期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 36, 期 18, 页码 11815-11824出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2011.06.029
关键词
Hydrogen storage; Ammonia cracking; Membrane reactor; CFD model
Ammonia decomposition in an integrated Catalytic Membrane Reactor for hydrogen production was studied by numerical simulation. The process is based on anhydrous NH(3) thermal dissociation inside a small size reactor (30 cm(3)), filled by a Ni/Al(2)O(3) catalyst. The reaction is promoted by the presence of seven Pd coated tubular membranes about 203 mm long, with an outer diameter of 1.98 mm, which shift the NH(3) decomposition towards the products by removing hydrogen from the reaction area. The system fluid-dynamics was implemented into a 2D and 3D geometrical model. Ammonia cracking reaction over the Nil Al(2)O(3) catalyst was simulated using the Temkin-Pyzhev equation. Introductory 2D simulations were first carried out for a hypothetic system without membranes. Because of reactor axial symmetry, different operative pressures, temperatures and input flows were evaluated. These introductory results showed an excellent ammonia conversion at 550 degrees C and 0.2 MPa for an input flow of 1.1 mg/s, with a residual NH3 of only a few ppm. 3D simulations were then carried out for the system with membranes. Hydrogen adsorption throughout the membranes has been modeled using the Sievert's law for the dissociative hydrogen flux. Several runs have been carried out at 1 MPa changing the temperature between 500 degrees C and 600 degrees C to point out the conditions for which the permeated hydrogen flux is the highest. With temperatures higher than 550 degrees C we obtained an almost complete ammonia conversion already before the membrane area. The working temperature of 550 degrees C resulted to be the most suitable for the reactor geometry. A good matching between membrane permeation and ammonia decomposition was obtained for an NH(3) input flow rate of 2.8 mg/s. Ammonia reaction shift due to the presence of H(2) permeable membranes in the reactor significantly fostered the dissociation: for the 550 degrees C case we obtained a conversion rate improvement of almost 18%. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
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