Ambient Pressure Hydrodesulfurization of Refractory Sulfur Compounds in Highly Sensitive μ-Reactor Platform Coupled to a Time-of-Flight Mass Spectrometer

Ann-Louise N. Christoffersen, Anders Bodin, Christian F. Elkjær, Jakob Ejler Sørensen, Jakob Kibsgaard, Ib Chorkendorff*

*Corresponding author for this work

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Abstract

Tightened restrictions call for cleaner transportation fuels to minimize environmental and societal problems caused by the presence of sulfur in transportation fuels. This emphasizes the need for new and better catalysts in the field of hydrodesulfurization (HDS), which aims at removing the refractory sulfur from different petroleum streams mostly found in the form of the alkyl-substituted dibenzothiophenes (β-DBTs). In this work we demonstrate how a setup dedicated to testing minute amounts (nanogram) of well-defined catalytic systems in μ-reactors can be used in the gas-phase HDS of the model compounds DBT and 4,6-dimethyldibenzothiophene (4,6-DMDBT) and the reaction pathways revealed by time-of-flight mass spectrometry. Specifically, we investigate HDS of DBT and 4,6-DMDBT on mass-selected Pt nanoparticles and show that only the direct desulfurization products are formed.The setup is a means to bridge the gap between structural characterization of model catalysts and their related activity in the HDS of DBT and 4,6-DMDBT.
Original languageEnglish
JournalJournal of Physical Chemistry C
Volume122
Issue number3
Pages (from-to)1699-1705
ISSN1932-7447
DOIs
Publication statusPublished - 2018

Cite this

@article{f3f62563b76b4628a98da897175bfd01,
title = "Ambient Pressure Hydrodesulfurization of Refractory Sulfur Compounds in Highly Sensitive μ-Reactor Platform Coupled to a Time-of-Flight Mass Spectrometer",
abstract = "Tightened restrictions call for cleaner transportation fuels to minimize environmental and societal problems caused by the presence of sulfur in transportation fuels. This emphasizes the need for new and better catalysts in the field of hydrodesulfurization (HDS), which aims at removing the refractory sulfur from different petroleum streams mostly found in the form of the alkyl-substituted dibenzothiophenes (β-DBTs). In this work we demonstrate how a setup dedicated to testing minute amounts (nanogram) of well-defined catalytic systems in μ-reactors can be used in the gas-phase HDS of the model compounds DBT and 4,6-dimethyldibenzothiophene (4,6-DMDBT) and the reaction pathways revealed by time-of-flight mass spectrometry. Specifically, we investigate HDS of DBT and 4,6-DMDBT on mass-selected Pt nanoparticles and show that only the direct desulfurization products are formed.The setup is a means to bridge the gap between structural characterization of model catalysts and their related activity in the HDS of DBT and 4,6-DMDBT.",
author = "Christoffersen, {Ann-Louise N.} and Anders Bodin and Elkj{\ae}r, {Christian F.} and S{\o}rensen, {Jakob Ejler} and Jakob Kibsgaard and Ib Chorkendorff",
year = "2018",
doi = "10.1021/acs.jpcc.7b11089",
language = "English",
volume = "122",
pages = "1699--1705",
journal = "The Journal of Physical Chemistry Part C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "3",

}

Ambient Pressure Hydrodesulfurization of Refractory Sulfur Compounds in Highly Sensitive μ-Reactor Platform Coupled to a Time-of-Flight Mass Spectrometer. / Christoffersen, Ann-Louise N.; Bodin, Anders; Elkjær, Christian F.; Sørensen, Jakob Ejler; Kibsgaard, Jakob; Chorkendorff, Ib.

In: Journal of Physical Chemistry C, Vol. 122, No. 3, 2018, p. 1699-1705.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Ambient Pressure Hydrodesulfurization of Refractory Sulfur Compounds in Highly Sensitive μ-Reactor Platform Coupled to a Time-of-Flight Mass Spectrometer

AU - Christoffersen, Ann-Louise N.

AU - Bodin, Anders

AU - Elkjær, Christian F.

AU - Sørensen, Jakob Ejler

AU - Kibsgaard, Jakob

AU - Chorkendorff, Ib

PY - 2018

Y1 - 2018

N2 - Tightened restrictions call for cleaner transportation fuels to minimize environmental and societal problems caused by the presence of sulfur in transportation fuels. This emphasizes the need for new and better catalysts in the field of hydrodesulfurization (HDS), which aims at removing the refractory sulfur from different petroleum streams mostly found in the form of the alkyl-substituted dibenzothiophenes (β-DBTs). In this work we demonstrate how a setup dedicated to testing minute amounts (nanogram) of well-defined catalytic systems in μ-reactors can be used in the gas-phase HDS of the model compounds DBT and 4,6-dimethyldibenzothiophene (4,6-DMDBT) and the reaction pathways revealed by time-of-flight mass spectrometry. Specifically, we investigate HDS of DBT and 4,6-DMDBT on mass-selected Pt nanoparticles and show that only the direct desulfurization products are formed.The setup is a means to bridge the gap between structural characterization of model catalysts and their related activity in the HDS of DBT and 4,6-DMDBT.

AB - Tightened restrictions call for cleaner transportation fuels to minimize environmental and societal problems caused by the presence of sulfur in transportation fuels. This emphasizes the need for new and better catalysts in the field of hydrodesulfurization (HDS), which aims at removing the refractory sulfur from different petroleum streams mostly found in the form of the alkyl-substituted dibenzothiophenes (β-DBTs). In this work we demonstrate how a setup dedicated to testing minute amounts (nanogram) of well-defined catalytic systems in μ-reactors can be used in the gas-phase HDS of the model compounds DBT and 4,6-dimethyldibenzothiophene (4,6-DMDBT) and the reaction pathways revealed by time-of-flight mass spectrometry. Specifically, we investigate HDS of DBT and 4,6-DMDBT on mass-selected Pt nanoparticles and show that only the direct desulfurization products are formed.The setup is a means to bridge the gap between structural characterization of model catalysts and their related activity in the HDS of DBT and 4,6-DMDBT.

U2 - 10.1021/acs.jpcc.7b11089

DO - 10.1021/acs.jpcc.7b11089

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VL - 122

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EP - 1705

JO - The Journal of Physical Chemistry Part C

JF - The Journal of Physical Chemistry Part C

SN - 1932-7447

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