期刊
CHEMCATCHEM
卷 13, 期 14, 页码 3247-3256出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202100235
关键词
Alkyne hydrogenation; Iron catalysts; Nuclearity effects; Single atoms; Carbon nitride
资金
- Swiss National Science Foundation
Nanostructuring earth-abundant metals as single atoms or controlled clusters on suitable carriers can develop high-performing heterogeneous catalysts, but resolving speciation trends remains challenging. Low-nuclearity iron catalysts exhibit higher activity than larger clusters, with atomistic simulations suggesting a central role of residual carbonyl species in enabling low-energy paths over isolated metal centers.
Nanostructuring earth-abundant metals as single atoms or clusters of controlled size on suitable carriers opens new routes to develop high-performing heterogeneous catalysts, but resolving speciation trends remains challenging. Here, we investigate the potential of low-nuclearity iron catalysts in the continuous liquid-phase semi-hydrogenation of various alkynes. The activity depends on multiple factors, including the nuclearity and ligand sphere of the metal precursor and their evolution upon interaction with the mesoporous graphitic carbon nitride scaffold. Density functional theory predicts the favorable adsorption of the metal precursors on the scaffold without altering the nuclearity and preserving some ligands. Contrary to previous observations for palladium catalysts, single atoms of iron exhibit higher activity than larger clusters. Atomistic simulations suggest a central role of residual carbonyl species in permitting low-energy paths over these isolated metal centers.
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