bluuebunny/crossref_metadata_2025_split huggingface dataset:
Emerging Applications of Solid Catalysts with Ionic Liquid Layer Concept in Electrocatalysis
Authors: Zhang Gui‐Rong , Etzold Bastian J. M. 
Published: May 2021

AbstractThe concept of solid catalysts with ionic liquid layer (SCILL) originates from the field of heterogeneous catalysis, where it offers a unique way to regulate both the catalytic activity and selectivity. In recent years, applying this concept in electrocatalysis represented a new, exciting, and growing research field. Herein, emerging applications of the SCILL concept in the context of electrocatalysis for key energy storage/conversion processes such as oxygen reduction, oxygen evolution, and CO2 reduction reactions are comprehensively reviewed. Alongside case studies highlighting the history, development and latest progress of the SCILL concept, mechanistic underpinnings on the roles of ILs in each application are critically discussed. At the same time, the key challenges and future opportunities in fully leveraging the SCILL concept for either regulating the performance of electrocatalysts or gaining mechanistic understandings for those electrocatalytic processes with complex reaction pathways are outlined.
Surpassing 13% Efficiency for Polythiophene Organic Solar Cells Processed from Nonhalogenated Solvent
Authors: Xiao Jingyang , Jia Xiao'e , Duan Chunhui , Huang Fei , Yip Hin‐Lap , Cao Yong 
Published: May 2021

AbstractBenefiting from low cost and simple synthesis, polythiophene (PT) derivatives are one of the most popular donor materials for organic solar cells (OSCs). However, polythiophene‐based OSCs still suffer from inferior power conversion efficiency (PCE) than those based on donor–acceptor (D–A)‐type conjugated polymers. Herein, a fluorinated polythiophene derivative, namely P4T2F‐HD, is introduced to modulate the miscibility and morphology of the bulk heterojunction (BHJ)‐active layer, leading to a significant improvement of the OSC performance. The Flory–Huggins interaction parameters calculated from the surface energy and differential scanning calorimetry results suggest that P4T2F‐HD shows moderate miscibility with the popular nonfullerene acceptor Y6‐BO (2,2′‐((2Z,2′Z)‐((12,13‐bis(2‐butyloctyl)‐3,9‐diundecyl‐12,13‐dihydro‐[1,2,5]thiadiazolo[3,4‐e]thieno[2′,3′:4′,5′]thieno[2′,3′:4,5]pyrrolo[3,2‐g]thieno[2′,3′:4,5]thieno[3,2‐b]indole‐2,10‐diyl)bis(methanylylidene))bis(5,6‐difluoro‐3‐oxo‐2,3‐dihydro‐1H‐indene‐2,1‐diylidene))dimalononitrile), while poly(3‐hexylthiophene) (P3HT) is very miscible with Y6‐BO. As a result, the P4T2F‐HD case forms desired nanoscale phase separation in the BHJ film while the P3HT case forms a completely mixed BHJ film, as revealed by transmission electron microscopy (TEM) and grazing‐incidence wide‐angle X‐ray scattering (GIWAXS). By optimizing the cathode interface and the morphology of the P4T2F‐HD:Y6‐BO films processed from nonhalogenated solvents, a new record PCE of 13.65% for polythiophene‐based OSCs is demonstrated. This work highlights the importance of controlling D/A interactions for achieving desired morphology and also demonstrates a promising OSC system for potential cost‐effective organic photovoltaics.
Dual‐Solvent Li‐Ion Solvation Enables High‐Performance Li‐Metal Batteries
Authors: Wang Hansen , Yu Zhiao , Kong Xian , Huang William , Zhang Zewen , Mackanic David G. , Huang Xinyi , Qin Jian , Bao Zhenan , Cui Yi 
Published: May 2021

