Modification of silicalite-1 with ammonium compounds aimed at preparation of acidic catalyst for acetalization of glycerol with acetone

E. Janiszewska , J. Kowalska-Kuś , K. Górka-Marek , Agnieszka M. Szymocha , K. Nowińska , S. Kowalak

Abstract

Post-synthesis modification of silicalite-1 (MFI) with solutions of ammonium compounds (NH4F, NH4Cl, NH4NO3, NH4OH) without any additional alkaline agent followed by further thermal treatment appeared a new, facile, and cheap method to generate the acidic sites in starting material. The number and strength of resulting acid sites depend on the nature of anion in the applied ammonium salt. Used procedure resulted in partial removal of external silanol groups and in the formation of acidic internal isolated as well as hydrogen bonded OH groups (e.g. silanol nests). The novel acidic sites show a high catalytic activity for acetalization of glycerol with acetone and high selectivity towards 2,2-dimethyl-1,3-dioxolane-4-methanol (solketal). The modified silicalite-1 indicates also high stability with time on stream. The proposed reaction mechanism considers a combined contribution of both Lewis and very weak Brønsted acid sites.
Author E. Janiszewska
E. Janiszewska,,
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, J. Kowalska-Kuś
J. Kowalska-Kuś,,
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, K. Górka-Marek
K. Górka-Marek,,
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, Agnieszka M. Szymocha (FoAaE / IoSSaA)
Agnieszka M. Szymocha,,
- Institute of Soil Science and Agrophysics
, K. Nowińska
K. Nowińska,,
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, S. Kowalak
S. Kowalak,,
-
Journal seriesApplied Catalysis A-General, [Applied Catalysis A: General], ISSN 0926-860X, e-ISSN 1873-3875, (N/A 100 pkt)
Issue year2019
No581
Pages1-10
Publication size in sheets0.5
Keywords in EnglishModified silicalite-1, Defective sites, Surface acidity, Glycerol acetalization
ASJC Classification1503 Catalysis; 1508 Process Chemistry and Technology
DOIDOI:10.1016/j.apcata.2019.05.012
URL https://www.sciencedirect.com/science/article/pii/S0926860X19302169
Languageen angielski
Score (nominal)100
Score sourcejournalList
Publication indicators WoS Citations = 2; Scopus SNIP (Source Normalised Impact per Paper): 2018 = 1.306; WoS Impact Factor: 2018 = 4.63 (2) - 2018=4.586 (5)
Citation count*
Additional fields
FinansowanieK. Góra-Marek acknowledges the Grant No. 2015/18/E/ST4/00191 from the National Science Centre, Poland.
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