bluuebunny/crossref_metadata_2025_split huggingface dataset:
Tuning the Charge Carrier Polarity of Organic Transistors by Varying the Electron Affinity of the Flanked Units in Diketopyrrolopyrrole‐Based Copolymers
Authors: Liu Qian , Wang Yang , Kohara Akihiro , Matsumoto Hidetoshi , Manzhos Sergei , Feron Krishna , Bottle Steven E. , Bell John , Michinobu Tsuyoshi , Sonar Prashant 
Published: December 2019

AbstractFine‐tuning of the charge carrier polarity in organic transistors is an important step toward high‐performance organic complementary circuits and related devices. Here, three new semiconducting polymers, namely, pDPF‐DTF2, pDPSe‐DTF2, and pDPPy‐DTF2, are designed and synthesized using furan, selenophene, and pyridine flanking group‐based diketopyrrolopyrrole cores, respectively. Upon evaluating their electrical properties in transistor devices, the best performance has been achieved for pDPSe‐DTF2 with the highest and average hole mobility of 1.51 and 1.22 cm2 V−1 s−1, respectively. Most intriguingly, a clear charge‐carrier‐polarity change is observed when the devices are measured under vacuum. The pDPF‐DTF2 polymer exhibits a balanced ambipolar performance with the µh/µe ratio of 1.9, whereas pDPSe‐DTF2 exhibits p‐type dominated charge carrier transport properties with the µh/µe ratio of 26.7. Such a charge carrier transport change is due to the strong electron‐donating nature of the selenophene. Furthermore, pDPPy‐DTF2 with electron‐withdrawing pyridine flanking units demonstrates unipolar n‐type charge transport properties with an electron mobility as high as 0.20 cm2 V−1 s−1. Overall, this study demonstrates a simple yet effective approach to switch the charge carrier polarity in transistors by varying the electron affinity of flanking groups of the diketopyrrolopyrrole unit.
Advanced MoSe2/Carbon Electrodes in Li/Na‐Ions Batteries
Authors: Ge Peng , Zhang Limin , Yang Yue , Sun Wei , Hu Yuehua , Ji Xiaobo 
Published: December 2019

AbstractSecondary charge batteries have captured numerous attentions, owing to their abundant raw, portability, and high energy density. As the main ions‐storage carrier, the electrode materials serve vital roles on the properties of whole battery system. Currently, MoSe2 is regarded as rising star of transition metal dichalcogenides, displaying unique layered structure, high electronic conductivity, as well as narrow energy band. These advantages enable their widely application on hydrogen evolution reactions and solar cells. Recently, a plenty of researching activities on MoSe2/carbon are triggered due to large interplanar spacing and high ions/e− migration rate. In this review, the recent achievements of diverse MoSe2/carbon on great energy‐storage domains are solidly summarized from bonding types (surface‐loading, internal‐wrapped) and dimensional controlling (1D nanotubes/nanofibers, 2D graphene/nanosheets, 3D carbon framework/sphere). Meanwhile, the related Li/Na ions‐storage mechanisms are also concluded. Furthermore, for MoSe2/carbon with better electrochemical properties, the opportunities and perspectives in the future are also suggested. This review throws light on the systematic developments of advanced MoSe2/carbon, and confirms its exploring potential on lithium‐ion batteries/sodium‐ion batteries.
Low‐Threshold Amplified Spontaneous Emission and Lasing from Thick‐Shell CdSe/CdS Core/Shell Nanoplatelets Enabled by High‐Temperature Growth
Authors: Zhang Lei , Yang Hongyu , Yu Buyang , Tang Ying , Zhang Chunfeng , Wang Xiaoyong , Xiao Min , Cui Yiping , Zhang Jiayu 
Published: December 2019

