bluuebunny/crossref_metadata_2025_split huggingface dataset:
Imaging the Single‐Electron Ln–Ln Bonding Orbital in a Dimetallofullerene Molecular Magnet
Authors: Paschke Fabian , Birk Tobias , Avdoshenko Stanislav M. , Liu Fupin , Popov Alexey A. , Fonin Mikhail 
Published: December 2021

AbstractChemically robust single‐molecule magnets (SMMs) with sufficiently high blocking temperatures TB are among the key building blocks for the realization of molecular spintronic or quantum computing devices. Such device applications require access to the magnetic system of a SMM molecule by means of electronic transport, which primarily depends on the interaction of magnetic orbitals with the electronic states of the metallic electrodes. Scanning tunneling microscopy in combination with ab initio calculations allows to directly address the unoccupied component of the single‐electron molecular orbital that mediates the ferromagnetic exchange coupling between two 4f ions within a lanthanide endohedral dimetallofullerene deposited on a graphene surface. The single‐electron metal–metal bond provides a direct access to the molecule's magnetic system in the transport experiments, paving the way for investigation and controlled manipulation of the spin system of individual dimetallofullerene SMMs, essential for molecular spintronics.
An Active‐Oxygen‐Scavenging Oriented Cathode‐Electrolyte‐Interphase for Long‐Life Lithium‐Rich Cathode Materials
Authors: Wang Yajing , Cai Senrong , Sun Zongqiang , Hou Qing , Huang Haihong , Cheng Jiancong , Fan Jingmin , Zheng Mingsen , Dong Quanfeng 
Published: December 2021

AbstractLithium‐rich layered oxides with high energy density are promising cathode materials, thus having attracted a large number of researchers. However, the materials cannot be commercialized for application so far. The crucial problem is the releasing of lattice oxygen at high voltage and resulting consequence, such as decomposition of electrolyte, irreversible phase transition of crystal structure, capacity degradation, and voltage decay. Therefore, capturing active‐oxygen and further constructing a cathode‐electrolyte‐interface (CEI) protective layer via the scavenging effects should be a fundamental step to solve these issues. Herein, β‐carotene with antioxidant properties is used as a scavenging molecule to achieve this goal. The control of active oxygen species effectively alleviates the decomposition of carbonate electrolyte under high voltage. The introduction of β‐carotene additives can also be adjusted in situ to generate a customized CEI film, which is a double‐layer structure with external organic components and internal inorganic components. Moreover, the β‐carotene‐containing electrolyte system exhibits better thermal stability. Benefited from these, Lithium‐rich cathode of β‐carotene‐containing electrolyte shows outstanding long‐life cycle stability, with 93.4% capacity retention rate after 200 cycles at 1 C; this electrochemical stability is superior to other electrolyte additive systems reported at present.
Sulfur Vacancies‐Engineered Ni3S4‐x Hollow Microspheres with Optimized Anionic Adsorption Energy for High‐Performance Supercapacitor
Authors: Zhang Jiawei , Li Yu , Liang Xinqi , Liu Qian , Chen Qingguo , Chen Minghua 
Published: December 2021

