Abstract
Active-sites play a pivotal role in catalyzing reactions at surfaces, yet engineering these active sites still remains a significant challenge. In this work, hydroxylated MgO nanosheets supported ultrasmall PtNi alloys approximately 2.6(1) nm (xPt-yNi/MgOhydr) has been investigated via active-site engineering. Experimental results and DFT calculations reveal that electron transfers from Ni to Pt and from hydroxyl groups to Pt 5d-orbitals generate active sites NiPt-(OH)x. In the preferential CO oxidation (CO-PROX) reaction, these active sites on xPt-yNi/MgOhydr switch the bicarbonates reaction pathway depending on temperature range. Consequently, the optimal catalyst, 5%Pt-0.5%Ni/MgOhydr, achieves 100% CO conversion at 100 °C, demonstrating a broad temperature operation window (100–200 °C) and excellent durability. The active site engineering approach presented in this study can promote the discovery of more excellent catalysts with the optimal reaction route for various applications.
Published Version
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