Modelling of packed bed membrane reactors for autothermal production of ultrapure hydrogen

T.P. Tiemersma, C.S. Patil, M. Sint Annaland, van, J.A.M. Kuipers

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Abstract

The conceptual feasibility of a packed bed membrane reactor for the autothermal reforming (ATR) of methane for the production of ultrapure hydrogen was investigated. By integrating H2 permselective Pd-based membranes under autothermal conditions, a high degree of process integration and intensification can be accomplished which is particularly interesting for small scale H2 production units. A two-dimensional pseudo-homogeneous packed bed membrane reactor model was developed that solves the continuity and momentum equations and the component mass and energy balances. In adiabatic operation, autothermal operation can be achieved; however, large axial temperature excursions were seen at the reactor inlet, which are disadvantageous for membrane life and catalyst performance. Different operation modes, such as cooling the reactor wall with sweep gas or distributive feeding of O2 along the reactor length to moderate the temperature profile, are evaluated. The concentration polarisation because of the selective hydrogen removal along the membrane length was found to become significant with increasing membrane permeability thereby constraining the reactor design. To decrease the negative effects of mass transfer limitations to the membrane wall, a small membrane tube diameter needs to be selected. For a relatively small ratio of the membrane tube diameter to the particle diameter, the porosity profile needs to be taken into account to prevent overestimation of the H2 removal rate. It is concluded that autothermal production of H2 in a PBMR is feasible, provided that the membranes are positioned outside the inlet region with large temperature gradients.
Original languageEnglish
Pages (from-to)1602-1616
Number of pages15
JournalChemical Engineering Science
Volume61
Issue number5
DOIs
Publication statusPublished - 2006

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Packed beds
Hydrogen
Membranes
Methane
Reforming reactions
Energy balance
Thermal gradients
Momentum
Mass transfer
Porosity
Gases
Polarization
Cooling
Temperature
Catalysts

Cite this

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title = "Modelling of packed bed membrane reactors for autothermal production of ultrapure hydrogen",
abstract = "The conceptual feasibility of a packed bed membrane reactor for the autothermal reforming (ATR) of methane for the production of ultrapure hydrogen was investigated. By integrating H2 permselective Pd-based membranes under autothermal conditions, a high degree of process integration and intensification can be accomplished which is particularly interesting for small scale H2 production units. A two-dimensional pseudo-homogeneous packed bed membrane reactor model was developed that solves the continuity and momentum equations and the component mass and energy balances. In adiabatic operation, autothermal operation can be achieved; however, large axial temperature excursions were seen at the reactor inlet, which are disadvantageous for membrane life and catalyst performance. Different operation modes, such as cooling the reactor wall with sweep gas or distributive feeding of O2 along the reactor length to moderate the temperature profile, are evaluated. The concentration polarisation because of the selective hydrogen removal along the membrane length was found to become significant with increasing membrane permeability thereby constraining the reactor design. To decrease the negative effects of mass transfer limitations to the membrane wall, a small membrane tube diameter needs to be selected. For a relatively small ratio of the membrane tube diameter to the particle diameter, the porosity profile needs to be taken into account to prevent overestimation of the H2 removal rate. It is concluded that autothermal production of H2 in a PBMR is feasible, provided that the membranes are positioned outside the inlet region with large temperature gradients.",
author = "T.P. Tiemersma and C.S. Patil and {Sint Annaland, van}, M. and J.A.M. Kuipers",
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Modelling of packed bed membrane reactors for autothermal production of ultrapure hydrogen. / Tiemersma, T.P.; Patil, C.S.; Sint Annaland, van, M.; Kuipers, J.A.M.

In: Chemical Engineering Science, Vol. 61, No. 5, 2006, p. 1602-1616.

Research output: Contribution to journalArticleAcademicpeer-review

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AB - The conceptual feasibility of a packed bed membrane reactor for the autothermal reforming (ATR) of methane for the production of ultrapure hydrogen was investigated. By integrating H2 permselective Pd-based membranes under autothermal conditions, a high degree of process integration and intensification can be accomplished which is particularly interesting for small scale H2 production units. A two-dimensional pseudo-homogeneous packed bed membrane reactor model was developed that solves the continuity and momentum equations and the component mass and energy balances. In adiabatic operation, autothermal operation can be achieved; however, large axial temperature excursions were seen at the reactor inlet, which are disadvantageous for membrane life and catalyst performance. Different operation modes, such as cooling the reactor wall with sweep gas or distributive feeding of O2 along the reactor length to moderate the temperature profile, are evaluated. The concentration polarisation because of the selective hydrogen removal along the membrane length was found to become significant with increasing membrane permeability thereby constraining the reactor design. To decrease the negative effects of mass transfer limitations to the membrane wall, a small membrane tube diameter needs to be selected. For a relatively small ratio of the membrane tube diameter to the particle diameter, the porosity profile needs to be taken into account to prevent overestimation of the H2 removal rate. It is concluded that autothermal production of H2 in a PBMR is feasible, provided that the membranes are positioned outside the inlet region with large temperature gradients.

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