AbstractNickel sulfides with high theoretical capacitance have aroused tremendous attention for next‐generation supercapacitors. Unfortunately, the structural durability of nickel sulfides is insufficient to support the long‐term working situation. Herein, Ni3S4‐x hollow microspheres with sulfur vacancies (Ni3S4‐x HMs) are constructed by a liquid‐phase anion exchange process using the Ni‐MOF as the precursor. Both experimental investigation and theoretical analysis suggest that the deliberately introduced sulfur vacancies effectively improve the anionic adsorptive ability of nickel sulfides in the KOH electrolyte, significantly enhancing the reversible capacitance and structural durability (1884 F g‐1 at 2 A g‐1, capacity retention of 97.9% after 10 000 cycles). In addition, an asymmetrical solid‐state supercapacitor consisting of Ni3S4‐x HMs cathode and activated carbon anode shows infusive energy/power density (33.05 Wh kg‐1/1.68 kW kg‐1) and remains 82.4% over 10 000 repeated charging/discharging processes in the KOH‐PVA gel electrolyte. The strategies can be developed to enlighten the structural design of various metal sulfides materials adopted in electrochemical energy storage devices including alkali ion batteries, supercapacitors, and electrocatalysts.
Quench‐Induced Surface Engineering Boosts Alkaline Freshwater and Seawater Oxygen Evolution Reaction of Porous NiCo2O4 Nanowires
Authors: Yang Jin , Wang Yanan , Yang Jie , Pang Yajun , Zhu Xinqiang , Lu Yinzhuo , Wu Yitian , Wang Jiajie , Chen Hao , Kou Zongkui , Shen Zhehong , Pan Zhenghui , Wang John 
Published: December 2021

AbstractThe electrochemical oxygen evolution reaction (OER) by efficient catalysts is a crucial step for the conversion of renewable energy into hydrogen fuel, in which surface/near‐surface engineering has been recognized as an effective strategy for enhancing the intrinsic activities of the OER electrocatalysts. Herein, a facile quenching approach is demonstrated that can simultaneously enable the required surface metal doping and vacancy generation in reconfiguring the desired surface of the NiCo2O4 catalyst, giving rise to greatly enhanced OER activities in both alkaline freshwater and seawater electrolytes. As a result, the quenched‐engineered NiCo2O4 nanowire electrode achieves a current density of 10 mA cm−2 at a low overpotential of 258 mV in 1 m KOH electrolyte, showing the remarkable catalytic performance towards OER. More impressively, the same electrode also displays extraordinary activity in an alkaline seawater environment and only needs 293 mV to reach 10 mA cm−2. Density functional theory (DFT) calculations reveal the strong electronic synergies among the metal cations in the quench‐derived catalyst, where the metal doping regulates the electronic structure, thereby yielding near‐optimal adsorption energies for OER intermediates and giving rise to superior activity. This study provides a new quenching method to obtain high‐performance transition metal oxide catalysts for freshwater/seawater electrocatalysis.
Regulating Interfacial Desolvation and Deposition Kinetics Enables Durable Zn Anodes with Ultrahigh Utilization of 80%
Authors: Jin Hongrun , Dai Simin , Xie Kefeng , Luo Yongxin , Liu Kaisi , Zhu Zehao , Huang Liwei , Huang Liang , Zhou Jun 
Published: December 2021

AbstractRechargeable aqueous zinc ion batteries (ZIBs) represent a promising technology for large‐scale energy storage due to their high capacity, intrinsic safety and low cost. However, Zn anodes suffer from poor reversibility and cycling stability caused by the side‐reactions and dendrite issues, which limit the Zn utilization in the ZIBs. Herein, to improve the durability of Zn under high utilization, an aluminum‐doped zinc oxide (AZO) interphase is presented. The AZO interphase inhibits side reactions by isolating active Zn from the bulk electrolyte, and enables facile and uniform Zn deposition kinetics by accelerating the desolvation of hydrated Zn2+ and homogenizing the electric field distribution. Accordingly, the AZO‐coated Zn (AZO@Zn) anode exhibits a long lifespan of 600 h with Zn utilization of 34.1% at the current density of 10 mA cm−2. Notably, even under ultrahigh Zn utilization of 80%, the AZO@Zn remains stable cycling over 200 h. Meanwhile, the V2O5/AZO@Zn full cell with limited Zn excess displays high capacity retention of 86.8% over 500 cycles at 2 A g−1. This work provides a simple and efficient strategy to ensure the reversibility and durability of Zn anodes under high utilization conditions, holding a great promise for commercially available ZIBs with competitive energy density.
Binder‐Free and High‐Loading Cathode Realized by Hierarchical Structure for Potassium–Sulfur Batteries
Authors: Yang Kaiwei , Kim Soochan , Yang Xin , Cho Misuk , Lee Youngkwan 
Published: December 2021

