40,963 research outputs found

    Newly developed electrosynthesis of Layered Double Hydroxides: application to sensing, energy storage and conversion

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    Layered Double hydroxides (LDHs) have been widely studied for their plethora of fascinating features and applications. The potentiostatic electrodeposition of LDHs has been extensively applied in the literature as a fast and direct method to substitute classical chemical routes. However, it does not usually allow for a fine control of the M(II)/M(III) ratio in the synthesized material and it is not suitable for large anions intercalation. Therefore, in this work a novel protocol has been proposed with the aim to overcome all these constraints using a method based on potentiodynamic synthesis. LDHs of controlled composition were prepared using different molar ratios of the trivalent to bivalent cations in the electrolytic solution ranging from 1:1 to 1:4. Moreover, we were able to produce electrochemically LDHs intercalated with carbon nanomaterials for the first time. A one-step procedure which contemporaneously allows for the Ni/Al-LDH synthesis, the reduction of graphene oxide (GO) and its intercalation inside the structure has been developed. The synthesised materials have been applied in several fields of interest. First of all, LDHs with a ratio 3:1 were exploited, and displayed good performances as catalysts for 5-(hydroxymethyl)furfural electro-oxidation, thus suggesting to carry out further investigation for applications in the field of industrial catalysis. The same materials, but with different metals ratios, were tested as catalysts for Oxygen Evolution Reaction, obtaining results comparable to LDHs synthesised by the classical co-precipitation method and also a better activity with respect to LDHs obtained by the potentiostatic approach. The composite material based on LDH and reduced graphene oxide was employed to fabricate a cathode of a hybrid supercapacitor coupled with an activated carbon anode. We can thus conclude that, to date, the potentiodynamic method has the greatest potential for the rapid synthesis of reproducible films of Co and Ni-based LDHs with controlled composition

    Improved electrochemical oxidation kinetics of La0.5Ba0.5FeO3-δ anode for solid oxide fuel cells with fluorine doping

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    Funding Information: The financial support from National Natural Science Foundation of China under contract number 22075205 and the support of Tianjin Municipal Science and Technology Commission under contract number 19JCYBJC21700 are gratefully acknowledged. The work has been also supported by the Program of Introducing Talents to the University Disciplines under file number B06006 , and the Program for Changjiang Scholars and Innovative Research Teams in Universities under file number IRT 0641 . Publisher Copyright: © 2021 Elsevier B.V.Sluggish anode kinetics and serious carbon deposition are two major obstacles to developing hydrocarbon fueled solid oxide fuel cells. A highly active and stable perovskite La0.5Ba0.5FeO3-δ anode material is studied in this work. The oxygen surface exchange and charge transfer steps are the rate-determining steps of the anode process, and the former is accelerated with fluorine doping on the anion sites due to the lowering of metal-oxygen bond energy. The oxygen surface exchange coefficients of La0.5Ba0.5FeO3-δ and La0.5Ba0.5FeO2.9-δF0.1 at 850 °C are 1.4 × 10−4 and 2.8 × 10−4 cm s−1, respectively. A single cell supported by a 300 μm-thick La0.8Sr0.2Ga0.8Mg0.2O3-δ electrolyte layer with La0.5Ba0.5FeO3-δ anode shows maximum power densities of 1446 and 691 mW cm−2 at 850 °C with wet hydrogen and methane fuels, respectively, which increase to 1860 and 809 mW cm−2 respectively when La0.5Ba0.5FeO2.9-δF0.1 is used as the anode. The cell exhibits a short-term durability of 40 h using wet methane as fuel without carbon deposition on the anode.Peer reviewe

    Cu-Ce0.8Sm0.2O2-δ anode for electrochemical oxidation of methanol in solid oxide fuel cell: Improved activity by La and Nd doping

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    Funding Information: The financial support from National Natural Science Foundation of China under contract number 22075205 and the support of Tianjin Municipal Science and Technology Commission under contract number 19JCYBJC21700 are gratefully acknowledged. The work has been also supported by the Program of Introducing Talents to the University Disciplines under file number B06006 , and the Program for Changjiang Scholars and Innovative Research Teams in Universities under file number IRT 0641 . Publisher Copyright: © 2021 Elsevier B.V.Cu–Ce0.8La0.1Sm0.1O2-δ and Cu–Ce0.8Nd0.1Sm0.1O2-δ are studied as anode materials for solid oxide fuel cells with methanol as fuel. The oxygen surface exchange and bulk diffusion coefficients of Ce0.8Sm0.2O2-δ both increase with La and Nd doping. The CH3OH temperature-programmed surface reaction results show that the addition of La and Nd accelerates the chemical oxidation of CH3OH. Furthermore, compared with Cu–Ce0.8Sm0.2O2-δ, the anodes with La and Nd show higher resistance to coking in CH3OH atmosphere. The Cu-based cermet anode exhibits a low catalytic activity for the electrochemical oxidation of H2, and a single cell supported by a Ce0.8Sm0.2O2-δ‑carbonate composite electrolyte with Cu–Ce0.8Sm0.2O2-δ anode exhibits a maximum power density of 160 mW cm−2 at 650 °C using dry hydrogen as fuel. However, the maximum power density reaches 550 mW cm−2 when CH3OH is used as fuel, and further increases to 730 and 830 mW cm−2 with the addition of La and Nd in the anode, respectively. The results indicate that withthe promotion of the oxygen activity, the Cu-based cermet is a promising anode material for solid oxide fuel cells using CH3OH as fuel.Peer reviewe

