bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Mechanistic and Quantitative Understanding of the Interactions between SiO and Graphite Particles
Authors: Gao Xiang , Li Suli , Xue Jiachen , Hu Dianyang , Xu Jun 
Published: November 2022

AbstractSiO, comprised of silicon and silicon dioxides (SiO2), is one of the most commercially promising anode materials to mix with current widely used graphite for the high energy density lithium‐ion batteries (LIBs). One of the major bottlenecks for SiO/Graphite (SiO/Gr) composite anode is the cyclability due to considerable stress and strain (deformation) caused within and among the composite particles. However, a sophisticated and quantitative understanding of the highly electrochemical–mechanical coupling behaviors is still lacking. Herein, an electro–chemo–mechanical model with a detailed geometric description to quantitatively reveal the underlying governing mechanisms of SiO/Gr composite anodes using the half‐cell configuration is established and validated. Results show that an 8–10 wt.% of SiO is an optimal choice regarding capacity delivery and minimizing Li plating under 1C constant current charging condition. Positioning SiO particles near the separator and reducing the sizes of SiO particles are also demonstrated to be beneficial for electrochemical performance with trivial influence on mechanical mismatch. This study highlights a promising multiphysics model for the design and evaluation of next‐generation batteries and unlocks the mechanistic and quantitative understanding of the interactions among composite particles in electrodes.
Revisiting the Role of Hydrogen in Lithium‐Rich Antiperovskite Solid Electrolytes: New Insight in Lithium Ion and Hydrogen Dynamics
Authors: Ling Sifan , Deng Bei , Zhao Ruo , Lin Haibin , Kong Long , Zhang Ruiqin , Lu Zhouguang , Bian Juncao , Zhao Yusheng 
Published: November 2022

AbstractLi2OHX(X= Cl or Br) with an antiperovskite structure possess the advantages of low melting point, low cost, and ease of scaling‐up, which show great promise for applications in all‐solid‐state Li metal batteries (ASSLMBs). However, Li‐ion transport mechanisms in Li2OHXare still debated and the influence of H on the electrochemical performance of Li2OHXis yet to be explored. Herein, combining the theoretical calculations and experimental measurements, it is found that H affects Li‐ion transport, crystal stability, electrochemical stability, and electronic conductivity of Li2OHX. Compared with H‐free Li3OCl, although H helps to generate vacancy‐like defects, the electrostatic repulsive force between H and Li‐ion leads to an increase in both the activation energy and the diffusion length (space compensation effect), resulting in special Li ion transport trajectories along the Li‐O plane. Decreasing H content reduces the electronic conductivity and enhances the reduction‐resistant ability of Li2OHX, promoting the cycling stability and rate performance of Li∣Li2OHX∣Li symmetric cells and the ASSLMBs. This work delivers a new insight into the role of H in antiperovskite Li2OHXand can serve as guidance for solid electrolyte design.
Dual‐Site Functionalization on Supported Metal Monolayer Electrocatalysts for Selective CO2 Reduction
Authors: Zhao Zhonglong , Lu Gang 
Published: November 2022

AbstractDevelopment of efficient catalysts for electrochemical carbon dioxide reduction reaction (CO2RR) represents a great challenge in renewable energy research. Although noble metals have long been explored as catalysts for CO2RR, their reactivity and selectivity remain rather low owing to the competing hydrogen evolution reaction (HER). Here, this work proposes that noble metal monolayers (MLs) supported by transition metal carbides (TMCs) and nitrides (TMNs) can become exceptional CO2RR catalysts with much suppressed HER. This work shows that there is a direct, antibonding interaction between the hydrogen adsorbate and the TMC/TMN substrates, while such interactions between CO2RR intermediates and the substrates are absent. This difference enables dual‐site functionalization of the ML catalysts, which circumvents the energy scaling relations dictating the competition between CO2RR and HER. Consequently, it is possible to reduce the binding of the H adsorbate to suppress HER and simultaneously increase the binding of CO2RR intermediates to boost the CO2RR. This work identifies several Ag and Au‐based catalysts that are thermodynamically and electrochemically stable and exhibit high activity and selectivity toward the production of formic acid. In addition, this work predicts that higher order CO2RR products including methanol and ethylene can also be produced on selected catalysts.
Pulse High Temperature Sintering to Prepare Single‐Crystal High Nickel Oxide Cathodes with Enhanced Electrochemical Performance
Authors: Huang Hao , Zhang Lipeng , Tian Huayang , Yan Junqing , Tong Junfan , Liu Xiaohang , Zhang Haoxuan , Huang Heqin , Hao Shu‐meng , Gao Jian , Yu Le , Li Hong , Qiu Jieshan , Zhou Weidong 
Published: November 2022

