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双修饰铂镓金属间化合物作为丙烷脱氢的稳定催化剂。

Doubly Decorated Platinum-Gallium Intermetallics as Stable Catalysts for Propane Dehydrogenation.

作者信息

Nakaya Yuki, Xing Feilong, Ham Hyungwon, Shimizu Ken-Ichi, Furukawa Shinya

机构信息

Institute for Catalysis, Hokkaido University, N-21, W-10, Sapporo, 001-0021, Japan.

Elements Strategy Initiative for Catalysts and Batteries, Kyoto University, Katsura, Kyoto, 615-8520, Japan.

出版信息

Angew Chem Int Ed Engl. 2021 Sep 1;60(36):19715-19719. doi: 10.1002/anie.202107210. Epub 2021 Jul 26.

DOI:10.1002/anie.202107210
PMID:34185941
Abstract

Propane dehydrogenation (PDH) is a promising chemical process that can satisfy the increasing global demand for propylene. However, the Pt-based catalysts that have been reported thus far are typically deactivated at ≥600 °C by side reactions and coke formation. Thus, such catalysts possess an insufficient life. Herein, we report a novel catalyst design concept, namely, the double decoration of PtGa intermetallics by Pb and Ca, which synergize the geometric and electronic promotion effects on the catalyst stability, respectively. Pb is deposited on the three-fold Pt sites of the PtGa nanoparticles to block them, whereas Ca, which affords an electron-enriched single-atom-like Pt site, is placed around the nanoparticles. Thus, PtGa-Ca-Pb/SiO exhibits an outstandingly high catalytic stability, even at 600 °C (k =0.00033 h , τ=3067 h), and almost no deactivation of the catalyst was observed for up to 1 month for the first time.

摘要

丙烷脱氢(PDH)是一种很有前景的化学工艺,能够满足全球对丙烯日益增长的需求。然而,迄今为止报道的基于铂的催化剂通常在≥600°C时因副反应和积炭而失活。因此,这类催化剂的使用寿命不足。在此,我们报道了一种新颖的催化剂设计概念,即通过铅和钙对PtGa金属间化合物进行双重修饰,它们分别对催化剂稳定性产生几何促进效应和电子促进效应。铅沉积在PtGa纳米颗粒的三重铂位点上以将其阻断,而能提供富电子单原子类铂位点的钙则置于纳米颗粒周围。因此,即使在600°C时,PtGa-Ca-Pb/SiO也表现出极高的催化稳定性(k =0.00033 h⁻¹,τ=3067 h),并且首次观察到催化剂在长达1个月的时间内几乎没有失活。

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