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Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study

Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron... HCHO has been confirmed as an active intermediate in the methanol‐to‐hydrocarbon (MTH) reaction, and is critical for interpreting the mechanisms of coke formation. Here, HCHO was detected and quantified during the MTH process over HSAPO‐34 and HZSM‐5 by in situ synchrotron radiation photoionization mass spectrometry. Compared with conventional methods, excellent time‐resolved profiles were obtained to study the formation and fate of HCHO, and other products during the induction, steady‐state reaction, and deactivation periods. Similar formation trends of HCHO and methane, and their close correlation in yields suggest that they are derived from disproportionation of methanol at acidic sites. In the presence of Y2O3, the amount of HCHO changes, affecting the hydrogen‐transfer processes of olefins into aromatics and aromatics into cokes. The yield of HCHO affects the aromatic‐based cycle and the formation of ethylene, indicating that ethylene is mainly formed from the aromatic‐based cycle. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Angewandte Chemie International Edition Wiley

Formation and Fate of Formaldehyde in Methanol‐to‐Hydrocarbon Reaction: In Situ Synchrotron Radiation Photoionization Mass Spectrometry Study

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Publisher
Wiley
Copyright
© 2020 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim
ISSN
1433-7851
eISSN
1521-3773
DOI
10.1002/anie.201914953
Publisher site
See Article on Publisher Site

Abstract

HCHO has been confirmed as an active intermediate in the methanol‐to‐hydrocarbon (MTH) reaction, and is critical for interpreting the mechanisms of coke formation. Here, HCHO was detected and quantified during the MTH process over HSAPO‐34 and HZSM‐5 by in situ synchrotron radiation photoionization mass spectrometry. Compared with conventional methods, excellent time‐resolved profiles were obtained to study the formation and fate of HCHO, and other products during the induction, steady‐state reaction, and deactivation periods. Similar formation trends of HCHO and methane, and their close correlation in yields suggest that they are derived from disproportionation of methanol at acidic sites. In the presence of Y2O3, the amount of HCHO changes, affecting the hydrogen‐transfer processes of olefins into aromatics and aromatics into cokes. The yield of HCHO affects the aromatic‐based cycle and the formation of ethylene, indicating that ethylene is mainly formed from the aromatic‐based cycle.

Journal

Angewandte Chemie International EditionWiley

Published: Mar 16, 2020

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