AbstractPotassium–sulfur batteries have attracted significant research attention owing to the naturally abundant resources of potassium and sulfur, and have promising applications in large‐scale energy storage systems. However, the sluggish reaction kinetics of K+, low reaction activity of sulfur species, shuttling effect of polysulfides, and large volume change impede the development of these batteries. Moreover, the conventional electrode fabrication method with binders and current collectors renders it difficult to improve the areal sulfur loading and energy density. In this study, a binder‐free and freestanding sulfur cathode is prepared by phase inversion and sulfurization of polyacrylonitrile. This sulfur cathode, with a hierarchically porous network, enables a high reversible capacity of 1345 mAh g−1 and a stable cycling performance with a capacity decay of 0.15% per cycle. Importantly, areal capacities of 3.1 and 4.2 mAh cm−2 are achieved even at high sulfur loadings of 3 and 7 mg cm−2, owing to the favorable electron/ion transport in the cathode. The facile preparation method and excellent electrochemical properties reported herein can pave the way for developing high‐performance K‐S batteries.
Interfacial Microenvironment Modulation Enhancing Catalytic Kinetics of Binary Metal Sulfides Heterostructures for Advanced Water Splitting Electrocatalysts
Authors: Qian Yongteng , Yu Jianmin , Zhang Ya , Zhang Fangfang , Kang Yingbo , Su Chenliang , Shi Hu , Kang Dae Joon , Pang Huan 
Published: December 2021

AbstractInterfacial microenvironment modulation has been proven to be a promising route to fabricate highly efficient catalysts. In this work, the lattice defect‐rich NiS2/MoS2 nanoflakes (NMS NFs) electrocatalysts are successfully synthesized by a simple strategy. Benefiting from the abundant lattice defects and modulated interfacial microenvironment between NiS2 and MoS2, the prepared NMS NFs show superior catalytic activity for water splitting. Particularly, the optimized NMS NFs (the molar ratio of Ni:Mo = 5:5) exhibit remarkable catalytic activity toward overall water splitting with a voltage of 1.60 V at 10 mA cm−2 in alkaline media, which is lower than that of the noble‐metal‐based electrocatalysts (1.68 V at 10 mA cm−2). The NMS NFs electrocatalysts also show exceptional long‐term stability (>50 h) for overall water splitting. The density functional theory results demonstrate that the injection of NiS2 into MoS2 can greatly optimize the catalytic kinetics and reduce the energy barrier for hydrogen/oxygen evolution reactions. The work does not only offer a promising candidate for a highly efficient water splitting electrocatalyst but also highlights that interfacial microenvironment modulation is a potential strategy to optimize the catalytic kinetics.
Zur Ermüdungsfestigkeit großer Schrauben im Stahlbau unter Berücksichtigung von Herstell‐ und Randschichteinflüssen – Teil 1: Bisheriger Kenntnisstand
Authors: Glienke Ralf , Schwarz Mathias , Marten Frithjof , Eichstädt Rasmus , Schwerdt Daniela , Meyer Melanie , Dörre Maik 
Published: December 2021

