Blurring the boundary between homogenous and heterogeneous catalysis using palladium nanoclusters with dynamic surfaces

Abstract Using a magnetron sputtering approach that allows size-controlled formation of nanoclusters, we have created palladium nanoclusters combine the features both heterogeneous and homogeneous catalysts. Here report atomic structures electronic environments series metal in ionic liquids at different stages formation, leading to discovery Pd with core ca . 2 nm surrounded by diffuse dynamic shell atoms [C 4 C 1 Im][NTf ]. Comparison catalytic activity alkene cyclopropanation reveals atomically surface is critically important, increasing factor when compared compact similar size. Catalyst poisoning tests using mercury dibenzo[ a,e ]cyclooctene show maintain their activity, which demonstrate combined catalysts within same material. Additionally, kinetic studies alkenes mediated reveal an observed catalyst order 1, underpinning pseudo-homogeneous character nanoclusters.