Surface-Modified Pd/CeO2 Single-Atom Catalyst Shows Increased Activity for Suzuki Cross-Coupling

Document Type

Article

Publication Date

12-25-2023

Publisher

American Chemical Society

Source Publication

Inorganic Chemistry

Source ISSN

0020-1669

Original Item ID

DOI: 10.1021/acs.inorgchem.3c03649

Abstract

Single-atom catalysts (SACs) comprise catalytically active atoms dispersed on supports; they combine the high activity and site uniformity of homogeneous catalysts with the ease of separability of heterogeneous catalysts. However, SACs lack fine control over the active site, provided by ligands in homogeneous catalysts. In this work, we demonstrate that modification of the support with an organic monolayer is a viable approach to improving the catalytic performance. The addition of catechol-type monolayers to a Pd/CeO2 SAC increases its catalytic activity for Suzuki cross-coupling, a central reaction in the synthesis of fine chemicals and pharmaceuticals. Kinetic trials reveal that the coating reduces the activation energy from 49 ± 9 to 22 ± 5 kJ/mol and produces a 4-fold rate enhancement at 25 °C, an effect we attribute to π–π interactions between the reactant and the catechol coating. Further development of this approach could vastly increase the utility of SACs in organic synthesis.

Comments

Inorganic Chemistry, Vol. 62, No. 51 (December 25, 2023): 21479-21486. DOI.

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