bluuebunny/crossref_metadata_2025_split huggingface dataset:
Bioinspired Catechol‐Grafting PEDOT Cathode for an All‐Polymer Aqueous Proton Battery with High Voltage and Outstanding Rate Capacity
Authors: Zhu Meihua , Zhao Li , Ran Qing , Zhang Yingchao , Peng Runchang , Lu Geyu , Jia Xiaoteng , Chao Danming , Wang Caiyun 
Published: December 2021

AbstractAqueous all‐polymer proton batteries (APPBs) consisting of redox‐active polymer electrodes are considered safe and clean renewable energy storage sources. However, there remain formidable challenges for APPBs to withstand a high current rate while maximizing high cell output voltage within a narrow electrochemical window of aqueous electrolytes. Here, a capacitive‐type polymer cathode material is designed by grafting poly(3,4‐ethylenedioxythiophene) (PEDOT) with bioinspired redox‐active catechol pendants, which delivers high redox potential (0.60 V vs Ag/AgCl) and remarkable rate capability. The pseudocapacitive‑dominated proton storage mechanism illustrated by the density functional theory (DFT) calculation and electrochemical kinetics analysis is favorable for delivering fast charge/discharge rates. Coupled with a diffusion‐type anthraquinone‐based polymer anode, the APPB offers a high cell voltage of 0.72 V, outstanding rate capability (64.8% capacity retention from 0.5 to 25 A g−1), and cycling stability (80% capacity retention over 1000 cycles at 2 A g−1), which is superior to the state‐of‐the‐art all‐organic proton batteries. This strategy and insight provided by DFT and ex situ characterizations offer a new perspective on the delicate design of polymer electrode patterns for high‐performance APPBs.
Ternary Logic with Stateful Neural Networks Using a Bilayered TaOX‐Based Memristor Exhibiting Ternary States
Authors: Kim Young Seok , An Jangho , Jeon Jae Bum , Son Myeong Won , Son Seoil , Park Woojoon , Lee Younghyun , Park Juseong , Kim Geun Young , Kim Gwangmin , Song Hanchan , Kim Kyung Min 
Published: December 2021

AbstractA memristive stateful neural network allowing complete Boolean in‐memory computing attracts high interest in future electronics. Various Boolean logic gates and functions demonstrated so far confirm their practical potential as an emerging computing device. However, spatio‐temporal efficiency of the stateful logic is still too limited to replace conventional computing technologies. This study proposes a ternary‐state memristor device (simply a ternary memristor) for application to ternary stateful logic. The ternary‐state implementable memristor device is developed with bilayered tantalum oxide by precisely controlling the oxygen content in each oxide layer. The device can operate 157 ternary logic gates in one operational clock, which allows an experimental demonstration of a functionally complete three‐valued Łukasiewicz logic system. An optimized logic cascading strategy with possible ternary gates is ≈20% more efficient than conventional binary stateful logic, suggesting it can be beneficial for higher performance in‐memory computing.
Pressure‐Perceptive Actuators for Tactile Soft Robots and Visual Logic Devices
Authors: Zhou Peidi , Lin Jian , Zhang Wei , Luo Zhiling , Chen Luzhuo 
Published: December 2021