AbstractFor the currently most dominant cathode of Li(NixCoyMnz)O2(NCM, x + y + z = 1) in lithium‐ion batteries, higher nickel content brings higher energy density but is accompanied by heavier interfacial reactions with electrolyte and worse safety performance. Single crystal cathode materials have the advantages of fewer grain boundaries, higher density, and greatly suppressed microcracks during cycling, these benefits in turn suppress interfacial side reactions, as well as the improve volumetric energy density and safety performance. Here, a strategy of pulse high‐temperature sintering (PHTS) is reported to prepare single‐crystal Li(Ni0.9Co0.05Mn0.05)O2 (SC‐NCM90), in which an extra PHTS at 1040 °C for 1 min is added in the traditional calcination process at 750 °C, yielding well defined octahedral particles with an initial capacity of 209 mAh g−1. Compared with the counterpart NCM90 secondary spheres, the tap density of SC‐NCM90 increases by 1/3 to 2.76 g cm−3 and the microcracks are successfully suppressed, improving both the cycling performance and thermal stability. The calcination time and temperature are optimized, showing that overlong time or overhigh temperature of the PHTS treatment would result in particles with better defined octahedral shape but heavier Li/Ni intermixing and capacity loss.
Duration of employment within occupations and incident stroke in a US general population cohort 45 years of age or older (REGARDS study)
Authors: Huynh Tran B. , McClure Leslie A. , Howard Virginia J. , Stafford Monika M. , Judd Suzanne E. , Burstyn Igor 
Published: November 2022

AbstractBackgroundThe work environment can contribute to the risk of cardiovascular diseases (CVD) including stroke. Our objective was to identify occupations with elevated risk of stroke within the Reasons for Geographic and Racial Differences in Stroke (REGARDS) cohort.MethodsWe analyzed incident stroke outcomes (ischemic and hemorrhagic strokes) from 2003 to 2020 and employment characteristics of 13,659 adults aged ≥45 years enrolled in a national population‐based cohort study. Using a modified Poisson regression approach, we estimated the relative risks (RRs) and the associated 95% confidence intervals (CI) of stroke in relation to years of employment within each occupation coded using the US Census two‐digit Standard Occupation Code. Models were adjusted for Framingham Stroke Risk Score, region, race, age, and body mass index. We conducted stratified analysis by sex, employment time period (pre‐1975 vs. post‐1975), and region.ResultsWorkers in the following occupations had a greater risk of stroke with longer duration of employment (per decade): protective service (RR: 2.35, 95% CI: 1.11, 4.97), food preparation and service (RR: 1.51, 95% CI: 1.05, 2.19), and transportation and material moving (RR: 1.30, 95% CI: 1.00, 1.69). The stroke risk in these occupations was disproportionately elevated in men, and differed by region and employment time period.ConclusionsLonger employment in protective service, food preparation and serving, and transportation and materials moving occupations may increase the risk of stroke. Surveillance may uncover specific work‐related risk factors in these occupations, leading to interventions to reduce the burden of stroke among US workers.
Personal social networks of people with Down syndrome
Authors: Skotko Brian G. , Krell Kavita , Haugen Kelsey , Torres Amy , Nieves Amber , Dhand Amar 
Published: November 2022

AbstractStudies in the neurotypical population have demonstrated that personal social networks can mitigate cognitive decline and the development of Alzheimer disease. To assess whether these benefits can also be extended to people with Down syndrome (DS), we studied whether and how personal networks can be measured in this population. We adapted a personal networks instrument previously created, validated, and implemented for the neurotypical population. We created two versions of the survey: one for participants with DS, ages 25 and older, and another for their study partners, who spent a minimum of 10 h/wk in a caregiver role. Participants with DS gave concordant data to those of study partners. Their personal networks included a median network size of 7.50, density 0.80, constraint 46.00, and effective size 3.07. Personal networks were composed of 50% kin, 80% who live within 15 miles, and 80% who eat a healthy diet. In this proof‐of‐principle study, we demonstrated that the personal networks of people with DS can be quantitatively analyzed, with no statistical difference between self‐report and parent‐proxy report. Future research efforts can now evaluate interventions to enhance personal networks for preventing Alzheimer disease in this population.
Expanding the Toolbox of Target Directed Bio‐Orthogonal Synthesis: In Situ Direct Macrocyclization by DNA Templates
Authors: Chaudhuri Ritapa , Prasanth Thumpati , Dash Jyotirmayee 
Published: November 2022

