Search Results Heading

MBRLSearchResults

mbrl.module.common.modules.added.book.to.shelf
Title added to your shelf!
View what I already have on My Shelf.
Oops! Something went wrong.
Oops! Something went wrong.
While trying to add the title to your shelf something went wrong :( Kindly try again later!
Are you sure you want to remove the book from the shelf?
Oops! Something went wrong.
Oops! Something went wrong.
While trying to remove the title from your shelf something went wrong :( Kindly try again later!
    Done
    Filters
    Reset
  • Discipline
      Discipline
      Clear All
      Discipline
  • Is Peer Reviewed
      Is Peer Reviewed
      Clear All
      Is Peer Reviewed
  • Item Type
      Item Type
      Clear All
      Item Type
  • Subject
      Subject
      Clear All
      Subject
  • Year
      Year
      Clear All
      From:
      -
      To:
  • More Filters
69 result(s) for "Howe, Jane Y."
Sort by:
Gold-in-copper at low CO coverage enables efficient electromethanation of CO2
The renewable-electricity-powered CO 2 electroreduction reaction provides a promising means to store intermittent renewable energy in the form of valuable chemicals and dispatchable fuels. Renewable methane produced using CO 2 electroreduction attracts interest due to the established global distribution network; however, present-day efficiencies and activities remain below those required for practical application. Here we exploit the fact that the suppression of *CO dimerization and hydrogen evolution promotes methane selectivity: we reason that the introduction of Au in Cu favors *CO protonation vs. C−C coupling under low *CO coverage and weakens the *H adsorption energy of the surface, leading to a reduction in hydrogen evolution. We construct experimentally a suite of Au-Cu catalysts and control *CO availability by regulating CO 2 concentration and reaction rate. This strategy leads to a 1.6× improvement in the methane:H 2 selectivity ratio compared to the best prior reports operating above 100 mA cm −2 . We as a result achieve a CO 2 -to-methane Faradaic efficiency (FE) of (56 ± 2)% at a production rate of (112 ± 4) mA cm −2 . The electroreduction of CO 2 offers a promising approach to produce carbon-neutral methane using renewable electricity. This study shows that the introduction of Au in Cu enables selective methane production from CO 2 by regulating *CO availability.
New black indium oxide—tandem photothermal CO2-H2 methanol selective catalyst
It has long been known that the thermal catalyst Cu/ZnO/Al 2 O 3 (CZA) can enable remarkable catalytic performance towards CO 2 hydrogenation for the reverse water-gas shift (RWGS) and methanol synthesis reactions. However, owing to the direct competition between these reactions, high pressure and high hydrogen concentration (≥75%) are required to shift the thermodynamic equilibrium towards methanol synthesis. Herein, a new black indium oxide with photothermal catalytic activity is successfully prepared, and it facilitates a tandem synthesis of methanol at a low hydrogen concentration (50%) and ambient pressure by directly using by-product CO as feedstock. The methanol selectivities achieve 33.24% and 49.23% at low and high hydrogen concentrations, respectively. Harsh reaction conditions are generally required for CO2 hydrogenation to shift the thermodynamic equilibrium towards methanol synthesis. Here, a new black indium oxide with two types of active sites, frustrated Lewis pairs and oxygen vacancies, is prepared, and facilitates a tandem synthesis of methanol at a low hydrogen concentration (50%) and ambient pressure.
The critical role of point defects in improving the specific capacitance of δ-MnO2 nanosheets
3D porous nanostructures built from 2D δ-MnO 2 nanosheets are an environmentally friendly and industrially scalable class of supercapacitor electrode material. While both the electrochemistry and defects of this material have been studied, the role of defects in improving the energy storage density of these materials has not been addressed. In this work, δ-MnO 2 nanosheet assemblies with 150 m 2  g −1 specific surface area are prepared by exfoliation of crystalline K x MnO 2 and subsequent reassembly. Equilibration at different pH introduces intentional Mn vacancies into the nanosheets, increasing pseudocapacitance to over 300 F g −1 , reducing charge transfer resistance as low as 3 Ω, and providing a 50% improvement in cycling stability. X-ray absorption spectroscopy and high-energy X-ray scattering demonstrate a correlation between the defect content and the improved electrochemical performance. The results show that Mn vacancies provide ion intercalation sites which concurrently improve specific capacitance, charge transfer resistance and cycling stability. Two-dimensional solids are of interest for energy storage due to their large accessible surface area, enabling rapid charge/discharge. Here, the authors quantify the point defects in oxide nanosheets, demonstrating that intentional introduction of charged point defects improves the charge storage behaviour.
