Adjustment of the Single Atom/Nanoparticle Ratio in Pd/CNT Catalysts for Phenylacetylene Selective Hydrogenation
Jérémy Audevard, Javier Navarro‐Ruiz, Vincent Bernardin, Yann Tison, Anna Corrias, Iker Del Rosal, Alain Favre‐Réguillon, Régis Philippe, Iann C. Gerber, Philippe Serp
Abstract
Abstract Pd/C catalysts are widely used for hydrogenation reactions in the chemical industry. One of the reasons for their high activity is the ability of Pd nanoparticles (Pd NP ) to dissociate H 2 and promote H‐spillover. Nevertheless, for selective hydrogenation unpromoted Pd/C catalysts show disappointing results. The use of supported Pd single atom (Pd SA ) catalysts permits to achieve high selectivity. However, Pd SA show low activity because they have difficulty in activating H 2 . A cooperative catalysis between Pd NP and Pd SA operates for the hydrogenation of alkenes thanks to the H‐spillover, which makes it possible to obtain active isolated Pd SA −H species. Here, we present experimental and computational results obtained for phenylacetylene hydrogenation on Pd/CNT catalysts showing different Pd SA /Pd NP ratios. Tuning this ratio allows doubling the activity while reaching high selectivity to styrene at high conversion. DFT calculations suggest that the first coordination sphere of Pd SA has a pronounced effect on their reactivity.