Details
| Originalsprache | Englisch |
|---|---|
| Aufsatznummer | 111920 |
| Fachzeitschrift | Microporous and Mesoporous Materials |
| Jahrgang | 337 |
| Frühes Online-Datum | 16 Apr. 2022 |
| Publikationsstatus | Veröffentlicht - Mai 2022 |
Abstract
Water permeation through a hydrophilic zeolite membrane can be used to promote reactions under equilibrium controlled conditions through the in situ removal of the by-product water. In the methylamine synthesis, mono- (MMA), di- (DMA) and trimethylamine (TMA) are formed by the successive methylation of ammonia with methanol (MeOH) over a mildly acidic catalyst. The methylamine yield can be increased through selective water extraction from the reactor through a membrane. Since both reactants and water have similar molecular kinetic diameters below 3.7 Å, because of the limited steam selectivity of the commonly used hydrophilic Na-LTA membrane (zeolite 4A), not only water has been removed. Therefore, in this work a K-LTA membrane, which was obtained by ion exchange with a reduced pore window diameter of 3 Å and thus with a higher water selectivity, was used in the membrane-supported methylamine synthesis. When replacing the Na-LTA with the K-LTA membrane, the H2O/MeOH mixed gas separation factor increases up to 1100 and the H2O/NH3 separation could also be improved. This in turn leads to an overall boost of the higher methylated amines DMA and TMA in methylamine synthesis. When using the narrow-pore aluminosilicate catalyst H-SSZ-13 with CHA structure, the application of the K-LTA membrane increases the share of the industrially desired product DMA from 51% without membrane to 74% with slightly increased conversion. When using the large-pore catalyst H-MOR, the thermodynamically most stable product TMA can be formed and the selectivity was increased from 35% without membrane to 41% with the K-LTA membrane.
ASJC Scopus Sachgebiete
- Chemie (insg.)
- Allgemeine Chemie
- Werkstoffwissenschaften (insg.)
- Allgemeine Materialwissenschaften
- Physik und Astronomie (insg.)
- Physik der kondensierten Materie
- Ingenieurwesen (insg.)
- Werkstoffmechanik
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in: Microporous and Mesoporous Materials, Jahrgang 337, 111920, 05.2022.
Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review
}
TY - JOUR
T1 - Controlled methylamine synthesis in a membrane reactor featuring a highly steam selective K+-LTA membrane
AU - Rieck genannt Best, Felix
AU - Mundstock, Alexander
AU - Richter, Hannes
AU - Kißling, Patrick A.
AU - Hindricks, Karen D.J.
AU - Huang, Aisheng
AU - Behrens, Peter
AU - Caro, Jürgen
N1 - Funding Information: The Deutsche Forschungsgemeinschaft ( DFG, German Research Foundation ) is thanked for financing the project ( CA147/21-1 ). Patrick A. Kiβling thanks the DFG (Project BI1708/5-1 ) [ 35 ]. Additionally, the project has in parts been funded by the DFG under Germany's Excellence Strategy within the Cluster of Excellence PhoenixD (EXC 2122, Project ID 390833453 ). Karen Hindricks is thankful for a grant from the Deutsche Studienstiftung.
PY - 2022/5
Y1 - 2022/5
N2 - Water permeation through a hydrophilic zeolite membrane can be used to promote reactions under equilibrium controlled conditions through the in situ removal of the by-product water. In the methylamine synthesis, mono- (MMA), di- (DMA) and trimethylamine (TMA) are formed by the successive methylation of ammonia with methanol (MeOH) over a mildly acidic catalyst. The methylamine yield can be increased through selective water extraction from the reactor through a membrane. Since both reactants and water have similar molecular kinetic diameters below 3.7 Å, because of the limited steam selectivity of the commonly used hydrophilic Na-LTA membrane (zeolite 4A), not only water has been removed. Therefore, in this work a K-LTA membrane, which was obtained by ion exchange with a reduced pore window diameter of 3 Å and thus with a higher water selectivity, was used in the membrane-supported methylamine synthesis. When replacing the Na-LTA with the K-LTA membrane, the H2O/MeOH mixed gas separation factor increases up to 1100 and the H2O/NH3 separation could also be improved. This in turn leads to an overall boost of the higher methylated amines DMA and TMA in methylamine synthesis. When using the narrow-pore aluminosilicate catalyst H-SSZ-13 with CHA structure, the application of the K-LTA membrane increases the share of the industrially desired product DMA from 51% without membrane to 74% with slightly increased conversion. When using the large-pore catalyst H-MOR, the thermodynamically most stable product TMA can be formed and the selectivity was increased from 35% without membrane to 41% with the K-LTA membrane.
AB - Water permeation through a hydrophilic zeolite membrane can be used to promote reactions under equilibrium controlled conditions through the in situ removal of the by-product water. In the methylamine synthesis, mono- (MMA), di- (DMA) and trimethylamine (TMA) are formed by the successive methylation of ammonia with methanol (MeOH) over a mildly acidic catalyst. The methylamine yield can be increased through selective water extraction from the reactor through a membrane. Since both reactants and water have similar molecular kinetic diameters below 3.7 Å, because of the limited steam selectivity of the commonly used hydrophilic Na-LTA membrane (zeolite 4A), not only water has been removed. Therefore, in this work a K-LTA membrane, which was obtained by ion exchange with a reduced pore window diameter of 3 Å and thus with a higher water selectivity, was used in the membrane-supported methylamine synthesis. When replacing the Na-LTA with the K-LTA membrane, the H2O/MeOH mixed gas separation factor increases up to 1100 and the H2O/NH3 separation could also be improved. This in turn leads to an overall boost of the higher methylated amines DMA and TMA in methylamine synthesis. When using the narrow-pore aluminosilicate catalyst H-SSZ-13 with CHA structure, the application of the K-LTA membrane increases the share of the industrially desired product DMA from 51% without membrane to 74% with slightly increased conversion. When using the large-pore catalyst H-MOR, the thermodynamically most stable product TMA can be formed and the selectivity was increased from 35% without membrane to 41% with the K-LTA membrane.
KW - Cation exchange
KW - Hydrophilic LTA membrane
KW - In situ water removal
KW - Membrane reactor
KW - Methylamines
KW - Zeolite membranes
UR - http://www.scopus.com/inward/record.url?scp=85129481489&partnerID=8YFLogxK
U2 - 10.1016/j.micromeso.2022.111920
DO - 10.1016/j.micromeso.2022.111920
M3 - Article
AN - SCOPUS:85129481489
VL - 337
JO - Microporous and Mesoporous Materials
JF - Microporous and Mesoporous Materials
SN - 1387-1811
M1 - 111920
ER -