously polymerized in the presence of [Pd(OAc)2] (5), then the Pd nanoparticle‐decorated material Pd@C_3 (900 m2 g−1) was obtained, which showed k values of −0.083 and −0.066 min−1 in the reduction of methylene blue and methyl orange, proving the accessibility of the Pd NPs.
Synthesis and Characterization of Dearomatized Pyridine‐Derived Alkyl‐Amido‐tert‐Butylphosphine Iron(II) Complexes
Authors: Gunasekera Parami S. , Paul Sanchita , MacMillan Samantha N. , Lacy David C. 
Published: January 2024

AbstractNeutral three‐coordinate iron alkylidenes of the form PN−Fe=CHR have been proposed as viable candidates for alkene metathesis. Indeed, during the final stages of preparing this current study, a separate report disclosed that dearomatized PN−Fe‐alkyl complexes are active precatalysts for ring‐opening metathesis polymerization (ROMP) of norbornene implicating PN−Fe=CHR species as possible intermediates. In yet another separate report, we prepared Zn analogues of PN−Fe‐alkyl complexes and herein provide an account for the synthesis, characterization, and reactivity of some new iron complexes with the same tBu substituted PN platform.
Adsorption of hydrocarbon pollutants from wastewater using Cu‐ and Zn‐loaded activated carbon derived from waste tires
Authors: Ahmad Waqas , Muhammad Taj , Ahmad Imtiaz , Khan Mumtaz , Nazneen Shahla 
Published: January 2024

AbstractPetroleum refinery effluents contain hazardous aromatic and polyaromatic hydrocarbons that causes environmental degradation, that is, water, land, and air pollution; therefore, it should be properly treated before its discharge into environment. Adsorption serves an efficient route to treatment of refinery wastewater; but the high production cost and selectivity of the modern adsorbent used limits their industrial scale application. On the other hand, activated carbon due to desirable adsorption characteristics and low cost seems to hold the promise if properly modified to improve its efficiency. In this study, Cu and Zn impregnated on activated carbon (AC) derived from waste tires was used for adsorption of hydrocarbon pollutants from wastewater. AC was prepared from scrap tires through thermal pyrolysis, followed by chemical activation with KOH. Cu and Zn were loaded on AC through wet impregnation method. Initial batch mode adsorption experiments were carried out using aniline and phenol as model hydrocarbons, which indicated that maximum adsorption of aniline and phenol over Zn/AC and Cu/AC occurs in 10 min contact time, temperature 30°C, pH 6, 100 ppm initial concentration, and adsorbent dose of 0.1 g/10 mL. The removal of hydrocarbon pollutants from real refinery wastewater was also investigated under optimized conditions. Results show that the COD of the refinery wastewater decreased from 963 to 73 mg/L in case of Cu/AC (92% removal) and 78 mg/L in case of Zn/AC (91% removal), respectively. The adsorbent showed many folds reusability, and in first cycle, the removal efficiency of phenol and aniline was observed to be above 95%, whereas in second, third and fourth cycles, the removal percentage was 85%, 80%, and 70%, respectively.
Evapotranspiration and surface energy fluxes across Europe, Africa and Eastern South America throughout the operational life of the Meteosat second generation satellite
Authors: Barrios J. M. , Arboleda A. , Dutra E. , Trigo I. , Gellens‐Meulenberghs F. 
Published: January 2024

AbstractThe exchange of energy and water fluxes between the Earth's surface and the atmosphere is crucial to a series of processes that impact human life. Noteworthy examples are agriculture yields, water availability, intensity and extent of droughts and the ability of ecosystems to provide services to society. The relevance of these processes has motivated the Satellite Application Facility on Land Surface Analysis (LSA SAF) programme to set up an operational framework to estimate—among other variables—evapotranspiration (ET) and surface energy fluxes (SEF) on the basis of observations by the Meteosat Second Generation (MSG) satellite. The LSA SAF programme has recently launched the reprocessing of the ET and SEF datasets on the basis of the most recent version of the algorithm and homogenous forcing datasets. This article features the resulting ET/SEF dataset, a Data Record that encompasses the period from the start of the operational life of the MSG satellite (2004) till 2020 and covers the field of view of the MSG satellite (i.e. Europe, Africa and Eastern South America). Details on the algorithm and the datasets driving the ET/SEF estimates are also provided as well as a quality assessment.
Negotiating structural barriers to environmental collaborations in doctoral programmes
Authors: Lait Joshua , Hayes Hannah , Hayes Sylvia , Auster Roger , Fox Ellie , Timmins Madeleine , Bauchot Augustin 
Published: January 2024

AbstractThis commentary reflects on the experiences of a cohort of human and physical geographers in enacting environmental collaborations during their doctoral studies. The authors identify three key structural barriers encountered whilst attempting a collaborative approach: (1) doctoral funding priorities, (2) doctoral resourcing and (3) assessing doctoral collaboration. The authors discuss how the negotiation of these encounters came to frame their understanding of collaborative approaches to environmental knowledge creation. Competitive application processes for doctoral studentships can encourage the overpromising of the impact of planned environmental collaboration, potentially co‐opting the voices of partners/communities to satisfy doctoral funding requirements. Given insufficient funding of collaborations, the authors argue that this overpromising of doctoral research's impact can later result in difficult trade‐offs between undertaking additional commitments at the expense of the career progression of the doctoral student, contributing to educational inequalities and scaling‐back the initial plans at the cost of collaborators encountering environmental crises. The trade‐off is further problematised by institutional assessment procedures that do not adequately recognise the more nuanced contributions of environmental collaborations and a prevailing culture promoting peer‐review publishing. Overall, the commentary argues that these barriers help to reproduce inequalities in the distribution of voice in environmental scholarship, undermining efforts to democratise environmental knowledge creation in doctoral research. The authors call for specific structural reforms of doctoral programmes to help address these challenges and support a broader resistance to the inadequate resourcing and evaluation of environmental collaborative research in UK higher education.