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Spectroscopic Definition of a Highly Reactive Site in Cu-CHA for Selective Methane Oxidation: Tuning a Mono-μ-Oxo Dicopper(II) Active Site for Reactivity

https://doi.org/10.1021/jacs.1c02835

Rhoda, Hannah M. ; Plessers, Dieter ; Heyer, Alexander J. ; Bols, Max L. ; Schoonheydt, Robert A. ; Sels, Bert F. ; Solomon, Edward I. ( May 2021 , Journal of the American Chemical Society)
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Spectroscopic Identification of the α-Fe/α-O Active Site in Fe-CHA Zeolite for the Low-Temperature Activation of the Methane C–H Bond

https://doi.org/10.1021/jacs.8b05877

Bols, Max L. ; Hallaert, Simon D. ; Snyder, Benjamin E. ; Devos, Julien ; Plessers, Dieter ; Rhoda, Hannah M. ; Dusselier, Michiel ; Schoonheydt, Robert A. ; Pierloot, Kristine ; Solomon, Edward I. ; et al ( September 2018 , Journal of the American Chemical Society)

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Cage effects control the mechanism of methane hydroxylation in zeolites

https://doi.org/10.1126/science.abd5803

Snyder, Benjamin E. R. ; Bols, Max L. ; Rhoda, Hannah M. ; Plessers, Dieter ; Schoonheydt, Robert A. ; Sels, Bert F. ; Solomon, Edward I. ( July 2021 , Science)

Catalytic conversion of methane to methanol remains an economically tantalizing but fundamentally challenging goal. Current technologies based on zeolites deactivate too rapidly for practical application. We found that similar active sites hosted in different zeolite lattices can exhibit markedly different reactivity with methane, depending on the size of the zeolite pore apertures. Whereas zeolite with large pore apertures deactivates completely after a single turnover, 40% of active sites in zeolite with small pore apertures are regenerated, enabling a catalytic cycle. Detailed spectroscopic characterization of reaction intermediates and density functional theory calculations show that hindered diffusion through small pore apertures disfavors premature release of CH₃radicals from the active site after C-H activation, thereby promoting radical recombination to form methanol rather than deactivated Fe-OCH₃centers elsewhere in the lattice.

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