bluuebunny/crossref_metadata_2025_split huggingface dataset:
HiGee Strategy toward Rapid Mass Production of Porous Covalent Organic Polymers with Superior Methane Deliverable Capacity
Authors: Zhang Weichao , Liu Yujia , Luo Yong , Xie Chengpeng , Xiang Zhonghua , Chen Jian‐Feng 
Published: January 2020

AbstractHigh porosity with well‐defined molecular reticulation along with strong stability is desired for natural gas delivery. The catalyzed Yamamoto‐type Ullmann cross‐coupling route with efficient terminal halogen removal capability is currently used to prepare porous organic materials with high specific surface area as well as ultrahigh hydrothermal stability. As a typical fast coupling reaction, the traditional stirred solvothermal approach shows the limitation of macroscopic reaction kinetics due to the increasing viscosity of the reaction mixture with the molecular network growth until it turns to a jelly‐like consistency. Herein, a high‐gravity chemical synthetic strategy to achieve rapid and economical preparation of a class of, but not limited to, covalent organic polymers (COPs) with high hydrothermal stability using the Ullman cross‐coupling route is described. The viscous fluid is vigorously split into homogeneous microdroplets through the rotating packed bed (RPB) under the HiGee environment. The HiGee approach shortens the traditional reaction time from 600 to 15 min as well as reduces the usage of high‐cost nickel (0) catalyst by 40 wt%. Specially, the COP‐10 obtained with the HiGee approach displays an excellent deliverable methane capacity of 415 cm3 STP g−1 at 298 K with working pressures 5–65 bar, which is higher than that of most reported porous organic materials.
Ultrasmall Pd‐Cu‐Pt Trimetallic Twin Icosahedrons Boost the Electrocatalytic Performance of Glycerol Oxidation at the Operating Temperature of Fuel Cells
Authors: Yang Fang , Ye JinYu , Yuan Qiang , Yang Xiaotong , Xie Zixuan , Zhao Fengling , Zhou Zhiyou , Gu Lin , Wang Xun 
Published: January 2020

AbstractRecently, in order to improve the energy conversion efficiency of direct polyol fuel cells, the engineering of effective Pd‐ and/or Pt‐based electrocatalysts to rupture CC bonds has received increasing attention. Here, an example is shown to synthesize highly uniform sub‐10 nm Pd‐Cu‐Pt twin icosahedrons by controlling the nucleation phase. Because of the synergies of the electronic effect, synergistic effect, geometric effect, and abundant surface active sites originating from the formation of near surface alloy and special icosahedral shape, the Pd‐Cu‐Pt twin icosahedrons exhibit excellent electrocatalytic performance in glycerol electrocatalysis at the operating temperature of direct alcohol fuel cells (70 °C) in KOH electrolyte. The Pd50.2Cu38.4Pt11.4 icosahedrons show mass activities of 9.7 A mg−1Pd+Pt and 13.7 A mg−1Pd. Furthermore, the Pd50.2Cu38.4Pt11.4 icosahedrons demonstrate long‐term durability in current–time test for 36 000 s and high in situ anti‐CO poisoning performance. In addition, the introduction of CO can enhance electro‐oxidation endurance on Pd50.2Cu38.4Pt11.4 icosahedrons, and the peak mass activity can reach to 14.4 A mg−1Pd+Pt. The in situ Fourier transform infrared spectroscopy spectra indicate that the Pd50.2Cu38.4Pt11.4 icosahedrons possess a high capacity to break CC bonds and may efficiently convert glycerol into CO2, thus improving the utilization efficiency of energy‐containing molecule glycerol.
Nanogenerators with Superwetting Surfaces for Harvesting Water/Liquid Energy
Authors: Wang Yang , Gao Shouwei , Xu Wanghuai , Wang Zuankai 
Published: January 2020

