期刊
ACS CATALYSIS
卷 13, 期 9, 页码 5906-5913出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.3c00297
关键词
silver; propylene epoxidation; chlorine; sulfur; NAP-XPS; operando
The development of catalysts for direct epoxidation of propylene to produce propylene oxide using oxygen is challenging. The low selectivity over silver catalysts is attributed to the lack of electrophilic oxygen. The addition of electrophilic-O via SO4 oxyanions and Cl activation of the oxyanion can significantly increase the selectivity to propylene oxide.
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.
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