Doubly Decorated Platinum-Gallium Intermetallics as Stable Catalysts for Propane Dehydrogenation
Doubly Decorated Platinum-Gallium Intermetallics as Stable Catalysts for Propane Dehydrogenation
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DOI：
10.1002/anie.202107210
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发表时间：
2021-07-26
影响因子：
16.6
通讯作者：
Furukawa, Shinya
中科院分区：
文献类型：
--
作者：
Nakaya, Yuki;Xing, Feilong;Furukawa, Shinya
丙烷脱氢（PDH）是一种很有前途的化学工艺，可以满足全球对丙烯日益增长的需求。然而，迄今为止报道的 Pt 基催化剂通常在 600 摄氏度以上时会因副反应和焦炭形成而失活。因此，这种催化剂的寿命不足。在此，我们报告了一种新颖的催化剂设计理念，即Pb和Ca对PtGa金属间化合物的双重修饰，分别协同几何和电子促进效应对催化剂稳定性的影响。 Pb 沉积在 PtGa 纳米颗粒的三倍 Pt-3 位点上以阻挡它们，而 Ca 则提供了一个富电子的单原子状 Pt-1 位点，放置在纳米颗粒周围。因此，PtGa-Ca-Pb/SiO2即使在600℃下也表现出极高的催化稳定性（k(d)=0.00033 h(-1)，tau=3067 h），并且首次在长达1个月的时间内几乎没有观察到催化剂失活。
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 degrees 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-3 sites of the PtGa nanoparticles to block them, whereas Ca, which affords an electron-enriched single-atom-like Pt-1 site, is placed around the nanoparticles. Thus, PtGa-Ca-Pb/SiO2 exhibits an outstandingly high catalytic stability, even at 600 degrees C (k(d)=0.00033 h(-1), tau=3067 h), and almost no deactivation of the catalyst was observed for up to 1 month for the first time.