AbstractWater covers about 70% of the earth's surface and contains tremendous energy that remains untapped. Despite success in harvesting hydrodynamic energy based on heavy‐weight and bulky electromagnetic generators, a great deal of water energies stored in the low‐frequency flow of water such as in the form of raindrops, river/ocean waves, and the tide, remain largely untapped. In spite of diversity in development strategies and working mechanisms, engineering efficient water energy harvesting devices, especially nanogenerators, requires the elegant control of interfacial properties of substrates for rapid liquid mass and momentum transfer and effective electron generation/transfer. In particular, inspired by various special wetting phenomena in nature, the design of superwetting surfaces offers a new dimension to fundamentally mediate the way the liquid, as well as the charge, interact with the substrate. Herein, the latest progress in the development of nanogenerators with three distinctive interface types—solid/liquid, solid/solid, and liquid/liquid interfaces—are summarized and their representative applications, challenges, and future perspectives are highlighted.
The Overlapped Electron‐Cloud Model for Electron Transfer in Contact Electrification
Authors: Lin Shiquan , Xu Cheng , Xu Liang , Wang Zhong Lin 
Published: January 2020

AbstractContact electrification (CE) is one of the oldest topics in physics, which has been discussed for more than 2600 years. Recently, an overlapped electron‐cloud (OEC) model was proposed by Wang to explain all types of CE phenomena for general materials in which a deep overlapping of electron clouds belonging to two atoms results in a lowered potential barrier for electron transfer from one to the other by applying a compressive force, which is simply referred to as Wang transition for CE. Here, the degree of electron‐cloud overlap between two atoms is controlled by using tapping mode atomic force microscopy. A temperature difference and electric field are applied between atoms of two surfaces. It is found that electron transfer only occurs when the contact tip and sample interact in the repulsive‐force region, which corresponds to a strong overlap of the electron clouds. Such a fact even preserves if the tip is at a higher temperature than the sample for 120 K. Alternatively, by applying a bias, electron tunneling would occur when the tip is in the attractive‐force region within which normal electron transfer would not occur. These studies solidify the overlapped electron‐cloud model first proposed by Wang. Further, the temperature and bias effects on the CE are explained based on a modified OEC model.
Electromagnetic Shielding of Monolayer MXene Assemblies
Authors: Yun Taeyeong , Kim Hyerim , Iqbal Aamir , Cho Yong Soo , Lee Gang San , Kim Myung‐Ki , Kim Seon Joon , Kim Daesin , Gogotsi Yury , Kim Sang Ouk , Koo Chong Min 
Published: January 2020

AbstractMiniaturization of electronics demands electromagnetic interference (EMI) shielding of nanoscale dimension. The authors report a systematic exploration of EMI shielding behavior of 2D Ti3C2Tx MXene assembled films over a broad range of film thicknesses, monolayer by monolayer. Theoretical models are used to explain the shielding mechanism below skin depth, where multiple reflection becomes significant, along with the surface reflection and bulk absorption of electromagnetic radiation. While a monolayer assembled film offers ≈20% shielding of electromagnetic waves, a 24‐layer film of ≈55 nm thickness demonstrates 99% shielding (20 dB), revealing an extraordinarily large absolute shielding effectiveness (3.89 × 106 dB cm2 g−1). This remarkable performance of nanometer‐thin solution processable MXene proposes a paradigm shift in shielding of lightweight, portable, and compact next‐generation electronic devices.
Methylation Status of the Nanog Promoter Determines the Switch between Cancer Cells and Cancer Stem Cells
Authors: Liu Shupeng , Cheng Kai , Zhang Hui , Kong Ruijiao , Wang Shuo , Mao Chuanbin , Liu Shanrong 
Published: January 2020