AbstractColloidal semiconductor nanoplatelets (NPLs) have recently emerged as highly promising optical gain medium because of their superior optical properties. Here, the shell‐thickness‐dependent optical gain properties of CdSe/CdS core/shell NPLs synthesized by high‐temperature growth are systematically investigated for the first time. The core/shell NPLs show the increased quantum yields and enhanced photostability as well as clear reduced emission blinking, thanks to the preferable passivation of nonradiative surface defects by the growth of the high‐quality CdS shells under high reaction temperature. Meanwhile, the amplified spontaneous emission (ASE) performance of CdSe/CdS NPLs indicates a nonmonotonic dependence on the shell thickness. The ASE threshold is achieved as low as ≈4.4 µJ cm−2 for thick‐shell NPLs with six monolayer CdS shells, and exhibiting ultrafast transient dynamics process (≈11 ps). Besides, an extremely long lifetime (>800 ps) and large bandwidth (>140 nm) of optical gain are observed by employing ultrafast transient absorption spectroscopy. Finally, a thick‐shell NPLs vertical cavity surface‐emitting laser is developed, which demonstrates spatially directional single‐mode operation with an ultralow lasing threshold of ≈1.1 µJ cm−2. These excellent results are attributed to the remarkable optical gain performance of core/shell NPLs and represent an important step toward practical NPL laser devices.
Theory‐Guided Defect Tuning through Topochemical Reactions for Accelerated Discovery of UVC Persistent Phosphors
Authors: Li Hong , Liu Qi , Ma Ju‐Ping , Feng Zhao‐Yang , Liu Jian‐Dang , Zhao Qing , Kuroiwa Yoshihiro , Moriyoshi Chikako , Ye Bang‐Jiao , Zhang Jun‐Ying , Duan Chang‐Kui , Sun Hong‐Tao 
Published: December 2019

AbstractLong persistent phosphors (LPPs) have attracted enduring attention owing to their wide applications. However, the discovery of LPPs is thus far largely the results of trial and error. Here, theory‐guided defect tuning through topochemical reactions is demonstrated for accelerated discovery of emerging LPPs. First‐principles calculations are employed to identify the thermodynamic charge‐transition levels of different defect states, which help examine whether the candidate structure is a suitable host for afterglow. Rationally tuning the species and concentrations of defects through topochemical reactions is then illustrated, which leads to discovery of Pr3+‐doped LaPO4 featuring ultraviolet C afterglow with a lasting time of over 2 h. Such a strategy, in conjunction with advanced characterizations including high‐resolution synchrotron X‐ray diffraction, positron annihilation lifetime spectroscopy, and electron spin resonance, suggests a radical‐involved afterglow mechanism. Importantly, it is illustrated that this concept can be extended for the discovery of more LPPs. It is suggested that theory‐guided defect engineering enabled by topochemical reactions can be used as a powerful tool to accelerate discovery of novel LPPs with much clearer afterglow mechanisms, with implications even for the design of other optoelectronic materials.
Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion
Authors: Zhu Yuanzhi , Sokolowski Joshua , Song Xiancheng , He Yanghua , Mei Yi , Wu Gang 
Published: December 2019

AbstractCarbon‐based heteroatom‐coordinated single‐atom catalysts (SACs) are promising candidates for energy‐related electrocatalysts because of their low‐cost, tunable catalytic activity/selectivity, and relatively homogeneous morphologies. Unique interactions between single metal sites and their surrounding coordination environments play a significant role in modulating the electronic structure of the metal centers, leading to unusual scaling relationships, new reaction mechanisms, and improved catalytic performance. This review summarizes recent advancements in engineering of the local coordination environment of SACs for improved electrocatalytic performance for several crucial energy‐convention electrochemical reactions: oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, CO2 reduction reaction, and nitrogen reduction reaction. Various engineering strategies including heteroatom‐doping, changing the location of SACs on their support, introducing external ligands, and constructing dual metal sites are comprehensively discussed. The controllable synthetic methods and the activity enhancement mechanism of state‐of‐the‐art SACs are also highlighted. Recent achievements in the electronic modification of SACs will provide an understanding of the structure–activity relationship for the rational design of advanced electrocatalysts.
Characteristics of decline in cognition and locomotion among the elderly in seven provinces of China
Authors: Liu Xiaoshuang , Luo Senlin , Zeng Ping , Gong Huan , Zhang Yan , Zhang Enyi , Han Yiwen , Pan Limin , Pang Jing , Zhang Tiemei 
Published: December 2019

