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Partial oxidation of methane to methyl chloride with tetrachloromethane on strontium hydroxyapatites ion-exchanged with lead

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Abstract

The partial oxidation of methane has been investigated in the presence and absence of tetrachloromethane (TCM) on strontium hydroxyapatites ion-exchanged with lead (SrPbHAp) at 773 K, at which temperature the apatites exist stably and do not convert to the corresponding phosphates. In the absence of TCM, the conversion of methane increased and the selectivity to carbon dioxide approached 100% as the lead content was increased. With a small quantity of TCM in the feedstream and at longer times-on-stream the selectivities to carbon dioxide decreased, those to carbon monoxide increased. Methyl chloride was formed at the higher times-on-stream on all catalyst compositions, but reached selectivities of 73% with those catalysts of Pb/Sr equal to or greater than 0.26. In contrast the conversion of methane decreased with increasing times-on-stream with the latter compositions. XRD and XPS measurements provide evidence for the introduction of Cl into the surface of PbSrAp, apparently forming the corresponding chlorapatite, although not precluding the existence of chlorine in additional configurations. Concomitantly a portion of the cationic lead is reduced to the metallic state. While TCM is evidently required for the production of methyl chloride, the presence of ion-exchanged lead appears to be required to achieve the highest selectivities for the aforementioned chloride.

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Authors
  1. S. Sugiyama
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  2. Y. Iguchi
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  3. T. Minami
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  4. H. Hayashi
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  5. J.B. Moffat
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Sugiyama, S., Iguchi, Y., Minami, T. et al. Partial oxidation of methane to methyl chloride with tetrachloromethane on strontium hydroxyapatites ion-exchanged with lead. Catalysis Letters 46, 279–285 (1997). https://doi.org/10.1023/A:1019039123113

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  • DOI: https://doi.org/10.1023/A:1019039123113

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