bluuebunny/crossref_metadata_2025_split huggingface dataset:
Lightweight 3D Graphene Metamaterials with Tunable Negative Thermal Expansion
Authors: He Peng , Du Tao , Zhao Keren , Dong Jiaqi , Liang Yusheng , Zhang Qiangqiang 
Published: November 2022

AbstractIn this study, a 3D graphene metamaterial (GM) showing negative thermal expansion is prepared using a strategy of hyperbolically oriented freezing under a dual temperature gradient along orthogonal directions after the π–π stacking‐derived assembly of 2D graphene sheets. As the fundamental construction element of the 3D GM, the graphene sheet displays anomalous shrinking deformation with a thermal expansion coefficient of (−6.12 ± 0.28) × 10−6 that is triggered by thermally induced out‐of‐plane vibrations of the CC bonds. A combination of numerical simulations and experimental investigations validates that anomalous negative thermal expansion (NTE) behavior can be effectively delivered to scalable 3D GM candidates at larger dimensions beyond the basic 2D graphene sheets at the microscale. The multiscale design and optimization of the structural characterization of the 3D GM further realize the desirable regulation of the NTE performance with the NTE coefficient ranging from negative ((−7.5± 0.65) × 10−6 K−1) to near‐zero values ((−0.8 ± 0.25) × 10−6 K−1). This is attributed to the NTE‐derived release regulation of the primary stress/strain of the microstructure, and the 3D GM exhibits high thermal stability while preserving the desirable structural robustness and fatigue resistance under thermo‐mechanical coupling conditions. Therefore, this 3D GM offers promising potential for applications as protective skin, thermal actuator, smart switcher, and packing filler.
Entering a New Dimension in Powder Processing for Advanced Ceramics Shaping
Authors: Sänger Johanna Christiane , Pauw Brian Richard , Riechers Birte , Zocca Andrea , Rosalie Julian , Maaß Robert , Sturm Heinz , Günster Jens 
Published: November 2022

AbstractFiligree structures can be manufactured via two‐photon polymerization (2PP) operating in the regime of nonlinear light absorption. For the first time, it is possible to apply this technique to the powder processing of ceramic structures with a feature size in the range of the critical defect sizes responsible for brittle fracture and, thus, affecting fracture toughness of high‐performance ceramics. In this way, tailoring of advanced properties can be achieved already in the shaping process. Traditionally, 2PP relies on transparent polymerizable resins, which are diametrically opposed to the usually completely opaque ceramic resins and slurries. Here a transparent and photocurable suspension of nanoparticles (resin) with very high mass fractions of yttria‐stabilized zirconia particles (YSZ) is presented. Due to the extremely well‐dispersed nanoparticles, scattering of light can be effectively suppressed at the process‐relevant wavelength of 800 nm. Sintered ceramic structures with a resolution of down to 500 nm are obtained. Even at reduced densities of 1–4 g cm−3, the resulting compressive strength with 4.5 GPa is equivalent or even exceeding bulk monolithic yttria‐stabilized zirconia. A ceramic metamaterial is born, where the mechanical properties of yttria‐stabilized zirconia are altered by changing geometrical parameters, and gives access to a new class of ceramic materials.
A New Class of Cluster–Matrix Nanocomposite Made of Fully Miscible Components
Authors: Iankevich Gleb , Sarkar Abhishek , Katnagallu Shyam , Chellali Mohammed Reda , Wang Di , Velasco Leonardo , Singh Ruby , Reisinger Thomas , Kruk Robert , Hahn Horst 
Published: November 2022

AbstractNanocomposite materials, consisting of two or more phases, at least one of which has a nanoscale dimension, play a distinctive role in materials science because of the multiple possibilities for tailoring their structural properties and, consequently, their functionalities. In addition to the challenges of controlling the size, size distribution, and volume fraction of nanometer phases, thermodynamic stability conditions limit the choice of constituent materials. This study goes beyond this limitation by showing the possibility of achieving nanocomposites from a bimetallic system, which exhibits complete miscibility under equilibrium conditions. A series of nanocomposite samples with different compositions are synthesized by the co‐deposition of 2000‐atom Ni‐clusters and a flux of Cu‐atoms using a novel cluster ion beam deposition system. The retention of the metastable nanostructure is ascertained from atom probe tomography (APT), magnetometry, and magnetotransport studies. APT confirms the presence of nanoscale regions with ≈100 at% Ni. Magnetometry and magnetotransport studies reveal superparamagnetic behavior and magnetoresistance stemming from the single‐domain ferromagnetic Ni‐clusters embedded in the Cu‐matrix. Essentially, the magnetic properties of the nanocomposites can be tailored by the precise control of the Ni concentration. The initial results offer a promising direction for future research on nanocomposites consisting of fully miscible elements.
Super‐Assembled Multi‐Level Asymmetric Mesochannels for Coupled Accelerated Dual‐Ion Selective Transport
Authors: Zhou Shan , Xie Lei , Zhang Xin , Yan Miao , Zeng Hui , Liang Kang , Jiang Lei , Kong Biao 
Published: November 2022

