Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol

Abstract Synthetic homogeneous system known to date performing methane to methanol conversion using O2 as terminal oxidant is unique and based on copper complex with piperazine-based ligand (Cu3L in Fig. 1) in a medium of acetonitrile. Prior work have shown that in order to achieve catalytic turnove...

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Autores principales:	Ehsan Moharreri, Tahereh Jafari, Dinithi Rathnayake, Harshul Khanna, Chung-Hao Kuo, Steven L. Suib, Partha Nandi
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/4056ade1d1d34f95ab7f023f0390b669
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spelling	oai:doaj.org-article:4056ade1d1d34f95ab7f023f0390b6692021-12-02T17:37:12ZRole of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol10.1038/s41598-021-98721-22045-2322https://doaj.org/article/4056ade1d1d34f95ab7f023f0390b6692021-09-01T00:00:00Zhttps://doi.org/10.1038/s41598-021-98721-2https://doaj.org/toc/2045-2322Abstract Synthetic homogeneous system known to date performing methane to methanol conversion using O2 as terminal oxidant is unique and based on copper complex with piperazine-based ligand (Cu3L in Fig. 1) in a medium of acetonitrile. Prior work have shown that in order to achieve catalytic turnover, hydrogen peroxide is needed to regenerate the active site. We show in this paper that reaction solvent based on organic nitrile decompose concurrently with methane activation and that in the absence of either acetonitrile, Cu complex or hydrogen peroxide, the catalytic turnover does not happen. We show in this manuscript that the direct methane oxidation to methanol might have been mediated by catalytic Radziszewski oxidation between acetonitrile and H2O2. Additionally we have discovered that in the absence of methane, peroxide mediated acetonitrile decomposition also makes methanol via a background reaction which was hitherto unknown.Ehsan MoharreriTahereh JafariDinithi RathnayakeHarshul KhannaChung-Hao KuoSteven L. SuibPartha NandiNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-7 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Ehsan Moharreri Tahereh Jafari Dinithi Rathnayake Harshul Khanna Chung-Hao Kuo Steven L. Suib Partha Nandi Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
description	Abstract Synthetic homogeneous system known to date performing methane to methanol conversion using O2 as terminal oxidant is unique and based on copper complex with piperazine-based ligand (Cu3L in Fig. 1) in a medium of acetonitrile. Prior work have shown that in order to achieve catalytic turnover, hydrogen peroxide is needed to regenerate the active site. We show in this paper that reaction solvent based on organic nitrile decompose concurrently with methane activation and that in the absence of either acetonitrile, Cu complex or hydrogen peroxide, the catalytic turnover does not happen. We show in this manuscript that the direct methane oxidation to methanol might have been mediated by catalytic Radziszewski oxidation between acetonitrile and H2O2. Additionally we have discovered that in the absence of methane, peroxide mediated acetonitrile decomposition also makes methanol via a background reaction which was hitherto unknown.
format	article
author	Ehsan Moharreri Tahereh Jafari Dinithi Rathnayake Harshul Khanna Chung-Hao Kuo Steven L. Suib Partha Nandi
author_facet	Ehsan Moharreri Tahereh Jafari Dinithi Rathnayake Harshul Khanna Chung-Hao Kuo Steven L. Suib Partha Nandi
author_sort	Ehsan Moharreri
title	Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
title_short	Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
title_full	Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
title_fullStr	Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
title_full_unstemmed	Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
title_sort	role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/4056ade1d1d34f95ab7f023f0390b669
work_keys_str_mv	AT ehsanmoharreri roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol AT taherehjafari roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol AT dinithirathnayake roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol AT harshulkhanna roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol AT chunghaokuo roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol AT stevenlsuib roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol AT parthanandi roleofcatalyticnitriledecompositionintricoppercomplexmediateddirectpartialoxidationofmethanetomethanol
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Role of catalytic nitrile decomposition in tricopper complex mediated direct partial oxidation of methane to methanol

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