231 research outputs found

    Bicarbonate or Carbonate Processes for Coupling Carbon Dioxide Capture and Electrochemical Conversion

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    Designing a scalable system to capture CO₂ from the air and convert it into valuable chemicals, fuels, and materials could be transformational for mitigating climate change. Climate models predict that negative greenhouse gas emissions will be required by the year 2050 in order to stay below a 2 °C change in global temperature. The processes of CO₂ capture, CO₂ conversion, and finally product separation all require significant energy inputs; devising a system that simultaneously minimizes the energy required for all steps is an important challenge. To date, a variety of prototype or pilot-level CO₂ capture and/or conversion systems have been designed and built targeting the individual objectives of either capture or conversion. One approach has focused on CO₂ removal from the atmosphere and storage of pure pressurized CO₂. Other efforts have concentrated on CO₂ conversion processes, such as electrochemical reduction or fermentation. Only a few concepts or analyses have been developed for complete end-to-end processes that perform both CO₂ capture and transformation

    Optical Excitation of a Nanoparticle Cu/p-NiO Photocathode Improves Reaction Selectivity for COâ‚‚ Reduction in Aqueous Electrolytes

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    We report the light-induced modification of catalytic selectivity for photoelectrochemical COâ‚‚ reduction in aqueous media using copper (Cu) nanoparticles dispersed onto p-type nickel oxide (p-NiO) photocathodes. Optical excitation of Cu nanoparticles generates hot electrons available for driving COâ‚‚ reduction on the Cu surface, while charge separation is accomplished by hot-hole injection from the Cu nanoparticles into the underlying p-NiO support. Photoelectrochemical studies demonstrate that optical excitation of plasmonic Cu/p-NiO photocathodes imparts increased selectivity for COâ‚‚ reduction over hydrogen evolution in aqueous electrolytes. Specifically, we observed that plasmon-driven COâ‚‚ reduction increased the production of carbon monoxide and formate, while simultaneously reducing the evolution of hydrogen. Our results demonstrate an optical route toward steering the selectivity of artificial photosynthetic systems with plasmon-driven photocathodes for photoelectrochemical COâ‚‚ reduction in aqueous media

    Analysis of the Space Shuttle main engine simulation

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    This is a final report on an analysis of the Space Shuttle Main Engine Program, a digital simulator code written in Fortran. The research was undertaken in ultimate support of future design studies of a shuttle life-extending Intelligent Control System (ICS). These studies are to be conducted by NASA Lewis Space Research Center. The primary purpose of the analysis was to define the means to achieve a faster running simulation, and to determine if additional hardware would be necessary for speeding up simulations for the ICS project. In particular, the analysis was to consider the use of custom integrators based on the Matrix Stability Region Placement (MSRP) method. In addition to speed of execution, other qualities of the software were to be examined. Among these are the accuracy of computations, the useability of the simulation system, and the maintainability of the program and data files. Accuracy involves control of truncation error of the methods, and roundoff error induced by floating point operations. It also involves the requirement that the user be fully aware of the model that the simulator is implementing

    Bicarbonate or Carbonate Processes for Coupling Carbon Dioxide Capture and Electrochemical Conversion

    Get PDF
    Designing a scalable system to capture CO₂ from the air and convert it into valuable chemicals, fuels, and materials could be transformational for mitigating climate change. Climate models predict that negative greenhouse gas emissions will be required by the year 2050 in order to stay below a 2 °C change in global temperature. The processes of CO₂ capture, CO₂ conversion, and finally product separation all require significant energy inputs; devising a system that simultaneously minimizes the energy required for all steps is an important challenge. To date, a variety of prototype or pilot-level CO₂ capture and/or conversion systems have been designed and built targeting the individual objectives of either capture or conversion. One approach has focused on CO₂ removal from the atmosphere and storage of pure pressurized CO₂. Other efforts have concentrated on CO₂ conversion processes, such as electrochemical reduction or fermentation. Only a few concepts or analyses have been developed for complete end-to-end processes that perform both CO₂ capture and transformation

