bluuebunny/crossref_metadata_2025_split huggingface dataset:
Magnetic Resonance Imaging–Defined Osteoarthritis Features and Anterior Knee Pain in Individuals With, or at Risk for, Knee Osteoarthritis: A Multicenter Study on Osteoarthritis
Authors: Macri Erin M. , Neogi Tuhina , Jarraya Mohamed , Guermazi Ali , Roemer Frank , Lewis Cora E. , Torner James C. , Lynch John A. , Tolstykh Irina , Jafarzadeh S. Reza , Stefanik Joshua J. 
Published: March 2021

ObjectiveThe lack of strong association between knee osteoarthritis (OA) structural features and pain continues to perplex researchers and clinicians. Evaluating the patellofemoral joint in addition to the tibiofemoral joint alone has contributed to explaining this structure–pain discordance, hence justifying a more comprehensive evaluation of whole‐knee OA and pain. The present study, therefore, was undertaken to evaluate the association between patellofemoral and tibiofemoral OA features with localized anterior knee pain (AKP) using 2 study designs.MethodsUsing cross‐sectional data from the Multicenter Osteoarthritis Study, our first approach was a within‐person, knee‐matched design in which we identified participants with unilateral AKP. We then assessed magnetic resonance imaging (MRI)–derived OA features (cartilage damage, bone marrow lesions [BMLs], osteophytes, and inflammation) in both knees and evaluated the association of patellofemoral and tibiofemoral OA features to unilateral AKP. In our second approach, MRIs from 1 knee per person were scored, and we evaluated the association of OA features to AKP in participants with AKP and participants with no frequent knee pain.ResultsUsing the first approach (n = 71, 66% women, mean ± SD age 69 ± 8 years), lateral patellofemoral osteophytes (odds ratio [OR] 5.0 [95% confidence interval (95% CI) 1.7–14.6]), whole‐knee joint effusion‐synovitis (OR 4.7 [95% CI 1.3–16.2]), and infrapatellar synovitis (OR 2.8 [95% CI 1.0–7.8]) were associated with AKP. Using the second approach (n = 882, 59% women, mean ± SD age 69 ± 7 years), lateral and medial patellofemoral cartilage damage (prevalence ratio [PR] 2.3 [95% CI 1.3–4.0] and PR 1.9 [95% CI 1.1–3.3], respectively) and lateral patellofemoral BMLs (PR 2.6 [95% CI 1.5–4.7]) were associated with AKP.ConclusionPatellofemoral but not tibiofemoral joint OA features and inflammation were associated with AKP.
Adaptive finite‐time control for output regulation of nonlinear systems with completely unknown control directions
Authors: Jia Fujin , Lu Junwei , Li Yongmin 
Published: March 2021

AbstractThis article studies the finite‐time output regulation problem for nonlinear strict‐feedback systems with completely unknown control directions and unknown functions. First, according to the necessary conditions for the solvability of the output regulation problem, the output regulation problem of nonlinear strict‐feedback systems and the external system is transformed into a stabilization problem of nonlinear systems. Second, an internal model with external signals is designed. Third, based on finite time, fuzzy control, output feedback control, and Nussbaum gain functions, the control law is designed so that all signals of the closed‐loop system are the semi‐global practically finite‐time stable (SGPFS), and the tracking error converges to a small neighborhood of the origin in a finite‐time. Finally, the proposed algorithm is applied to the finite‐time tracking problem of Chua's oscillator system.
Reversible Transformation between CsPbBr3 Perovskite Nanowires and Nanorods with Polarized Optoelectronic Properties
Authors: Wang Yongkai , Liu Xiaoyu , He Qiqian , Chen Gaoyu , Xu Dongdong , Chen Xudong , Zhao Wenbo , Bao Jianchun , Xu Xiangxing , Liu Junli , Wang Xun 
Published: March 2021