AbstractAsymmetric nanofluidic devices hold great potential in energy conversion applications. However, most of the existing asymmetric nanofluidic devices remain a single‐level asymmetric structure and a single‐ion selective layer, which results in weak ion selectivity and limited energy conversion efficiency. Herein, a multi‐level asymmetric mesoporous carbon/anodized aluminum/mesoporous silica (MC/AAO/MS) nanofluidic device with abundant and ordered mesochannels is constructed from super‐assembly strategy. The resultant MC/AAO/MS exhibits diode‐like ion transport and outstanding ion storage‐release performance. Importantly, MC/AAO/MS couples the MC and MS dual‐ion selective layers, which ensures a high ionic conductance and evidently enhances the cation selectivity. Thereby, the MC/AAO/MS demonstrates ascendant salinity gradient energy conversion performance. The power density and conversion efficiency can reach up to 5.37 W m−2and 32.79%, respectively. Noteworthy, a good energy conversion performance of 63 mW m−2can still be achieved upon high working area, outperforming 300% of the performance of MC/AAO and MS/AAO single‐level asymmetric nanochannels. Theoretical calculation further verifies that the multi‐level asymmetric structure and dual‐ion selective transport are the reason for the enhanced cation selectivity and energy conversion efficiency. This work opens a new avenue for constructing multi‐level asymmetric structured nanofluidic devices for various applications.
Inter‐Metal Interaction with a Threshold Effect in NiCu Dual‐Atom Catalysts for CO2 Electroreduction
Authors: Yao Dazhi , Tang Cheng , Zhi Xing , Johannessen Bernt , Slattery Ashley , Chern Shane , Qiao Shi‐Zhang 
Published: November 2022

AbstractDual‐atom catalysts (DACs) have become an emerging platform to provide more flexible active sites for electrocatalytic reactions with multi‐electron/proton transfer, such as the CO2 reduction reaction (CRR). However, the introduction of asymmetric dual‐atom sites causes complexity in structure, leaving an incomprehensive understanding of the inter‐metal interaction and catalytic mechanism. Taking NiCu DACs as an example, herein, a more rational structural model is proposed, and the distance‐dependent inter‐metal interaction is investigated by combining theoretical simulations and experiments, including density functional theory computation, aberration‐corrected transmission electron microscopy, synchrotron‐based X‐ray absorption fine structure, and Monte Carlo experiments. A distance threshold around 5.3 Å between adjacent NiN4 and CuN4 moieties is revealed to trigger effective electronic regulation and boost CRR performance on both selectivity and activity. A universal macro‐descriptor rigorously correlating the inter‐metal distance and intrinsic material features (e.g., metal loading and thickness) is established to guide the rational design and synthesis of advanced DACs. This study highlights the significance of identifying the inter‐metal interaction in DACs, and helps bridge the gap between theoretical study and experimental synthesis of atomically dispersed catalysts with highly correlated active sites.
Enantioselective Allenylation of Ketimines Derived from Isatins Using Chiral Bis(imidazoline)‐Palladium Catalysts
Authors: Oyamada Yusuke , Yamasaki Shintaro , Tsuzuki Mika , Kitagawa Takumi , Kondo Masaru , Sasamori Takahiro , Nakamura Shuichi 
Published: November 2022

AbstractThe catalytic enantioselective allenylation of ketimines derived from isatins is described. Products with high regio‐ and enantioselectivities were obtained in the presence of a bis(imidazoline)‐palladium catalyst. The obtained products were then converted into various chiral amines. The stereoselectivity origin was revealed by DFT calculations of the transition state.magnified image
Thienothiophene‐Assisted Property Optimization for Dopant‐Free π‐Conjugation Polymeric Hole Transport Material Achieving Over 23% Efficiency in Perovskite Solar Cells
Authors: Xie Zhiqing , Park Hyungjin , Choi SeungJu , Park Ho‐Yeol , Gokulnath Thavamani , Kim Hyerin , Kim Jeonghyun , Kim Hak‐Beom , Choi In Woo , Jo Yimhyun , Kim Dong Suk , Kim Young‐Yong , Yoon Seog Young , Yoon Jinhwan , Cho Yong‐Rae , Jin Sung‐Ho 
Published: November 2022

