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Howard, Jack B.

Publications and source records attributed to Howard, Jack B..

Combustion Synthesis of Fullerenes and Fullerenic Nanostructures In Microgravity

The objectives of the proposed research were to determine the effects of gravity on fullerenes formation in flames and, based on the observed effects, to develop fundamental understanding of fullerenes formation and to identify engineering principles for fullerenes production. The research method consisted of the operation of laminar diffusion flames under normal- and reduced-gravity conditions, and the collection from the flames and subsequent analysis of condensables including any fullerenes present, using coupled high performance liquid chromatography/mass spectrometry and high resolution transmission electron microscopy. The focus included fullerene molecules C60 and C70 and fullerenic nanostructures including tubes, spherules and other shapes. The normal-gravity experiments were performed at MIT and complementary reduced-gravity experiments were to have been contributed by NASA. The independent variables of interest are gravity, fuel type, fuel/oxygen ratio, pressure, gas velocity at burner, diluent type and concentration. Given the large number of variables and the absence of data on either fullerene formation in diffusion flames or gravitational effects on fullerene formation in diffusion or premixed flames, the first part of the work was exploratory while the later part involved detailed study of the most interesting mechanisms. Samples of condensable material from laminar low pressure benzene/argon/oxygen diffusion flames were collected and analyzed by high-performance liquid chromatography to determine the yields of fullerenes, and by high-resolution transmission electron microscopy (HRTEM) to characterize the fullerenic material, i.e., curved-layer nanostructures, on and within the soot particles. The highest concentration of fullerenes was always detected just above the visible stoichiometric surface of a flame. The percentage of fullerenes in the condensable material increases with decreasing pressure. The overall highest amount of fullerenes was found for a surprisingly high dilution fuel with argon. The maximum flame temperature seems to be of minor importance in fullerene formation. The HRTEM analysis of the soot showed an increase of the curvature of the carbon layers, and hence increased fullerenic character. After this maximum, the curvature decreases. In addition to the soot, the samples included fullerenic nanostructures, such as tubes and spheroids including highly-ordered multilayered or onion-like structures. The soot itself shows highly ordered regions that appear to have been cells of ongoing fullerenic nanostructure formation.

Howard, Jack B.↗

Synthesis of Fullerenes in Low Pressure Benzene/Oxygen Diffusion Flames

The interest in fullerenes is strongly increasing since their discovery by Kroto et al. in 1985 as products of the evaporation of carbon into inert gas at low pressure. Due to their all carbon closed-shell structure, fullerenes have many exceptional physical and chemical properties and a large potential for applications such as superconductors, sensors, catalysts, optical and electronic devices, polymers, high energy fuels, and biological and medical materials. This list is still growing, because the research on fullerenes is still at an early stage. Fullerenes can be formed not only in a system containing only carbon and an inert gas, but also in premixed hydrocarbon flames under reduced pressure and fuel rich conditions. The highest yields of fullerenes in flames are obtained under conditions of substantial soot formation. There is a need for more information on the yields of fullerenes under different conditions in order to understand the mechanisms of their formation and to enable the design of practical combustion systems for large-scale fullerene production. Little work has been reported on the formation of fullerenes in diffusion flames. In order to explore the yields of fullerenes and the effect of low pressure in diffusion flames, therefore we constructed and used a low pressure diffusion flame burner in this study.

Hebgen, Peter↗

Fullerenes, PAH, Carbon Nanostructures, and Soot in Low Pressure Diffusion Flames

The formation of fullerenes C60 and C7O is known to occur in premixed laminar benzene/oxygen/argon flames operated at reduced pressures. High resolution transmission electron microscopy (HRTEM) images of material collected from these flames has identified a variety of multishelled nanotubes and fullerene 'onions' as well as some trigonous structures. These fullerenes and nanostructures resemble the material that results from commercial fullerene production systems using graphite vaporization. As a result, combustion is an interesting method for fullerenes synthesis. If commercial scale operation is to be considered, the use of diffusion flames might be safer and less cumbersome than premixed flames. However, it is not known whether diffusion flames produce the types and yields of fullerenes obtained from premixed benzene/oxygen flames. Therefore, the formation of fullerenes and carbon nanostructures, as well as polycyclic aromatic hydrocarbons (PAH) and soot, in acetylene and benzene diffusion flames is being studied using high performance liquid chromatography (HPLC) and high resolution transmission electron microscopy (HRTEM).

Grieco, William J.↗

Fullerenes formation in flames

Fullerenes are composed of carbon atoms arranged in approximately spherical or ellipsoidal cages resembling the geodesic domes designed by Buckminster Fuller, after whom the molecules were named. The approximately spherical fullerene, which resembles a soccer ball and contains sixty atoms (C60), is called buckminsterfullerene. The fullerene containing seventy carbon atoms (C70) is approximately ellipsoidal, similar to a rugby ball. Fullerenes were first detected in 1985, in carbon vapor produced by laser evaporation of graphite. The closed shell structure, which has no edge atoms vulnerable to reaction, was proposed to explain the observed high stability of certain carbon clusters relative to that of others at high temperatures and in the presence of an oxidizing gas.

Howard, Jack B.↗