    Efficient Bayesian inference under the structured coalescent

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    Motivation: Population structure significantly affects evolutionary dynamics. Such structure may be due to spatial segregation, but may also reflect any other gene-flow-limiting aspect of a model. In combination with the structured coalescent, this fact can be used to inform phylogenetic tree reconstruction, as well as to infer parameters such as migration rates and subpopulation sizes from annotated sequence data. However, conducting Bayesian inference under the structured coalescent is impeded by the difficulty of constructing Markov Chain Monte Carlo (MCMC) sampling algorithms (samplers) capable of efficiently exploring the state space. Results: In this article, we present a new MCMC sampler capable of sampling from posterior distributions over structured trees: timed phylogenetic trees in which lineages are associated with the distinct subpopulation in which they lie. The sampler includes a set of MCMC proposal functions that offer significant mixing improvements over a previously published method. Furthermore, its implementation as a BEAST 2 package ensures maximum flexibility with respect to model and prior specification. We demonstrate the usefulness of this new sampler by using it to infer migration rates and effective population sizes of H3N2 influenza between New Zealand, New York and Hong Kong from publicly available hemagglutinin (HA) gene sequences under the structured coalescent. Availability and implementation: The sampler has been implemented as a publicly available BEAST 2 package that is distributed under version 3 of the GNU General Public License at http://compevol.github.io/MultiTypeTree. Contact: [email protected] Supplementary information: Supplementary data are available at Bioinformatics onlin

    Hot Hole Collection and Photoelectrochemical CO_2 Reduction with Plasmonic Au/p-GaN Photocathodes

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    Harvesting nonequilibrium hot carriers from plasmonic-metal nanostructures offers unique opportunities for driving photochemical reactions at the nanoscale. Despite numerous examples of hot electron-driven processes, the realization of plasmonic systems capable of harvesting hot holes from metal nanostructures has eluded the nascent field of plasmonic photocatalysis. Here, we fabricate gold/p-type gallium nitride (Au/p-GaN) Schottky junctions tailored for photoelectrochemical studies of plasmon-induced hot-hole capture and conversion. Despite the presence of an interfacial Schottky barrier to hot-hole injection of more than 1 eV across the Au/p-GaN heterojunction, plasmonic Au/p-GaN photocathodes exhibit photoelectrochemical properties consistent with the injection of hot holes from Au nanoparticles into p-GaN upon plasmon excitation. The photocurrent action spectrum of the plasmonic photocathodes faithfully follows the surface plasmon resonance absorption spectrum of the Au nanoparticles and open-circuit voltage studies demonstrate a sustained photovoltage during plasmon excitation. Comparison with Ohmic Au/p-NiO heterojunctions confirms that the vast majority of hot holes generated via interband transitions in Au are sufficiently hot to inject above the 1.1 eV interfacial Schottky barrier at the Au/p-GaN heterojunction. We further investigated plasmon-driven photoelectrochemical CO_2 reduction with the Au/p-GaN photocathodes and observed improved selectivity for CO production over H_2 evolution in aqueous electrolytes. Taken together, our results offer experimental validation of photoexcited hot holes more than 1 eV below the Au Fermi level and demonstrate a photoelectrochemical platform for harvesting hot carriers to drive solar-to-fuel energy conversion

    Optical Excitation of a Nanoparticle Cu/p-NiO Photocathode Improves Reaction Selectivity for COâ‚‚ Reduction in Aqueous Electrolytes

    Get PDF
    We report the light-induced modification of catalytic selectivity for photoelectrochemical COâ‚‚ reduction in aqueous media using copper (Cu) nanoparticles dispersed onto p-type nickel oxide (p-NiO) photocathodes. Optical excitation of Cu nanoparticles generates hot electrons available for driving COâ‚‚ reduction on the Cu surface, while charge separation is accomplished by hot-hole injection from the Cu nanoparticles into the underlying p-NiO support. Photoelectrochemical studies demonstrate that optical excitation of plasmonic Cu/p-NiO photocathodes imparts increased selectivity for COâ‚‚ reduction over hydrogen evolution in aqueous electrolytes. Specifically, we observed that plasmon-driven COâ‚‚ reduction increased the production of carbon monoxide and formate, while simultaneously reducing the evolution of hydrogen. Our results demonstrate an optical route toward steering the selectivity of artificial photosynthetic systems with plasmon-driven photocathodes for photoelectrochemical COâ‚‚ reduction in aqueous media

