Nakaya Yuki, Hirayama Jun, Yamazoe Seiji, Shimizu Ken-Ichi, Furukawa Shinya
Institute for Catalysis, Hokkaido University, N21, W10, Sapporo, 001-0021, Japan.
Department of Chemistry, Graduate School of Science, Tokyo Metropolitan University, Hachioji-shi, Tokyo, 192-0397, Japan.
Nat Commun. 2020 Jun 5;11(1):2838. doi: 10.1038/s41467-020-16693-9.
Propylene production via propane dehydrogenation (PDH) requires high reaction temperatures to obtain sufficient propylene yields, which results to prominent catalyst deactivation due to coke formation. Developing highly stable catalysts for PDH without deactivation even at high temperatures is of great interest and benefit for industry. Here, we report that single-atom Pt included in thermally stable intermetallic PtGa works as an ultrastable and selective catalyst for PDH at high temperatures. Intermetallic PtGa displays three-hold-Pt ensembles and single Pt atoms isolated by catalytically inert Ga at the surface, the former of which can be selectively blocked and disabled by Pb deposition. The PtGa-Pb/SiO catalyst exhibits 30% conversion with 99.6% propylene selectivity at 600 °C for 96 h without lowering the performance. The single-atom Pt well catalyzes the first and second C-H activation, while effectively inhibits the third one, which minimizes the side reactions to coke and drastically improves the selectivity and stability.
通过丙烷脱氢(PDH)生产丙烯需要高温以获得足够的丙烯产率,这会由于焦炭形成导致显著的催化剂失活。开发即使在高温下也不会失活的用于PDH的高度稳定催化剂对工业具有极大的吸引力和益处。在此,我们报道热稳定金属间化合物PtGa中包含的单原子Pt在高温下作为用于PDH的超稳定且选择性的催化剂。金属间化合物PtGa在表面显示出三原子Pt组合以及被催化惰性的Ga隔离的单个Pt原子,其中前者可通过Pb沉积被选择性地阻断和失活。PtGa-Pb/SiO催化剂在600°C下96小时内表现出30%的转化率和99.6%的丙烯选择性,且性能不降低。单原子Pt很好地催化了第一次和第二次C-H活化,同时有效抑制了第三次C-H活化,这使生成焦炭的副反应最小化,并极大地提高了选择性和稳定性。