New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy

Christian Gründling; Victor A. Veefkind; Gabriele Eder-Mirth; Johannes A. Lercher

doi:10.1016/S0167-2991(97)80605-2

New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy

Christian Gründling
, Victor A. Veefkind
, Gabriele Eder-Mirth
, Johannes A. Lercher

Catalytic Processes and Materials

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › Academic › peer-review

9 Citations (Scopus)

Abstract

Amination of alcohols over Brønsted acidic molecular sieves such as H-mordenites proceeds via a bimolecular precursor consisting of an ammonium ion and an alcohol molecule. The rate of transformation of that complex into a sorbed alkyl ammonium ion is fast. Desorption of the formed amines, however, is difficult under reaction conditions (633K) and only proceeds in the presence of excess ammonia. Two mechanisms are proposed for the release of the alkylamines in the gasphase, i.e., adsorption assisted desorption and alkyl scavenging by ammonia. The vast majority of the alkylamines are formed by scavenging alkyl groups of chemisorbed alkyl ammonium ions by ammonia. A linear relation of the initial rate of monomethylamine formation and the total surface concentration of methyl groups (present as mono-up to tetramethylammonium ions) inside the pores of the mordenites was found.

Original language	English
Title of host publication	Progress in Zeolite and Microporous Materials
Subtitle of host publication	Proceedings of the 11th International Zeolite Conference 12-17 August 1996, Seoul, Korea
Publisher	Elsevier
Pages	591-598
Number of pages	8
DOIs	https://doi.org/10.1016/S0167-2991(97)80605-2
Publication status	Published - 1997
Event	11th International Zeolite Conference 1996 - Seoul, Korea, Republic of Duration: 12 Aug 1997 → 17 Aug 1997 Conference number: 11

Publication series

Name	Studies in surface science and catalysis
Publisher	Elsevier
Volume	105
ISSN (Print)	0167-2991

Conference

Conference	11th International Zeolite Conference 1996
Country/Territory	Korea, Republic of
City	Seoul
Period	12/08/97 → 17/08/97

Keywords

n/a OA procedure

Access to Document

10.1016/S0167-2991(97)80605-2

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Gründling, C., Veefkind, V. A., Eder-Mirth, G., & Lercher, J. A. (1997). New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy. In Progress in Zeolite and Microporous Materials: Proceedings of the 11th International Zeolite Conference 12-17 August 1996, Seoul, Korea (pp. 591-598). (Studies in surface science and catalysis; Vol. 105). Elsevier. https://doi.org/10.1016/S0167-2991(97)80605-2

Gründling, Christian ; Veefkind, Victor A. ; Eder-Mirth, Gabriele et al. / New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy. Progress in Zeolite and Microporous Materials: Proceedings of the 11th International Zeolite Conference 12-17 August 1996, Seoul, Korea. Elsevier, 1997. pp. 591-598 (Studies in surface science and catalysis).

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title = "New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy",

abstract = "Amination of alcohols over Br{\o}nsted acidic molecular sieves such as H-mordenites proceeds via a bimolecular precursor consisting of an ammonium ion and an alcohol molecule. The rate of transformation of that complex into a sorbed alkyl ammonium ion is fast. Desorption of the formed amines, however, is difficult under reaction conditions (633K) and only proceeds in the presence of excess ammonia. Two mechanisms are proposed for the release of the alkylamines in the gasphase, i.e., adsorption assisted desorption and alkyl scavenging by ammonia. The vast majority of the alkylamines are formed by scavenging alkyl groups of chemisorbed alkyl ammonium ions by ammonia. A linear relation of the initial rate of monomethylamine formation and the total surface concentration of methyl groups (present as mono-up to tetramethylammonium ions) inside the pores of the mordenites was found.",

keywords = "n/a OA procedure",

author = "Christian Gr{\"u}ndling and Veefkind, \{Victor A.\} and Gabriele Eder-Mirth and Lercher, \{Johannes A.\}",

year = "1997",

doi = "10.1016/S0167-2991(97)80605-2",

language = "English",

series = "Studies in surface science and catalysis",

publisher = "Elsevier",

pages = "591--598",

booktitle = "Progress in Zeolite and Microporous Materials",

address = "Spain",

note = "11th International Zeolite Conference 1996 ; Conference date: 12-08-1997 Through 17-08-1997",