AbstractSoft actuators with sensing capabilities are important in intelligent robots and human–computer interactions. However, present perceptive actuating systems rely on the integration of multiple functional units with complex circuit design. Here, a new‐type pressure‐perceptive actuator is reported, which integrates functions of sensing, actuating, and decision making at material level without complex combination. The actuator is composed of an actuating unit and a pressure‐sensing unit, both of which are fabricated by carbon nanotube (CNT), silk, and polymer composite. On the one hand, the actuating unit can be driven by low voltages (<13 V), owing to a Joule‐heating effect. On the other hand, the current passing the pressure‐sensing unit can be controlled by tactile pressure. In the integrated actuator, it is able to control the deformation amplitude of actuating unit by applying different pressures on the pressure‐sensing unit. A portable tactile‐activated gripper is fabricated to operate an object through pressure control, demonstrating its application in tactile soft robots. Finally, three visual logic gates (AND, OR, and NOT) are proposed, which convert “tactile” inputs into “visible” deformation outputs, using the CNT‐silk‐based material for sensing and actuating in the decision‐making process. This study provides a new path for intelligent soft robots and new‐generation logic devices.
Catalytic Halogen‐Exchange Fluorination of 4‐Chlorobenzaldehyde to 4‐Fluorobenzaldehyde, a Greener Process
Authors: Li Xiukai , Yongcai Wu , Lijuan Shi , Zhang Yugen 
Published: December 2021

AbstractThe direct halogen‐exchange fluorination of 4‐chlorobenzaldehyde was studied under solvent‐free and various diphenyl solvents conditions using spray‐dried KF as a fluorinating agent. Aspects influencing the selectivity and yield of product were investigated in detail, including catalysts and solvents selection, reaction conditions optimization, and side product control. We paid more attention to issues from a perspective of industrial process, such as product separation and catalyst/solvent recycling. The reaction works efficiently with tetraphenyl phosphonium bromide as a phase transfer catalyst under solvent free conditions and in diphenyl solvents. Under the optimum reaction conditions, the yield of 4‐fluorobenzaldehyde reached 90% with a selectivity of 98%.
Enantioselective Synthesis of Oxazaborolidines by Palladium‐Catalyzed N−H/B−H Double Activation of 1,2‐Azaborines
Authors: Morita Taiki , Murakami Hiroki , Asawa Yasunobu , Nakamura Hiroyuki 
Published: December 2021

AbstractA palladium‐catalyzed N−H/B−H double activation of 1,2‐dihydro‐1,2‐benzazaborines proceeded via cycloaddition with vinyl ethylene carbonate to produce polycyclic oxazaborolidines in 31–96 % yield. The key step in this process is the release of molecular hydrogen from a borate intermediate. Using a SPINOL‐derived phosphoramidite as a chiral ligand, chiral oxazaborolidines were synthesized in good to high yields with excellent enantioselectivity (up to 95 % ee). The vinyl group of the resulting oxazaborolidine underwent metathesis, Heck reaction, and Wacker oxidation without affecting the oxazaborolidine framework.
Mesoporosity‐Enabled Selectivity of Mesoporous Palladium‐Based Nanocrystals Catalysts in Semihydrogenation of Alkynes
Authors: Lv Hao , Qin Huaiyu , Sun Mingzi , Jia Fengrui , Huang Bolong , Liu Ben 
Published: December 2021

AbstractWe reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1‐phenyl‐1‐propyne, all of which are remarkably better than commercial Lindlar catalysts. Mechanistic investigations ascribed high semihydrogenation selectivity to the continuous crystalline framework and penetrated mesoporous channel of catalysts that weakened the adsorption and interaction capacity of alkenes and thus inhibited over‐hydrogenation of alkenes to industrially unfavorable alkanes. Density functional theory calculations further demonstrated that convex crystalline mesoporosity of nanobundles catalysts electronically optimized the coordination environment of Pd active sites and energetically changed hydrogenation trends, resulting in a superior semihydrogenation selectivity to targeted alkenes.
12b,24b‐Diborahexabenzo[a,c,fg,l,n,qr]pentacene: A Low‐LUMO Boron‐Doped Polycyclic Aromatic Hydrocarbon
Authors: Mützel Carina , Farrell Jeffrey M. , Shoyama Kazutaka , Würthner Frank 
Published: December 2021