AbstractDie Ermüdungsfestigkeit von Stahlbauschrauben wird maßgeblich von Herstellungseinflüssen beeinflusst. In den Bemessungsgrundlagen werden diese Einflussfaktoren, abhängig vom jeweils herangezogenen Regelwerk, sehr uneinheitlich berücksichtigt. Insbesondere für Schrauben großer Durchmesser, wie sie z. B. bei Windenergieanlagen in hoher Stückzahl zum Einsatz kommen, war eine experimentelle Grundlage zur Bewertung verschiedener Einflüsse in der Vergangenheit nur sehr begrenzt verfügbar. Im Teil 1 des vorliegenden Beitrags wird der bisherige Kenntnisstand dargelegt, der die maßgebenden Einflussgrößen auf die Ermüdungsfestigkeit von Schrauben im Stahlbau beschreibt. Hieraus werden von den Verfassern die Grundlagen zur Bewertung von bestehenden und (242) bislang unveröffentlichten Ergebnissen aus Schwingfestigkeitsuntersuchungen an axial belasteten Schraube‐Mutter‐Verbindungen bis zur Nenngröße M64 abgeleitet, die im Teil 2 dieses Beitrags enthalten sind. Im Vordergrund stehen dabei der Größen‐ und Randschichteinfluss, der Einfluss der Gewindeherstellung sowie der Beanspruchungszustand aus der ziehenden Anziehpraxis.
Zur Ermüdungsfestigkeit großer Schrauben im Stahlbau unter Berücksichtigung von Herstell‐ und Randschichteinflüssen – Teil 2: Versuchsergebnisse und Bewertung
Authors: Glienke Ralf , Schwarz Mathias , Marten Frithjof , Eichstädt Rasmus , Schwerdt Daniela , Meyer Melanie , Dörre Maik 
Published: December 2021

AbstractDie Ermüdungsfestigkeit von Stahlbauschrauben wird maßgeblich von Herstellungseinflüssen beeinflusst. In den Bemessungsgrundlagen werden diese Einflussfaktoren, abhängig vom jeweils herangezogenen Regelwerk, sehr uneinheitlich berücksichtigt. Insbesondere für Schrauben großer Durchmesser, wie sie z. B. bei Windenergieanlagen in hoher Stückzahl zum Einsatz kommen, war eine experimentelle Grundlage zur Bewertung verschiedener Einflüsse in der Vergangenheit nur sehr begrenzt verfügbar. In diesem Beitrag werden Ergebnisse von 20 verschiedenen, größtenteils in der jüngeren Vergangenheit durchgeführten Versuchsserien an drei unterschiedlichen hochfesten Schraubensystemen mit variierenden Herstellungsbedingungen vorgestellt und bewertet. Die Datenbasis streckt sich über einen Durchmesserbereich zwischen M12 und M64 und legt den Fokus auf Versuche mit hohem repräsentativem Mittelspannungsniveau. Die Ergebnisse werden unter Einbeziehung der in der Fachliteratur beschriebenen Erkenntnisse in Bezug auf unterschiedliche Herstellungseinflüsse bewertet und den Regelungen der relevanten internationalen normativen Bemessungsgrundlagen gegenübergestellt. Dabei werden zusätzlich zu den Ergebnissen von Schwingfestigkeitsversuchen ergänzende metallografische Untersuchungen zur Bruchflächengestalt sowie zum Rand‐ und Schutzschichtzustand herangezogen. Auf dieser Basis werden abschließend Handlungsempfehlungen abgeleitet und ein Ausblick auf weitere zielführende Untersuchungen gegeben.
Recent Advances in Processing and Applications of Heterobimetallic Oxide Thin Films by Aerosol‐Assisted Chemical Vapor Deposition
Authors: Ehsan Muhammad Ali , Shah Syed Shaheen , Basha Shaik Inayath , Hakeem Abbas Saeed , Aziz Md. Abdul 
Published: December 2021

