Effective ethylene polymerization requires that the ethylene feed stream contain minimal acetylene to avoid poisoning the polymerization catalyst. The selective hydrogenation of acetylene to ethylene, while avoiding over-hydrogenation to ethane, is, therefore, an important problem in industrial catalysis. The high selectivity required in this reaction makes it a prime candidate for study with single-atom catalysts, in which isolated metal centers are designed with uniform chemical activity. In this work, we design on-surface metal-organic complexation, which acts to bridge the gap between homogeneous catalysis and heterogeneous catalysis, and provides metal sites on powder oxide supports that are active and selective for hydrogenation of acetylene to ethylene. We investigate the effect of organic ligand and its impact on the activity, selectivity, and stability of supported single-atom Pd metal. In the metal-ligand approach we are employing, the supported metal species form Pd-ligand single-atom catalysts (SAC) on pristine powder supports. The activity of these catalysts shows a significant dependence on the choice of ligand and type of support. Understanding the support-metal interaction is crucial to advance the design of highly dispersed single-site catalysts for heterogeneous reactions.

Reactivity and selectivity of single atom catalysts on metal oxide surfaces for the selective hydrogenation of acetylene

ACS Spring 2022

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