AbstractHerein we devise and execute a new synthesis of a pristine boron‐doped nanographene. Our target boron‐doped nanographene was designed based on DFT calculations to possess a low LUMO energy level and a narrow band gap derived from its precise geometry and B‐doping arrangement. Our synthesis of this target, a doubly B‐doped hexabenzopentacene (B2‐HBP), employs six net C−H borylations of an alkene, comprising consecutive hydroboration/electrophilic borylation/dehydrogenation and BBr3/AlCl3/2,6‐dichloropyridine‐mediated C−H borylation steps. As predicted by our calculations, B2‐HBP absorbs strongly in the visible region and emits in the NIR up to 1150 nm in o‐dichlorobenzene solutions. Furthermore, B2‐HBP possesses a very low LUMO level, showing two reversible reductions at −1.00 V and −1.17 V vs. Fc+/Fc. Our methodology is surprisingly selective despite its implementation of unfunctionalized precursors and offers a new approach to the synthesis of pristine B‐doped polycyclic aromatic hydrocarbons.
Supported σ‐Complexes of Li−C Bonds from Coordination of Monomeric Molecules of LiCH3, LiCH2CH3 and LiC6H5 to Mo≣Mo Bonds
Authors: Pérez‐Jiménez Marina , Campos Jesús , Jover Jesús , Álvarez Santiago , Carmona Ernesto 
Published: December 2021

AbstractLiCH3 and LiCH2CH3 react with the complex [Mo2(H)2(μ‐AdDipp2)2(thf)2] (1⋅thf) with coordination of two molecules of LiCH2R (R=H, CH3) and formation of complexes [Mo2{μ‐HLi(thf)CH2R}2(AdDipp2)2], 5⋅LiCH3 and 5⋅LiCH2CH3, respectively (AdDipp2=HC(NDipp)2; Dipp=2,6‐iPr2C6H3; thf=C4H8O). Due to steric hindrance, only one molecule of LiC6H5 adds to 1⋅thf generating the complex [Mo2(H){μ‐HLi(thf)C6H5}(μ‐AdDipp2)2], (4⋅LiC6H5). Computational studies disclose the existence of five‐center six‐electron bonding within the H−Mo≣Mo−C−Li metallacycles, with a mostly covalent H−Mo≣Mo−C group and predominantly ionic Li−C and Li−H interactions. However, the latter bonds exhibit non‐negligible covalency, as indicated by X‐ray, computational data and the large one‐bond 6,7Li,1H and 6,7Li,13C NMR coupling constants found for the three‐atom H−Li−C chains. By contrast, the phenyl group in 4⋅LiC6H5 coordinates in an η2 fashion to the lithium atom through the ipso and one of the ortho carbon atoms.
A Heme‐Acquisition Protein Reconstructed with a Cobalt 5‐Oxaporphyrinium Cation and Its Growth‐Inhibition Activity Toward Multidrug‐Resistant Pseudomonas aeruginosa
Authors: Takiguchi Asahi , Sakakibara Erika , Sugimoto Hiroshi , Shoji Osami , Shinokubo Hiroshi 
Published: December 2021

AbstractUsing artificial hemes for the reconstruction of natural heme proteins represents a fascinating approach to enhance the bioactivity of the latter. We report the synthesis of various metal 5‐oxaporphyrinium cations as cofactors, and a cobalt 5‐oxaporphyrinium cation was successfully incorporated into the heme‐acquisition protein (HasA) secreted by Pseudomonas aeruginosa. We hypothesize that the oxaporphyrinium cation strongly binds to the HasA‐specific outer membrane receptor (HasR) due to its cationic charge, which prevents the subsequent acquisition of heme. In fact, the reconstructed HasA inhibited the growth of Pseudomonas aeruginosa and even of multidrug‐resistant P. aeruginosa.
Design of a near‐infrared‐triggered photo/thermal dual‐responsive composite carrier with excellent biocompatibility for controllable drug release
Authors: Tian Mengyuan , Xin Fuhua , Gao Yanjing , Nie Jun , Sun Fang 
Published: December 2021

