Understanding the mechanism of catalytic fast pyrolysis by unveiling reactive intermediates in heterogeneous catalysis

Patrick Hemberger; Victoria B. F. Custodis; Andras Bodi; Thomas Gerber; Jeroen A. van Bokhoven

doi:10.1038/ncomms15946

journal article Open Access Jun 29, 2017

Understanding the mechanism of catalytic fast pyrolysis by unveiling reactive intermediates in heterogeneous catalysis

Patrick Hemberger Victoria B. F. Custodis Andras Bodi Thomas Gerber

Jeroen A. van Bokhoven

Nature Communications Vol. 8 No. 1 · Springer Science and Business Media LLC

View at Publisher Save 10.1038/ncomms15946

Abstract

AbstractCatalytic fast pyrolysis is a promising way to convert lignin into fine chemicals and fuels, but current approaches lack selectivity and yield unsatisfactory conversion. Understanding the pyrolysis reaction mechanism at the molecular level may help to make this sustainable process more economic. Reactive intermediates are responsible for product branching and hold the key to unveiling these mechanisms, but are notoriously difficult to detect isomer-selectively. Here, we investigate the catalytic pyrolysis of guaiacol, a lignin model compound, using photoelectron photoion coincidence spectroscopy with synchrotron radiation, which allows for isomer-selective detection of reactive intermediates. In combination with ambient pressure pyrolysis, we identify fulvenone as the central reactive intermediate, generated by catalytic demethylation to catechol and subsequent dehydration. The fulvenone ketene is responsible for the phenol formation. This technique may open unique opportunities for isomer-resolved probing in catalysis, and holds the potential for achieving a mechanistic understanding of complex, real-life catalytic processes.

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Published: Jun 29, 2017
Vol/Issue: 8(1)
License: View

Authors

P

Patrick Hemberger

V

Victoria B. F. Custodis

Jeroen A. van Bokhoven

Department of Energy and Environment Paul Scherrer Institut Forschungsstrasse 111 5232 Villigen PSI Switzerland; Department of Chemistry and Applied Biosciences ETH Zurich Vladimir-Prelog-Weg 1–5/10 8093 Zürich Switzerland

Cite This Article

Patrick Hemberger, Victoria B. F. Custodis, Andras Bodi, et al. (2017). Understanding the mechanism of catalytic fast pyrolysis by unveiling reactive intermediates in heterogeneous catalysis. Nature Communications, 8(1). https://doi.org/10.1038/ncomms15946

Understanding the mechanism of catalytic fast pyrolysis by unveiling reactive intermediates in heterogeneous catalysis

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