NO activation of Cu-MOR enhanced methanol production at elevated temperatures, to a greater extent than activation by O under optimal conditions. The increase in methanol production by NO activation was attributed to the facile formation of an active copper center with no formation of inactive intermediate species.
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http://dx.doi.org/10.1039/c7cc00467b | DOI Listing |
J Am Chem Soc
August 2024
Department of Chemistry, Stanford University, Stanford, California 94305, United States.
Methane is one of the most potent greenhouse gases; developing technology for its abatement is essential for combating climate change. Copper zeolites can activate methane at low temperatures and pressures, demonstrating promise for this technology. However, a barrier to industrial implementation is the inability to recycle the Cu(II) active site.
View Article and Find Full Text PDFPhys Chem Chem Phys
February 2024
School of Physical Science and Technology, ShanghaiTech University, 393 Huaxia Middle Road, Shanghai 201210, China.
A comprehensive study combining the density functional theory (DFT) and thermodynamic analysis was conducted to unravel the active sites and adsorption mechanisms of ethanol, acetaldehyde, and ethylene on various copper-modified mordenite (Cu-MOR) configurations, including Cu/MOR, CuO/MOR, and Cu/MOR. This research involved an exhaustive exploration of structural and formation energies, revealing that the formation energies of these structures are temperature-dependent. Despite all three structures thermodynamically accommodating ethanol adsorption, their respective adsorption mechanisms differ significantly.
View Article and Find Full Text PDFChem Sci
September 2023
Department of Chemistry, NIS Center and INSTM Reference Center, University of Turin, 10125 Turin Via P. Giuria 7 Italy
The direct activation of methane to methanol (MTM) proceeds through a chemical-looping process over Cu-oxo sites in zeolites. Herein, we extend the overall understanding of oxidation reactions over metal-oxo sites and C-H activation reactions by pinpointing the evolution of Cu species during reduction. To do so, a set of temperature-programmed reduction experiments were performed with CH, CH and CO.
View Article and Find Full Text PDFACS Omega
August 2023
National & Local Joint Engineering Research Center of Precision Coal Mining, Anhui University of Science and Technology, Huainan 232001, China.
The direct oxidation of low-concentration methane to value-added chemicals can not only reduce carbon emission but also provide an alternative production route for fossil fuels. Herein, we proposed a novel catalyst for the direct oxidation of low-concentration methane to methanol via the impregnation method, which selected copper and zinc as co-modifiers to modify the MOR catalyst. The highest methanol yield of 71.
View Article and Find Full Text PDFACS Catal
February 2023
Department of Microbial and Molecular Systems, Center for Sustainable Catalysis and Engineering, KU Leuven-University of Leuven, B-3001 Leuven, Belgium.
The industrial implementation of a direct methane to methanol process would lead to environmental and economic benefits. Copper zeolites successfully execute this reaction at relatively low temperatures, and mordenite zeolites in particular enable high methanol production. When loaded to a Cu/Al ratio of 0.
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