AbstractA near‐infrared (NIR)‐triggered photo/thermal dual‐responsive composite carrier (UCNPs‐NG‐PDA) was designed and fabricated by the incorporation of upconversion nanoparticles (UCNPs), coumarin‐based photo/thermal‐responsive nanogel (NG) with uniform particle size (193 nm) and polydopamine (PDA) particles. UCNPs‐NG‐PDA has good photothermal conversion capability because of the introduction of PDA. The light and heat dual‐responsiveness of coumarin‐based nanogels markedly enhances the drug release of UCNPs‐NG‐PDA. Under NIR irradiation for only 20 min, the final cumulative release reaches 79.4% and is much higher than that (58.8%) under UV irradiation. More remarkably, the UCNPs‐NG‐PDA exhibits an excellent biocompatibility and has fascinating application prospects in drug delivery fields.
Balancing load and performance for different failure models
Authors: Finkelstein Maxim , Cha Ji Hwan , Chackraborty Niladri 
Published: December 2021

AbstractIn this article, we discuss an optimal loading for items with lifetimes described by failure models that are popular in reliability and statistics. The obtained results can be relevant, for example, for production/manufacturing systems. The expected productivity and the mission success probability are maximized with respect to the value of a load. It is shown that the optimal load for the considered settings is not necessarily the load that maximizes the production rate. The crucial function in our discussion is the production rate over the load. It is shown that, depending on the model, the optimal load can be equal, smaller or larger than the value of the load that achieves the maximum of this function. The accelerated life and the proportional hazards failure models are considered, as well as the additive hazards model. Illustrative examples confirm our theoretical findings.
Hedging and utility valuation of a defaultable claim driven by Hawkes processes
Authors: Pasricha Puneet , Selvamuthu Dharmaraja , Tardelli Paola 
Published: December 2021

AbstractThis article studies the problem of hedging a defaultable claim via the maximization of the mean value of exponential utility, over a set of admissible strategies. The dynamics of the underlying asset is assumed to be governed by mutually exciting Hawkes processes, which captures the jumps clustering phenomenon observed in the market. The resulting market is incomplete and does not allow perfect replication. Hence, a dynamic programming approach is adopted to characterize the value function as the largest solution to a suitable backward stochastic differential equation (BSDE) with a non‐Lipschitz generator. The value function of the optimal investment problem and of the indifference prices are represented in terms of limits of the sequence of value functions of suitable Lipschitz BSDEs and, further, a result of uniqueness is achieved. Finally, numerical experiments are performed to demonstrate the applicability of the proposed framework and to understand the impact of the jump‐clustering on the values of the claims.
The imperfect fit: Fetal alcohol spectrum disorder as the basis to commit individuals involuntarily as sexually violent predators/persons
Authors: Abbott Brian R. 
Published: December 2021

AbstractPrenatal alcohol exposure produces a broad range of primary disabilities that lead to adverse life course outcomes in children raised in adverse environments. Inappropriate sexual behaviors are a commonly occurring secondary disability, with a large minority of individuals with fetal alcohol spectrum disorder (FASD) displaying sexual aggression. Adults with FASD who commit repeated criminal sexual acts may be subject to legal proceedings for indefinite involuntary civil confinement as sexually violent predators/persons (SVP) in certain jurisdictions in the United States. Studies about the diagnostic practices among psychologists and psychiatrists retained by states to evaluate individuals as SVP do not recognize FASD as a mental disorder, despite the likelihood that hundreds of individuals petitioned for involuntary commitment suffer from FASD. Establishing an FASD diagnosis may provide exculpatory evidence to refute a government petition that an individual suffers from a mental condition that affects emotional or volitional capacity by predisposing the person to committing criminal sexual behavior. This article provides a framework for identifying, assessing, and deciding whether individuals with the FASD diagnosis suffer from the legally defined mental disorder that is necessary to indefinitely confine individuals as SVP.
Impact of Barrett oesophagus diagnoses and endoscopies on oesophageal cancer survival in the UK: A cohort study
Authors: Offman Judith , Pesola Francesca , Fitzgerald Rebecca C. , Hamilton Willie , Sasieni Peter 
Published: December 2021

