@article{241e0dfd7d03412792303e898a12976a,
title = "Coordination and activation of nitrous oxide by iron zeolites",
abstract = "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 M{\"o}ssbauer, 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. This highlights a mechanism for structural control over function in Fe-zeolite catalysts. [Figure not available: see fulltext.]",
author = "Bols, {Max L.} and Snyder, {Benjamin E.R.} and Rhoda, {Hannah M.} and Pieter Cnudde and Ghinwa Fayad and Schoonheydt, {Robert A.} and {Van Speybroeck}, Veronique and Solomon, {Edward I.} and Sels, {Bert F.}",
note = "Funding Information: This investigation has been supported by the Flemish Science Foundation (FWO, grant no. G0A2216N to B.F.S. and R.A.S.) and the National Science Foundation (grant no. CHE-1660611 to E.I.S.). B.E.R.S. acknowledges support from the National Science Foundation Graduate Research Fellowship Program under grant no. DGE-11474 and from the Munger, Pollock, Reynolds, Robinson, Smith & Yoedicke Stanford Graduate Fellowship. M.L.B. acknowledges the Research Foundation–Flanders for funding of his stay at Stanford University (grant no. V417018N). E.I.S. acknowledges support from the Stanford Woods Institute for the Environment. P.C. and V.V.S. acknowledge the Research Board of Ghent University (BOF) and funding from the European Union{\textquoteright}s Horizon 2020 research and innovation programme (consolidator ERC grant agreement no. 647755– DYNPOR (2015–2020)). The work by G.W. was supported by the ANR-Total {\textquoteleft}Nanoclean Energy{\textquoteright} chair and Normandy{\textquoteright}s RIN program. The computational resources and services for the periodic calculations were provided by Ghent University (Stevin Supercomputer Infrastructure) and the VSC (Flemish Supercomputer Centre), funded by the Research Foundation–Flanders (FWO). Publisher Copyright: {\textcopyright} 2021, The Author(s), under exclusive licence to Springer Nature Limited.",
year = "2021",
month = apr,
doi = "10.1038/s41929-021-00602-4",
language = "English (US)",
volume = "4",
pages = "332--340",
journal = "Nature Catalysis",
issn = "2520-1158",
publisher = "Nature Publishing Group",
number = "4",
}