    Antihypertensive response to prolonged tempol in the spontaneously hypertensive rat

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    Antihypertensive response to prolonged tempol in the spontaneously hypertensive rat.IntroductionTempol is a permeant nitroxide superoxide dismutase (SOD) mimetic that lowers mean arterial pressure (MAP) in spontaneously hypertensive rats (SHRs). We investigated the hypothesis that the antihypertensive response entails a negative salt balance, blunting of plasma renin activity (PRA), endothelin-1 (ET-1), or catecholamines or correction of oxidative stress as indexed by 8-isoprostane prostaglandin F2α (PGF2α) (8-Iso).MethodsGroups (N = 6 to 8) of SHRs were infused for 2 weeks with vehicle or tempol (200 nmol/kg/min) or given tempol (2 mmol/L) in drinking water.ResultsTempol infusion reduced the MAP of anesthetized SHRs (150 ± 5 vs. 126 ± 6mm Hg) (P < 0.005). Oral tempol did not change the heart rate but reduced the MAP of conscious SHRs (-23 ± 6mm Hg) (P < 0.01) but not Wistar-Kyoto (WKY) rats. Tempol infusion increased the PRA (2.2 ± 0.2 vs. 5.0 ± 0.9 ng/mL/hour) (P < 0.005), did not change excretion of nitric oxide (NO) [NO2 + NO3 (NOx)], ET-1, or catecholamines but reduced excretion of 8-Iso (13.2 ± 1.4 vs. 9.6 ± 0.9 ng/24 hours; P < 0.01). Cumulative Na+ balance and gain in body weight were unaltered by tempol infusion. Tempol prevented a rise in MAP with high salt intake.ConclusionTempol corrects hypertension without a compensatory sympathoadrenal activation or salt retention. The response is independent of nitric oxide, endothelin, or catecholamines and occurs despite increased PRA. It is accompanied by a reduction in oxidative stress and is maintained during increased salt intake

    Hot Hole Collection and Photoelectrochemical CO_2 Reduction with Plasmonic Au/p-GaN Photocathodes

    Get PDF
    Harvesting nonequilibrium hot carriers from plasmonic-metal nanostructures offers unique opportunities for driving photochemical reactions at the nanoscale. Despite numerous examples of hot electron-driven processes, the realization of plasmonic systems capable of harvesting hot holes from metal nanostructures has eluded the nascent field of plasmonic photocatalysis. Here, we fabricate gold/p-type gallium nitride (Au/p-GaN) Schottky junctions tailored for photoelectrochemical studies of plasmon-induced hot-hole capture and conversion. Despite the presence of an interfacial Schottky barrier to hot-hole injection of more than 1 eV across the Au/p-GaN heterojunction, plasmonic Au/p-GaN photocathodes exhibit photoelectrochemical properties consistent with the injection of hot holes from Au nanoparticles into p-GaN upon plasmon excitation. The photocurrent action spectrum of the plasmonic photocathodes faithfully follows the surface plasmon resonance absorption spectrum of the Au nanoparticles and open-circuit voltage studies demonstrate a sustained photovoltage during plasmon excitation. Comparison with Ohmic Au/p-NiO heterojunctions confirms that the vast majority of hot holes generated via interband transitions in Au are sufficiently hot to inject above the 1.1 eV interfacial Schottky barrier at the Au/p-GaN heterojunction. We further investigated plasmon-driven photoelectrochemical CO_2 reduction with the Au/p-GaN photocathodes and observed improved selectivity for CO production over H_2 evolution in aqueous electrolytes. Taken together, our results offer experimental validation of photoexcited hot holes more than 1 eV below the Au Fermi level and demonstrate a photoelectrochemical platform for harvesting hot carriers to drive solar-to-fuel energy conversion
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