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Rhodium Single-Atom Catalyst Design through Oxide Support Modulation for Selective Gas-Phase Ethylene
Marcos G Farpón1, Wilson Henao1, Philipp N Plessow2
1ITQ Instituto de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC), Av. Los Naranjos s/n, 46022, Valencia, Spain.
Designing inorganic single-atom (SA) catalysts remains a challenge. This study demonstrates that Rh single atoms on oxygen-defective SnO2 achieve high selectivity and activity in ethylene hydroformylation, matching molecular catalysts.
Area of Science:
- Heterogeneous catalysis
- Surface chemistry
- Inorganic materials
Background:
- Designing single-atom (SA) catalysts with high selectivity is crucial.
- Organometallic catalysts offer high selectivity but are limited to homogeneous systems.
- Modulating the coordination environment of SA sites using support surface chemistry is an underexplored strategy.
Purpose of the Study:
- To develop fully inorganic single-atom sites for high reaction selectivity.
- To investigate the role of oxide support surface chemistry in modulating SA site performance.
- To achieve selectivity in gas-phase hydroformylation comparable to homogeneous molecular catalysts.
Main Methods:
- Stabilization of isolated Rh atoms on oxygen-defective SnO2.
- Gas-phase hydroformylation of ethylene.
- Density Functional Theory (DFT) calculations.
- Surface characterization techniques.
Main Results:
- Isolated Rh atoms on oxygen-defective SnO2 exhibit excellent turnover frequency (TOF).
- Achieved nearly full selectivity in ethylene hydroformylation, suppressing olefin hydrogenation.
- Demonstrated performance comparable to molecular catalysts in liquid media.
Conclusions:
- Oxygen-defective SnO2 supports Rh single atoms effectively.
- Lattice oxygen depletion on SnO2 enhances coordination pliability of Rh centers.
- This strategy enables highly selective and active inorganic SA catalysts for hydroformylation.
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