AbstractBackgroundCurrent guidelines recommend endoscopic surveillance for Barrett oesophagus (BE), but the value of surveillance is still debated. Using a combination of primary care, secondary care and cancer registry datasets, we examined the impact of a prior BE diagnosis, clinical and risk factors on survival from oesophageal cancer and adenocarcinoma.MethodsRetrospective cohort study of patients aged 50 and above diagnosed with malignant oesophageal cancer between 1993 and 2014 using Clinical Practice Research Datalink (CPRD). All prior BE diagnoses and endoscopies were identified from CPRD and Hospital Episode Statistics. Histology information was obtained from linked cancer registry data. We used flexible parametric models to estimate excess hazard ratios (EHRs) for relative survival. We simulated the potential impact of lead‐time by adding random lead‐times from a variety of distributions to all those with prior BE.ResultsAmong our oesophageal cancer (n = 7503) and adenocarcinoma (n = 1476) cohorts only small percentages, 3.4% and 5.3%, respectively, had a prior BE diagnosis. Two‐year relative survival was better among patients with BE: 48.0% (95% CI 41.9–54.9) compared to 25.2% (24.3–26.2) without. Patients with BE had a better prognosis (EHR = 0.53, 0.41–0.68). Survival was higher even if patients with BE had fewer than two endoscopies (50.0%; 43.6–57.3). A survival benefit was still observed after lead‐time adjustment, with a 20% absolute difference in 2‐year survival using a 5 year mean sojourn time.ConclusionsPatients with a prior BE diagnosis had a survival advantage. This was not fully explained by surveillance endoscopies.
Fast Charge Transfer Kinetics Enabled by Carbon‐Coated, Heterostructured SnO2/SnSx Arrays for Robust, Flexible Lithium‐Ion Batteries
Authors: Xue Lichun , Chen Feiming , Zhang Zhenbao , Gao Yang , Chen Dengjie 
Published: December 2021

AbstractTin (Sn)‐based materials possessing high theoretical capacity have shown great potential for next‐generation lithium‐ion batteries (NGLIBs). Its poor conductivity and severe volume expansion, however, hinder practical applications. Herein, we prepare flexible carbon cloth supported SnO2/SnSx heterostructured arrays coated with carbon (SnO2/SnSx@C) with an easy hydrothermal process and carbonization. The resulting SnO2/SnSx@C electrode is capable of providing high capacity, good rate capability, and long‐term stability. Specifically, SnO2/SnSx@C shows an initial discharge specific capacity of 1898.7 mAh g−1 with Coulombic efficiency of 77.5 % and retains 1047.5 mAh g−1 after 100 cycles at 0.2 A g−1. The superior electrochemical performance of SnO2/SnSx@C is attributed to the well‐established unique structure: (1) the carbon cloth offers a flexible framework that can enhance the integrity of nanostructures and facilitate charge transfer; (2) both experimental and theoretical studies demonstrate that the SnO2/SnSx heterostructure can speed up charge transfer, and this heterostructure as a buffer framework can also mitigate expansion in volume; and (3) carbon arrays are beneficial for preventing the SnO2/SnSx electrode from pulverization and enhancing charge transfer. Our findings clearly indicate that Sn‐based heterostructures are promising for high‐capacity and stable NGLIBs.
Structural, Dielectric and Raman Spectroscopy of La3+–Ni2+–Zn2+ Substituted M‐Type Strontium Hexaferrites
Authors: Musa Ibrahim Murtala , Abdu Yunusa , Mohammed Jibrin , Srivastava Ajeet Kumar 
Published: December 2021

