High-Entropy Intermetallics Serve Ultrastable Single-Atom Pt for Propane Dehydrogenation

被引:104
作者
Nakaya, Yuki [1 ]
Hayashida, Eigo [1 ]
Asakura, Hiroyuki [2 ]
Takakusagi, Satoru [1 ]
Yasumura, Shunsaku [1 ]
Shimizu, Ken-ichi [1 ,2 ]
Furukawa, Shinya [1 ,2 ,3 ]
机构
[1] Hokkaido Univ, Inst Catalysis, Sapporo 0010021, Japan
[2] Kyoto Univ, Elements Strategy Initiat Catalysts & Batteries, Kyoto 6158520, Japan
[3] Japan Sci & Technol Agcy, Precursory Res Embryon Sci & Technol, Tokyo 1020076, Japan
关键词
SYNCHRONOUS-TRANSIT METHOD; STATE; CATALYSTS; ALLOYS;
D O I
10.1021/jacs.2c01200
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Propane dehydrogenation has been a promising propylene production process that can compensate for the increasing global demand for propylene. However, Pt-based catalysts with high stability at >= 600 ? have barely been reported because the catalysts typically result in short catalyst life owing to side reactions and coke formation. Herein, we report a new class of heterogeneous catalysts using high-entropy intermetallics (HEIs). Pt-Pt ensembles, which cause side reactions, are entirely diluted by the component inert metals in PtGe-type HEIs. The resultant HEI (PtCoCu) (GeGeSn)/Ca-SiO(2 )exhibited an outstandingly high catalytic stability, even at 600 ? (k(d)(-1) = tau = 4146 h = 173 d), and almost no deactivation of the catalyst was observed for 2 months for the first time. Detailed experimental studies and theoretical calculations demonstrated that the combination of the site-isolation and entropy effects upon multi-metallization of PtGe drastically enhanced the desorption of propylene and the thermal stability, eventually suppressing the side reactions even at high reaction temperatures.
引用
收藏
页码:15944 / 15953
页数:10
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