Coordination and activation of nitrous oxide by iron zeolites

Bols, Max L.; Snyder, Benjamin E. R.; Rhoda, Hannah M.; Cnudde, Pieter; Fayad, Ghinwa; Schoonheydt, Robert A.; Speybroeck, Veronique Van; Solomon, Edward I.; Sels, Bert F.

doi:10.1038/s41929-021-00602-4

Title: Coordination and activation of nitrous oxide by iron zeolites

Journal Article · Thu Apr 22 00:00:00 EDT 2021 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-021-00602-4· OSTI ID:1798511

^[1]; Snyder, Benjamin E. R. ^[2];

^[3];

^[4]; Fayad, Ghinwa ^[5];

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KU Leuven (Belgium)
Univ. of California, Berkeley, CA (United States); Stanford Univ., CA (United States)
Stanford Univ., CA (United States)
Ghent Univ., Zwijnaarde (Belgium)
Univ. de Caen (France)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Iron-containing zeolites are heterogeneous catalysts that exhibit remarkable activity in the selective oxidation of inert hydrocarbons and catalytic decomposition of nitrous oxide (N₂O). The reduction of N₂O is critical to both these functions, but experimental data tracking the iron active sites during N₂O binding and activation are limited. Here, the N₂O-ligated Fe(ii) active site in iron-exchanged zeolite beta is isolated and characterized by variable-temperature Mössbauer, diffuse reflectance UV-vis-NIR and Fourier transform infrared spectroscopy. N₂O binds through the terminal nitrogen atom with substantial backbonding from the Fe(ii) centre at low temperature. At higher temperatures, the Fe–N₂O interaction is weakened, facilitating isomerization to the O-bound form, which is competent in O-atom transfer. Density functional theory calculations show the geometric and electronic structure requirements for N₂O binding and activation. A geometric distortion imposed by the zeolite lattice plays an important role in activating N₂O. As a result, this highlights a mechanism for structural control over function in Fe-zeolite catalysts.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Flemish Science Foundation; National Science Foundation (NSF); National Science Foundation Graduate Research Fellowship Program

Grant/Contract Number:: AC02-76SF00515; G0A2216N; V417018N; DGE-11474; CHE-1660611; 647755

OSTI ID:: 1798511

Journal Information:: Nature Catalysis, Vol. 4, Issue 4; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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