Main-Group Catalysts with Atomically Dispersed In Sites for Highly Efficient Oxidative Dehydrogenation

Transition metal oxides are well-known catalysts for oxidative dehydrogenation thanks to their excellent ability to activate alkanes. However, they suffer from an inferior alkene yield due to the trade-off between the conversion and selectivity induced by more reactive alkenes than alkanes, which obscures the optimization of catalysts. Herein, we attempt to overcome this challenge by activating a selective main-group indium oxide considered to be inactive for oxidative dehydrogenation in conventional wisdom. Atomically dispersed In sites with the local structure of [InOH](2)(+) anchored by substituting the protons of supercages in HY are enclosed to be active centers that enable the activation of ethane with a metal-normalized turnover number of almost one magnitude higher than those of their supported In2O3 counterparts. Furthermore, the structure of isolated [InOH](2+) sites could be stabilized by in situ formed H2O from the selective oxidation of hydrogen by In2O3 nanoparticles. As a result, the as-designed main-group In catalysts exhibit 80% ethene selectivity at 80% ethane conversion, thus achieving 60% ethene yield due to active isolated [InOH](2+) sites and selective H2O3 nanoparticles, outperforming state-of-the-art transition metal oxide catalysts. This study unlocks new opportunities for the utilization of main-group elements and could pave the way toward a more rational design of catalysts for highly efficient selective oxidation catalysis.

Automated summary

This study demonstrates successful activation of a main-group indium oxide, which was previously considered inactive, for the conversion of ethane, achieving improved conversion rate and selectivity. The active centers in the catalyst are atomically dispersed indium sites and selective H2O3 nanoparticles. This research opens up new opportunities for the rational design of catalysts for highly efficient selective oxidation.