Hydroxy‐ or chlorine‐anchored Pt single‐atom in Al2O3: Which is better for propane dehydrogenation?

Abstract

AbstractPlatinum‐based single‐atom catalysts (Pt1 SACs) can significantly improve the catalytic activity for propane dehydrogenation (PDH) because of their elevated atomic utilization. However, maintaining the high‐temperature stability of the Pt1 species is of utmost importance. To answer the key question: Hydroxy‐ or chlorine‐anchored Pt1 single atoms in Al2O3: Which is the better choice for PDH? We have designed two types of single‐atom Pt catalysts on Al2O3 via a surface group trapping strategy: Pt1–Al2O3 with isolated Pt–O species and Pt1Cl1–Al2O3 with isolated Pt–Cl species. When tested in PDH, Pt1Cl1–Al2O3 showed an exceptional activity of 145 molpropene molPt−1 min−1 at 600°C, which was 3.8 times higher than that of Pt1–Al2O3. It has been demonstrated that the isolated Pt–Cl species in Pt1Cl1–Al2O3 act as an active site and undergoes a dehydrogenation pathway with a lower energy barrier, while Pt1 in Pt1–Al2O3 undergoes a dissociation‐desorption pathway, resulting in few propene productions.