AbstractHerein, we demonstrate for the first time that noncanonical DNA can direct macrocyclization‐like challenging reactions to synthesize gene modulators. The planar G‐quartets present in DNA G‐quadruplexes (G4s) provide a size complementary reaction platform for the bio‐orthogonal macrocyclization of bifunctional azide and alkyne fragments over oligo‐ and polymerization. G4s immobilized on gold‐coated magnetic nanoparticles have been used as target templates to enable easy identification of a selective peptidomimetic macrocycle. Structurally similar macrocycles have been synthesized to understand their functional role in the modulation of gene function. The innate fluorescence of the in situ formed macrocycle has been utilized to monitor its cellular localization using a G4 antibody and its in cell formation from the corresponding azide and alkyne fragments. The successful execution of in situ macrocyclization in vitro and in cells would open up a new dimension for target‐directed therapeutic applications.
Manipulating OH−‐Mediated Anode‐Cathode Cross‐Communication Toward Long‐Life Aqueous Zinc‐Vanadium Batteries
Authors: Liu Dao‐Sheng , Zhang Zhaoyu , Zhang Yufei , Ye Minghui , Huang Song , You Shunzhang , Du Zijian , He Jiangfeng , Wen Zhipeng , Tang Yongchao , Liu Xiaoqing , Li Cheng Chao 
Published: November 2022

AbstractThe anode‐cathode interplay is an important but rarely considered factor that initiates the degradation of aqueous zinc ion batteries (AZIBs). Herein, to address the limited cyclability issue of V‐based AZIBs, Al2(SO4)3 is proposed as decent electrolyte additive to manipulate OH−‐mediated cross‐communication between Zn anode and NaV3O8 ⋅ 1.5H2O (NVO) cathode. The hydrolysis of Al3+ creates a pH≈0.9 strong acidic environment, which unexpectedly prolongs the anode lifespan from 200 to 1000 h. Such impressive improvement is assigned to the alleviation of interfacial OH− accumulation by Al3+ adsorption and solid electrolyte interphase formation. Accordingly, the strongly acidified electrolyte, associated with the sedated crossover of anodic OH− toward NVO, remarkably mitigate its undesired dissolution and phase transition. The interrupted OH−‐mediated communication between the two electrodes endows Zn||NVO batteries with superb cycling stability, at both low and high scan rates.
Parahydrogen‐Induced Carbon‐13 Radiofrequency Amplification by Stimulated Emission of Radiation
Authors: Nelson Christopher , Schmidt Andreas B. , Adelabu Isaiah , Nantogma Shiraz , Kiselev Valerij G. , Abdurraheem Abubakar , de Maissin Henri , Lehmkuhl Sören , Appelt Stephan , Theis Thomas , Chekmenev Eduard Y. 
Published: November 2022

AbstractThe feasibility of Carbon‐13 Radiofrequency (RF) Amplification by Stimulated Emission of Radiation (C‐13 RASER) is demonstrated on a bolus of liquid hyperpolarized ethyl [1‐13C]acetate. Hyperpolarized ethyl [1‐13C]acetate was prepared via pairwise addition of parahydrogen to vinyl [1‐13C]acetate and polarization transfer from nascent parahydrogen‐derived protons to the carbon‐13 nucleus via magnetic field cycling yielding C‐13 nuclear spin polarization of approximately 6 %. RASER signals were detected from samples with concentration ranging from 0.12 to 1 M concentration using a non‐cryogenic 1.4T NMR spectrometer equipped with a radio‐frequency detection coil with a quality factor (Q) of 32 without any modifications. C‐13 RASER signals were observed for several minutes on a single bolus of hyperpolarized substrate to achieve 21 mHz NMR linewidths. The feasibility of creating long‐lasting C‐13 RASER on biomolecular carriers opens a wide range of new opportunities for the rapidly expanding field of C‐13 magnetic resonance hyperpolarization.
A Novel Electrode for Value‐Generating Anode Reactions in Water Electrolyzers at Industrial Current Densities
Authors: Wang Changlong , Wu Yufeng , Bodach Alexander , Krebs Moritz Lukas , Schuhmann Wolfgang , Schüth Ferdi 
Published: November 2022