AbstractCancer stem cells (CSCs) are the main cause of tumor development, metastasis, and relapse. CSCs are thus considered promising targets for cancer therapy. However, it is hard to eradicate CSCs due to their inherent plasticity and heterogeneity, and the underlying mechanism of the switch between non‐CSCs and CSCs remains unclear. Here, it is shown that miR‐135a combined with SMYD4 activates Nanog expression and induces the switch of non‐CSCs into CSCs. The miR‐135a level, once elevated, lowers the methylation level of the CG5 site in the Nanog promoter by directly targeting DNMT1. SMYD4 binds to the unmethylated Nanog promoter to activate Nanog expression in Nanog‐negative tumor cells. The in vivo regulation of miR‐135a levels could significantly affect both the CSCs proportion and tumor progression. These findings indicate that DNA methylation of the Nanog promoter modulates the switch of non‐CSCs into CSCs under the control of the miRNA‐135 level. In addition, the related pathways, miR‐135a/DNMT1 and SMYD4, involved in these processes are potential targets for CSC‐targeted therapy.
Solution‐Processed High‐Performance p‐Type Perovskite NdAlO3 Thin Films for Transparent Electronics
Authors: Xin Zhijie , Ding Yanan , Zhu Yixin , Fu Chuanyu , Yao Zhao , Chen Qian , Liu Guoxia , Shan Fukai 
Published: January 2020

AbstractTransparent oxide semiconductors exhibit great potential as fundamental building blocks for electronic applications. However, the lack of high‐performance p‐type oxide materials limits their potential applications for transparent electronics. Ternary p‐type perovskite NdAlO3 thin films are prepared by spin coating and annealed at various temperatures. It is demonstrated that neodymium vacancies (VNd) is generated in NdAlO3 thin film, and the presence of VNd results in high hole mobility. The thin‐film transistors (TFTs) based on NdAlO3 thin film are integrated and exhibit typical p‐channel transistor behavior. The TFT based on NdAlO3 thin film annealed at 700 °C exhibits an optimized electrical performance, including a field‐effect mobility (µFE) of 0.19 cm2V−1s−1 and an on/off current ratio (Ion/Ioff) of ≈105. When high‐k Al2O3 dielectric is integrated into the TFTs, the µFE and Ion/Ioff are further improved to 9.93 cm2V−1s−1 and ≈106, respectively. The fabrication of a p–n junction based on p‐NdAlO3/n‐In2O3 heterojunction further confirms the excellent p‐type performance of the perovskite NdAlO3 thin films. This work not only demonstrates the possibility of p‐type perovskite NdAlO3 thin films applicable for transparent electronics, but also provides guidelines for the design of novel p‐type oxide semiconductors.
Fundamentals of Organic Anti‐Ambipolar Ternary Inverters
Authors: Kim Chang‐Hyun , Hayakawa Ryoma , Wakayama Yutaka 
Published: January 2020

AbstractDigital logic accommodating more than two data levels is at the forefront of future high‐information‐density electronics. The fundamental mechanisms of the organic ternary inverters relying on anti‐ambipolarity are revealed. Ideally combining the analytical and predictive capabilities of simulation, the three distinctive regimes of operation are identified, and systematic guidelines for how to balance the “0,” “1/2,” and “1” voltage levels are suggested. Most importantly, the junction energy barrier and minority carrier penetration are found to be critical to this type of inverter. In time with the increasing viability of flexible multi‐valued logic circuits, such theoretical insights are positioned to spearhead the next engineering efforts on optimized performances.
Anisotropic In‐Plane Ballistic Transport in Monolayer Black Arsenic‐Phosphorus FETs
Authors: Zhou Wenhan , Zhang Shengli , Wang Yangyang , Guo Shiying , Qu Hengze , Bai Pengxiang , Li Zhi , Zeng Haibo 
Published: January 2020

