Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions
Nishtha Agarwal,Simon J. Freakley,Rebecca McVicker,Sultan Althahban,Nikolaos Dimitratos,Qian He,David J. Morgan,Robert Leyshon Jenkins,David J. Willock,Stuart Hamilton Taylor,Christopher J. Kiely,Christopher J. Kiely,Graham J. Hutchings +12 more
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It is demonstrated that the resulting methanol incorporated a substantial fraction of gas-phase O2, suggesting that the controlled breakdown of H2O2 activates methane, which subsequently incorporates molecular oxygen through a radical process.Abstract:
The selective oxidation of methane, the primary component of natural gas, remains an important challenge in catalysis. We used colloidal gold-palladium nanoparticles, rather than the same nanoparticles supported on titanium oxide, to oxidize methane to methanol with high selectivity (92%) in aqueous solution at mild temperatures. Then, using isotopically labeled oxygen (O2) as an oxidant in the presence of hydrogen peroxide (H2O2), we demonstrated that the resulting methanol incorporated a substantial fraction (70%) of gas-phase O2. More oxygenated products were formed than the amount of H2O2 consumed, suggesting that the controlled breakdown of H2O2 activates methane, which subsequently incorporates molecular oxygen through a radical process. If a source of methyl radicals can be established, then the selective oxidation of methane to methanol using molecular oxygen is possible.read more
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Toward the Decentralized Electrochemical Production of H2O2: A Focus on the Catalysis
Sungeun Yang,Arnau Verdaguer-Casadevall,Logi Arnarson,Luca Silvioli,Viktor Colic,Rasmus Frydendal,Jan Rossmeisl,Ib Chorkendorff,Ifan E. L. Stephens,Ifan E. L. Stephens +9 more
TL;DR: In this article, the influence of the geometry of the active site and its influence on active site activity and selectivity is discussed. And the role of cell geometry and mass transport in liquid half-cells in H2O2 production is analyzed.
Journal ArticleDOI
Hydrophobic zeolite modification for in situ peroxide formation in methane oxidation to methanol
Zhu Jin,Liang Wang,Erik Zuidema,Kartick Mondal,Ming Zhang,Jian Zhang,Chengtao Wang,Xiangju Meng,Hengquan Yang,Carl Mesters,Feng-Shou Xiao +10 more
TL;DR: A heterogeneous catalyst system for enhanced meethanol productivity in methane oxidation by in situ generated hydrogen peroxide at mild temperature (70°C) and methanol selectivity reached 92%, corresponding to methanl productivity up to 91.6 millimoles per gram of AuPd per hour.
Journal ArticleDOI
Highly selective oxidation of methane to methanol at ambient conditions by titanium dioxide-supported iron species
Jijia Xie,Renxi Jin,Ang Li,Yingpu Bi,Qiushi Ruan,Yucheng Deng,Yajun Zhang,Siyu Yao,Gopinathan Sankar,Ding Ma,Junwang Tang +10 more
TL;DR: In this paper, a photocatalytic approach based on TiO2-supported iron oxide species is described, which affords methanol in high yield and selectivity at ambient conditions.
Journal ArticleDOI
In Situ/Operando Electrocatalyst Characterization by X-ray Absorption Spectroscopy
TL;DR: The fundamental principles of the XAS method are discussed and the progress in the instrumentation and data analysis approaches undertaken for deciphering X-ray absorption near edge structure (XANES) and extended X- Ray absorption fine structure (EXAFS) spectra are described.
Journal ArticleDOI
Direct Methane Conversion under Mild Condition by Thermo-, Electro-, or Photocatalysis
Xianguang Meng,Xiaoju Cui,Xiaoju Cui,Xiaoju Cui,N. Pethan Rajan,Liang Yu,Liang Yu,Dehui Deng,Dehui Deng,Dehui Deng,Xinhe Bao,Xinhe Bao +11 more
TL;DR: In this paper, the typical catalytic processes employed in these reaction systems and in particular highlight the potential heterogeneous catalysts with noteworthy C-H activation performance are summarized along with their perspectives on catalyst design, theoretical simulations, the choice of reaction condition, and the method of reaction product analysis.
References
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Platinum Catalysts for the High-Yield Oxidation of Methane to a Methanol Derivative
TL;DR: Mechanistic studies show that platinum(II) is the most active oxidation state of platinum for reaction with methane, and are consistent with reaction proceeding through carbon-hydrogen bond activation of methane to generate a platinum-methyl intermediate that is oxidized to generate the methyl ester product.
Journal ArticleDOI
Solvent-Free Oxidation of Primary Carbon-Hydrogen Bonds in Toluene Using Au-Pd Alloy Nanoparticles
Lokesh Kesavan,Ramchandra Tiruvalam,Mohd Hasbi Ab. Rahim,Mohd Izham Saiman,Dan I. Enache,Robert Leyshon Jenkins,Nikolaos Dimitratos,Jose Antonio Lopez-Sanchez,Stuart Hamilton Taylor,David W. Knight,Christopher J. Kiely,Graham J. Hutchings +11 more
TL;DR: It is reported here that supported gold-palladium nanoparticles on carbon or TiO2 are active for the oxidation of the primary carbon-hydrogen bonds in toluene and related molecules, giving high selectivities to benzyl benzoate under mild solvent-free conditions.
Journal ArticleDOI
The soluble methane mono-oxygenase of Methylococcus capsulatus (Bath). Its ability to oxygenate n-alkanes, n-alkenes, ethers, and alicyclic, aromatic and heterocyclic compounds.
TL;DR: Methane mono-oxygenase of Methylococcus capsulatus (Bath) catalyses the oxidation of various substituted methane derivatives including methanol and, in some of its catalytic properties, apparently resembles the analogous enzyme from Methylomonas methanica but differs from those found in Methylosinus trichosporium and M methylomonas albus.
Journal ArticleDOI
Selective Oxidation of Methane by the Bis(μ-oxo)dicopper Core Stabilized on ZSM-5 and Mordenite Zeolites
TL;DR: Three lines of evidence firmly support the key role of the bis(mu-oxo)dicopper core in this selective, low-temperature hydroxylation of methane.
Journal ArticleDOI
A Mercury-Catalyzed, High-Yield System for the Oxidation of Methane to Methanol
Roy A. Periana,Douglas J. Taube,Eric R. Evitt,Daniel G. Löffler,Paul R. Wentrcek,George Voss,Toshihiko Masuda +6 more
TL;DR: A homogeneous system for the selective, catalytic oxidation of methane to methanol via methyl bisulfate is reported and the essential elements of the mechanism were identified.
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