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Abstract

The development of catalysts for propylene oxide production from direct epoxidation using propylene and oxygen remains a challenge. Compared to ethylene epoxidation, where selectivity on silver catalysts is high, the low selectivity to produce propylene oxide over silver is partially attributed to the lack of electrophilic oxygen under propylene epoxidation reaction conditions. Here, we investigate how to mediate the chemical reactivity of oxygen by theory-inspired experiments for propylene epoxidation. We show how adding electrophilic-O via SO₄ oxyanions to the surface of silver increases epoxide selectivity. Moreover, we show how the addition of Cl to the SO₄-modified catalyst activates the oxyanion, giving a more than 4-fold increase in selectivity to propylene oxide. Finally, we explore different systems using DFT and draw a picture on how the next catalyst/co-catalyst systems should be tuned to design a catalyst with high selectivity for direct propylene oxidation.