AbstractThe performance limits of monolayer arsenic‐phosphorus (AsP) field‐effect transistors (FETs) are explored by first‐principles simulations of ballistic transport in nanoscale devices. The monolayer AsP holds a direct bandgap of 0.92 eV with significantly anisotropic electronic properties. Transfer characteristics of n‐type and p‐type AsP FETs are thoroughly investigated by scaling channel length in the armchair and zigzag direction, respectively. The simulation results indicate that AsP FETs exhibit exceptional device characteristics, such as high on‐state current, short delay time, and low power consumption. Moreover, transfer characteristics demonstrate superior anisotropy on in‐plane electrical transport properties. In particular, in the zigzag direction, even if the channel length is scaled down to 4 nm, the device performance still can satisfy the International Technology Roadmap for Semiconductors high‐performance requirement. Finally, through benchmarking energy‐delay product against other typical 2D FETs, AsP FETs are revealed to be strongly competitive 2D FETs.
A Pure 2H‐MoS2 Nanosheet‐Based Memristor with Low Power Consumption and Linear Multilevel Storage for Artificial Synapse Emulator
Authors: Wang Kaiyang , Li Liteng , Zhao Rujie , Zhao Jianhui , Zhou Zhenyu , Wang Jingjuan , Wang Hong , Tang Baokun , Lu Chao , Lou Jianzhong , Chen Jingsheng , Yan Xiaobing 
Published: January 2020

AbstractTwo‐dimensional (2D) transition metal dichalcogenide has attracted significant attention recently due to its unique electrical and optical properties. However, MoS2 nanosheets fabricated by traditional methods exhibit poor electrical performance due to the existence of the 1T metal phase. A solution‐processable pure 2H semiconductor phase MoS2 nanosheet for use as the functional layer of high‐performance memristors is presented. The resulting memristor based on a Ag/MoS2/Pt structure exhibits excellent resistive switching properties including high endurance and multilevel retention. Moreover, the power consumption and programming current of the SET operation can be as low as 7.35 nW and 100 nA, respectively. Interestingly, it is demonstrated that the resistance of the Ag/MoS2/Pt device can be bidirectionally modulated over a wide range (pulse number >500) with an approximately linear trend. Furthermore, the accuracy of pattern recognition with handwritten data can reach 90.37%. This work provides a simple and practical method for the realization of fabrication of pure 2H‐MoS2 and application in biological neural computing systems.
Soil carbon sequestration in bermudagrass golf course fairways in Lubbock, Texas
Authors: Gautam Prativa , Young Joseph R. , Sapkota Manish , Longing Scott , Weindorf David C. 
Published: January 2020

AbstractTurfgrasses benefit the environment through conversion of CO2 into stable C stored in soils. Limited research on the sequestration potential of bermudagrass (Cynodon spp.) has been conducted in semiarid climates. The objective of this study was to evaluate soil physiochemical properties of golf courses in Lubbock, TX, to determine C sequestration potential and longevity. Soil was obtained from fairways of five golf courses ranging in age from 13 to 93 yr. Shallow (0–7.5 cm) and deeper (7.5–15 cm) soil depths were tested for soil pH, electrical conductivity, soil organic matter, soil organic C (SOC), inorganic C, total N, inorganic N, and texture. After ANOVA and mean separation, principal component analysis (PCA) was used to group golf courses by soil depth or age. Soil organic matter and SOC decreased with depth, but the rate of SOC accumulation (0.22 Mg C ha−1 yr−1) was lower when compared with previous studies. Maximal C (35.1 and 23.7 Mg C ha−1 in the upper and lower depths) was consistent with previous studies, indicating that C accumulated for a longer period of time. The PCA explained 52.7% of variability in soil physiochemical properties on two axes, but PCA more effectively differentiated soil sampling depth than golf course age. High variability in data among fairways at a single golf course likely resulted in limited grouping capabilities. Including a broader regional representation of golf courses or sampling golf courses between 40 and 70 yr to quantify soils near maximal accumulation would strengthen future studies.
Novel Recessive TNNT1 Congenital Core‐Rod Myopathy in French Canadians
Authors: Pellerin David , Aykanat Asli , Ellezam Benjamin , Troiano Emily C. , Karamchandani Jason , Dicaire Marie‐Josée , Petitclerc Marc , Robertson Rebecca , Allard‐Chamard Xavier , Brunet Denis , Konersman Chamindra G. , Mathieu Jean , Warman Chardon Jodi , Gupta Vandana A. , Beggs Alan H. , Brais Bernard , Chrestian Nicolas 
Published: January 2020

