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Kinetic modeling and packed bed membrane reactor scale-up for ammonia decomposition

Hydrogen economy is capitalizing the decarbonization of transport and industrial sectors. Ammonia is an attractive intermediate to store and transport hydrogen, due to its low production cost, well developed storage and transportation infrastruc- ture, high hydrogen density in its liquified form (for transportation) and the potential production from renewable energy sources. Although there have been significant ad- vancements in catalyst development for ammonia decomposition, the potential of this technology cannot be fully exploited until significant process development is made. In this sense, catalytic membrane reactors show promising features and performances.
In this work, ammonia decomposition has been studied using the following ap- proach: (1) Catalytic Packed Bed Reactor (CPBR) and kinetic modeling, (2) Cat- alytic Packed Bed Membrane Reactor (CPBMR) modeling and (3) CPBMR scale-up.
Stage (1) was performed using Ru-K/CaO and Co-Ce catalysts over a wide range of experimental conditions (including pressures up to 16 bar). Stage (2) includes 1-D and 2-D models that were further validated experimentally, also using different software to tackle the stage (3), which aims to give the optimized geometry and properties of a CPBMR for a production of 5 N m3 h−1 of high purity H2 .
The results presented in this Thesis enabled to: (1) obtain a reliable kinetic model
capable of describing the ammonia decomposition under a wide range of operating conditions, using Ru-K/CaO and Co-Ce catalysts. (2) identify a range of operat- ing conditions where the CPBMR performs better than the CPBR in terms of NH3

conversion, H2 recovery and H2 purity. This range includes: reaction temperature between 250◦C and 500◦C; reaction pressures between 1 and 16 bar; space times be- tween 1 and 15 gcat h mol−1 and H2 permeate pressure higher than the atmospheric
pressure (up to 5 bar). (3) scale-up the CPBMR for ammonia decomposition at a
pilot scale, encountering that a pilot plant for a production of 5 N m3 h−1 of pure H2 ( >99.99%) could be obtained with a relatively small multitubular arraignment, that might be even smaller than the needed for the same product using other technology.

Identiferoai:union.ndltd.org:kaust.edu.sa/oai:repository.kaust.edu.sa:10754/668818
Date04 1900
CreatorsRealpe, Natalia
ContributorsCastaño, Pedro, Physical Science and Engineering (PSE) Division, Gascon, Jorge, Roberts, William L.
Source SetsKing Abdullah University of Science and Technology
LanguageEnglish
Detected LanguageEnglish
TypeThesis
Rights2024-04-16, At the time of archiving, the student author of this thesis opted to temporarily restrict access to it. The full text of this thesis will become available to the public after the expiration of the embargo on 2024-04-16.

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