AbstractNovel electrolyte designs to further enhance the lithium (Li) metal battery cyclability are highly desirable. Here, fluorinated 1,6‐dimethoxyhexane (FDMH) is designed and synthesized as the solvent molecule to promote electrolyte stability with its prolonged –CF2– backbone. Meanwhile, 1,2‐dimethoxyethane is used as a co‐solvent to enable higher ionic conductivity and much reduced interfacial resistance. Combining the dual‐solvent system with 1 m lithium bis(fluorosulfonyl)imide (LiFSI), high Li‐metal Coulombic efficiency (99.5%) and oxidative stability (6 V) are achieved. Using this electrolyte, 20 µm Li||NMC batteries are able to retain ≈80% capacity after 250 cycles and Cu||NMC anode‐free pouch cells last 120 cycles with 75% capacity retention under ≈2.1 µL mAh−1 lean electrolyte conditions. Such high performances are attributed to the anion‐derived solid‐electrolyte interphase, originating from the coordination of Li‐ions to the highly stable FDMH and multiple anions in their solvation environments. This work demonstrates a new electrolyte design strategy that enables high‐performance Li‐metal batteries with multisolvent Li‐ion solvation with rationally optimized molecular structure and ratio.
Laser‐Scanning‐Guided Assembly of Quasi‐3D Patterned Arrays of Plasmonic Dimers for Information Encryption
Authors: Yang Fan , Ye Shunsheng , Dong Wenhao , Zheng Di , Xia Yifan , Yi Chenglin , Tao Jing , Sun Chang , Zhang Lei , Wang Lu , Chen QianYun , Wang Yazi , Nie Zhihong 
Published: May 2021

AbstractThe application of plasmonic dimeric nanostructures in color displays, data storage, and especially metamaterials necessitates the patterning of dimers into ordered arrays, but controllable assembly of plasmonic nanoparticles into patterned dimer arrays on substrates still remains a challenge. Here, a facile laser‐scanning‐based strategy to fabricate quasi‐3D patterned arrays of plasmonic nanoparticle dimers with controlled orientation for plasmonic information encryption is reported. Laser scanning of polymer‐covered plasmonic nanoparticle (e.g., gold) arrays selectively exposes the surface of irradiated nanoparticle via localized photothermal heating, guiding the assembly of another type of nanoparticles onto the exposure nanoparticle surface to form dimers on substrates. This combined top‐down/bottom‐up approach is highly flexible in forming high‐resolution patterns of plasmonic dimers from nanoparticles of different sizes and shapes. The z‐axis orientation, interparticle spacing, and nanoparticle size and shape of plasmonic dimers can be precisely tuned, enabling the modulation of the coupled resonances of the dimer arrays. Moreover, it is demonstrated that the patterned dimer arrays can be used in information encryption where their plasmonic color can be repeatedly displayed and erased. This work provides an important addition to tools for the fabrication of patterned complex plasmonic nanostructures from as‐synthesized nanoparticles with broad applications.
K‐Ion Battery Cathode Design Utilizing Trigonal Prismatic Ligand Field
Authors: Wu Nanzhong , Zhou Xiaolong , Kidkhunthod Pinit , Yao Wenjiao , Song Tianyi , Tang Yongbing 
Published: May 2021

AbstractThe intrinsic physical and chemical properties of materials are largely governed by the bonding and electronic structures of their fundamental building units. The majority of cathode materials contain octahedral TMO6 (TM = transition metal), which dominates the redox chemistry during electrochemical operation. As a less symmetric form of TMO6, the trigonal prismatic geometry is not a traditionally favored coordination configuration as it tends to lose the crystal‐field stabilization energy and thus generate large ligand repulsion. Herein, a K‐ion battery cathode design, K2Fe(C2O4)2, is shown​, where the TMO6 trigonal prism (TP) is not only electrochemically active but stable enough to allow for excellent cycling stability. Detailed synchrotron X‐ray absorption spectroscopy measurements reveal the evolution of localized fine structure, evidencing the electrochemical activity, reversibility, and stability of the TP motif. The findings are expected to expand the toolbox for the rational design of electrode materials by taking advantage of TP as a structural gene.
Impact of Hierarchization on the Textural Properties of MCM‐22 Based Zeolites
Authors: Sachse Alexander , Aumond Thibaud , Rousseau Julie , Batonneau‐Gener Isabelle 
Published: May 2021

