Design, Synthesis, and Properties of Chemical Vapor Deposited Diamond on Inorganic Oxide Catalysts: Experimentation and Simulation

Khushrav E. Nariman, Jan Joseph Lerou, Kenneth B. Bischoff, Henry C. Foley

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

The effects of a porous diamond coating on the physical and chemical properties of catalytic inorganic oxides have been studied with experimentation and simulation. A layer of diamond 20–50 µm thick has been grown on pellets of silica alumina, using voltage-biased, hot-filament chemical vapor deposition. The morphology and thickness of the coating is examined by scanning electron microscopy. Nitrogen and argon porosimetry indicate that the surface area, pore volume, and pore-size distribution of the diamond-coated silica alumina are virtually identical to those of the native oxide (surface area = 73 m2/g, pore volume = 0.38 cm3/g r̄ = 34 Å). Dehydration of methanol over the diamond-coated and uncoated silica alumina pellets leads to experimentally equivalent levels of conversion over the full range of temperatures tested (∼20% at 175 °C to ∼80% at 475 °C). Despite these physical similarities at the pellet level, thermal conductivities were measurably enhanced by the diamond coating. This effect is clear from the ratio of the thermal conductivities of the coated and uncoated pellets (50-µm film λctdλuc = 2.4, 20-µm film λctduc = 1.6). Simulation was used to consider the extent of the effect that a porous diamond coating could have on heat transport through a packed bed. Oxidation of o-xylene was simulated, for diamond-coated and uncoated vanadium pentoxide catalysts, using the two-dimensional, heterogeneous model of DeWasch and Froment and with thermal conductivities based on our own experimental results with diamond on silica alumina. The results of the simulation indicate that, for a fixed bed of diamond-coated particles, temperature gradients could be reduced and selectivity increased versus those obtained with uncoated particles.

Original languageEnglish (US)
Pages (from-to)263-273
Number of pages11
JournalIndustrial and Engineering Chemistry Research
Volume32
Issue number2
DOIs
StatePublished - Jan 1 1993

Fingerprint

Diamond
Oxides
Diamonds
Vapors
Catalysts
Aluminum Oxide
Silicon Dioxide
Alumina
Silica
Coatings
Thermal conductivity
Argon
Packed beds
Xylene
Dehydration
Vanadium
Thermal gradients
Chemical properties
Pore size
Methanol

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

Cite this

Nariman, Khushrav E. ; Lerou, Jan Joseph ; Bischoff, Kenneth B. ; Foley, Henry C. / Design, Synthesis, and Properties of Chemical Vapor Deposited Diamond on Inorganic Oxide Catalysts : Experimentation and Simulation. In: Industrial and Engineering Chemistry Research. 1993 ; Vol. 32, No. 2. pp. 263-273.
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abstract = "The effects of a porous diamond coating on the physical and chemical properties of catalytic inorganic oxides have been studied with experimentation and simulation. A layer of diamond 20–50 µm thick has been grown on pellets of silica alumina, using voltage-biased, hot-filament chemical vapor deposition. The morphology and thickness of the coating is examined by scanning electron microscopy. Nitrogen and argon porosimetry indicate that the surface area, pore volume, and pore-size distribution of the diamond-coated silica alumina are virtually identical to those of the native oxide (surface area = 73 m2/g, pore volume = 0.38 cm3/g r̄ = 34 {\AA}). Dehydration of methanol over the diamond-coated and uncoated silica alumina pellets leads to experimentally equivalent levels of conversion over the full range of temperatures tested (∼20{\%} at 175 °C to ∼80{\%} at 475 °C). Despite these physical similarities at the pellet level, thermal conductivities were measurably enhanced by the diamond coating. This effect is clear from the ratio of the thermal conductivities of the coated and uncoated pellets (50-µm film λctdλuc = 2.4, 20-µm film λctd/λuc = 1.6). Simulation was used to consider the extent of the effect that a porous diamond coating could have on heat transport through a packed bed. Oxidation of o-xylene was simulated, for diamond-coated and uncoated vanadium pentoxide catalysts, using the two-dimensional, heterogeneous model of DeWasch and Froment and with thermal conductivities based on our own experimental results with diamond on silica alumina. The results of the simulation indicate that, for a fixed bed of diamond-coated particles, temperature gradients could be reduced and selectivity increased versus those obtained with uncoated particles.",
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Design, Synthesis, and Properties of Chemical Vapor Deposited Diamond on Inorganic Oxide Catalysts : Experimentation and Simulation. / Nariman, Khushrav E.; Lerou, Jan Joseph; Bischoff, Kenneth B.; Foley, Henry C.

