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J Phys Chem A. 2010 Jun 17;114(23):6502-14. doi: 10.1021/jp102049c.

Selective removal of ethylene, a deposit precursor, from a "dirty" synthesis gas stream via gas-phase partial oxidation.

The journal of physical chemistry. A

Stephanie M Villano, Jessica Hoffmann, Hans-Heinrich Carstensen, Anthony M Dean

Affiliations

  1. Chemical Engineering Department, Colorado School of Mines, Golden, Colorado 80401, USA.

PMID: 20496944 DOI: 10.1021/jp102049c

Abstract

A fundamental issue in the gasification of biomass is that in addition to the desired synthesis gas product (a mixture of H(2) and CO), the gasifier effluent contains other undesirable products that need to be removed before any further downstream processing can occur. This work assesses the potential to selectively remove hydrocarbons from a synthesis gas stream via gas-phase partial oxidation. Specifically, the partial oxidation of methane-doped, ethylene-doped, and methane/ethylene-doped model synthesis gas mixtures has been investigated at ambient pressures over a temperature range of 760-910 degrees C and at residence times ranging from 0.4 to 2.4 s using a tubular flow reactor. For the synthesis gas mixtures that contain either methane or ethylene, the addition of oxygen substantially reduces the hydrocarbon concentration while only a small reduction in the hydrogen concentration is observed. For the synthesis gas mixtures doped with both methane and ethylene, the addition of oxygen preferentially removes ethylene while the concentrations of methane and hydrogen remain relatively unaffected. These results are compared to the predictions of a plug flow model using a reaction mechanism that is designed to describe the pyrolysis and partial oxidation of small hydrocarbon species. The agreement between the experimental observations and the model predictions is quite good, allowing us to explore the underlying chemistry that leads to the hydrocarbon selective oxidation. The implications of these results are briefly discussed in terms of using synthesis gas to produce liquid fuels and electrical power via a solid oxide fuel cell.

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