GB657585A - Improvements in or relating to the production of gases containing carbon monoxide and hydrogen from hydrocarbons - Google Patents

Abstract

In the production of carbon monoxide and hydrogen mixtures by the oxidation of gaseous hydrocarbons such as methane with a metal oxide using the fluidized solid technique, copper oxide, supported on a finely-divided carrier of magnesia, alumina, zirconia, thoria or preferably silica, is used to supply oxygen in stoichiometric or slightly greater proportions relative to the feed, and the resulting supported metallic copper acts as a reforming catalyst for the reaction of carbon dioxide and water formed by the oxidation, with unreacted methane to form carbon monoxide and hydrogen. Temperatures from 1500-1850 DEG F. are employed at atmospheric pressure or up to 2400 DEG F. at 400 p.s.i. The catalyst, containing 3-30 per cent copper, may be prepared by adding silica gel to copper nitrate solution, drying, heating to decompose the nitrate, grinding and reducing with methane at 1600 DEG F. Control of the reaction is effected by providing a small <PICT:0657585/III/1> additional pilot reforming zone to which samples of the exit gases may be passed, a highly-active reforming catalyst and higher temperatures such as 2000-2400 DEG F. being provided to ensure completion of reformation. The oxygen feed to the main process is adjusted to provide under normal conditions, from 1/2 to 3 per cent carbon dioxide content in the pilot outflow. Determinations of carbon dioxide content by known methods are then made (a) in the main process exit gases and (b) in the pilot exit gases. If (a) is excessive, either the reformation is incomplete or the oxygen feed is excessive. If (b) is also excessive too much oxide is being fed to the main process, whereas if (b) is normal and (a) excessive, the reforming reaction in the main process is incomplete and reduction of gas velocity or increase in temperature is necessary. In the Figure, the reactor 101 is supplied with hydrocarbon via line 109 and supported copper oxide from regenerator 102 via line 107. The product gas is separated from entrained fines in separator 117, the fines returning to overflow pipe 106 which carries the catalyst from the reactor to the base of the regenerator where oxidizing gas via pipe 111 oxidizes the copper to copper oxide for return to the reactor via pipe 107. The product gas effluent through pipe 119 is sampled via line 120 for carbon dioxide content in device 122 and a further sample withdrawn via line 123 to pass through the pilot reforming zone 124 and carbon dioxide analyzer 126. Specification 635,909 is referred to.