AbstractIn this work, M‐type strontium nanohexaferrites with chemical composition Ba0.8−xSr0.2LaxFe12−x−yNixZnyO19 (x = 0.00, 0.05, 0.10; y = 0.00, 0.08, 0.16) are prepared using sol–gel auto‐combustion technique. The formation of single phase hexagonal ferrites is confirmed from XRD analysis. It also reveals the presence of magnetite and the crystallites sizes are in the range of 21.31–29.91nm. The lattice constants are found to decrease with an increase in cation substitution. The FTIR spectra of the sample show three dominant peaks in the range of 400–600 cm–1 which indicate the formation of the desired hexaferrite structure. The field emission scanning electron microscope images reveal large crystallites with shapes close to the hexagonal platelet‐like whose sizes are nonuniformly distributed. Also, agglomeration is observed due to magnetic interactions between the crystallites. The dielectric constant, dielectric loss, conductivity, and dielectric modulus are analyzed using the Maxwell–Wagner model. Dielectric constant is enhanced at high frequency in the entire sample and reduction of dielectric loss is also observed with further cations substitutions.
Formation of Hierarchical Cobalt Hydroxychloride Nanostructures with Enhanced Performance for Lithium‐Ion Batteries
Authors: Wang G. , Liang J. , Li D. , Li M. , Li L. 
Published: December 2021

AbstractLayered metal hydroxide salts have attracted considerable attention in various applications due to their superior photoelectric, physical, and chemical properties. Here, a simple in situ growth hydrothermal approach is reported to prepare hierarchical cobalt hydrochloride (Co2(OH)3Cl) microspheres composed of octahedron‐like subunits. Based on the multiple functional triethanolamine and time‐dependent morphology evolution, the formation of the unique sphere structures can be elucidated by a hierarchical self‐assembly of anisotropic nanoparticles. When used as lithium ion battery (LIB) anodes, this Co2(OH)3Cl microsphere shows very large reversible specific capacity (1196 mA h g–1 at 0.2 A g–1), excellent rate capability (720.4 mA h g−1 at 4.0 A g−1), and long‐life stability (802 mA h g–1 with 81.1% retention after 500 cycle tests at 4.0 A g–1). The excellent electrochemical performance is attributed to the improvement of electrical conductivity and fast ionic diffusion in the electrode by improving the microarchitecture and functionally introducing Cl–.
Changes and drivers of zooplankton diversity patterns in the middle reach of Yangtze River floodplain lakes, China
Authors: Lu Quanfeng , Liu Xiongjun , Qiu Xuemei , Liang Tao , Chen Jinping , Zhao Shuai , Ouyang Shan , Jin Binsong , Wu Xiaoping 
Published: December 2021

AbstractAnthropogenic habitat alteration interferes the natural aquatic habitats and the system's hydrodynamics in the Yangtze River floodplain lakes, resulting in a serious decline in freshwater biodiversity. Zooplankton communities possess major position in freshwater ecosystems, which play essential parts in maintaining biological balance of freshwater habitats. Knowledge of processes and mechanisms for affecting variations in abundance, biomass, and diversity of zooplankton is important for maintaining biological balance of freshwater ecosystems. Here, we analyzed that the temporal and spatial changes in the structure of zooplankton community and their temporal and spatial variations respond to changes in environmental factors in the middle reach of Yangtze River floodplain lakes. The results showed that zooplankton samples were classified into 128 species, and Rotifera was the most common taxa. Significant seasonal differences were found among the abundance and diversity of zooplankton. Similarly, we also found significant seasonal differences among the biomass of zooplankton functional groups. The spatial turnover component was the main contributor to the β diversity pattern, which indicated that study areas should establish habitat restoration areas to restore regional biodiversity. The NMDS plot showed that the structure of zooplankton community exhibited significant seasonal changes, where the community structure was correlated with pH, water temperature, water depth, salinity, total nitrogen, chlorophyll‐a, and total phosphorus based on RDA. This study highlights that it is very important to ensure the floodplain ecosystem's original state of functionality for maintaining the regional diversity of the ecosystem as a whole.