}

Gründling, C, Veefkind, VA, Eder-Mirth, G & Lercher, JA 1997, New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy. in Progress in Zeolite and Microporous Materials: Proceedings of the 11th International Zeolite Conference 12-17 August 1996, Seoul, Korea. Studies in surface science and catalysis, vol. 105, Elsevier, pp. 591-598, 11th International Zeolite Conference 1996, Seoul, Korea, Republic of, 12/08/97. https://doi.org/10.1016/S0167-2991(97)80605-2

New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy. / Gründling, Christian; Veefkind, Victor A.; Eder-Mirth, Gabriele et al.
Progress in Zeolite and Microporous Materials: Proceedings of the 11th International Zeolite Conference 12-17 August 1996, Seoul, Korea. Elsevier, 1997. p. 591-598 (Studies in surface science and catalysis; Vol. 105).

Research output: Chapter in Book/Report/Conference proceeding › Conference contribution › Academic › peer-review

TY - GEN

T1 - New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy

AU - Gründling, Christian

AU - Veefkind, Victor A.

AU - Eder-Mirth, Gabriele

AU - Lercher, Johannes A.

N1 - Conference code: 11

PY - 1997

Y1 - 1997

N2 - Amination of alcohols over Brønsted acidic molecular sieves such as H-mordenites proceeds via a bimolecular precursor consisting of an ammonium ion and an alcohol molecule. The rate of transformation of that complex into a sorbed alkyl ammonium ion is fast. Desorption of the formed amines, however, is difficult under reaction conditions (633K) and only proceeds in the presence of excess ammonia. Two mechanisms are proposed for the release of the alkylamines in the gasphase, i.e., adsorption assisted desorption and alkyl scavenging by ammonia. The vast majority of the alkylamines are formed by scavenging alkyl groups of chemisorbed alkyl ammonium ions by ammonia. A linear relation of the initial rate of monomethylamine formation and the total surface concentration of methyl groups (present as mono-up to tetramethylammonium ions) inside the pores of the mordenites was found.

AB - Amination of alcohols over Brønsted acidic molecular sieves such as H-mordenites proceeds via a bimolecular precursor consisting of an ammonium ion and an alcohol molecule. The rate of transformation of that complex into a sorbed alkyl ammonium ion is fast. Desorption of the formed amines, however, is difficult under reaction conditions (633K) and only proceeds in the presence of excess ammonia. Two mechanisms are proposed for the release of the alkylamines in the gasphase, i.e., adsorption assisted desorption and alkyl scavenging by ammonia. The vast majority of the alkylamines are formed by scavenging alkyl groups of chemisorbed alkyl ammonium ions by ammonia. A linear relation of the initial rate of monomethylamine formation and the total surface concentration of methyl groups (present as mono-up to tetramethylammonium ions) inside the pores of the mordenites was found.

KW - n/a OA procedure

U2 - 10.1016/S0167-2991(97)80605-2

DO - 10.1016/S0167-2991(97)80605-2

M3 - Conference contribution

T3 - Studies in surface science and catalysis

SP - 591

EP - 598

BT - Progress in Zeolite and Microporous Materials

PB - Elsevier

T2 - 11th International Zeolite Conference 1996

Y2 - 12 August 1997 through 17 August 1997

ER -

Gründling C, Veefkind VA, Eder-Mirth G, Lercher JA. New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy. In Progress in Zeolite and Microporous Materials: Proceedings of the 11th International Zeolite Conference 12-17 August 1996, Seoul, Korea. Elsevier. 1997. p. 591-598. (Studies in surface science and catalysis). doi: 10.1016/S0167-2991(97)80605-2

New insight into the mechanism of zeolite catalyzed nucleophilic amination Via In Situ infrared spectroscopy

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