AbstractCsPbX3 (X = Cl, Br, I) perovskite nanowires and nanorods are important 1D and quasi 1D semiconductor nanomaterials. They have shown significant prospect in optic and optoelectronic applications, especially for their adaptability to flexible devices, good carrier transport performance, polarized absorption, and emission properties. Due to the high dependence of the property to the morphology, it is crucial to develop synthesis methods with continuous diameter and length tunability of the 1D/quasi 1D perovskites. In this report, a feasibly room temperature synthesis method was developed for ultrathin CsPbX3(X = Cl, Br, I) perovskite nanowires. By aging the CsPbBr3 nanowires (≈2*500 nm) under ambient condition with proper concentration and time, the nanowires are transformed to nanorods with controllable diameter and length. Reversibly, the nanorods can be transformed back to nanowires. Equilibrium mechanism is adopted to understand the morphology evolution, and hopefully could be generally applied to many other nano materials. The polarized optoelectronic properties of the nanowires and nanorods are interpreted by a model based on the two‐channel anisotropies measurement. Polarized light detectors constructed by oriented assembled nanowires are fabricated to demonstrate their application potentials.
Understanding of Neighboring Fe‐N4‐C and Co‐N4‐C Dual Active Centers for Oxygen Reduction Reaction
Authors: Li Huanxin , Wen Yongliang , Jiang Min , Yao Yong , Zhou Haihui , Huang Zhongyuan , Li Jiawen , Jiao Shuqiang , Kuang Yafei , Luo Shenglian 
Published: March 2021

AbstractSingle atomic dispersed M‐N‐C (M = Fe, Co, Ni, Cu, etc.) composites display excellent performance for catalytic reactions. However, the analysis and understanding of neighboring M‐N‐C centers at the atomic level are still insufficient. Here, FeCo‐N‐doped hollow carbon nanocages (FeCo‐N‐HCN) with neighboring Fe‐N4‐C and Co‐N4‐C dual active centers as efficient catalysts are reported. Spherical aberration‐corrected high angle annular dark‐field scanning transmission electron microscopy, small area (1 nm2) electron energy loss spectroscopy, and X‐ray absorption spectroscopy data analysis and fitting prove the neighboring Fe‐N4‐C and Co‐N4‐C dual active structure in FeCo‐N‐HCN. Experimental tests and density functional theory calculation results reveal that the FeCo‐N‐HCN catalyst displays better catalytic activity than Fe single‐metal catalyst for oxygen reduction reaction (ORR), which is attributed to the synergistic effect of Fe‐N4‐C and Co‐N4‐C dual active centers reducing the reaction energy barriers for ORR. Although the catalytic performance of the FeCo‐N‐HCN catalyst is not comparable to the‐state‐of‐art catalysts reported due to the low metal contents (Fe: 1.96 wt% and Co: 1.31 wt%), these results can refresh the understanding of neighboring M‐N‐C centers at the atomic level and provide guidance for the design of catalysts in the future.
Efficient Fabrication of Ultralight YBa2Cu3O7−x Superconductors with Programmable Shape and Structure
Authors: Zhang Baoqiang , Zhang Qiangqiang , He Peng , Ma Yanbin , Shen Lei , Zhang Xingyi , Zhou Youhe 
Published: March 2021

AbstractSuperconducting YBa2Cu3O7−x (YBCO) bulks have demonstrated promising applications in quasi‐permanent magnets, levitation, etc. Recently, the applications of bulk superconductors have been proposed, such as in portable, ultralight superconducting devices. These applications require bulk superconductors with lightweight, complex morphology, and good processability. However, the traditional fabrication method of YBCO bulks requires prolonged supplemental oxygenation and produces limited geometries with many randomly distributed cracks. This, combined with the inherent brittleness of the ceramic material, seriously impedes its wide application. In this study, a YBCO bulk with a multiscale hierarchical geometric configuration is constructed by a direct‐ink‐writing‐based 3D‐printing process. The 3D‐printed YBCO green bodies exhibit a robust structure after directional freezing, which promotes intimate contact between the precursor particles in the deposited layers. This technology offers the advantage of a low shrinkage of 13.6 vol% after sintering at 920 °C. The 3D‐printed bulks show lightweight, highly crystalline, and good electromagnetic properties compared with those produced by traditional cold‐pressed sintering. Importantly, the multilevel void structure with a large specific surface area significantly reduces the oxygenation time and retains superconductivity. The proposed 3D‐printing process can be adopted for the industrial production of superconducting bulk with complex geometries for novel applications.
Droplet‐Based Techniques for Printing of Functional Inks for Flexible Physical Sensors
Authors: Abdolmaleki Hamed , Kidmose Preben , Agarwala Shweta 
Published: March 2021

