Semi-hydrogenation of acetylene to ethylene is an important process to purify ethylene streams in industry. However, among current approaches reported in the literature, high ethylene selectivity has been generally achieved at the expense of activity. Herein, we show that a Ga2 O3 coating of Ag@Pd core-shell bimetallic nanoparticle catalysts, allows improvement of the ethylene selectivity to a much greater extent than the coating of monometallic Pd nanoparticles, while preserving a remarkable intrinsic activity, approximately 50 times higher than the benchmark catalyst of Pd1 Ag single-atom alloys (SAAs). Importantly, the resulting catalyst also shows excellent long-term stability, by suppressing coke formation efficiently. Spectroscopic characterization reveals that weakened ethylene adsorption by bimetallic electronic synergy, and oxide site isolation are both essential for the high ethylene selectivity and high-coking resistance. H-D exchange measurements further show that the Ga2 O3 -coated Ag@Pd catalyst possesses a much higher activity of H2 activation than that of Pd1 Ag SAAs, thus boosting the hydrogenation activity at the same time.
Keywords: atomic layer deposition; bimetallic catalysts; hydrogenation; oxide overcoating; selectivity.
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