In-situ restructuring of Ni-based metal organic frameworks for photocatalytic CO2 hydrogenation
As the global quest for sustainable energy keeps rising, exploring novel efficient and practical photocatalysts remains a research and industrial urge. Particularly, metal organic frameworks were proven to contribute to various stages of the carbon cycle, from CO 2 capture to its conversion. Herein, we report the photo-methanation activity of three isostructural, nickel-based metal organic frameworks incorporating additional niobium, iron, and aluminum sites, having demonstrated exceptional CO 2 capture abilities from thin air in previous reports. The niobium version exhibits the highest performance, with a CO 2 to CH 4 conversion rate in the order of 750–7500 µmol*g catalyst −1 *h −1 between 180 °C and 240 °C, achieving 97% selectivity under light irradiation and atmospheric pressure. The in-depth characterization of this framework before and after catalysis reveals the occurrence of an in-situ restructuring process, whereas active surface species are formed under photocatalytic conditions, thus providing comprehensive structure-performance correlations for the development of efficient CO 2 conversion photocatalysts. This study correlates the structure and the CO 2 photohydrogenation performance of a series of isostructural Ni-based MOFs. Comparative characterization reveals the occurrence of an in situ restructuring, yielding different surface active sites.
Reactive capture of CO2 via amino acid
Reactive capture of carbon dioxide (CO 2 ) offers an electrified pathway to produce renewable carbon monoxide (CO), which can then be upgraded into long-chain hydrocarbons and fuels. Previous reactive capture systems relied on hydroxide- or amine-based capture solutions. However, selectivity for CO remains low (<50%) for hydroxide-based systems and conventional amines are prone to oxygen (O 2 ) degradation. Here, we develop a reactive capture strategy using potassium glycinate (K-GLY), an amino acid salt (AAS) capture solution applicable to O 2 -rich CO 2 -lean conditions. By employing a single-atom catalyst, engineering the capture solution, and elevating the operating temperature and pressure, we increase the availability of dissolved in-situ CO 2 and achieve CO production with 64% Faradaic efficiency (FE) at 50 mA cm −2 . We report a measured CO energy efficiency (EE) of 31% and an energy intensity of 40 GJ t CO −1 , exceeding the best hydroxide- and amine-based reactive capture reports. The feasibility of the full reactive capture process is demonstrated with both simulated flue gas and direct air input. The electrosynthesis of CO via integrated capture and conversion of dilute CO 2 suffers from low energy efficiency. Here, the authors report an amino acid salt-based system that employs a single-atom catalyst and operates at an elevated temperature and pressure, which enables efficient CO production.
Constraining CO coverage on copper promotes high-efficiency ethylene electroproduction
The availability of inexpensive industrial CO gas streams motivates efficient electrocatalytic upgrading of CO to higher-value feedstocks such as ethylene. However, the electrosynthesis of ethylene by the CO reduction reaction (CORR) has suffered from low selectivity and energy efficiency. Here we find that the recent strategy of increasing performance through use of highly alkaline electrolyte—which is very effective in CO 2 RR—fails in CORR and drives the reaction to acetate. We then observe that ethylene selectivity increases when we constrain (decrease) CO availability. Using density functional theory, we show how CO coverage on copper influences the reaction pathways of ethylene versus oxygenate: lower CO coverage stabilizes the ethylene-relevant intermediates whereas higher CO coverage favours oxygenate formation. We then control local CO availability experimentally by tuning the CO concentration and reaction rate; we achieve ethylene Faradaic efficiencies of 72% and a partial current density of >800 mA cm −2 . The overall system provides a half-cell energy efficiency of 44% for ethylene production. The electrocatalytic upgrading of CO to higher-value feedstocks provides a promising route to multicarbon products. Here, the authors show that high ethylene selectivity can be achieved by constraining CO availability on copper, with an ethylene Faradaic efficiency of 72% and a partial current density of >800 mA cm −2 .
Copper adparticle enabled selective electrosynthesis of n-propanol
The electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products; however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation. Density functional theory calculations suggest that copper adparticles increase CO binding energy and stabilize two-carbon intermediates, facilitating coupling between adsorbed *CO and two-carbon intermediates to form three-carbon products. We form adparticle-covered catalysts in-situ by mediating catalyst growth with strong CO chemisorption. The new catalysts exhibit an n-propanol Faradaic efficiency of 23% from CO reduction at an n-propanol partial current density of 11 mA cm −2 . Upgrading wasted carbon emissions to high-value, multi-carbon products provides an economic route to reduce carbon dioxide levels, but such conversions have proven challenging. Here, authors explore copper adparticles as highly active surfaces that convert CO to n-propanol with high selectivities.