AbstractPrinted electronics (PE) is an emerging technology that uses functional inks to print electrical components and circuits on variety of substrates. This technology has opened up new possibilities to fabricate flexible, bendable, and form‐fitting devices at low‐cost and fast speed. There are different printing technologies in use, among which droplet‐based techniques are of great interest as they provide the possibility of printing computer‐controlled design patterns with high resolution, and greater production flexibility. Nanomaterial inks form the heart of this technology, enabling different functionalities. To this end, intensive research has been carried out on formulating inks with conductive, semiconductive, magnetic, piezoresistive, and piezoelectric properties. Here, a detailed landscape view on different droplet‐based printing technologies (inkjet, aerosol jet, and electrohydrodynamic jet) is provided, with comprehensive discussion on their working principals. This is followed by a detailed research overview of different functional inks (metal, carbon, polymer, and ceramic). Different sintering methods and common substrates being used in printed electronics are also discussed, followed by an in‐depth review of different physical sensors fabricated by droplet‐based techniques. Finally, the challenges facing the field are considered and a perspective on possible ways to overcome them is provided.
Narrowing Bandgap of HfS2 by Te Substitution for Short‐Wavelength Infrared Photodetection
Authors: Ye Jiafu , Liao Ke , Ge Xun , Wang Zhen , Wang Yang , Peng Meng , He Ting , Wu Peisong , Wang Hailu , Chen Yunfeng , Cui Zhuangzhuang , Gu Yue , Xu Hangyu , Xu Tengfei , Li Qing , Zhou Xiaohao , Luo Man , Li Ning , Zubair Muhammad , Wu Feng , Wang Peng , Shan Chongxin , Wang Gang , Miao Jinshui , Hu Weida 
Published: March 2021

AbstractInfrared photodetectors are widely used in the field of remote sensing, communications, biomedical imaging, etc. Most photodetection based on 2D transition‐metal dichalcogenides (TMDs) is limited to the visible (Vis) to near‐infrared (NIR) due to large intrinsic bandgaps (≈1.2–2 eV). Here, a bandgap engineering of HfS2 by a tellurium (Te)‐replacement strategy is obtained via chemical vapor transport method. The bandgap values of HfS2(1−x)Te2x decrease from 1.7 to 0.88 eV with Te composition changing from 0 to 0.095. Few‐layer HfS1.81Te0.19 based field‐effect transistors exhibit a high current on/off ratio of 106 and decent electron mobility of 12.6 cm2 V−1 s−1 at room temperature. The photodetectors show a responsivity of 2 A W−1 with a remarkable photocurrent of ≈3 μA and a fast response speed of 8.8/75 ms at 830 nm simultaneously. Further, the response spectrum of HfS2(1−x)Te2x based photodetectors is broadened from Vis to short‐wavelength infrared (SWIR), covering the free‐space laser communications wavelength and the second NIR region in medicine. Bandgap engineering of 2D TMDs proposed in this work offer a promising route to develop bandgap‐variable 2D materials for infrared photodetection applications.
Stochastic Estimations of the Total Number of Classes for a Clustering having Extremely Large Samples to be Included in the Clustering Engine
Authors: Utimula Keishu , Prayogo Genki I. , Nakano Kousuke , Hongo Kenta , Maezono Ryo 
Published: March 2021

AbstractNumerous reports have elucidated the classification of a large amount of data using various clustering techniques. However, an increase in data size hinders the applicability of these methods. Here, it is investigated how to deal with the exploding number of possibilities to be sorted into irreducible classes by using a clustering technique when its input capacity cannot accommodate the total number of possibilities. This can be exemplified by atomic substitutions in the supercell modeling of alloys. The number of possibilities is sometimes equal to trillions, which is extremely large to be accommodated in a cluster. Thus, it is not practically feasible to identify directly how many irreducible classes exist even though several techniques are available to perform the clustering. In this regard, a stochastic framework is developed to avoid the shortage limitations, providing a method to estimate the total number of irreducible classes (the order of classes), as a statistical estimate. The main conclusion is that the statistical variation of the number of classes, at each sampling trial, can serve as a promising measure to estimate the total number of irreducible classes. Characteristics of this approach is also discussed by comparing with the conventional one based on Polya's theorem.
From Micromagnetic to In Silico Modeling of Magnetic Nanodisks for Hyperthermia Applications
Authors: Manzin Alessandra , Ferrero Riccardo , Vicentini Marta 
Published: March 2021

