Journal
JOURNAL OF MEMBRANE SCIENCE
Volume 337, Issue 1-2, Pages 188-199Publisher
ELSEVIER
DOI: 10.1016/j.memsci.2009.03.040
Keywords
Steam reforming of methane; One-dimensional model; Two-dimensional model; Silica-alumina membrane; Membrane reactor; General criterion
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Studies of the steam reforming of methane were carried out at high temperature (773-923 K) and pressure (0.1-2.0 MPa (1-20 atm)) using a commercial Ni/MgAl2O4 catalyst in a reactor equipped with a tubular hydrogen-selective silica-alumina membrane. The membrane was prepared using a chemical vapor deposition (CVD) method which gave a H-2 permeance of 1.6 x 10(-7) mol m(-2) s(-1) Pa-1 with a H-2/CH4 selectivity of 710 at 923 K. Operation as a membrane reactor gave improved methane conversions and hydrogen yields compared to use as a packed-bed reactor at all temperatures and pressures. One-dimensional (1D) and two-dimensional (2-D) models without adjustable parameters were developed to describe the performance of the two reactors. The 2-D model gave a slightly better fit to the membrane reactor results than the 1-D model, which predicted higher conversion at high pressure than observed experimentally. This was because the 2-D model correctly accounted for decreased permeant concentrations in the vicinity of the membrane (concentration polarization) which reduce the driving force for permeation and give lower conversions. A general criterion, denoted as the Order-Hierarchy Criterion, is developed for predicting when a 2-D model should be applied instead of a 1-D model for describing reactor performance. The 2-D description is necessary when both deviations from plug-flow behavior occur and when the rate of permeation > the rate of reaction, calculated at entrance conditions. (C) 2009 Elsevier B.V. All rights reserved.
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