Lipid-Coated Mesoporous Silica Nanoparticles for the Delivery of the ML336 Antiviral to Inhibit Encephalitic Alphavirus Infection
Venezuelan equine encephalitis virus (VEEV) poses a major public health risk due to its amenability for use as a bioterrorism agent and its severe health consequences in humans. ML336 is a recently developed chemical inhibitor of VEEV, shown to effectively reduce VEEV infection in vitro and in vivo . However, its limited solubility and stability could hinder its clinical translation. To overcome these limitations, lipid-coated mesoporous silica nanoparticles (LC-MSNs) were employed. The large surface area of the MSN core promotes hydrophobic drug loading while the liposome coating retains the drug and enables enhanced circulation time and biocompatibility, providing an ideal ML336 delivery platform. LC-MSNs loaded 20 ± 3.4 μg ML336/mg LC-MSN and released 6.6 ± 1.3 μg/mg ML336 over 24 hours. ML336-loaded LC-MSNs significantly inhibited VEEV in vitro in a dose-dependent manner as compared to unloaded LC-MSNs controls. Moreover, cell-based studies suggested that additional release of ML336 occurs after endocytosis. In vivo safety studies were conducted in mice, and LC-MSNs were not toxic when dosed at 0.11 g LC-MSNs/kg/day for four days. ML336-loaded LC-MSNs showed significant reduction of brain viral titer in VEEV infected mice compared to PBS controls. Overall, these results highlight the utility of LC-MSNs as drug delivery vehicles to treat VEEV.
New yellow Ba0.93Eu0.07Al2O4 phosphor for warm-white light-emitting diodes through single-emitting-center conversion
Phosphor-converted white light-emitting diodes for indoor illumination need to be warm-white (i.e., correlated color temperature <4000 K) with good color rendition (i.e., color rendering index >80). However, no single-phosphor, single-emitting-center-converted white light-emitting diodes can simultaneously satisfy the color temperature and rendition requirements due to the lack of sufficient red spectral component in the phosphors’ emission spectrum. Here, we report a new yellow Ba 0.93 Eu 0.07 Al 2 O 4 phosphor that has a new orthorhombic lattice structure and exhibits a broad yellow photoluminescence band with sufficient red spectral component. Warm-white emissions with correlated color temperature <4000 K and color rendering index >80 were readily achieved when combining the Ba 0.93 Eu 0.07 Al 2 O 4 phosphor with a blue light-emitting diode (440–470 nm). This study demonstrates that warm-white light-emitting diodes with high color rendition (i.e., color rendering index >80) can be achieved based on single-phosphor, single-emitting-center conversion. Light-emitting diodes: Warm-white lighting Scientists have developed a yellow phosphor that can be used to provide a pleasing white light with a warm color temperature when combined with a blue light-emitting diode (LED) chip. Although YAG: Ce-based white LEDs show great promise as a highly efficient and long-lasting form of domestic lighting, their cool bluish-white light makes them undesirable for use in the home. Scientists from the USA and China have now shown that a new phosphor, Ba 0.93 Eu 0.07 Al 2 O 4 , when combined with a blue InGaN LED, provides a pleasing white light with a warm colour temperature of less than 4000K and a high colour-rendering index of more than 80. The phosphor has an orthorhombic structure and was manufactured by carbothermal reduction and vapour phase deposition in a tube furnace system. This work suggests that high-quality, warm-white lighting can be achieved using a combination of a single phosphor with single-emitting-center and a blue LED chip.
Redox Active Organic-Carbon Composites for Capacitive Electrodes: A Review
The pressing concerns of environmental sustainability and growing needs of clean energy have raised the demands of carbon and organic based energy storage materials to a higher level. Redox-active organic-carbon composites electrodes are emerging to be enablers for high-performance, high power and long-lasting energy storage solutions, especially for electrochemical capacitors (EC). This review discusses the electrochemical redox active organic compounds and their composites with various carbonaceous materials focusing on capacitive performance. Starting with the most common conducting polymers, we expand the scope to other emerging redox active molecules, compounds and polymers as well as common carbonaceous substrates in composite electrodes, including graphene, carbon nanotube and activated carbon. We then discuss the first-principles computational studies pertaining to the interactions between the components in the composites. The fabrication methodologies for the composites with thin organic coatings are presented with their merits and shortcomings. The capacitive performances and features of the redox active organic-carbon composite electrodes are then summarized. Finally, we offer some perspectives and future directions to achieve a fundamental understanding and to better design organic-carbon composite electrodes for ECs.