AbstractMagnetic nanodisks have been recently proposed as biomedical tools for therapeutics at the nanoscale level, with a special focus on hyperthermia for cancer cure. Here we present a detailed study of permalloy nanodisks to be used in alternative to superparamagnetic iron oxide nanoparticles, as efficient heating agents that release heat via magnetic hysteresis. A micromagnetic modeling analysis is carried out to identify sizes and ac field parameters that maximize the specific loss power (SLP), guaranteeing the fulfillment of biophysical constraints (Hergt–Dutz limit) and vortex state at remanence (reduced agglomeration effects). The highest SLP (790 W g−1) is found for 100 nm diameter and 20 nm thickness nanodisks, excited at a frequency of 75 kHz. Further analysis elucidates the influence of magnetostatic interactions and local nanodisk‐field orientation on the SLP of nanodisk clusters, which originate from the deposition in target tissues. At high concentrations, magnetostatic interactions can lead to a reduction of 40–50% in the hysteresis losses. From thermal simulations, we finally demonstrate that in a murine model temperature increments comparable to that obtained in calorimetric measurements under quasi‐adiabatic conditions can be achieved only by using an order of magnitude larger dosage of nanodisks, due to blood perfusion effects.
Patterned Blade Coating Strategy Enables the Enhanced Device Reproducibility and Optimized Morphology of Organic Solar Cells
Authors: Yuan Jian , Liu Dongjie , Zhao Heng , Lin Baojun , Zhou Xiaobo , Naveed Hafiz Bilal , Zhao Chao , Zhou Ke , Tang Zheng , Chen Fei , Ma Wei 
Published: March 2021

AbstractMorphology evolution kinetics at multi‐scale regime is a challenging problem which is critical for industrial fabrication of high‐performance organic solar cells (OSCs). An innovative strategy utilizing a patterned blade to print non‐fullerene (NF) based devices in ambient conditions is demonstrated. A specially designed patterned blade with micro‐cylinder arrays exhibit a reasonable control over the fluid flow at high extensional and shear strain rate to enhance lateral mass transport during blade‐coating. Comparison of patterned and normal blade in printing polymer:NF blend film at different speeds reveals interesting avenues to optimize the blend films morphology. Patterned blade printed PM6:Y6 films yield a PCE of 15.93% as compared to 14.55% from a normal blade. Through in situ and ex situ morphology characterization techniques, the use of patterned blades induce conformational changes in PM6 chains, enabling Y6 to crystallize faster and more efficiently. Such improved blend morphology enables favorable charge transfer and transport to realize superior device performance. A lower stick‐slip effect at the macro‐scale with the patterned blade results in a smoother film promoting device reproducibility. Applications in efficient large‐scale devices, confirming the choice of patterned blade design are reported. The efforts collaborating device engineering, morphology evolution kinetics would enable reproducibility and eased commercialization of OSCs at large scale.
New Cysteine Covalent Modification Strategies Enable Advancement of Proteome‐wide Selectivity of Kinase Modulators
Authors: Guan Ivy , Williams Kayla , Pan Jolyn , Liu Xuyu 
Published: March 2021

AbstractThere has been tremendous progress in covalent inhibitors as evidenced by the ascent of innovative electrophilic warheads with suppressed non‐specific reactivity but enhanced capacity for proximity‐driven covalent reactions with nucleophilic residues in the targeted site. Kinases, a central player in cancers, autoimmune disorders and chronic diseases, represent a highly targeted class of enzymes by covalent inhibitors. However, innovative strategies to afford high selectivity in target recognition remain a pressing need. This minireview focuses on four promising strategies to achieve superior target selectivity through rational design of the covalent engagement. Special emphasis is placed on examples where the selectivity had arisen by complementing the reactivity of protein cysteines with electrophilic warheads specified for distinct covalent chemistry, or inspired from native electrophile signalling in cells.
Iron‐Catalyzed Water Oxidation: O–O Bond Formation via Intramolecular Oxo–Oxo Interaction
Authors: Zhang Hong‐Tao , Su Xiao‐Jun , Xie Fei , Liao Rong‐Zhen , Zhang Ming‐Tian 
Published: March 2021

AbstractHerein, we report the importance of structure regulation on the O−O bond formation process in binuclear iron catalysts. Three complexes, [Fe2(μ‐O)(OH2)2(TPA)2]4+(1), [Fe2(μ‐O)(OH2)2(6‐HPA)]4+(2) and [Fe2(μ‐O)(OH2)2(BPMAN)]4+(3), have been designed as electrocatalysts for water oxidation in 0.1 M NaHCO3solution (pH 8.4). We found that1and2are molecular catalysts and that O−O bond formation proceeds via oxo–oxo coupling rather than by the water nucleophilic attack (WNA) pathway. In contrast, complex3displays negligible catalytic activity. DFT calculations suggested that theantitosynisomerization of the two high‐valent Fe=O moieties in these catalysts takes place via the axial rotation of one Fe=O unit around the Fe‐O‐Fe center. This is followed by the O−O bond formation via an oxo–oxo coupling pathway at the FeIVFeIVstate or via oxo–oxyl coupling pathway at the FeIVFeVstate. Importantly, the rigid BPMAN ligand in complex3limits theantitosynisomerization and axial rotation of the Fe=O moiety, which accounts for the negligible catalytic activity.
Vapochromism and Magnetochemical Switching of a Nickel(II) Paddlewheel Complex by Reversible NH3 Uptake and Release
Authors: Fürpaß Katharina M. , Peschel Lydia M. , Schachner Jörg A. , Borisov Sergey M. , Krenn Heinz , Belaj Ferdinand , Mösch‐Zanetti Nadia C. 
Published: March 2021

