bluuebunny/crossref_metadata_2025_split huggingface dataset:
A General Strategy for Antimony‐Based Alloy Nanocomposite Embedded in Swiss‐Cheese‐Like Nitrogen‐Doped Porous Carbon for Energy Storage
Authors: Yang Tao , Zhong Jiasong , Liu Jianwen , Yuan Yongjun , Yang Dexin , Mao Qinan , Li Xinyue , Guo Zaiping 
Published: January 2021

AbstractDue to its suitable working voltage and high theoretical storage capacity, antimony is considered a promising negative electrode material for lithium‐ion batteries (LIBs) and has attracted widespread attention. The volume effect during cycling, however, will cause the antimony anode to undergo a severe structural collapse and a rapid decrease in capacity. Here, a general in situ self‐template‐assisted strategy is proposed for the rational design and preparation of a series of MSb (M = Ni, Co, or Fe) nanocomposites with MNC coordination, which are firmly anchored on Swiss‐cheese‐like nitrogen‐doped porous carbon as anodes for LIBs. The large interface pore network structure, the introduction of heteroatoms, and the formation of strong metalNC bonds effectively enhance their electronic conductivity and structural integrity, and provide abundant interfacial lithium storage. The experimental results have proved the high rate performance and excellent cycling stability of antimony‐based composite materials. Electrochemical kinetics studies have demonstrated that the increase in capacity during cycling is mainly controlled by the diffusion mechanism rather than the pseudocapacitance contribution. This facile strategy can provide a new pathway for low‐cost and high‐yield synthesis of Sb‐based composites with high performance, and is expected to be applied in other energy‐related fields such as sodium‐/potassium‐ion batteries or electrocatalysis.
Magnetothermal Miniature Reactors Based on Fe3O4 Nanocube‐Coated Liquid Marbles
Authors: Li Hualin , Liu Peng , Gunawan Renardi , Simeneh Zemenu Mengistie , Liang Chen , Yao Xi , Yang Mengsu 
Published: January 2021

AbstractLiquid marbles have recently attracted much interest in various scientific fields because of their isolated environment and robustness. However, conventional liquid marbles lack a reliable heating mechanism, which is critical in many potential applications. Here, the development of iron oxide (Fe3O4) nanocube‐coated liquid marbles (iNLMs), which can be homogeneously heated with an alternating magnetic field (AMF) to as high as 86 °C, is reported. Through tuning the power of the AMF, the iNLMs canbe heated to desired temperatures in controllable patterns. Furthermore, multicenter and selective heating is realized based on the unique magnetothermal properties of iNLMs. As heatable miniature reactors, the iNLMs are further demonstrated to facilitate the kinetic study of temperature‐dependent chemical reactions. DNA amplification is successfully performed in liquid marbles, achieving a 25% superior amplification rate compared with that in a common thermal cycler. These results confirm the feasibility of coating liquid marbles with Fe3O4 nanocubes to form delicate magnetothermal miniature reactors, which provides a reliable method of applying liquid marbles in areas such as biosensor technology, point‐of‐care testing, and theranostics.
Electronic Conductive Inorganic Cathodes Promising High‐Energy Organic Batteries
Authors: Mao Minglei , Wang Shu , Lin Zejing , Liu Tao , Hu Yong‐Sheng , Li Hong , Huang Xuejie , Chen Liquan , Suo Liumin 
Published: January 2021

AbstractThe electrochemical utilization of organic electrode materials (OEMs) is highly dependent on an excess amount of inactive carbon at the expense of low packing density and energy density. In this work, the challenges by substituting inactive carbon with electronic conductive inorganic cathode (ECIC) materials, which are endowed with high electronic conductivity to transport electrons for redox reactions of the whole electrodes, high ion‐storage capacity to act as secondary active materials, and strong affinity with OEMs to inhibit their dissolution, are addressed. Combining representative ECICs (TiS2 and Mo6S8) with organic electrode materials (perylene‐3,4,9,10‐tetracarboxylic dianhydride (PTCDA) and hexaazatrinaphthalene (HATN)) simultaneously achieves high capacity, low porosity, lean electrolyte, and thus high energy density. High gravimetric and volumetric energy densities of 153 Wh kg−1 and 200 Wh L−1 are delivered with superior cycling stability in a 30 mA h‐level Li/PTCDA‐TiS2 pouch cell. The proof‐of‐concept of organic–ECIC electrodes is also successfully demonstrated in monovalent Na, divalent Mg, and trivalent Al batteries, indicating their feasibility and generalizability. With the discovery of more ECIC materials and OEMs, it is anticipated that the proposed organic–ECIC system can result in further improvements at cell level to compete with transition metal‐based Li‐ion batteries.
Great Location: About Effects of Surface Bound Neighboring Groups for Passive and Active Fine‐Tuning of CO2 Adsorption Properties in Model Carbon Capture Materials
Authors: Klinkenberg Nele , Kraft Sophia , Polarz Sebastian 
Published: January 2021