AbstractBackgroundDecline in cognition and in locomotion is associated with aging. However, the relationship between them and the current occurrence of them in Chinese elderly people was weak.MethodsTo investigate the details of these two functions in Chinese elderly people and to try to find some early recognition and intervention clues, data of MMSE test and usual gait speed from 4487 elderly people from seven provinces in China were analysed.ResultsThe prevalence of mild cognitive impairment (MCI) and dementia in persons aged 60 and over was 17.83% and 4.08%, respectively. Among 11 items of MMSE, calculation, three‐word recall, drawing two pentagons, and temporal orientation were the most commonly impaired items in persons with MCI or dementia. The gait speed of old persons with dementia was significantly slower than that of persons with MCI or NCI. Meanwhile, old persons with gait speed >1.39 m/s fast gait speed also had high MMSE scores and no dementia was detected by MMSE.ConclusionThe prevalence of dementia observed in this population was similar to that reported 20 years ago. Loss of temporal orientation and drawing two pentagons may supply more information for early recognition of cognitive impairment. Maintaining locomotion in a proper way may help old persons to prevent cognitive function decline.
Food retail expansion patterns in Sub‐Saharan Africa and the Middle East and North Africa: Institutional and regional perspectives
Authors: Bahn Rachel A. , Abebe Gumataw K. 
Published: December 2019

AbstractFood retail transformation in developing countries continues to receive attention due to its implications for business expansion and food system development. We assess the dynamism of supermarketization in two relatively understudied regions—Sub‐Saharan Africa and the Middle East and North Africa—applying the institution‐based view and econometric analysis of a pooled cross‐sectional dataset of over 700 country‐year observations. While modern food retail has shown rapid growth, the traditional food retail segment is still dominant in both regions. The observed food retail patterns may be attributed to economic factors (income levels), sociodemographic (female labor force participation, urbanization, and religion), and institutional factors (control of corruption, ease of starting a business, time to enforce a contract, and World Trade Organization membership). However, while economic and sociodemographic variables exhibit similar effects in both regions, results are mixed regarding the institutional factors; potential explanations are suggested [EconLit citations: O100, L100].
Sulfonated poly(ether ether ketone)/s–TiO2composite membrane for a vanadium redox flow battery
Authors: Wang Gang , Wang Fei , Li Anfeng , Zhang Miaomiao , Zhang Jie , Chen Jinwei , Wang Ruilin 
Published: December 2019

ABSTRACTThe SPEEK/s‐TiO2composite membrane was prepared by blending sulfonated poly(ether ether ketone) (SPEEK) and sulfonated titanium dioxide (s‐TiO2) nanoparticles. The important physiochemical parameters such as proton conductivity, water uptake, swelling degree and ion exchange capacity of the composite membrane were measured. The thermal stability and chemical stability were also tested. It was observed that the SPEEK/s‐TiO2composite membrane exhibited the best selectivity (7.13 × 104 S·min·cm−3) accompanying high proton conductivity (0.061 S·cm−1) and low tetravalent vanadium ion (VO2+) permeability (8.55 × 10−7cm2·min−1) compared with Nafion117, SPEEK and SPEEK/TiO2membranes. The battery performance with these membranes was characterized by charge–discharge cycling tests and it was found that the SPEEK/s‐TiO2composite membrane showed the highest energy efficiency (EE) up to 82.3%, indicating the SPEEK/s‐TiO2composite membrane is a candidate for vanadium redox flow battery (VRFB) application. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci.2020,137, 48830.
Hybrid control of synchronization of fractional order nonlinear systems
Authors: Mohadeszadeh Milad , Pariz Naser 
Published: December 2019