AbstractThe impact of zeolite hierarchization is often highlighted in terms of increased mesopore volume or specific surface area and preservation of micropore volume. Yet, although these targets may be achieved, the accessibility to certain micropores might be negatively affected during hierarchization. A set of hierarchical MCM‐22 based materials is prepared based on desilication treatments of MCM‐22, of the layered precursor MCM‐22(P) and of the hexadecyltrimethylammonium bromide (CTAB) swollen precursor swMCM‐22(P), and by the pillaring of swMCM‐22(P) leading to MCM‐36. A new methodology is presented based on comparing the micropore volume of pristine materials with their n‐nonane retaining counterparts. A definition of the accessible micropore volume fraction is given, which relates to the amount of surface 12‐MR cups. This approach hence allows quantifying which type of microporosity is preferentially destroyed during hierarchization treatments of MCM‐22. Besides comparing the development of mesoporosity, specific surface area, and the evolution of micropore volume during hierarchization treatments, the accessible micropore volume fraction allows for a distinct definition of the hierarchization quality for MCM‐22 based materials. Despite an important increase in interlayer‐mesopore volume and specific surface area for MCM‐36, the accessible micropore volume fraction is found to be just 3% higher than for MCM‐22.
Intramolecular Through‐Space Charge Transfer Based TADF‐Active Multifunctional Emitters for High Efficiency Solution‐Processed OLED
Authors: Li Bing , Yang Zhan , Gong Wenqi , Chen Xinhui , Bruce Duncan W. , Wang Shengyue , Ma Huili , Liu Yu , Zhu Weiguo , Chi Zhenguo , Wang Yafei 
Published: May 2021

AbstractThermally activated delayed fluorescence (TADF) has been explored actively in luminescent organic materials. Yet, realizing such TADF‐active, multifunctional emitters with high emission efficiency still remains hugely challenging. In this context, a series of twist‐conjugated organic molecules bearing diphenylsulfone and 9,9‐dimethylacridine moieties are designed and prepared, and are found to show, in one molecule, TADF, room‐temperature phosphorescence, triboluminescence, and aggregation‐induced emission enhancement. In addition, remarkably high photoluminescence quantum efficiency, up to ≈100%, is achieved for these novel molecules. Single‐crystal analysis and theoretical calculations reveal that the through‐space charge transfer (TSCT) effect in these molecules is responsible for both the multifunctional emission and high emission efficiency. A maximum external quantum efficiency of 20.1% is achieved, which is among the highest recorded in a solution‐processable device containing TSCT‐based TADF materials. These results illustrate a new approach to achieving highly efficient TADF‐active, multifunctional emitters.
Enhanced Ferroelectric Properties in Hf0.5Zr0.5O2 Films Using a HfO0.61N0.72 Interfacial Layer
Authors: Kim Beom Yong , Park Hyeon Woo , Hyun Seung Dam , Lee Yong Bin , Lee Suk Hyun , Oh Minsik , Ryoo Seung Kyu , Lee In Soo , Byun Seungyong , Shim Doosup , Cho Deok‐Yong , Park Min Hyuk , Hwang Cheol Seong 
Published: May 2021