AbstractImproved carbon capture materials are crucial for managing the CO2 level in the atmosphere. The past focus was on increasing adsorption capacities. It is widely known that controlling the heat of adsorption (ΔHads) is equally important. If it is too low, CO2 uptake takes place at unfavorable conditions and with insufficient selectivity. If it is too high, chemisorption occurs, and the materials can hardly be regenerated. The conventional approach for influencing ΔHads is the modification of the adsorbing center. This paper proposes an alternative strategy. The hypothesis is that fine‐tuning of the molecular environment around the adsorbing center is a powerful tool for the adjustment of CO2‐binding properties. Via click chemistry, any desired neighboring group (NG) can be incorporated on the surfaces of the nanoporous organosilica model materials. Passive NGs induce a change in the polarity of the surface, whereas active NGs are capable of direct interaction with the active center/CO2 pair. The effects on ΔHads and on the selectivity are studied. A situation can be realized which resembles frustrated Lewis acid–base pairs, and the investigation of the binding‐species by solid‐state NMR indicates that the push–pull effects could play an essential role not only in CO2 adsorption but also in its activation.
Energy Harvesters for Wearable Electronics and Biomedical Devices
Authors: Hasan Md. Nazibul , Sahlan Shafishuhaza , Osman Khairuddin , Mohamed Ali Mohamed Sultan 
Published: January 2021

AbstractEnergy harvesters (EHs) are widely used to transform ambient energy sources into electrical energy, and have tremendous potential to power wearables electronics and biomedical devices by eliminating, or at least increasing, the battery life. Nevertheless, the use of EHs for a specific application depends on various aspects including the form of energy source, the structural configuration of the device, and the properties of materials. This paper presents a comprehensive review of the classification of EHs, notably thermoelectric generators (TEGs), triboelectric nanogenerators (TENGs), and piezoelectric generators (PEGs) that allows a wide variety of devices to be operated. The EHs are discussed in terms of their operating principles, optimization factors, state‐of‐the‐art materials, and device structure, that directly influence their operational efficiency. Besides, the breakthrough performance of each of the EHs listed above is highlighted. From the review and analysis, the maximum output power density of 9.2 mW cm−2, 50 mW cm−2, and 64.9 µW cm−2, respectively, are obtained from the TEG, TENG, and PEG, respectively. Furthermore, recent applications relevant to a specific EH and their output performance, are also enlightened. Eventually, the essential outcomes and future direction from this review are discussed and encapsulated.
Multifunctional Metasurface Design with a Generative Adversarial Network
Authors: An Sensong , Zheng Bowen , Tang Hong , Shalaginov Mikhail Y. , Zhou Li , Li Hang , Kang Myungkoo , Richardson Kathleen A. , Gu Tian , Hu Juejun , Fowler Clayton , Zhang Hualiang 
Published: January 2021

AbstractMetasurfaces have enabled precise electromagnetic (EM) wave manipulation with strong potential to obtain unprecedented functionalities and multifunctional behavior in flat optical devices. These advantages in precision and functionality come at the cost of tremendous difficulty in finding individual meta‐atom structures based on specific requirements (commonly formulated in terms of EM responses), which makes the design of multifunctional metasurfaces a key challenge in this field. In this paper, a generative adversarial network that can tackle this problem and generate meta‐atom/metasurface designs to meet multifunctional design goals is presented. Unlike conventional trial‐and‐error or iterative optimization design methods, this new methodology produces on‐demand free‐form structures involving only a single design iteration. More importantly, the network structure and the robust training process are independent of the complexity of design objectives, making this approach ideal for multifunctional device design. Additionally, the ability of the network to generate distinct classes of structures with similar EM responses but different physical features can provide added latitude to accommodate other considerations such as fabrication constraints and tolerances. The network's ability to produce a variety of multifunctional metasurface designs is demonstrated by presenting a bifocal metalens, a polarization‐multiplexed beam deflector, a polarization‐multiplexed metalens, and a polarization‐independent metalens.
Hydrogel Microsphere Encapsulation Enhances the Flow Properties of Monoclonal Antibody Crystal Formulations
Authors: Schieferstein Jeremy M. , Reichert Paul , Narasimhan Chakravarthy N. , Yang Xiaoyu , Doyle Patrick S. 
Published: January 2021

