Catalyst instabilities during the liquid phase partial oxidation of methane

Research output: Contribution to journalArticle

  • 6 Citations

Abstract

A promising catalytic system for the low temp. oxidn. of methane to a methanol deriv. was studied under both batch and semi-continuous operation in two different reactor types. The system comprises of a bimetallic palladium and copper (II) chloride catalyst contained in a trifluoroacetic acid (TFA) and an aq. phase. Methane, oxygen and a co-reductant carbon monoxide constitute the gas phase. Typical operating conditions were a temp. of 85 Deg and a pressure of 83 bar and the yields of the Me trifluoroacetate product obsd. in this present work were less than those obtained in other batch autoclave works, which employed only 4 mL of liq. phase, compared with 50 mL in this study. Furthermore, an encouraging initial product formation rate of ca. 40 mol/m3 h, quickly decreased after the first hour, and came to an apparent end after only 2 h. This observation had not been reported previously and the work performed in a semi-continuous porous tube reactor (300 mL of re-circulating liq. phase) also showed the same reaction characteristics as in the batch reactor. Thus, the deteriorating product formation rate cannot be attributed to gaseous reactant depletion (batch operation). The results suggest problems assocd. with catalyst instabilities, e.g. with the previously elucidated Wacker chem. [on SciFinder (R)]
LanguageEnglish
Pages631-640
Number of pages10
JournalCatalysis Today
Volume81
Issue number4
StatusPublished - 2003

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Trifluoroacetic Acid
Methane
Trifluoroacetic acid
Oxidation
Catalysts
Reducing Agents
Autoclaves
Palladium
Batch reactors
Liquids
Carbon Monoxide
Carbon monoxide
Methanol
Gases
Oxygen
Copper
cupric chloride

Keywords

  • Oxidation catalysts (partial
  • bimetallic catalyst for liq. phase partial oxidn. of methane and the catalyst instabilities thereof)
  • bimetallic palladium copper chloride catalyst methane partial oxidn
  • Reactors (batch
  • semicontinuous
  • Oxidation (of methane using bimetallic catalyst and the catalyst instabilities thereof)
  • Reactors (tubular
  • for liq. phase partial oxidn. of methane using bimetallic palladium and copper (II) chloride catalyst and the catalyst instabilities thereof)

Cite this

Catalyst instabilities during the liquid phase partial oxidation of methane. / Williams, Gareth R; Kolaczkowski, Stan T; Plucinski, Pawel.

In: Catalysis Today, Vol. 81, No. 4, 2003, p. 631-640.

Research output: Contribution to journalArticle

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abstract = "A promising catalytic system for the low temp. oxidn. of methane to a methanol deriv. was studied under both batch and semi-continuous operation in two different reactor types. The system comprises of a bimetallic palladium and copper (II) chloride catalyst contained in a trifluoroacetic acid (TFA) and an aq. phase. Methane, oxygen and a co-reductant carbon monoxide constitute the gas phase. Typical operating conditions were a temp. of 85 Deg and a pressure of 83 bar and the yields of the Me trifluoroacetate product obsd. in this present work were less than those obtained in other batch autoclave works, which employed only 4 mL of liq. phase, compared with 50 mL in this study. Furthermore, an encouraging initial product formation rate of ca. 40 mol/m3 h, quickly decreased after the first hour, and came to an apparent end after only 2 h. This observation had not been reported previously and the work performed in a semi-continuous porous tube reactor (300 mL of re-circulating liq. phase) also showed the same reaction characteristics as in the batch reactor. Thus, the deteriorating product formation rate cannot be attributed to gaseous reactant depletion (batch operation). The results suggest problems assocd. with catalyst instabilities, e.g. with the previously elucidated Wacker chem. [on SciFinder (R)]",
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