AbstractUnder the existence of model uncertainties and external disturbance, finite‐time projective synchronization between two identical complex and two identical real fractional‐order (FO) chaotic systems are achieved by employing FO sliding mode control approach. In this paper, to ensure the occurrence of synchronization and asymptotic stability of the proposed methods, a sliding surface is designed and the Lyapunov direct method is used. By using integer and FO derivatives of a Lyapunov function, three different FO real and complex control laws are derived. A hybrid controller based on a switching law is designed. Its behavior is more efficient that if the individual controllers were designed based on the minimization of an appropriate cost function. Numerical simulations are implemented for verifying the effectiveness of the methods.
LncRNA GMDS‐AS1 inhibits lung adenocarcinoma development by regulating miR‐96‐5p/CYLD signaling
Authors: Zhao Ming , Xin Xiao‐Feng , Zhang Jian‐Ya , Dai Wei , Lv Tang‐Feng , Song Yong 
Published: December 2019

AbstractAccording to the global cancer statistic, lung cancer is one of the most dangerous tumors, which poses a serious threat to human health. Exploration the mechanism of lung cancer and new targeted therapeutic measures is always the hot topic. Long noncoding RNA (lncRNA) is an important factor affecting the development of tumors. However, the research on the mechanism of lncRNA in the progress of lung cancer needs to be further expanded. In this study, we found that the expression of lncRNA GMDS‐AS1 was significantly reduced in lung adenocarcinoma (LUAD) tissues and cells. Upregulated GMDS‐AS1 can significantly inhibit the proliferation of LUAD cells and promote cell apoptosis in vitro and in vivo. The results indicate that GMDS‐AS1 acts as a tumor suppressor gene to affect the development of LUAD. Further studies revealed that GMDS‐AS1 is a target gene of miR‐96‐5p, and GMDS‐AS1 regulates proliferation and apoptosis of LUAD cells in association with miR‐96‐5p. In addition, we also confirmed that CYLD lysine 63 deubiquitinase (CYLD) is also a target gene of miR‐96‐5p. Through various validations, we confirmed that GMDS‐AS1 can act as a ceRNA to upregulate the expression of CYLD by sponging miR‐96‐5p. Moreover, the intervention of GMDS‐AS1/miR‐96‐5p/CYLD network can regulate the proliferation and apoptosis of LUAD cells. In this study, we revealed that the GMDS‐AS1/miR‐96‐5p/CYLD network based on ceRNA mechanism plays an important role in the development of LUAD and provides a new direction and theoretical basis for targeted therapy of LUAD.
Analysis of the Destabilization of Bacterial Membranes by Quaternary Ammonium Compounds: A Combined Experimental and Computational Study
Authors: Alkhalifa Saleh , Jennings Megan C. , Granata Daniele , Klein Michael , Wuest William M. , Minbiole Kevin P. C. , Carnevale Vincenzo 
Published: December 2019

AbstractThe mechanism of action of quaternary ammonium compound (QAC) antiseptics has long been assumed to be straightforward membrane disruption, although the process of approaching and entering the membrane has little modeling precedent. Furthermore, questions have more recently arisen regarding bacterial resistance mechanisms, and why select classes of QACs (specifically, multicationic QACs) are less prone to resistance. In order to better understand such subtleties, a series of molecular dynamics simulations were utilized to help identify these molecular determinants, directly comparing mono‐, bis‐, and triscationic QACs in simulated membrane intercalation models. Three distinct membranes were simulated, mimicking the surfaces of Escherichia coli and Staphylococcus aureus, as well as a neutral phospholipid control. By analyzing the resulting trajectories in the form of a timeseries analysis, insight was gleaned regarding the significant steps and interactions involved in the destabilization of phospholipid bilayers within the bacterial membranes. Finally, to more specifically probe the effect of the hydrophobic section of the amphiphile that presumably penetrates the membrane, a series of alkyl‐ and ester‐based biscationic quaternary ammonium compounds were prepared, tested for antimicrobial activity against both Gram‐positive and Gram‐negative bacteria, and modeled.
Case report describing late balloon dilatation as a treatment for paravalvular leak with intuity elite rapid deployment valve
Authors: Pal Nikhil , Jones Dylan , Rice Gregory , Sinhal Ajay 
Published: December 2019