AbstractMonoclonal antibodies are therapeutic molecules known for their high specificity and versatility in the treatment of cancer and autoimmune disorders, but dosage forms are typically limited to low concentrations and large fluid volumes due to formulation challenges. Hydrogel microsphere formulations offer a route to quicker, patient‐friendly dosing regimens for monoclonal antibodies with high loading and favorable flow properties needed for injection through a narrow syringe needle under moderate applied force. Crystals of an intact monoclonal antibody are prepared as a concentrated suspension (>300 mg mL−1) which is then encapsulated within hydrogel microspheres with diameters as small as 30 µm. The hydrogel microspheres contain up to 56 wt% (dry basis) monoclonal antibody and release within 4 days under in vitro dissolution conditions. The hydrogel microspheres are concentrated into densely packed suspensions containing up to 300 mg mL−1 monoclonal antibody to evaluate their flow. These hydrogel formulations shear‐thin and have lower viscosity when compared to both liquid and suspended crystal forms of the monoclonal antibody, demonstrating the potential of hydrogel microsphere encapsulants as a carrier which can mask undesirable flow properties of concentrated antibody therapeutics.
Targeting Glioblastoma Using a Novel Peptide Specific to a Deglycosylated Isoform of Brevican
Authors: von Spreckelsen Niklas , Fadzen Colin M. , Hartrampf Nina , Ghotmi Yarah , Wolfe Justin M. , Dubey Shipra , Yang Bo Yeun , Kijewski Marie F. , Wang Shuyan , Farquhar Charlotte , Bergmann Sonja , Zdioruk Mykola , Wasserburg J. Roscoe , Scott Benjamin , Murrell Emily , Bononi Fernanda C. , Luyt Leonard G. , DiCarli Marcelo , Lamfers Martine L. M. , Ligon Keith L. , Chiocca E. Antonio , Viapiano Mariano S. , Pentelute Bradley L. , Lawler Sean E. , Cho Choi‐Fong 
Published: January 2021

AbstractGlioblastoma (GBM) is the most common and deadliest form of brain tumor and remains amongst the most difficult cancers to treat. Brevican (Bcan), a central nervous system (CNS)‐specific extracellular matrix protein, is upregulated in high‐grade glioma cells, including GBM. A Bcan isoform lacking most glycosylation, dg‐Bcan, is found only in GBM tissues. Here, dg‐Bcan is explored as a molecular target for GBM. In this study, a d‐peptide library is screened to identify a small 8‐amino acid dg‐Bcan‐Targeting Peptide (BTP) candidate, called BTP‐7 that binds dg‐Bcan with high affinity and specificity. BTP‐7 is preferentially internalized by dg‐Bcan‐expressing patient‐derived GBM cells. To demonstrate GBM targeting, BTP‐7 is radiolabeled with 18F, a radioisotope of fluorine, and increased radiotracer accumulation is found in intracranial GBM established in mice using positron emission tomography (PET) imaging. dg‐Bcan is an attractive molecular target for GBM, and BTP‐7 represents a promising lead candidate for further development into novel imaging agents and targeted therapeutics.
Modeling Sorption and Diffusion of Alkanes, Alkenes, and their Mixtures in Silicalite: From MD and GCMC Molecular Simulations to Artificial Neural Networks
Authors: Gurras Arsenios , Gergidis Leonidas N. 
Published: January 2021