AbstractFluorite structured ferroelectrics, such as (Hf, Zr)O2, attract much interest due to their scalability and compatibility with complementary metal‐oxide semiconductors, which make them superior to the conventional ferroelectrics. However, their reliability issues, including their limited endurance, are yet to be resolved. Such issues have been reported to be strongly correlated to the formation and drift of oxygen vacancies concentrated in the interfacial region adjacent to TiN electrodes. In this study, the effect of inserting a sacrificial HfO0.61N0.72 interfacial layer between a TiN bottom electrode and a ferroelectric Hf0.5Zr0.5O2 thin film is investigated. The insertion of the 2 nm‐thick HfO0.61N0.72 interfacial layer decreases the inclusion of the undesirable non‐ferroelectric phase by ≈60% and increases the remanent polarization by more than 30%. The reaction barrier property of the sacrificial HfO0.61N0.72 layer significantly enhances the reliability of the Hf0.5Zr0.5O2 film, and thus, improves the endurance of the film beyond 1.5 × 1011 switching cycles. This is the highest endurance among the reported values for fluorite‐structured ferroelectrics with the remanent polarization kept higher than 10 µC cm‐2.
Transcranial color‐coded duplex sonography reliably identifies intracranial vasculopathy in adult patients with sickle cell disease
Authors: Edjlali Myriam , Gobin‐Metteil Marie‐Pierre , Mélé Nicolas , Maïer Benjamin , Habibi Anoosha , Kauv Paul , Hosseini Hassan , Mas Jean‐Louis , Oppenheim Catherine , Galactéros Frédéric , Bartolucci Pablo , Calvet David 
Published: May 2021

AbstractIn order to prevent stroke, screening for disease‐related intracranial vasculopathy using Doppler ultrasound is recommended in sickle‐cell disease (SCD) children. How to screen such vasculopathy in adults remains largely unknown. The objective of this study was to assess whether transcranial color‐coded duplex sonography (TCCD) is sensitive and specific enough to identify SCD adult patients with vasculopathy, compared with magnetic resonance angiography (MRA). Sickle cell disease adults followed in referral centers at high risk of vasculopathy were included in this study. Transcranial color‐coded duplex sonography examination and 3‐D time‐of‐flight MRA were performed on the same day. On MRA, vasculopathy was defined by the presence of at least one ≥50% arterial stenosis. On TCCD, vasculopathy was defined by a time‐averaged mean of the maximum velocity (TAMx) stenotic/prestenotic ratio ≥ 3, an occlusion, or a Moyamoya pattern. Vasculopathy was also considered as present when TAMx ratio could not be calculated because of the presence of severe cervical lesions. Among 80 included patients, quality of MRA was insufficient in three patients. Among the 38 patients with vasculopathy on MRA, 37 had a vasculopathy according to TCCD criteria: TAMx ratio ≥ 3 or intracranial occlusion in 33 patients and cervical lesion in four patients. A Moyamoya pattern was identified with TCCD in all 17 patients with Moyamoya on MRA. Sensitivity and specificity of TCCD to identify patients with ≥50% vasculopathy on MRA were (n = 37/38) 97% and (n = 28/34) 82%, respectively. Positive and negative predictive values were (n = 37/43) 86% and (n = 28/29) 97%, respectively. Note, TCCD may be used to identify SCD adult patients with vasculopathy.
Reproductive males are effective at managing conflict in captive Sulawesi crested macaques (Macaca nigra)
Authors: Cowl Veronica B. , Walker Susan L. , Shultz Susanne 
Published: May 2021

AbstractGroup size, density, and composition significantly influence the expression of agonism and, as demography is frequently manipulated in captivity, natural mechanisms of conflict management may be disrupted. Here, we examine how changes to the social and physical environment of a captive group of Sulawesi crested macaques,Macaca nigra, influenced mechanisms of conflict management. The initial group was comprised of females, juveniles, and castrated males; under a series of management interventions, the group was moved to a new enclosure, 75% of the castrated adult males were removed, 67% of the females were contracepted, a novel, intact male was introduced, and the group was allowed access to an outdoor enclosure. Despite a decreasing trend in aggression following the changes to the social group, we found no significant differences in aggression or intervention behavior in the 5‐week periods immediately following changes to the social group, apart from a significant decrease in aggression following the introduction of the novel male. This decrease in the frequency of aggression was still evident 10 weeks after the interventions occurred, and was coupled with a decrease in the intensity of aggression. Moreover, the intensity of aggression as well as the frequency of aggression and intervention were significantly lower under low‐density conditions. Our results highlight how management changes to the social and physical environment can influence aggressive behavior, albeit following a period of acclimation. We discuss the relative impacts of social group composition, social density, and individual reproductive status on the management of conflict behavior in a captive setting.
Performance of shear wave elastography: A single centre pilot study of mixed etiology liver disease patients with normal BMI
Authors: Laroia Shalini Thapar , Vellore Srinivasan Shyam , Yadav Komal , Rastogi Archana , Kumar Senthil , Kumar Guresh , Kumar Manoj 
Published: May 2021

