Journal ArticleDOI
Room-Temperature Oxidation of Methane by α-Oxygen and Extraction of Products from the FeZSM-5 Surface
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TLDR
In this article, a new generation FeZSM-5 samples were used to investigate the room-temperature oxidation of methane to methanol by α-oxygen and showed that 6−7% of the reaction products contained DME.Abstract:
Room-temperature oxidation of methane to methanol by α-oxygen is of great mechanistic interest for both conventional and biomimetic oxidation catalysis. This work was carried out using new-generation FeZSM-5 samples that have the Oα concentration of 100 μmol/g. This value exceeds 3−15 times the Oα concentration on the earlier studied samples, thus providing more precise quantitative measurements related to the reaction mechanism. Fourier transform infrared spectroscopy data confirmed an earlier conclusion that CH4 + Oα surface reaction proceeds by the hydrogen abstraction mechanism. This mechanism leads to hydroxy and methoxy groups residing on α-sites. The methanol formation takes place by hydrolysis of (Fe-OCH3)α groups at the step of extraction. For the first time dimethyl ether (DME) was identified in the reaction products, its amount comprising 6−7% of the methane reacted. In distinction to methanol, DME is readily extracted both by dry solvents (acetonitrile, tetrahydrofuran, ethanol) and their mixt...read more
Citations
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Journal ArticleDOI
Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol.
Sebastian Grundner,Monica A. C. Markovits,Guanna Li,Moniek Tromp,Evgeny A. Pidko,Emiel J. M. Hensen,Andreas Jentys,Maricruz Sanchez-Sanchez,Johannes A. Lercher +8 more
TL;DR: The mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol.
Journal ArticleDOI
Reactivity of Surface Species in Heterogeneous Catalysts Probed by In Situ X-ray Absorption Techniques
TL;DR: (Article begins on next page)
Journal ArticleDOI
Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts
TL;DR: Mononuclear rhodium species, anchored on a zeolite or titanium dioxide support suspended in aqueous solution, catalyse the direct conversion of methane to methanol and acetic acid, using oxygen and carbon monoxide under mild conditions, and it is found that the two products form through independent pathways, which allows to tune the conversion.
Journal ArticleDOI
The Direct Catalytic Oxidation of Methane to Methanol-A Critical Assessment.
TL;DR: Mhanol protection is identified as being indispensable for future research on homogeneous and heterogeneous catalysis by establishing the severe limitations related to the direct catalytic synthesis of methanol from methane.
Journal ArticleDOI
Oxidation of ethane to ethanol by N2O in a metal–organic framework with coordinatively unsaturated iron(II) sites
Dianne J. Xiao,Eric D. Bloch,Jarad A. Mason,Wendy L. Queen,Matthew R. Hudson,Nora Planas,Joshua Borycz,Allison L. Dzubak,Pragya Verma,Kyuho Lee,Francesca Bonino,Valentina Crocellà,Junko Yano,Silvia Bordiga,Donald G. Truhlar,Laura Gagliardi,Craig M. Brown,Jeffrey R. Long +17 more
TL;DR: It is shown that the metal-organic framework Fe2(dobdc) and its magnesium-diluted analogue, Fe0.1Mg1.9( dobdc), are able to activate the C-H bonds of ethane and convert it into ethanol and acetaldehyde using nitrous oxide as the terminal oxidant.
References
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Journal ArticleDOI
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Journal ArticleDOI
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Journal ArticleDOI
Selective Oxidation of Methane by the Bis(μ-oxo)dicopper Core Stabilized on ZSM-5 and Mordenite Zeolites
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