AbstractHydrogen generated in electrolyzers is discussed as a key element in future energy scenarios, but oxygen evolution as the standard anode reaction is a complex multi‐step reaction requiring a high overpotential. At the same time,it does not add value‐the oxygen is typically released into the atmosphere. Alternative anode reactions which can proceed at similar current densities as the hydrogen evolution are, therefore, of highest interest. We have discovered a high‐performance electrode based on earth‐abundant elements synthesized in the presence of H2O2, which is able to sustain current densities of close to 1 A cm−2 for the oxidation of many organic molecules, which are partly needed at high production volumes. Such anode reactions could generate additional revenue streams, which help to solve one of the most important problems in the transition to renewable energy systems, i.e. the cost of hydrogen electrolysis.
Upconversion Luminescence through Cooperative and Energy‐Transfer Mechanisms in Yb3+‐Metal‐Organic Frameworks
Authors: Xie Yao , Sun Guotao , Mandl Gabrielle A. , Maurizio Steven L. , Chen Jiabo , Capobianco John A. , Sun Lining 
Published: November 2022

AbstractLanthanide‐doped metal–organic frameworks (Ln‐MOFs) have versatile luminescence properties, however it is challenging to achieve lanthanide‐based upconversion luminescence in these materials. Here, 1,3,5‐benzenetricarboxylic acid (BTC) and trivalent Yb3+ions were used to generate crystalline Yb‐BTC MOF 1D‐microrods with upconversion luminescence under near infrared excitation via cooperative luminescence. Subsequently, the Yb‐BTC MOFs were doped with a variety of different lanthanides to evaluate the potential for Yb3+‐based upconversion and energy transfer. Yb‐BTC MOFs doped with Er3+, Ho3+, Tb3+, and Eu3+ions exhibit both the cooperative luminescence from Yb3+and the characteristic emission bands of these ions under 980 nm irradiation. In contrast, only the 497 nm upconversion emission band from Yb3+is observed in the MOFs doped with Tm3+, Pr3+, Sm3+, and Dy3+. The effects of different dopants on the efficiency of cooperative luminescence were established and will provide guidance for the exploitation of Ln‐MOFs exhibiting upconversion.
Mapping the Complete Photocycle that Powers a Large Stokes Shift Red Fluorescent Protein
Authors: Wang Ziyu , Zhang Ya , Chen Cheng , Zhu Ruixue , Jiang Jiaming , Weng Tsu‐Chien , Ji Quanjiang , Huang Yifan , Fang Chong , Liu Weimin 
Published: November 2022

AbstractLarge Stokes shift (LSS) red fluorescent proteins (RFPs) are highly desirable for bioimaging advances. The RFP mKeima, with coexisting cis‐ and trans‐isomers, holds significance as an archetypal system for LSS emission due to excited‐state proton transfer (ESPT), yet the mechanisms remain elusive. We implemented femtosecond stimulated Raman spectroscopy (FSRS) and various time‐resolved electronic spectroscopies, aided by quantum calculations, to dissect the cis‐ and trans‐mKeima photocycle from ESPT, isomerization, to ground‐state proton transfer in solution. This work manifests the power of FSRS with global analysis to resolve Raman fingerprints of intermediate states. Importantly, the deprotonated trans‐isomer governs LSS emission at 620 nm, while the deprotonated cis‐isomer's 520 nm emission is weak due to an ultrafast cis‐to‐trans isomerization. Complementary spectroscopic techniques as a table‐top toolset are thus essential to study photochemistry in physiological environments.
Innovative Electrochemical Strategies for Hydrogen Production: From Electricity Input to Electricity Output
Authors: Yan Dafeng , Mebrahtu Chalachew , Wang Shuangyin , Palkovits Regina 
Published: November 2022

AbstractRenewable H2 production by water electrolysis has attracted much attention due to its numerous advantages. However, the energy consumption of conventional water electrolysis is high and mainly driven by the kinetically inert anodic oxygen evolution reaction. An alternative approach is the coupling of different half‐cell reactions and the use of redox mediators. In this review, we, therefore, summarize the latest findings on innovative electrochemical strategies for H2 production. First, we address redox mediators utilized in water splitting, including soluble and insoluble species, and the corresponding cell concepts. Second, we discuss alternative anodic reactions involving organic and inorganic chemical transformations. Then, electrochemical H2 production at both the cathode and anode, or even H2 production together with electricity generation, is presented. Finally, the remaining challenges and prospects for the future development of this research field are highlighted.
Halogen‐Bonding Heteroditopic [2]Catenanes for Recognition of Alkali Metal/Halide Ion Pairs
Authors: Tay Hui Min , Tse Yuen Cheong , Docker Andrew , Gateley Christian , Thompson Amber L. , Kuhn Heike , Zhang Zongyao , Beer Paul D. 
Published: November 2022

