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Fine-Tuning of Pt Dispersion on Al 2 O 3 and Understanding the Nature of Active Pt Sites for Efficient CO and NH 3 Oxidation Reactions.

Wei TanShaohua XieXing ZhangKailong YeMurtadha AlmousawiDaekun KimHaowei YuYandi CaiHanchen XiLu MaSteven N EhrlichFei GaoLin DongFudong Liu
Published in: ACS applied materials & interfaces (2023)
Fine-tuning the dispersion of active metal species on widely used supports is a research hotspot in the catalysis community, which is vital for achieving a balance between the atomic utilization efficiency and the intrinsic activity of active sites. In this work, using bayerite Al(OH) 3 as support directly or after precalcination at 200 or 550 °C, Pt/Al 2 O 3 catalysts with distinct Pt dispersions from single atoms to clusters ( ca . 2 nm) were prepared and evaluated for CO and NH 3 removal. Richer surface hydroxyl groups on AlO x (OH) y support were proved to better facilitate the dispersion of Pt. However, Pt/Al 2 O 3 with relatively lower Pt dispersion could exhibit better activity in CO/NH 3 oxidation reactions. Further reaction mechanism study revealed that the Pt sites on Pt/Al 2 O 3 with lower Pt dispersion could be activated to Pt 0 species much easier under the CO oxidation condition, on which a higher CO adsorption capacity and more efficient O 2 activation were achieved simultaneously. Compared to Pt single atoms, PtO x clusters could also better activate NH 3 into -NH 2 and -HNO species. The higher CO adsorption capacity and the more efficient NH 3 /O 2 activation ability on Pt/Al 2 O 3 with relatively lower Pt dispersion well explained its higher CO/NH 3 oxidation activity. This study emphasizes the importance of avoiding a singular pursuit of single-atom catalyst synthesis and instead focusing on achieving the most effective Pt species on Al 2 O 3 support for targeted reactions. This approach avoids unnecessary limitations and enables a more practical and efficient strategy for Pt catalyst fabrication in emission control applications.
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