Enabling Pd Catalytic Selectivity via Engineering Intermetallic Core@Shell Structure

doi:10.1021/acsnano.3c05193

Enabling Pd Catalytic Selectivity via Engineering Intermetallic Core@Shell Structure

2023-12-20

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DOI：10.1021/acsnano.3c05193

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Core@shell nanoparticles (NPs) have been widely explored to enhance catalysis due to the synergistic effects introduced by their nanoscale interface and surface structures. However, creating a catalytically functional core@shell structure is often a synthetic challenge due to the need to control the shell thickness. Here, we report a one-step synthetic approach to core-shell CuPd@Pd NPs with an intermetallic B2-CuPd core and a thin (similar to 0.6 nm) Pd shell. This core@shell structure shows enhanced activity toward selective hydrogenation of Ar-NO2 and allows one-pot tandem hydrogenation of Ar-NO2 to Ar-NH2 and its condensation with Ar-CHO to form Ar-N & boxH;CH-Ar. DFT calculations indicate that the B2-CuPd core promotes the Pd shell binding to Ar-NO2 more strongly than to Ar-CHO, thereby selectively activating Ar-NO2. The chemoselective catalysis demonstrated by B2-CuPd@Pd can be extended to a broader scope of substrates, allowing green chemistry synthesis of a wide range of functional chemicals and materials.

Keywords:

chemoselective hydrogenation

core@shell structure

tandem reactions

green chemistry

rigid-rodpolymer

DFT calculations

Enabling Pd Catalytic Selectivity via Engineering Intermetallic Core@Shell Structure

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