AbstractPurposeTo assess the performance of shear wave ultrasound elastography (SWE) for non‐invasive grading of fibrosis in normal BMI patients with varied aetiology chronic liver disease.MethodProspective SWE liver and spleen stiffness (LS, SS respectively) of 124 patients (94 men, mean age 45.4 ± 12.4 years, mean BMI 19.66 ± 1.49) with CLD of mixed aetiology, who underwent liver biopsy, between January 2019–20 was analysed using receiver operating curve (ROC) and classification analysis regression tree (CART) to determine fibrosis cut‐off values and nominal logistical regression to quantify fibrosis.ResultsOf 124 patients, 50 (40%) had non‐alcoholic steatohepatitis (NASH), 31 (25%) chronic hepatitis B (CHB) and 43 (35%) alcoholic liver disease (ALD) on biopsy. Overall mean LS and SS of the study population was 11.81 ± 5.9 and 16.88 ± 10.8 kPa, respectively. LS cut‐off value <8 kPa was consistent with F0, 9–14 kPa for F1‐F2 and >14.9 kPa for F3‐F4 fibrosis on biopsy. On application of CART, LS value < 5.3 kPa was discriminative for NASH, 5.32 to <12.64 kPa for CHB, >12.64 kPa for ALD, SS <15.3 kPa was discriminative for NASH, 15.3–30 kPa for CHB and >30 kPa for ALD in our study population.ConclusionSWE is a viable non‐invasive tool for assessment of liver fibrosis grading in a population of mixed aetiology CLD. LS values in conjunction with SS are promising predictors of F2‐F3 fibrosis with potential to discriminate select categories like CHB and NASH in such a population.
Adaptive Bayesian phase I clinical trial designs for estimating the maximum tolerated doses for two drugs while fully utilizing all toxicity information
Authors: Zhang Yuzi , Kutner Michael , Chen Zhengjia 
Published: May 2021

AbstractThe combined treatments with multiple drugs are very common in the contemporary medicine, especially for medical oncology. Therefore, we developed a Bayesian adaptive Phase I clinical trial design entitled escalation with overdoing control using normalized equivalent toxicity score for estimating maximum tolerated dose (MTD) contour of two drug combination (EWOC‐NETS‐COM) used for oncology trials. The normalized equivalent toxicity score (NETS) as the primary endpoint of clinical trial is assumed to follow quasi‐Bernoulli distribution and treated as quasi‐continuous random variable in the logistic linear regression model which is used to describe the relationship between the doses of the two agents and the toxicity response. Four parameters in the dose–toxicity model were re‐parameterized to parameters with explicit clinical meanings to describe the association between NETS and doses of two agents. Noninformative priors were used and Markov chain Monte Carlo was employed to update the posteriors of the four parameters in dose–toxicity model. Extensive simulations were conducted to evaluate the safety, trial efficiency, and MTD estimation accuracy of EWOC‐NETS‐COM under different scenarios, using the EWOC as reference. The results demonstrated that EWOC‐NETS‐COM not only efficiently estimates MTD contour of multiple drugs but also provides better trial efficiency by fully utilizing all toxicity information.
Blood pressure in dementia, mild cognitive impairment, and subjective cognitive decline related to time of death
Authors: Hestad Knut Asbjørn , Engedal Knut , Selbæk Geir , Strand Bjørn Heine 
Published: May 2021