AbstractReaction of [NiCl2(PnH)4] (1) (PnH=6‐tert‐butyl‐pyridazine‐3‐thione) with NiCl2 affords the binuclear paddlewheel (PW) complex [Ni2(Pn)4] (2). Diamagnetic complex 2 is the first example of a PW complex capable of reversibly binding and releasing NH3. The NH3 ligand in [Ni2(Pn)4(NH3)] (2⋅NH3) enforces major spectroscopic and magnetic susceptibility changes, thus displaying vapochromic properties (λmax(2)=532 nm, λmax(2⋅NH3)=518 nm) and magnetochemical switching (2: S=0; 2⋅NH3: S=1). Upon repeated adsorption/desorption cycles of NH3 the PW core remains intact. Compound 2 can be embedded into thin polyurethane films (2P) under retention of its sensing abilities. Therefore, 2 qualifies as reversible optical probe for ammonia. The magnetochemical switching of 2 and 2⋅NH3 was studied in detail by SQUID measurements showing that in 2⋅NH3, solely the Ni atom coordinated the NH3 molecule is responsible for the paramagnetic behavior.
The Interrelated Effect of Cations and Electrolyte pH on the Hydrogen Evolution Reaction on Gold Electrodes in Alkaline Media
Authors: Goyal Akansha , Koper Marc T. M. 
Published: March 2021

AbstractIn this work we study the role of alkali metal cation concentration and electrolyte pH in altering the kinetics of the hydrogen evolution reaction (HER) at gold (Au) electrodes. We show that at moderately alkaline pH (pH 11), increasing the cation concentration significantly enhances the HER activity on Au electrodes (with a reaction order ≈0.5). Based on these results we suggest that cations play a central role in stabilizing the transition state of the rate‐determining Volmer step by favorably interacting with the dissociating water molecule (*H–OHδ−–cat+). Moreover, we show that increasing electrolyte pH (pH 10 to pH 13) tunes the local field strength, which in turn indirectly enhances the activity of HER by tuning the near‐surface cation concentration. Interestingly, a too high near‐surface cation concentration (at high pH and high cation concentration) leads to a lowering of the HER activity, which we ascribe to a blockage of the surface by near‐surface cations.
Reduction of the environmental footprint of thermo‐alkali pretreatment by reusing black liquor during anaerobic digestion of lignocellulosic biomasses
Authors: Peyrelasse Christine , Kaparaju Prasad , Lallement Audrey , Marques Melissa , Monlau Florian 
Published: March 2021

AbstractIn this study, the effect of thermo‐alkaline pretreatment and recycling of the liquid fraction (black liquor) for successive pretreatment steps on chemical composition and methane yields from horse manure was investigated. At first, horse manure was subjected to alkaline pretreatment at 70 °C for 1 h (8.6 g NaOH/100 g total solids). Pretreated biomass was then separated into solid and liquid fractions (black liquor). In the subsequent stages, black liquor was mixed with 20% (v/v) of fresh NaOH and was reused to pretreat subsequent batches of horse manure (cycles 1–4). Chemical analyses showed that thermo‐alkaline pretreatment was effective in the delignification and solubilization of organic matter and thereby increased the holocellulose (cellulose and hemicelluloses) content in the solid fraction of horse manure. On comparison with untreated horse manure methane yields (225 ± 1 L CH4 kg−1 VSadded), thermo‐alkaline pretreatment improved the methane yields of horse manure by 39% (313 ± 16 L CH4 kg−1 VSadded). However, the effectiveness of black liquor recycling on methane production decreased (from 39 to 12%) with an increase in the number of recycling steps (from 1 to 4). Nevertheless, recycling of black liquor reduced the consumption of NaOH (40%) and water use (60%). Thus, thermo‐alkaline pretreatment with liquor recycling was found to be an effective pretreatment with an economic gain of 2.4 to 10.4 compared to pretreatment without recycling. © 2021 Society of Chemical Industry and John Wiley & Sons, Ltd