화학공학소재연구정보센터
Journal of Catalysis, Vol.176, No.2, 503-512, 1998
Oxygenate formation from n-butane oxidation at short contact times : Different gauze sizes and multiple steady states
The production of olefins and oxygenates by partial oxidation of n-butane over a single layer of Pt-10% Rh gauze has been examined at atmospheric pressure in the fuel rich regime and in the space velocity range of 3.3 x 10(6) to 1.6 x 10(7) h(-1) (contact times of similar to 1000 to 200 mu s) using a single gauze reactor. We show that there is an optimum regime of space velocities to maximize the oxygenate selectivity and that at least 75% selectivity to olefins and oxygenates can be obtained. Nitrogen diluent in the feed lowers the production of oxygenates, and coarser mesh gauze gives higher oxygenate yield than finer mesh. In addition, at a specific range of fuel/oxygen feed ratios, multiple steady states are observed on the more open gauze. Analysis of the product distribution of these steady states indicates that initially the exothermic complete combustion of the butane on the gauze surface to CO2 and H2O provides most of the necessary heat for this process. Oxygenates and olefins are then produced by homogeneous reaction in the quench zone downstream of the gauze. A detailed model of homogeneous chemistry confirms that oxygenates are produced by homogeneous reactions.