Bimetallic overlayer catalysts with core-shell nanostructures have attracted long-standing attention and have been applied in a wide range of chemical reactions in heterogeneous catalysis. How to appropriately select core and shell composition to optimize lattice strain and ligand effect for a target reaction remains a significant but challenging issue, and the resulting geometric and electronic structures of catalysts play key roles in tailoring adsorption properties and thus improving catalytic performances. In our work, we disclose by joint theoretical and experimental investigations that tensile strain of Pt or Pd overlayer on Au terrace upshifts the surface d-band center and increases reaction activity in chemoselective hydrogenation of p-chloronitrobenzene and benzyl alcohol oxidation compared to their monometallic counterparts by enhancing adsorption and activation of reactants as key steps. On the contrary, lattice compression of Pd overlayer on Ru downshifts d-band center and weakens binding, improving selectivity toward ethylene by promoting its desorption in semi-hydrogenation of acetylene. Specific activity is also increased based on sensitive dependence of adsorption for different intermediates on metal surfaces resulting from molecule saturation. These findings provide a valuable rationale of designing strained bimetallic overlayer nanostructures with desired chemical properties in target reactions.

Synergistic improvement of activity and selectivity on strained bimetallic overalyers by tailoring adsorption

Where thousands of chemistry professionals meet to share ideas and advance scientific and technical knowledge. Spring 2023 abstracts, posters, and presentations will launch at the end of March.

ACS Spring 2023

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.