AbstractThe first examples of halogen bonding (XB) heteroditopic homo[2]catenanes were prepared by discrete Na+ template‐directed assembly of oligo(ethylene glycol) units derived from XB donor‐containing macrocycles and acyclic bis‐azide precursors, followed by a CuI‐mediated azide‐alkyne cycloaddition macrocyclisation reaction. Extensive 1H NMR spectroscopic studies show the [2]catenane hosts exhibit positive cooperative ion‐pair recognition behaviour, wherein XB‐mediated halide recognition is enhanced by alkali metal cation pre‐complexation. Notably, subtle changes in the catenanes’ oligo(ethylene glycol) chain length dramatically alters their ion‐binding affinity, stoichiometry, complexation mode, and conformational dynamics. Solution‐phase and single‐crystal X‐ray diffraction studies provide evidence for competing host‐separated and direct‐contact ion‐pair binding modes. We further demonstrate the [2]catenanes are capable of extracting solid alkali‐metal halide salts into organic media.
How Crystal Symmetry Dictates Non‐Local Vibrational Circular Dichroism in the Solid State
Authors: Jähnigen Sascha , Le Barbu‐Debus Katia , Guillot Régis , Vuilleumier Rodolphe , Zehnacker Anne 
Published: November 2022

AbstractSolid‐State Vibrational Circular Dichroism (VCD) can be used to determine the absolute structure of chiral crystals, but its interpretation remains a challenge in modern spectroscopy. In this work, we investigate the effect of a twofold screw axis on the solid‐state VCD spectrum in a combined experimental and theoretical analysis of P21 crystals of (S)‐(+)‐1‐indanol. Even though the space group is achiral, a single proper symmetry operation has an important impact on the VCD spectrum, which reflects the supramolecular chirality of the crystal. Distinguishing between contributions originating from molecular chirality and from chiral crystal packing, we find that while IR absorption hardly depends on the symmetry of the space group, the situation is different for VCD, where completely new non‐local patterns emerge. Understanding the two underlying mechanisms, namely gauge transport and direct coupling, will help to use VCD to distinguish polymorphic forms.
Crystalline Unipolymer Monolayer with High Modulus and Conductivity
Authors: Wang Jinxin , Zhang Hao , Li Shumu , Ding Caijun , Zhao Yongjie , Long Xiuzhen , Wei Chang , Wang Yanfang , Li Yongfang , Shen Lingyun , Cui Shuxun , Hong Wenjing , Li Mao 
Published: November 2022

AbstractThe synthesis of crystalline polymer with a well‐defined orientated state and a two‐dimensional crystalline size beyond a micrometer will be essential to achieve the highest physical feature of polymer material but remain challenging. Herein, we show the synthesis of the crystalline unipolymer monolayer with an unusual ultrahigh modulus that is higher than the ITO substrate and high conductance by simultaneous electrosynthesis and manipulation. We find that the polymer monolayer has fully extended in the vertical and unidirectional orientation, which is proposed to approach their theoretically highest density, modulus, and conductivity among all aggregation formations of the current polymer. The modulus and current density can reach 40 and 1000 times higher than their amorphous counterpart. It is also found that these monolayers exhibit the bias‐ and length‐dependent multiple charge states and asymmetrically negative differential resistance (NDR) effect, indicating that this unique molecular tailoring and ordering design is promising for multilevel resistive memory devices. Our work demonstrates the creation of a crystalline polymer monolayer for approaching the physical limit of polymer electronic materials and also provides an opportunity to challenge the synthetically iterative limit of an isolated ultra‐long polymer.
Results of the 2022 AORN Salary and Compensation Survey
Authors: Bacon Donald R. , Stewart Kim A. 
Published: November 2022

ABSTRACTAORN conducted its 20th annual compensation survey for perioperative nurses in June of 2022. A multiple regression model was used to examine how several variables, including job title, education level, certification, experience, and geographic region, affect perioperative nurse compensation. Comparisons between the 2022 data and data from previous years are presented. The effects of other forms of compensation (eg, on‐call compensation, overtime, bonuses, shift differentials, benefits) on total compensation are also examined. Additional analyses explore the current state of the nursing shortage and the sources of job satisfaction and dissatisfaction.