AbstractMolecular dynamics (MD) in canonical (NVT) statistical ensemble and grand canonical‐Monte Carlo (GCMC) simulations along with artificial neural network (ANN) techniques are used for the study of diffusion and sorption characteristics of small alkanes, alkenes, and their mixtures in silicalite. In particular, sorption isotherms and self‐diffusion coefficients of alkanes (ethane to hexane), alkenes (ethene to hexene), and the respective alkane–alkene mixtures (consisting of the same number of carbon atoms) in silicalite are studied. The findings are directly compared with recent magic‐angle spinning pulsed field‐gradient nuclear magnetic resonance experimental diffusivity measurements and are in close agreement. Furthermore, new results are provided for the alkane–alkene systems. The sorption data from GCMC simulations, the self‐diffusivity calculations from the MD simulations along with available experimental data are used for the development of ANN predictive modeling procedures in order to give generic sorption and diffusion predictions for pure alkanes, alkenes in different input values of fugacity, temperature, and sorbate loadings at the minimum computational resources and time. Finally, structural characteristics for pure alkane, alkenes, and alkane–alkene mixtures when confined in the silicalite framework are computed revealing sorption domains and siting preferences.
Surface‐Bound Domain Penetration and Large Wall Current
Authors: Jiang Jun , Wang Chao , Chai Xiaojie , Zhang Qinghua , Hou Xu , Meng Fanqi , Gu Lin , Wang Jie , Jiang An Quan 
Published: January 2021

AbstractBy controlling the domain nucleation in ferroelectric mesa‐like cells formed at the surfaces of X‐cut LiNbO3 single‐crystal films that are integrated with Si substrates, growth of a surface‐bound needle‐like domain is observed in a quarter‐ellipsoidal shape. This domain, which extends in the major polar direction, contracts into several equilibrium segments with unequal lengths after removal of the in‐plane applied electric fields. The curved wall region located near the domain tip that connects the two top nanoelectrodes exhibits 12‐fold magnification of the on‐current when compared with the straight wall region near the tail. The field‐dependent flexible domain length and the high electrical conduction in the tip region promote crossbar integration of high‐density multilevel information‐storing memory devices and selectors with sufficient readout currents, thus enabling data‐intensive applications to be performed using domain wall microelectronics.
A New Functional Composite for Photovoltaic and Sensor Applications
Authors: Ghosh Puja , Roy Anurag , Mukhopadhyay Soumita , Narjinary Mousumi , Sundaram Senthilarasu , Sen Shrabanee , Devi Parukuttyamma Sujatha 
Published: January 2021

AbstractAs a preliminary drive to eventually develop dye‐sensitized solar cell (DSSC)‐powered gas sensors, many oxide‐based systems have been explored to fabricate sensors that can show response at room temperature for any analyte gas. As an outcome of recent work in this endeavor, a composite nanorod of anatase TiO2 with Na0.23TiO2 is found to exhibit both photovoltaic performance and gas sensing at room temperature as demonstrated here. An interesting morphology change along with a phase change from nanoparticle to nanorod is observed during the hydrothermal synthesis of anatase TiO2 nanoparticles with sodium hydroxide under a highly basic condition. In order to understand the effect of the minor phase Na0.23TiO2 on the inherent properties of anatase TiO2, the application of nanorod composite in two unique potential application areas, DSSC and acetone sensings is investigated. The composite material exhibits an enhanced efficiency of 7.85% for a DSSC. Surprisingly, a resistive sensor fabricated with the synthesized composite material exhibits room temperature p‐type sensing behavior toward different concentrations of acetone (10, 5, 3, 2, and 1 ppm) with high selectivity.
Au‐Promoted Pt nanoparticles supported on MgO/SBA‐15 as an efficient catalyst for selective oxidation of glycerol
Authors: Liu Yibin , Zha Minghao , Qin Hansong , Yao Shuang , Zhou Xin , Zhao Siming , Sheng Nan , Sun Yinghao , Jin Xin , Yan Hao , Feng Xiang , Chen Xiaobo , Yang Chaohe 
Published: January 2021

AbstractA systematic study of Au‐promoted and unpromoted Pt/MgO/SBA‐15 catalyst is developed to separate the promoter effect from electron transfer effect between Au and Pt. Multi‐characterizations revealed that Au and Pt metals in these bimetallic catalysts mainly exist in the form of alloy, and the main role of Au is to reduce the size of AuPt alloy nanoparticles, thus enhancing the adsorption and activation of intermediate products. Through the optimization of various factors (including MgO content, Au/Pt molar ratio, reaction temperature and time), the Au1Pt2/MgO/SBA‐15 (0.05) catalyst exhibits excellent catalytic activity and glyceric acid selectivity for the selective oxidation of glycerol. Density functional theory calculation confirmed that the synergistic effect between Pt and Au active sites could facilitate the oxidation of primary hydroxyl group by promoting the activation of CH bond and the oxidation of aldehyde group. The results may give insights on designing effective Pt based bimetallic catalyst for selective oxidation of glycerol.
Quasi‐continuous synthesis of iron single atom catalysts via a microcapsule pyrolysis strategy
Authors: Huang Liyun , Wu Kui , He Qian , Xiong Chao , Gan Tao , He Xiaohui , Ji Hongbing 
Published: January 2021

