Propane Dehydrogenation on PtxSny (x, y ≤ 4) Clusters on Al2O3(110),ACS Catalysis

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Propane Dehydrogenation on PtxSny (x, y ≤ 4) Clusters on Al2O3(110)
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-02-09 , DOI: 10.1021/acscatal.2c05671
Yilang Liu ₁ , Xue Zong _{1,

2} , Abhirup Patra ₁ , Stavros Caratzoulas ₁ , Dionisios G. Vlachos _{1,

2}

Affiliation

With increasing interest in atomically dispersed and sub-nanometer Pt and Pt–Sn cluster catalysts for propane dehydrogenation (PDH), understanding structure–property relationships is of great importance. In this work, we present density functional theory calculations and microkinetic modeling of PDH on eight alumina-supported Pt_x (x = 1–4) and Pt_xSn_y (x = 1–3, y = 1 and x = 2, y = 2) model catalysts and elucidate the effects of Pt nuclearity and Sn heteroatoms. Pt_x clusters are prone to sintering, and their stability is improved with the addition of Sn. The Pt_x activity changes nonmonotonically with cluster size. Pt₁ presents the most favorable dehydrogenation barriers, but its PDH rate is highly limited by the blocking of sites by hydrogen. A volcano-like activity–nuclearity relation is found, with Pt₂ being the most active cluster. An increase in Pt nuclearity beyond x = 2 leads to lower rates due to increased dehydrogenation barriers. Moderate addition of Sn somewhat depresses the Pt activity, whereas Pt_xSn_y clusters with a Pt/Sn ratio of 1:1 become inactive. The Pt₃Sn₁ cluster exhibits good activity with improved stability compared to Pt₃ and Pt₂ and could be an experimental target. While Sn promotes propylene desorption, propane hydrogenolysis to C1 and C2 species on single atoms and small Pt_x and Pt_xSn_y clusters is unfavorable. Low selectivity to propylene seen experimentally should instead stem from other routes.

更新日期：2023-02-09

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