AbstractHole transport materials (HTMs) play essential roles in achieving high photovoltaic performance and long‐term stability in the n–i–p structure of perovskite solar cell (PSC) devices. Recently, dopant‐free polymeric materials as HTMs in PSCs have attracted considerable attention owing to high carrier mobility and excellent hydrophobicity. However, achieving similar efficiencies to those of doped small molecule HTMs such as Spiro‐OMeTAD is a big challenge. Herein, a thienothiophene π‐bridge is selected as a stabilizer and energy level regulator incorporated into a donor–acceptor‐type HTM to synthesize a new polymer, Nap‐SiBTA. The incorporation of the thienothiophene group improves the thermal stability and favors the high planarity and face‐on orientation, promoting high charge carrier mobility and tunable optical band gap. Finally, the dopant‐free polymer Nap‐SiBTA‐based PSC achieves an excellent power conversion efficiency (PCE) of 23.07% with a high fill factor of 80.85%. To the best of the authors’ knowledge, this is one of the best efficiencies in dopant‐free HTM PSCs. Moreover, the unencapsulated device retains 93% of its initial PCE after 1000 h owing to the excellent hydrophobicity of Nap‐SiBTA. This work provides a general and practical method to design dopant‐free HTMs for the high efficiency and long‐term stability of PSCs.
Electrochemo‐Mechanical Stresses and Their Measurements in Sulfide‐Based All‐Solid‐State Batteries: A Review
Authors: Gu Jiabao , Liang Ziteng , Shi Jingwen , Yang Yong 
Published: November 2022

AbstractSulfide‐based all‐solid‐state batteries (ASSBs) are one of the most promising energy storage devices due to their high energy density and good safety. However, due to the volume (stress) changes of the solid active materials during the charging and discharging process, the generation and evolution of electrochemomechanical stresses are becoming serious and unavoidable problems during the operation of all‐solid‐state batteries due to the lack of a liquid electrolyte to partially buffer the stress generated in the electrodes. To understand these electrochemo‐mechanical effects, including the origins and evolution of mechanical or internal stresses, it is necessary to develop some highly sensitive probing techniques to measure them precisely and bridge the relationship between the electrochemical reaction process and internal stress evolution. Herein, recent progress on uncovering the origins of the internal stresses, the working principle and experimental devices for stress measurement, and the application of those stress‐measuring techniques in the study of electrochemical reactions in sulfide‐based ASSBs are briefly summarized and overviewed. The investigation of precise and operando monitoring techniques and strategies for suppressing or relaxing these electrochemomechanical stresses will be an important direction in future solid‐state batteries.
Specific Metal Nanostructures toward Electrochemical CO2 Reduction: Recent Advances and Perspectives
Authors: Yu Mulin , Sui Peng‐Fei , Fu Xian‐Zhu , Luo Jing‐Li , Liu Subiao 
Published: November 2022

AbstractElectrochemically converting CO2 (CO2 reduction reaction(CO2RR)) to value‐added fuels is an advanced technology to effectively alleviate global warming and the energy crisis. However, thermodynamically high energy barriers, sluggish reaction kinetics, and inadequate CO2 conversion rate as well as poor selectivity of target products and rapid materials degradation severely limit its further large‐scale application, which highlights the importance of high‐performance electrocatalysts. Metal nanomaterials, due to their intrinsically high but still insufficient reactivity, selectivity, and stability, have been brought to the forefront and have lead to many reviews from various points of view. However, reviews which comprehensively unravel the importance and excellence of specific metal nanostructures and their associated properties for CO2RR are quite limited. To bridge this gap, various specific monometal and bimetal nanostructures are summarized, with an emphasis on the deep understanding of crystal orientation, surface structure, surface crystallography, surface modification, and many associated effects benefiting from the constructed specific metal nanostructures as well as the intrinsic relationships of specific metal nanostructure‐property‐CO2RR activities. Finally, the challenges and the perspectives to advance CO2RR are proposed to pay particularly more attention to architecture evolution during CO2RR with in situ/operando techniques, high‐throughput theoretical computations, and facile synthetic strategies with high yield and production for scale‐up applications.
Pesticide trends in a tailwater recovery system in the Mississippi Delta
Authors: Nelson Amanda M. , Moore Matthew T. , Witthaus Lindsey M. 
Published: November 2022