ObjectiveRecessive null variants of the slow skeletal muscle troponin T1 (TNNT1) gene are a rare cause of nemaline myopathy that is fatal in infancy due to respiratory insufficiency. Muscle biopsy shows rods and fiber type disproportion. We report on 4 French Canadians with a novel form of recessive congenital TNNT1 core‐rod myopathy.MethodsPatients underwent full clinical characterization, lower limb magnetic resonance imaging (MRI), muscle biopsy, and genetic testing. A zebrafish loss‐of‐function model using morpholinos was created to assess the pathogenicity of the identified variant. Wild‐type or mutated human TNNT1 mRNAs were coinjected with morpholinos to assess their abilities to rescue the morphant phenotype.ResultsThree adults and 1 child shared a novel missense homozygous variant in the TNNT1 gene (NM_003283.6: c.287T > C; p.Leu96Pro). They developed from childhood very slowly progressive limb‐girdle weakness with rigid spine and disabling contractures. They suffered from restrictive lung disease requiring noninvasive mechanical ventilation in 3 patients, as well as recurrent episodes of rhabdomyolysis triggered by infections, which were relieved by dantrolene in 1 patient. Older patients remained ambulatory into their 60s. MRI of the leg muscles showed fibrofatty infiltration predominating in the posterior thigh and the deep posterior leg compartments. Muscle biopsies showed multiminicores and lobulated fibers, rods in half the patients, and no fiber type disproportion. Wild‐type TNNT1 mRNA rescued the zebrafish morphants, but mutant transcripts failed to do so.InterpretationThis study expands the phenotypic spectrum of TNNT1 myopathy and provides functional evidence for the pathogenicity of the newly identified missense mutation. ANN NEUROL 2020;87:568–583
Mitochondrial‐DNA‐Targeted IrIII‐Containing Metallohelices with Tunable Photodynamic Therapy Efficacy in Cancer Cells
Authors: Li Xuezhao , Wu Jinguo , Wang Lei , He Cheng , Chen Liyong , Jiao Yang , Duan Chunying 
Published: January 2020

AbstractThe development of DNA‐targeted photodynamic therapy (PDT) agents for cancer treatment has drawn substantial attention. Herein, the design and synthesis of dinuclear IrIII‐containing luminescent metallohelices with tunable PDT efficacy that target mitochondrial DNA in cancer cells are reported. The metallohelices are fabricated using dynamic imine‐coupling chemistry between aldehyde end‐capped fac‐Ir(ppy)3handles and linear alkanediamine spacers, followed by reduction of the imine linkages. The length and odd–even character of the diamine alkyl linker determined the stereochemistry (helicates vs. mesocates). Compared to the helicates, the mesocates exhibit improved apoptosis‐induction upon white‐light irradiation. Molecular docking studies indicate that the mesocate with a proper length of diamine spacers shows stronger affinity for the minor groove of DNA. This study highlights the potential of DNA‐targeting IrIII‐containing metallohelices as PDT agents.
Modulation of Prins Cyclization by Vibrational Strong Coupling
Authors: Hirai Kenji , Takeda Rie , Hutchison James A. , Uji‐i Hiroshi 
Published: January 2020

