Details
| Original language | English |
|---|---|
| Pages (from-to) | 307-316 |
| Number of pages | 10 |
| Journal | Industrial and Engineering Chemistry Research |
| Volume | 61 |
| Issue number | 1 |
| Early online date | 22 Dec 2021 |
| Publication status | Published - 12 Jan 2022 |
Abstract
Mono-, di-, and trimethylamine are the products of the successive methylation of ammonia. Using narrow-pore acidic catalysts of the CHA family like H-SAPO-34 or H-SSZ-13, the formation of the thermodynamically but bulky trimethylamine can be suppressed due to steric effects; thus, methylation is stopped at dimethylamine. In this work, the continuous in situ removal of the byproduct water through the 4 Å wide pores in an LINDE Type A (LTA) (grown on an α-Al2O3 support) membrane reactor further increased the selectivity toward the economically desired product dimethylamine by 50%. This experimental finding can be explained by the release of adsorbed water blocking the catalytic site. Water removal through the hydrophilic LTA zeolite membrane allows methanol to adsorb at the acidic catalyst sites, which in turn accelerates the methylation rate of monomethylamine to the desired product dimethylamine. Further methylation to trimethylamine as the thermodynamically most favored product is not possible in narrow-pore catalysts because of space restrictions, but it takes place in the 12-membered-ring H-Mordenite (H-MOR) catalyst.
ASJC Scopus subject areas
- Chemistry(all)
- General Chemistry
- Chemical Engineering(all)
- General Chemical Engineering
- Engineering(all)
- Industrial and Manufacturing Engineering
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In: Industrial and Engineering Chemistry Research, Vol. 61, No. 1, 12.01.2022, p. 307-316.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Boosting Dimethylamine Formation Selectivity in a Membrane Reactor by In Situ Water Removal
AU - Rieck genannt Best, Felix
AU - Mundstock, Alexander
AU - Kißling, Patrick A.
AU - Richter, Hannes
AU - Hindricks, Karen D.J.
AU - Huang, Aisheng
AU - Behrens, Peter
AU - Caro, Jürgen
N1 - Funding Information: The H-SAPO-34 catalyst was kindly provided by Zhongmin Liu of the Dalian Institute for Chemical Physics of the Chinese Academy of Sciences. The LTA membranes on tubular alumina supports have been prepared at Fraunhofer IKTS Dresden/Hermsdorf. Further thanks to Frank Steinbach for preparing and taking the SEM cross-sectional images. The Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) is thanked for financing the project (CA147/21-1) by F.R.g.B. and J.C., P.A.K. thanks the DFG (Project BI1708/5-1). Funding Information: The Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) is thanked for financing the project (CA147/21-1) by F.R.g.B. and J.C., P.A.K. thanks the DFG (Project BI1708/5-1). Additionally, the project has in part been funded by the German Science Foundation (DFG, German Research Foundation) under Germany’s Excellence Strategy within the Cluster of Excellence PhoenixD (EXC 2122, Project ID 390833453).
PY - 2022/1/12
Y1 - 2022/1/12
N2 - Mono-, di-, and trimethylamine are the products of the successive methylation of ammonia. Using narrow-pore acidic catalysts of the CHA family like H-SAPO-34 or H-SSZ-13, the formation of the thermodynamically but bulky trimethylamine can be suppressed due to steric effects; thus, methylation is stopped at dimethylamine. In this work, the continuous in situ removal of the byproduct water through the 4 Å wide pores in an LINDE Type A (LTA) (grown on an α-Al2O3 support) membrane reactor further increased the selectivity toward the economically desired product dimethylamine by 50%. This experimental finding can be explained by the release of adsorbed water blocking the catalytic site. Water removal through the hydrophilic LTA zeolite membrane allows methanol to adsorb at the acidic catalyst sites, which in turn accelerates the methylation rate of monomethylamine to the desired product dimethylamine. Further methylation to trimethylamine as the thermodynamically most favored product is not possible in narrow-pore catalysts because of space restrictions, but it takes place in the 12-membered-ring H-Mordenite (H-MOR) catalyst.
AB - Mono-, di-, and trimethylamine are the products of the successive methylation of ammonia. Using narrow-pore acidic catalysts of the CHA family like H-SAPO-34 or H-SSZ-13, the formation of the thermodynamically but bulky trimethylamine can be suppressed due to steric effects; thus, methylation is stopped at dimethylamine. In this work, the continuous in situ removal of the byproduct water through the 4 Å wide pores in an LINDE Type A (LTA) (grown on an α-Al2O3 support) membrane reactor further increased the selectivity toward the economically desired product dimethylamine by 50%. This experimental finding can be explained by the release of adsorbed water blocking the catalytic site. Water removal through the hydrophilic LTA zeolite membrane allows methanol to adsorb at the acidic catalyst sites, which in turn accelerates the methylation rate of monomethylamine to the desired product dimethylamine. Further methylation to trimethylamine as the thermodynamically most favored product is not possible in narrow-pore catalysts because of space restrictions, but it takes place in the 12-membered-ring H-Mordenite (H-MOR) catalyst.
UR - http://www.scopus.com/inward/record.url?scp=85122349286&partnerID=8YFLogxK
U2 - 10.1021/acs.iecr.1c04149
DO - 10.1021/acs.iecr.1c04149
M3 - Article
AN - SCOPUS:85122349286
VL - 61
SP - 307
EP - 316
JO - Industrial and Engineering Chemistry Research
JF - Industrial and Engineering Chemistry Research
SN - 0888-5885
IS - 1
ER -