AbstractTailwater recovery (TWR) systems are an important best management practice (BMP) used to address both water quality and quantity issues in the Mississippi Delta region. Tailwater recovery systems are surface water capture‐and‐irrigation reuse systems using a combination of ditches to capture surface water, an on‐farm storage (OFS) reservoir to store captured surface water, and pumps to move surface water from ditches to the reservoir and from the reservoir to irrigate nearby fields. It is anticipated that TWR systems improve water quality by allowing agricultural contaminants to settle out in ditches and reservoirs rather than being transported during irrigation to nearby fields and downstream aquatic systems. To determine if TWR systems are an effective way to reduce downstream pesticide transport, water samples from a ditch‐and‐reservoir TWR system in Sunflower County, MS, were routinely collected and analyzed for 5 yr. Objectives of this study were to assess seasonal pesticide and pesticide metabolite concentrations throughout the different components of the TWR system and identify any trends that may exist. Atrazine‐desethyl, atrazine‐desisopropyl, atrazine, clomazone, propanil, fipronil desulfinyl, metolachlor, fipronil, p,p'‐DDT, bifenthrin, beta‐cyfluthrin, and zeta‐cypermethrin were found in every season in both ditch and reservoir samples. Several pesticides that have not been used in the United States for decades were detected including DDT and its metabolites as well as dieldrin, heptachlor, lindane, and methyl parathion, demonstrating their environmental persistence. The reservoir featured more types and higher concentrations of pesticides, indicating a possible risk of cross‐crop injury from the recycling of the water from the reservoir for irrigation.
Impacts of long‐term fertilization on crop yield and microbial communities under rice–rapeseed rotation
Authors: Li Jifu , Gan Guoyu , Zeng Qianqian 
Published: November 2022

AbstractSoil microbes play an integral role in agricultural production and soil fertility, while limited information is available about the effects of long‐term fertilization on rice (Oryza sativa L.)–rapeseed (Brassica napus L.) rotation yield, soil properties, and microbial communities in central China. Here, we report the response of plant–soil system to different mineral fertilizer inputs, including the balanced fertilization with N, P, and K (NPK) fertilizers and unbalanced fertilizers without one of the major nutrients (PK, NK, and NP) for 10 years. Compared with the NPK treatment, the average annual decrease rates of rice and rapeseed yield in the PK, NK, and NP treatments were 12.5%, 18.1%, 6.4% and 33.1%, 54.8%, 16.0%, respectively. Long‐term fertilization significantly changed the soil chemical properties, especially the pH and available K content. Compared with the NPK fertilization, the NK treatment increased the soil microbial composition and diversity, whereas PK and NP treatments had a reverse impact. Available K, pH, and slowly available K were closely related to alterations of the dominant bacterial community. On the contrary, the Olsen‐P, slowly available K, and pH were significantly correlated with the fungal community. Soil properties changed by fertilization had a more direct effect on crop yield than the microbial community; moreover, the bacterial group had a higher influence than the fungal group on crop yield. Therefore, a balanced nutrient input using NPK fertilization is an effective management strategy for soil biological fertility and sustainable crop yield.
Validity of anthropometric equation‐based estimators of fat mass in Samoan adults
Authors: Heinsberg Lacey W. , Hawley Nicola L. , Duckham Rachel L. , Pomer Alysa , Rivara Anna C. , Naseri Take , Reupena Muagututi‘a Sefuiva , Weeks Daniel E. , McGarvey Stephen T. , Minster Ryan L. 
Published: November 2022

