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...

Descripción completa

Guardado en:
Detalles Bibliográficos
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:
R
Q
Acceso en línea:https://doaj.org/article/4056ade1d1d34f95ab7f023f0390b669
Etiquetas: Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
id oai:doaj.org-article:4056ade1d1d34f95ab7f023f0390b669
record_format dspace
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
_version_ 1718379878227640320