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Atomically Dispersed Pt1-Polyoxometalate Catalysts: How Does Metal-Support Interaction Affect Stability and
Bin Zhang1, Geng Sun2, Shipeng Ding1
1Department of Chemical and Biomolecular Engineering , National University of Singapore , 4 Engineering Drive 4 , 117585 Singapore.
Journal of the American Chemical Society
|April 30, 2019
Summary
Supported single-atom catalysts (SACs) with platinum atoms on polyoxometalates show high stability and activity. These platinum SACs offer improved performance in hydrogenation reactions without compromising catalytic power.
Area of Science:
- Heterogeneous Catalysis
- Materials Science
- Surface Chemistry
Background:
- Supported single-atom catalysts (SACs) feature atomically dispersed metal atoms, leading to significant metal-support interactions.
- Understanding the stability and catalytic influence of these interactions is crucial for designing advanced catalysts.
Purpose of the Study:
- To quantitatively investigate the stability of platinum (Pt) atoms on polyoxometalate supports.
- To elucidate how Pt-support interactions affect catalytic performance in hydrogenation reactions.
Main Methods:
- Synthesis and characterization of polyoxometalate-supported Pt catalysts.
- Experimental evaluation of catalytic performance in hydrogenation reactions.
- Density Functional Theory (DFT) calculations to simulate reaction pathways and energetics.
Main Results:
- Pt atoms preferentially adsorb at 4-fold hollow sites on polyoxometalates, with a minimum adsorption energy of 5.50 eV ensuring sintering resistance.
- Catalytic activity in hydrogenation reactions shows similar pathways and low effective barriers (24 kJ/mol) across different Pt-support interactions.
- DFT confirms reactions occur solely on Pt atoms, with hydrogenation proceeding via molecularly adsorbed H2, and weaker H2 adsorption on SACs.
Conclusions:
- Achieving highly stable platinum SACs on polyoxometalates is possible without sacrificing catalytic activity.
- The observed low activation barriers are attributed to weaker H2 adsorption on Pt SACs compared to clusters or surfaces.
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