AbstractUse of sutureless bioprostheses for aortic valve replacement has increased in recent years as compared to conventional prostheses, though with the potential issue of paravalvular leak, which requires close follow‐up. We present this case report describing the successful treatment of paravalvular leak in a 65 year old man, who had NYHA class III symptoms post implantation of a 21 mm Intuity Elite rapid deployment bioprosthesis (Edwards Lifesciences, Irvine, CA). Diagnosis was established using TTE, TOE, and Cardiac MRI. Performing balloon dilatation using an Atlas Gold balloon (BARD Peripheral Vascular Inc., Tempe, AZ) treated the likely inadequate expansion of the subvalvular stent, leading to significant reduction in the paravalvular leak. At one month follow‐up patient reported complete resolution of his symptoms. Successful percutaneous treatment of paravalvular leak following implantation of rapid deployment sutureless bioprosthesis provides a new treatment strategy for these patients; this strategy requires further validation.
Doping‐Assisted Phase Changing Effect on MoS2 Towards Hydrogen Evolution Reaction in Acidic and Alkaline pH
Authors: Bolar Saikat , Shit Subhasis , Murmu Naresh C. , Kuila Tapas 
Published: December 2019

AbstractHydrogen evolution reaction (HER) was improved through nitrogen (N) doping in molybdenum disulfide (MoS2) due to the formation of 1T‐metallic phase as compared to the thermodynamically stable 2H‐semiconducting phase. Generally, the phase transition of MoS2 from semiconducting 2H to metallic 1T was carried out by chemical intercalation method. A facile solvothermal synthetic procedure is used to organize 1T@2H MoS2 nanoflower by incorporating N in MoS2 crystal lattice which improved the catalytic activity with the generation of metallic property of MoS2. Optimized N doping is an effective strategy for the development of mixed phase MoS2. Physicochemical characterization techniques confirmed the formation of hybrid phase (1T@2H) MoS2 by N incorporation. A tuned dopant concentration in MoS2 crystal lattice effectively enhanced the catalytic performance by modifying the physical and chemical properties. Moreover, optimal N doped MoS2 offered a very low overpotential of ∼108 and ∼141 mV to reach the benchmarking current density of 10 mA cm−2 for HER in acidic and basic medium, respectively. This work elucidated a rational implantation of phase engineering, which is an efficient strategy to develop efficient electrocatalysts, shedding light on the improvement of transition metal‐based electrocatalyst in renewable energy technologies.
Effect of Dual‐Salt Concentrated Electrolytes on the Electrochemical Performance of Silicon Nanoparticles
Authors: Chang Zeng‐hua , Li Xiang , Yun Feng‐ling , Shao Ze‐chao , Wu Zhao‐hui , Wang Jian‐tao , Lu Shi‐gang 
Published: December 2019