AbstractThe fabrication of smart, efficient, and innovative devices critically needs highly refined thin‐film nanomaterials; therefore, facile, scalable, and economical methods of thin films production are highly sought‐after for the sustainable growth of the hi‐tech industry. The chemical vapor deposition (CVD) technique is widely implemented at the industrial level due to its versatile features. However, common issues with a precursor, such as reduced volatility and thermal stability, restrict the use of CVD to produce novel and unique materials. A modified CVD approach, named aerosol‐assisted CVD (AACVD), has been the center of attention due to its remarkable tendency to fabricate uniform, homogenous, and distinct nano‐architecture thin films in an uncomplicated and straightforward manner. Above all, AACVD can utilize any custom‐made or commercially available precursors, which can be transformed into a transparent solution in a common organic solvent; thus, a vast array of compounds can be used for the formation of nanomaterial thin films. This review article highlights the importance of AACVD in fabricating heterobimetallic oxide thin films and their potential in making energy production (e. g., photoelectrochemical water splitting), energy storage (e. g., supercapacitors), and environmental protection (e. g., electrochemical sensors) devices. A heterobimetallic oxide system involves two metallic species either in a composite, solid solution, or metal‐doped metal oxides. Moreover, the AACVD tunable parameters, such as temperature, deposition time, and precursor, which drastically affect thin films microstructure and their performance in device applications, are also discussed. Lastly, the key challenges and issues of scaling up AACVD to the industrial level and processing for emerging functional materials are also highlighted.
Influence of tower shadow on downwind flexible rotors: Field tests and simulations
Authors: Simpson Juliet G. , Kaminski Meghan , Loth Eric 
Published: December 2021

AbstractAs wind turbine rotors become larger, the blades become more flexible, requiring extra stiffness and cost to avoid the risk of tower strike. Wind turbines in a downwind configuration have a reduced risk of tower strike because the rotor thrust acts away from the tower. However, downwind blades pass through the wake of the tower, and the resulting load variation may contribute to blade fatigue. To date, there have been no field tests to quantify this tower shadow effect on unsteady blade moments. The present study reports on the first field testing of a flexible, downwind, coned rotor and compares the experimental data against simulations run in OpenFAST. The tower shadow effect is simulated using the conventional Powles model and a new Eames model (developed herein), which includes the influence of upstream turbulence. Both models reasonably predict the blade root out‐of‐plane bending moment data and the tower shadow dip magnitude when compared to field test data in Region 3. Tower shadow was found to increase the short‐term Damage Equivalent Loads (DELs) by less than 10% compared to other effects (gravity, shear, and turbulence), and the predictions were consistent with experiments. These results indicate that the tower shadow effect can be reasonably modeled with the simpler Powles model and that the tower shadow effect can be small compared to the effect of turbulence. However, long‐term fatigue due to tower shadow should be included in detailed structural analysis and design of the rotor and the tower.
Erklärbarkeit der altersadjustierten Übersterblichkeit mit den COVID-19-attribuierten Sterbefällen von Januar 2020 bis Juli 2021
Authors: Wollschläger Daniel , Schmidtmann Irene , Fückel Sebastian , Blettner Maria , Gianicolo Emilio 
Published: December 2021

Zusammenfassung
Hintergrund
Unsicherheiten in der Todesursachencodierung erschweren die Bestimmung der durch COVID-19 verursachten Mortalität. Dagegen ist die altersadjustierte Übersterblichkeit ein robuster Indikator für Auswirkungen der COVID-19-Pandemie auf die öffentliche Gesundheit. Die Übersterblichkeit spiegelt neben COVID-19-Sterbefällen aber potenziell auch negative Folgen der Maßnahmen zur Pandemieeindämmung wider.

Ziele
Diese Studie prüft, ob es in Deutschland von 01/2020 bis 07/2021 eine Übersterblichkeit gab, die nicht durch COVID-19 erklärbar ist, sondern für indirekte Effekte gesundheitspolitischer Maßnahmen auf die Mortalität spricht.

Methoden
Übersterblichkeitstrends im Zeitraum von 01/2020 bis 07/2021, jeweils in den Bundesländern sowie in den Kreisen von Rheinland-Pfalz, wurden auf Konsistenz mit COVID-19 zugeschriebenen Sterbefällen geprüft. Die erwarteten monatlichen Sterbefälle wurden auf Basis der Daten von 2015 bis 2019 vorhergesagt. Dabei wurden die Bevölkerungsstruktur, Lufttemperatur, saisonale Influenzaaktivität sowie zyklische und langfristige Zeittrends berücksichtigt.