AbstractObjectiveIt is unknown whether systolic blood pressure (SBP) drop is part of the normal aging process or due to the onset of dementia for some people. SBP drop is referring to the decrease in blood pressure often seen before death. Thus, the aim of this study was to examine whether SBP at time of diagnosis of dementia, mild cognitive impairment, or subjective cognitive decline was associated with years prior to death, and whether these associations were modified by diagnoses, age, and sex.MethodsParticipants were 2,236 patients from the Norwegian Registry of Persons Assessed for Cognitive Symptoms (NorCog), who died during follow‐up (2009–2017) for whom we had valid blood pressure measurements. Mean age at diagnosis was 77.5 years (SD 8.3), and patients were followed for an average of 3.9 years (SD 2.2, maximum 10.5 years). The patients had subjective cognitive decline (95), mild cognitive impairment (573), dementia (1,401), or no diagnoses related to cognitive deficits (167). SBP as dependent variable was regressed against years prior to death.ResultsIn men, SBP was 1.8 mmHg lower per year closer to death (p < .01), and this trend was linear without any acceleration. This association between years prior to death and SBP in men was not modified by age, year of diagnosis, or diagnosis. There was no such association in women.ConclusionSBP was significantly lower for those diagnosed close to death in men, but not in women. This association was not modified by either age or onset of diagnosis. Thus, the lowering of SBP is more related to closeness to death and sex than to dementia or age. The downward trend was linear all 10 years prior to death, with no acceleration closer to death.
Metal‐Free Deoxygenation of Amine N‐Oxides: Synthetic and Mechanistic Studies
Authors: Lecroq William , Schleinitz Jules , Billoue Mallaury , Perfetto Anna , Gaumont Annie‐Claude , Lalevée Jacques , Ciofini Ilaria , Grimaud Laurence , Lakhdar Sami 
Published: May 2021

AbstractWe report herein an unprecedented combination of light and P(III)/P(V) redox cycling for the efficient deoxygenation of aromatic amine N‐oxides. Moreover, we discovered that a large variety of aliphatic amine N‐oxides can easily be deoxygenated by using only phenylsilane. These practically simple approaches proceed well under metal‐free conditions, tolerate many functionalities and are highly chemoselective. Combined experimental and computational studies enabled a deep understanding of factors controlling the reactivity of both aromatic and aliphatic amine N‐oxides.
Treatment of donor‐specific antibody‐mediated rejection after heart transplantation by IgM‐enriched human immunoglobulin
Authors: Immohr Moritz Benjamin , Akhyari Payam , Aubin Hug , Westenfeld Ralf , Mehdiani Arash , Bruno Raphael Romano , Sipahi Nihat Firat , Erbel‐Khurtsidze Sophiko , Reinecke Petra , Tudorache Igor , Lichtenberg Artur , Boeken Udo 
Published: May 2021

AbstractAntibody‐mediated graft rejection caused by donor‐specific antibodies (DSA‐MR) remains a serious problem after heart transplantation (HTx). IgM‐enriched human intravenous immunoglobulin (IGM‐IVIG) consists of 76% IgG, 12% IgM, and 12% IgA and provides a new multifactorial approach for DSA‐MR. Between 2017 and 2020, four (P1–4) of 102 patients developed DSA‐MR after HTx in our department and were repetitively treated with IGM‐IVIG in combination with anti‐thymocyte globulin. While in P1 and P4, DSA‐MR occurred within the early post‐operative interval, P2 and P3 developed DSA‐MR approximately 1 year after transplantation. An impairment of ventricular function was observed in three of four patients. Furthermore, P1 and P4 suffered from malign ventricular arrhythmias. After the application of IGM‐IVIG, the ventricular function recovered, and all patients could be discharged from the hospital. As part of a multifactorial therapeutic approach, treatment with IGM‐IVIG seems to be a safe and effective strategy to address DSA‐MR.