AbstractIntroductionIn 1999, a set of highly accurate Polynesian‐specific equations to estimate adult body fat from non‐invasive field measures of age, sex, height, and weight (Equation 1), age, sex, height, weight, and bioelectrical impedance analysis (BIA) resistance (Equation 2), and age, sex, height, weight, and the sum of two skinfold thicknesses (Equation 3) were published. The purpose of this study was to evaluate the performance of the equation‐based estimators in a sample of Samoan adults recruited 20 years later between 2017 and 2019.MethodsAge, sex, height, weight, BIA resistance, skinfold thickness, and fat mass as measured using dual energy x‐ray absorptiometry (DXA) were available for 432 Samoan adults (mean age 50.9 years, 56% female) seen in 2017/2019. We compared equation‐derived fat mass and DXA‐derived fat mass using scatterplots and Pearson correlation coefficients. We then updated the equation coefficient estimates in a training set (2/3 of the sample) and evaluated the performance of the updated equations in a testing set (the remaining 1/3 of the sample).ResultsEquation‐derived fat mass was strongly correlated with DXA‐derived fat mass for Equation (1) (r2 = 0.95, n = 432), Equation (2) (r2 = 0.97, n = 425), and Equation (3) (r2 = 0.95, n = 426). Updating the equation coefficient estimates resulted in mostly similar coefficients and nearly identical testing set performance for Equation (1) (r2 = 0.96, n = 153), Equation (2) (r2 = 0.98, n = 150), and Equation (3) (r2 = 0.96, n = 150).ConclusionsThe Polynesian‐specific body fat estimation equations remained stable despite changing social and environmental factors and marked increase in obesity prevalence in Samoa.
Further expansion and confirmation of phenotype in rare loss of YWHAE gene distinct from Miller–Dieker syndrome
Authors: Baker Elizabeth K. , Brewer Casey J. , Ferreira Leonardo , Schapiro Mark , Tenney Jeffrey , Wied Heather M. , Kline‐Fath Beth M. , Smolarek Teresa A. , Weaver K. Nicole , Hopkin Robert J. 
Published: November 2022

AbstractDeletion of 17p13.3 has varying degrees of severity on brain development based on precise location and size of the deletion. The most severe phenotype is Miller–Dieker syndrome (MDS) which is characterized by lissencephaly, dysmorphic facial features, growth failure, developmental disability, and often early death. Haploinsufficiency of PAFAH1B1 is responsible for the characteristic lissencephaly in MDS. The precise role of YWHAE haploinsufficiency in MDS is unclear. Case reports are beginning to elucidate the phenotypes of individuals with 17p13.3 deletions that have deletion of YWHAE but do not include deletion of PAFAH1B1. Through our clinical genetics practice, we identified four individuals with 17p13.3 deletion that include YWHAE but not PAFAH1B1. These patients have a similar phenotype of dysmorphic facial features, developmental delay, and leukoencephalopathy. In a review of the literature, we identified 19 patients with 17p13.3 microdeletion sparing PAFAH1B1 but deleting YWHAE. Haploinsufficiency of YWHAE is associated with brain abnormalities including cystic changes. These individuals have high frequency of epilepsy, intellectual disability, and dysmorphic facial features including prominent forehead, epicanthal folds, and broad nasal root. We conclude that deletion of 17p13.3 excluding PAFAH1B1 but including YWHAE is associated with a consistent phenotype and should be considered a distinct condition from MDS.
Clinical overview on RASopathies
Authors: Zenker Martin 
Published: November 2022

AbstractRASopathies comprise a group of clinically overlapping developmental disorders caused by genetic variations affecting components or modulators of the RAS‐MAPK signaling cascade, which lead to dysregulation of signal flow through this pathway. Noonan syndrome and the less frequent, clinically related disorders, Costello syndrome, cardiofaciocutaneous syndrome, Noonan syndrome with multiple lentigines, and Noonan syndrome‐like disorder with loose anagen hair are part of the RASopathy spectrum and share a recognizable pattern of multisystem involvement. This review describes the “Noonan syndrome‐like” phenotype as a common phenotypic signature of generalized developmental RAS pathway dysregulation. Distinctive features of the different entities are revisited against the background of the understanding of underlying genetic alterations and genotype correlations, which has evolved rapidly during the past 20 years, thereby leading to suggestions regarding the nosology of RASopathies.
A Review on Molecular Iodine Catalyzed/Mediated Multicomponent Reactions
Authors: Monika  , Chander  , Ram Sita , Sharma Pawan K. 
Published: November 2022

AbstractIn multicomponent reactions, three or more reactants combine in one pot to form a product without the isolation of intermediate and most of the reactants contribute to newly formed product reducing number of steps involved and waste generated. Molecular iodine is mild, efficient, relatively nontoxic, inexpensive, commercially available, and catalyzes various organic reactions due to its Lewis acidic behaviour. The development of multicomponentreactions catalyzed by molecular iodine indeed is a good green alternative for synthetic organic chemistry. The aim of this article is to review all important multicomponent reactions catalyzed by molecular iodine reported since 2013 in order to envisage some new efficient protocols for the synthesis of structurally complex molecules.