AI Article Synopsis
- A key challenge in single-atom (SA) catalysis is creating fully inorganic sites that can achieve the high reaction selectivity typically seen in organometallic catalysts used in homogeneous catalysis.
- Researchers have found that isolated rhodium (Rh) atoms on oxygen-defective SnO can achieve high turnover frequency (TOF) and excellent selectivity for gas-phase hydroformylation of ethylene while preventing unwanted olefin hydrogenation.
- The study demonstrates that a significant reduction of lattice oxygen in the SnO surface allows for greater flexibility in the coordination of Rh atoms, resulting in exceptional catalytic performance comparable to liquid-phase molecular catalysts.
Article Abstract
A frontier challenge in single-atom (SA) catalysis is the design of fully inorganic sites capable of emulating the high reaction selectivity traditionally exclusive of organometallic counterparts in homogeneous catalysis. Modulating the direct coordination environment in SA sites, via the exploitation of the oxide support's surface chemistry, stands as a powerful albeit underexplored strategy. We report that isolated Rh atoms stabilized on oxygen-defective SnO uniquely unite excellent TOF with essentially full selectivity in the gas-phase hydroformylation of ethylene, inhibiting the thermodynamically favored olefin hydrogenation. Density Functional Theory calculations and surface characterization suggest that substantial depletion of the catalyst surface in lattice oxygen, energetically facile on SnO , is key to unlock a high coordination pliability at the mononuclear Rh centers, leading to an exceptional performance which is on par with that of molecular catalysts in liquid media.
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| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10099584 | PMC |
| http://dx.doi.org/10.1002/anie.202214048 | DOI Listing |
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