AbstractLight‐molecule strong coupling has emerged within the last decade as a new method to control chemical reactions. A few years ago it was discovered that chemical reactivity could be altered by vibrational strong coupling (VSC). Only a limited number of reactions have been investigated under VSC to date, including solvolysis and deprotection reactions. Here the effect of VSC on a series of aldehydes and ketones undergoing Prins cyclization, an important synthetic step in pharmaceutical chemistry, is investigated. A decrease of the second‐order rate constant with VSC of the reactant carbonyl stretching groups is observed. We also observe an increased activation energy due to VSC, but proportional changes in activation enthalpy and entropy, suggesting no substantive change in reaction pathway. The addition of common cycloaddition reactions to the stable of VSC‐modified chemical reactions is another step towards establishing VSC as a genuine tool for synthetic chemistry.
Intrinsically Low Thermal Conductivity and High Carrier Mobility in Dual Topological Quantum Material, n‐Type BiTe
Authors: Samanta Manisha , Pal Koushik , Waghmare Umesh V. , Biswas Kanishka 
Published: January 2020

AbstractA challenge in thermoelectrics is to achieve intrinsically low thermal conductivity in crystalline solids while maintaining a high carrier mobility (μ). Topological quantum materials, such as the topological insulator (TI) or topological crystalline insulator (TCI) can exhibit high μ. Weak topological insulators (WTI) are of interest because of their layered hetero‐structural nature which has a low lattice thermal conductivity (κlat). BiTe, a unique member of the (Bi2)m(Bi2Te3)n homologous series (m:n=1:2), has both the quantum states, TCI and WTI, which is distinct from the conventional strong TI, Bi2Te3 (where m:n=0:1). Herein, we report intrinsically low κlat of 0.47–0.8 W m−1 K−1 in the 300–650 K range in BiTe resulting from low energy optical phonon branches which originate primarily from the localized vibrations of Bi bilayer. It has high μ≈516 cm2 V−1 s−1 and 707 cm2 V−1 s−1 along parallel and perpendicular to the spark plasma sintering (SPS) directions, respectively, at room temperature.
Electron Configuration Modulation of Nickel Single Atoms for Elevated Photocatalytic Hydrogen Evolution
Authors: Jin Xixiong , Wang Rongyan , Zhang Lingxia , Si Rui , Shen Meng , Wang Min , Tian Jianjian , Shi Jianlin 
Published: January 2020

AbstractThe emerging metal single‐atom catalyst has aroused extensive attention in multiple fields, such as clean energy, environmental protection, and biomedicine. Unfortunately, though it has been shown to be highly active, the origins of the activity of the single‐atom sites remain unrevealed to date owing to the lack of deep insight on electronic level. Now, partially oxidized Ni single‐atom sites were constructed in polymeric carbon nitride (CN), which elevates the photocatalytic performance by over 30‐fold. The 3d orbital of the partially oxidized Ni single‐atom sites is filled with unpaired d‐electrons, which are ready to be excited under irradiation. Such an electron configuration results in elevated light response, conductivity, charge separation, and mobility of the photocatalyst concurrently, thus largely augmenting the photocatalytic performance.
Determination of Complex Small‐Molecule Structures Using Molecular Alignment Simulation
Authors: Ibáñez de Opakua Alain , Klama Frederik , Ndukwe Ikenna E. , Martin Gary E. , Williamson R. Thomas , Zweckstetter Markus 
Published: January 2020

AbstractCorrect structural assignment of small molecules and natural products is critical for drug discovery and organic chemistry. Anisotropy‐based NMR spectroscopy is a powerful tool for the structural assignment of organic molecules, but it relies on the utilization of a medium that disrupts the isotropic motion of molecules in organic solvents. Here, we establish a quantitative correlation between the atomic structure of the alignment medium, the molecular structure of the small molecule, and molecule‐specific anisotropic NMR parameters. The quantitative correlation uses an accurate three‐dimensional molecular alignment model that predicts residual dipolar couplings of small molecules aligned by poly(γ‐benzyl‐l‐glutamate). The technique facilitates reliable determination of the correct stereoisomer and enables unequivocal, rapid determination of complex molecular structures from extremely sparse NMR data.