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

Patrick Hemberger (), Victoria B. F. Custodis, Andras Bodi, Thomas Gerber and Jeroen A. van Bokhoven ()
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Patrick Hemberger: Laboratory for Femtochemistry and Synchrotron Radiation, Paul Scherrer Institute
Victoria B. F. Custodis: Institute for Chemical and Bioengineering
Andras Bodi: Laboratory for Femtochemistry and Synchrotron Radiation, Paul Scherrer Institute
Thomas Gerber: Molecular Dynamics Group, Paul Scherrer Institute
Jeroen A. van Bokhoven: Institute for Chemical and Bioengineering

Nature Communications, 2017, vol. 8, issue 1, 1-9

Abstract: Abstract Catalytic 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.

Date: 2017
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DOI: 10.1038/ncomms15946

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