AbstractSingle atom catalysts (SACs), featured with atomically dispersed metal species, have been considered as one of the most promising catalytic materials because of the excellent performance in various high‐value‐added reactions. However, the large‐scale and continuous‐type production of such SACs is still challenging. Herein, a novel and facile microcapsule strategy for the quasi‐continuous synthesis of iron SACs supported on S, N co‐doped carbon (Fe/SNC) is developed, and the Fe species are presented as isolated active sites and stabilized as the FeN3S‐like structure. The as‐prepared Fe/SNC catalysts exhibit excellent catalytic properties for selective oxidation of arylalkanes, which followed pseudo‐first‐order kinetics with an Ea = 41.5 kJ/mol. More importantly, the two Fe/SNC catalysts synthesized at different continuous times showed essentially identical catalyst structure and catalytic performance, demonstrating the superior reliability of our microcapsule strategy for the quasi‐continuous production of SACs, which can be easily scaled up to industrial application.
Contact Charge Transfer between Nominally Identical Materials
Authors: Angus John C. , Greber Isaac 
Published: January 2021

AbstractDifferences in concentrations of excited electrons arising from geometry‐dependent differences in de‐excitation paths lead to differences in Fermi energies, which enable contact charge transfer between otherwise identical solids of different size. This model is used with a quasi‐equilibrium description of the Fermi energy to estimate a lower bound of the magnitude of charging of pairs of like particles and the charge distribution in groups of interacting like particles. The predictions agree with observed charge transfer directions between large and small particles and with the broad particle size range over which charging is observed. Estimates of charging are compared to available measurements, the breakdown limits of air, and the relative strengths of interparticle electrostatic and gravitational forces. The influence of particle size distribution on the charge distribution in groups of particles is examined.
Carbene‐Catalyzed Activation of Remote Nitrogen Atoms of (Benz)imidazole‐Derived Aldimines for Enantioselective Synthesis of Heterocycles
Authors: Yang Xing , Xie Yongtao , Xu Jun , Ren Shichao , Mondal Bivas , Zhou Liejin , Tian Weiyi , Zhang Xinglong , Hao Lin , Jin Zhichao , Chi Yonggui Robin 
Published: January 2021

AbstractA new mode of carbene‐catalyzed heteroatom activation and asymmetric reactions is disclosed. The reaction starts with addition of a carbene catalyst to a (benz)imidazole‐derived aldimine substrate. Subsequent oxidation and proton transfer lead to the formation of a catalyst‐bound triaza‐diene as the key intermediate, in which the nitrogen atom at a site remote to the catalyst‐substrate bond is activated. This unusual triaza‐diene intermediate then undergoes highly enantioselective reactions with activated ketones through a concerted asynchronous pathway, as supported by mechanistic studies and preliminary density function theory calculation.
“NAD‐display”: Ultrahigh‐Throughput in Vitro Screening of NAD(H) Dehydrogenases Using Bead Display and Flow Cytometry
Authors: Lindenburg Laurens , Hollfelder Florian 
Published: January 2021

AbstractNAD(H)‐utiliing enzymes have been the subject of directed evolution campaigns to improve their function. To enable access to a larger swath of sequence space, we demonstrate the utility of a cell‐free, ultrahigh‐throughput directed evolution platform for dehydrogenases. Microbeads (1.5 million per sample) carrying both variant DNA and an immobilised analogue of NAD+ were compartmentalised in water‐in‐oil emulsion droplets, together with cell‐free expression mixture and enzyme substrate, resulting in the recording of the phenotype on each bead. The beads’ phenotype could be read out and sorted for on a flow cytometer by using a highly sensitive fluorescent protein‐based sensor of the NAD+:NADH ratio. Integration of this “NAD‐display” approach with our previously described Split & Mix (SpliMLiB) method for generating large site‐saturation libraries allowed straightforward screening of fully balanced site saturation libraries of formate dehydrogenase, with diversities of 2×104. Based on modular design principles of synthetic biology NAD‐display offers access to sophisticated in vitro selections, avoiding complex technology platforms.