In: Industrial and Engineering Chemistry Research, Vol. 32, No. 2, 01.01.1993, p. 263-273.

Research output: Contribution to journalArticle

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T1 - Design, Synthesis, and Properties of Chemical Vapor Deposited Diamond on Inorganic Oxide Catalysts

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AU - Nariman, Khushrav E.

AU - Lerou, Jan Joseph

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AU - Foley, Henry C.

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N2 - The effects of a porous diamond coating on the physical and chemical properties of catalytic inorganic oxides have been studied with experimentation and simulation. A layer of diamond 20–50 µm thick has been grown on pellets of silica alumina, using voltage-biased, hot-filament chemical vapor deposition. The morphology and thickness of the coating is examined by scanning electron microscopy. Nitrogen and argon porosimetry indicate that the surface area, pore volume, and pore-size distribution of the diamond-coated silica alumina are virtually identical to those of the native oxide (surface area = 73 m2/g, pore volume = 0.38 cm3/g r̄ = 34 Å). Dehydration of methanol over the diamond-coated and uncoated silica alumina pellets leads to experimentally equivalent levels of conversion over the full range of temperatures tested (∼20% at 175 °C to ∼80% at 475 °C). Despite these physical similarities at the pellet level, thermal conductivities were measurably enhanced by the diamond coating. This effect is clear from the ratio of the thermal conductivities of the coated and uncoated pellets (50-µm film λctdλuc = 2.4, 20-µm film λctd/λuc = 1.6). Simulation was used to consider the extent of the effect that a porous diamond coating could have on heat transport through a packed bed. Oxidation of o-xylene was simulated, for diamond-coated and uncoated vanadium pentoxide catalysts, using the two-dimensional, heterogeneous model of DeWasch and Froment and with thermal conductivities based on our own experimental results with diamond on silica alumina. The results of the simulation indicate that, for a fixed bed of diamond-coated particles, temperature gradients could be reduced and selectivity increased versus those obtained with uncoated particles.

AB - The effects of a porous diamond coating on the physical and chemical properties of catalytic inorganic oxides have been studied with experimentation and simulation. A layer of diamond 20–50 µm thick has been grown on pellets of silica alumina, using voltage-biased, hot-filament chemical vapor deposition. The morphology and thickness of the coating is examined by scanning electron microscopy. Nitrogen and argon porosimetry indicate that the surface area, pore volume, and pore-size distribution of the diamond-coated silica alumina are virtually identical to those of the native oxide (surface area = 73 m2/g, pore volume = 0.38 cm3/g r̄ = 34 Å). Dehydration of methanol over the diamond-coated and uncoated silica alumina pellets leads to experimentally equivalent levels of conversion over the full range of temperatures tested (∼20% at 175 °C to ∼80% at 475 °C). Despite these physical similarities at the pellet level, thermal conductivities were measurably enhanced by the diamond coating. This effect is clear from the ratio of the thermal conductivities of the coated and uncoated pellets (50-µm film λctdλuc = 2.4, 20-µm film λctd/λuc = 1.6). Simulation was used to consider the extent of the effect that a porous diamond coating could have on heat transport through a packed bed. Oxidation of o-xylene was simulated, for diamond-coated and uncoated vanadium pentoxide catalysts, using the two-dimensional, heterogeneous model of DeWasch and Froment and with thermal conductivities based on our own experimental results with diamond on silica alumina. The results of the simulation indicate that, for a fixed bed of diamond-coated particles, temperature gradients could be reduced and selectivity increased versus those obtained with uncoated particles.

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