AbstractAs a promising anode material, silicon has attracted extensive attention. The instability of the electrode/electrolyte interphase due to the inherent volume variation upon (de)lithiation is one of the major factors limiting the commercialization of silicon anode materials. Here, we report a concentrated electrolyte with lithium bis(fluorosulfonyl)imide (LiFSI) and lithium difluoro (oxalate) borate (LiDFOB) dual salt to enhance the control of the species constituting the solid electrolyte interphase (SEI) on the surface of the silicon material. The silicon nanoparticle (SiNP) electrode with the dual‐salt LiFSI0.7LiDFOB0.3‐(PC)4 concentrated electrolyte delivers a relatively high average coulombic efficiency of 97.68 % and a remarkably improved cycling performance with an initial capacity of approximately 3300 mAh g−1 and a capacity retention around 2000 mAh g−1 after 100 cycles. It is found that the polarity of the B−F bond of LiDFOB decreases when the molar ratio of LiDFOB to LiFSI is greater than 0.3 : 0.7. Therefore, the reduction of LiDFOB through a ring‐opening reaction coupled with a ring‐opening reaction of PC becomes dominant. The SEI layer rich in the corresponding products Li(BF2O)n polymer could suppress the rupture of the Si particles and excessive growth of the SEI layer, thus could further mitigate the decrease of coulombic efficiency.
A General Pathway to Heterobimetallic Triple‐Decker Complexes
Authors: Piesch Martin , Dielmann Fabian , Reichl Stephan , Scheer Manfred 
Published: December 2019

AbstractA systematic study on the reactivity of the triple‐decker complex [(Cp’’’Co)2(μ,η4:η4‐C7H8)] (A) (Cp’’’=1,2,4‐tritertbutyl‐cyclopentadienyl) towards sandwich complexes containing cyclo‐P3, cyclo‐P4, and cyclo‐P5 ligands under mild conditions is presented. The heterobimetallic triple‐decker sandwich complexes [(Cp*Fe)(Cp’’’Co)(μ,η5:η4‐P5)] (1) and [(Cp’’’Co)(Cp’’’Ni)(μ,η3:η3‐P3)] (3) (Cp*=1,2,3,4,5‐pentamethylcyclopentadienyl) were synthesized and fully characterized. In solution, these complexes exhibit a unique fluxional behavior, which was investigated by variable temperature NMR spectroscopy. The dynamic processes can be blocked by coordination to {W(CO)5} fragments, leading to the complexes [(Cp*Fe)(Cp’’’Co)(μ3,η5:η4:η1‐P5){W(CO)5}] (2 a), [(Cp*Fe)(Cp’’’Co)(μ4,η5:η4:η1:η1‐P5){(W(CO)5)2}] (2 b), and [(Cp’’’Co)(Cp’’’Ni)(μ3,η3:η2:η1‐P3){W(CO)5}] (4), respectively. The thermolysis of 3 leads to the tetrahedrane complex [(Cp’’’Ni)2(μ,η2:η2‐P2)] (5). All compounds were fully characterized using single‐crystal X‐ray structure analysis, NMR spectroscopy, mass spectrometry, and elemental analysis.
Transition‐Metal‐Free Multiple Functionalization of Piperidines to 4‐Substituted and 3,4‐Disubstituted 2‐Piperidinones
Authors: Chamorro‐Arenas Delfino , Nolasco‐Hernández Alejandro A. , Fuentes Lilia , Quintero Leticia , Sartillo‐Piscil Fernando 
Published: December 2019

AbstractRemote and multiple functionalization of piperidines without the use of transition‐metal catalysts and elaborate directing groups is one of the major challenges in organic synthesis. Herein is reported an unprecedented two‐step protocol that enables the multiple functionalization of piperidines to either 4‐substituted ortrans‐3,4‐disubstituted 2‐piperidones. First, by exploiting the duality of TEMPO reactivity, which under oxidative and thermal conditions fluctuates between cationic and persistent‐radical form, a novel multiple C(sp3)‐H oxidation of piperidines to α,β‐unsaturated 2‐piperidones was developed. Second, the intrinsic low reactivity of the unsaturated piperidones toward conjugated Grignard additions was overcome by using trimethylsilyl chloride (TMSCl) as Lewis acid. Subsequently, conjugated Grignard addition/electrophilic trapping protocol provided substituted 2‐piperidone intermediates, some of which were then transformed into pharmaceutical alkaloids.