Alternative Oxidants for the Catalytic Oxidative Coupling of Methane

Allison M. Arinaga; Morgan C. Ziegelski; Tobin J. Marks

doi:10.1002/anie.202012862

Alternative Oxidants for the Catalytic Oxidative Coupling of Methane

Allison M. Arinaga, Morgan C. Ziegelski, Tobin J. Marks^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Review article › peer-review

68 Scopus citations

Abstract

The catalytic oxidative coupling of methane (OCM) to C₂ hydrocarbons with oxygen (O₂-OCM) has garnered renewed worldwide interest in the past decade due to the emergence of enormous new shale gas resources. However, the C₂ selectivity of typical OCM processes is significantly challenged by overoxidation to CO_x products. Other gaseous reagents such as N₂O, CO₂, and S₂ have been investigated to a far lesser extent as alternative, milder oxidants to replace O₂. Although several authoritative review articles have summarized OCM research progress in depth, recent oxidative coupling developments using alternative oxidants (X-OCM) have not been overviewed in detail. In this perspective, we review and analyze OCM research results reporting the implementation of N₂O, CO₂, S₂, and other non-O₂ oxidants, highlighting the unique chemistries of these systems and their advantages/challenges compared to O₂-OCM. Current outlook and potential areas for future study are also discussed.

Original language	English (US)
Pages (from-to)	10502-10515
Number of pages	14
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	19
DOIs	https://doi.org/10.1002/anie.202012862
State	Published - May 3 2021

Funding

This work was supported by the NSF Engineering Research Center (ERC), Center for Innovative and Strategic Transformation of Light Alkane Resources (CISTAR; NSF award number 1647722). This work was supported by the NSF Engineering Research Center (ERC), Center for Innovative and Strategic Transformation of Light Alkane Resources (CISTAR; NSF award number EEC-1647722). . Morgan C. Ziegelski is an undergraduate student at the Georgia Institute of Technology. She is pursuing a BS in Chemical and Biomolecular Engineering and conducting research under Prof. Rachel Chem. Previously, she conducted research at Northwestern University under Prof. Tobin J. Marks within the NSF Center for Innovative and Strategic Transformation of Alkane Resources (CISTAR). Her research interests include sustainability, catalysis, and biotechnology

Keywords

alkanes
heterogeneous catalysis
methane activation
oxidative coupling of methane
soft oxidants

ASJC Scopus subject areas

General Chemistry
Catalysis

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10.1002/anie.202012862

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title = "Alternative Oxidants for the Catalytic Oxidative Coupling of Methane",

abstract = "The catalytic oxidative coupling of methane (OCM) to C2 hydrocarbons with oxygen (O2-OCM) has garnered renewed worldwide interest in the past decade due to the emergence of enormous new shale gas resources. However, the C2 selectivity of typical OCM processes is significantly challenged by overoxidation to COx products. Other gaseous reagents such as N2O, CO2, and S2 have been investigated to a far lesser extent as alternative, milder oxidants to replace O2. Although several authoritative review articles have summarized OCM research progress in depth, recent oxidative coupling developments using alternative oxidants (X-OCM) have not been overviewed in detail. In this perspective, we review and analyze OCM research results reporting the implementation of N2O, CO2, S2, and other non-O2 oxidants, highlighting the unique chemistries of these systems and their advantages/challenges compared to O2-OCM. Current outlook and potential areas for future study are also discussed.",

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AU - Arinaga, Allison M.

AU - Ziegelski, Morgan C.

AU - Marks, Tobin J.

PY - 2021/5/3

Y1 - 2021/5/3

N2 - The catalytic oxidative coupling of methane (OCM) to C2 hydrocarbons with oxygen (O2-OCM) has garnered renewed worldwide interest in the past decade due to the emergence of enormous new shale gas resources. However, the C2 selectivity of typical OCM processes is significantly challenged by overoxidation to COx products. Other gaseous reagents such as N2O, CO2, and S2 have been investigated to a far lesser extent as alternative, milder oxidants to replace O2. Although several authoritative review articles have summarized OCM research progress in depth, recent oxidative coupling developments using alternative oxidants (X-OCM) have not been overviewed in detail. In this perspective, we review and analyze OCM research results reporting the implementation of N2O, CO2, S2, and other non-O2 oxidants, highlighting the unique chemistries of these systems and their advantages/challenges compared to O2-OCM. Current outlook and potential areas for future study are also discussed.

AB - The catalytic oxidative coupling of methane (OCM) to C2 hydrocarbons with oxygen (O2-OCM) has garnered renewed worldwide interest in the past decade due to the emergence of enormous new shale gas resources. However, the C2 selectivity of typical OCM processes is significantly challenged by overoxidation to COx products. Other gaseous reagents such as N2O, CO2, and S2 have been investigated to a far lesser extent as alternative, milder oxidants to replace O2. Although several authoritative review articles have summarized OCM research progress in depth, recent oxidative coupling developments using alternative oxidants (X-OCM) have not been overviewed in detail. In this perspective, we review and analyze OCM research results reporting the implementation of N2O, CO2, S2, and other non-O2 oxidants, highlighting the unique chemistries of these systems and their advantages/challenges compared to O2-OCM. Current outlook and potential areas for future study are also discussed.

KW - alkanes

KW - heterogeneous catalysis

KW - methane activation

KW - oxidative coupling of methane

KW - soft oxidants

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Alternative Oxidants for the Catalytic Oxidative Coupling of Methane

Abstract

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