    Finding and Counting Patterns in Sparse Graphs

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    The stumbling block in ‘the race of our lives’: transition-critical materials, financial risks and the NGFS climate scenarios

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    Several ‘critical’ raw materials, including metals, minerals and Rare Earth Elements (REEs), play a central role in the low-carbon transition and are needed to expand the deployment of low-carbon technologies. The reliable and affordable supply of these resources is subject to supply-side risks and demand-induced pressures. This paper empirically estimates the material demand requirements for ‘Transition-Critical Materials’ (TCMs) implied under two NGFS Climate Scenarios, namely the ‘Net Zero by 2050’ and ‘Delayed Transition’ scenarios. We apply material intensity estimates to the underlying assumptions on the deployment of low-carbon technologies to determine the implied material demand between 2021 and 2040 for nine TCMs. We find several materials to be subject to significant demand-induced pressures under both scenarios. Subsequently, the paper examines the possible emergence of material bottlenecks for three materials, namely copper, lithium and nickel. The results indicate possible substantial mismatches between supply and demand, which would be further exacerbated if the transition is delayed rather than realised immediately. We discuss these findings in the context of different possible transmission channels through which these bottlenecks could affect financial and price stability, and propose avenues for future research

    Highly Stable Garnet Fe2Mo3O12 Cathode Boosts the Lithium–Air Battery Performance Featuring a Polyhedral Framework and Cationic Vacancy Concentrated Surface

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    Lithium–air batteries (LABs), owing to their ultrahigh theoretical energy density, are recognized as one of the next-generation energy storage techniques. However, it remains a tricky problem to find highly active cathode catalyst operating within ambient air. In this contribution, a highly active Fe2Mo3O12 (FeMoO) garnet cathode catalyst for LABs is reported. The experimental and theoretical analysis demonstrate that the highly stable polyhedral framework, composed of FeO octahedrons and MO tetrahedrons, provides a highly effective air catalytic activity and long-term stability, and meanwhile keeps good structural stability. The FeMoO electrode delivers a cycle life of over 1800 h by applying a simple half-sealed condition in ambient air. It is found that surface-rich Fe vacancy can act as an O2 pump to accelerate the catalytic reaction. Furthermore, the FeMoO catalyst exhibits a superior catalytic capability for the decomposition of Li2CO3. H2O in the air can be regarded as the main contribution to the anode corrosion and the deterioration of LAB cells could be attributed to the formation of LiOH·H2O at the end of cycling. The present work provides in-depth insights to understand the catalytic mechanism in air and constitutes a conceptual breakthrough in catalyst design for efficient cell structure in practical LABs

    Biochemical characterization and identification of ferulenol and embelin as potent inhibitors of malate:quinone oxidoreductase from Campylobacter jejuni

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    Campylobacter jejuni infection poses a serious global threat to public health. The increasing incidence and antibiotic resistance of this bacterial infection have necessitated the adoption of various strategies to curb this trend, primarily through developing new drugs with new mechanisms of action. The enzyme malate:quinone oxidoreductase (MQO) has been shown to be essential for the survival of several bacteria and parasites. MQO is a peripheral membrane protein that catalyses the oxidation of malate to oxaloacetate, a crucial step in the tricarboxylic acid cycle. In addition, MQO is involved in the reduction of the quinone pool in the electron transport chain and thus contributes to cellular bioenergetics. The enzyme is an attractive drug target as it is not conserved in mammals. As a preliminary step in assessing the potential application of MQO from C. jejuni (CjMQO) as a new drug target, we purified active recombinant CjMQO and conducted, for the first time, biochemical analyses of MQO from a pathogenic bacterium. Our study showed that ferulenol, a submicromolar mitochondrial MQO inhibitor, and embelin are nanomolar inhibitors of CjMQO. We showed that both inhibitors are mixed-type inhibitors versus malate and noncompetitive versus quinone, suggesting the existence of a third binding site to accommodate these inhibitors; indeed, such a trait appears to be conserved between mitochondrial and bacterial MQOs. Interestingly, ferulenol and embelin also inhibit the in vitro growth of C. jejuni, supporting the hypothesis that MQO is essential for C. jejuni survival and is therefore an important drug target