Ergebnisse
In 232/304 (76,3 %) Monat-Bundesland- bzw. in 607/684 (88,7 %) Monat-Kreis-Kombinationen lag die COVID-19 zugeschriebene Mortalität innerhalb der 95 %-Vorhersageintervalle für die Übersterblichkeit. Die Rangkorrelation zwischen Übersterblichkeit und COVID-19-attribuierter Mortalität betrug für die Bundesländer 0,42 (95 %-Konfidenzintervall [0,31; 0,53]) und für die Kreise 0,21 (95 %-Konfidenzintervall [0,13; 0,29]).

Diskussion
Die gute Übereinstimmung der räumlich-zeitlichen Übersterblichkeitsmuster mit den COVID-19 zugeschriebenen Sterbefällen ist konsistent mit der Annahme, dass die Maßnahmen zur Eindämmung der COVID-19-Pandemie zwischen 01/2020 und 07/2021 nicht wesentlich zur Übersterblichkeit in Deutschland beigetragen haben.
Development and application of an in-house library and workflow for gas chromatography–electron ionization–accurate-mass/high-resolution mass spectrometry screening of environmental samples
Authors: Castro Verónica , Quintana José Benito , López-Vázquez Javier , Carro Nieves , Cobas Julio , Bilbao Denis , Cela Rafael , Rodil Rosario 
Published: December 2021

Abstract This work presents an optimized gas chromatography–electron ionization–high-resolution mass spectrometry (GC-EI-HRMS) screening method. Different method parameters affecting data processing with the Agilent Unknowns Analysis SureMass deconvolution software were optimized in order to achieve the best compromise between false positives and false negatives. To this end, an accurate-mass library of 26 model compounds was created. Then, five replicates of mussel extracts were spiked with a mixture of these 26 compounds at two concentration levels (10 and 100 ng/g dry weight in mussel, 50 and 500 ng/mL in extract) and injected in the GC-EI-HRMS system. The results of these experiments showed that accurate mass tolerance and pure weight factor (combination of reverse-forward library search) are the most critical factors. The validation of the developed method afforded screening detection limits in the 2.5–5 ng range for passive sampler extracts and 1–2 ng/g for mussel sample extracts, and limits of quantification in the 0.6–3.2 ng and 0.1–1.8 ng/g range, for the same type of samples, respectively, for 17 model analytes. Once the method was optimized, an accurate-mass HRMS library, containing retention indexes, with ca. 355 spectra of derivatized and non-derivatized compounds was generated. This library (freely available at https://doi.org/10.5281/zenodo.5647960), together with a modified Agilent Pesticides Library of over 800 compounds, was applied to the screening of passive samplers, both of polydimethylsiloxane and polar chemical integrative samplers (POCIS), and mussel samples collected in Galicia (NW Spain), where a total of 75 chemicals could be identified.
Cauda equina syndrome—a practical guide to definition and classification
Authors: Lavy Chris , Marks Paul , Dangas Katerina , Todd Nicholas 
Published: December 2021

Abstract

Purpose
International uniformity of definition and classification are crucial for diagnosis and management of cauda equina syndrome (CES). They are also useful for clinicians when discussing CES with patients and relatives, and for medicolegal purposes.

Methods
We reviewed published literature using PubMed on definition and classification of cauda equina syndrome since 2000 (21 years). Using the search terms ‘cauda equina’ and ‘definition’ or ‘classification’, we found and reviewed 212 papers.

Results
There were 17 different definitions of CES used in the literature. There were three well-defined methods of classification of CES. The two-stage system of incomplete CES (CESI) versus CES with retention (CESR) is the most commonly used classification, and has prognostic value although the details of this continue to be debated.

Conclusion
We used the existing literature to propose a clear definition of CES. We also drew on peer-reviewed published literature that has helped to amplify and expand the CESI/CESR dichotomy, adding categories that are both less severe than CESI, and more severe than CESR, and we propose clear definitions in a table form to assist current and future discussion and management of CES.