    Understanding sodium storage properties of ultra-small Fe3S4Fe_3S_4 nanoparticles – a combined XRD, PDF, XAS and electrokinetic study

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    Various electrode materials are considered for sodium-ion batteries (SIBs) and one important prerequisite for developments of SIBs is a detailed understanding about charge storage mechanisms. Herein, we present a rigorous study about Na storage properties of ultra-small Fe3_3S4_4 nanoparticles, synthesized applying a solvothermal route, which exhibit a very good electrochemical performance as anode material for SIBs. A closer look into electrochemical reaction pathways on the nanoscale, utilizing synchrotron-based X-ray diffraction and X-ray absorption techniques, reveals a complicated conversion mechanism. Initially, separation of Fe3_3S4_4 into nanocrystalline intermediates occurs accompanied by reduction of Fe3+^{3+} to Fe2+^{2+} cations. Discharge to 0.1 V leads to formation of strongly disordered Fe0^0 finely dispersed in a nanosized Na2_2S matrix. The resulting volume expansion leads to a worse long-term stability in the voltage range 3.0–0.1 V. Adjusting the lower cut-off potential to 0.5 V, crystallization of Na2_2S is prevented and a completely amorphous intermediate stage is formed. Thus, the smaller voltage window is favorable for long-term stability, yielding highly reversible capacity retention, e.g., 486 mAh g−1^{−1} after 300 cycles applying 0.5 A g−1^{−1} and superior coulombic efficiencies >99.9%. During charge to 3.0 V, Fe3_3S4_4 with smaller domains are reversibly generated in the 1st cycle, but further cycling results in loss of structural long-range order, whereas the local environment resembles that of Fe3_3S4_4 in subsequent charged states. Electrokinetic analyses reveal high capacitive contributions to the charge storage, indicating shortened diffusion lengths and thus, redox reactions occur predominantly at surfaces of nanosized conversion products

    Preparation, modification, and clinical application of porous tantalum scaffolds

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    Porous tantalum (Ta) implants have been developed and clinically applied as high-quality implant biomaterials in the orthopedics field because of their excellent corrosion resistance, biocompatibility, osteointegration, and bone conductivity. Porous Ta allows fine bone ingrowth and new bone formation through the inner space because of its high porosity and interconnected pore structure. It contributes to rapid bone integration and long-term stability of osseointegrated implants. Porous Ta has excellent wetting properties and high surface energy, which facilitate the adhesion, proliferation, and mineralization of osteoblasts. Moreover, porous Ta is superior to classical metallic materials in avoiding the stress shielding effect, minimizing the loss of marginal bone, and improving primary stability because of its low elastic modulus and high friction coefficient. Accordingly, the excellent biological and mechanical properties of porous Ta are primarily responsible for its rising clinical translation trend. Over the past 2 decades, advanced fabrication strategies such as emerging manufacturing technologies, surface modification techniques, and patient-oriented designs have remarkably influenced the microstructural characteristic, bioactive performance, and clinical indications of porous Ta scaffolds. The present review offers an overview of the fabrication methods, modification techniques, and orthopedic applications of porous Ta implants

    Countermeasures for the majority attack in blockchain distributed systems

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    La tecnología Blockchain es considerada como uno de los paradigmas informáticos más importantes posterior al Internet; en función a sus características únicas que la hacen ideal para registrar, verificar y administrar información de diferentes transacciones. A pesar de esto, Blockchain se enfrenta a diferentes problemas de seguridad, siendo el ataque del 51% o ataque mayoritario uno de los más importantes. Este consiste en que uno o más mineros tomen el control de al menos el 51% del Hash extraído o del cómputo en una red; de modo que un minero puede manipular y modificar arbitrariamente la información registrada en esta tecnología. Este trabajo se enfocó en diseñar e implementar estrategias de detección y mitigación de ataques mayoritarios (51% de ataque) en un sistema distribuido Blockchain, a partir de la caracterización del comportamiento de los mineros. Para lograr esto, se analizó y evaluó el Hash Rate / Share de los mineros de Bitcoin y Crypto Ethereum, seguido del diseño e implementación de un protocolo de consenso para controlar el poder de cómputo de los mineros. Posteriormente, se realizó la exploración y evaluación de modelos de Machine Learning para detectar software malicioso de tipo Cryptojacking.DoctoradoDoctor en Ingeniería de Sistemas y Computació
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