Activating Lattice Oxygen at the Twisted Surface in a Mesoporous CeO2 Single Crystal for Efficient and Durable Catalytic CO Oxidation

Activating lattice oxygen linked to active sites at surface remains a fundamental challenge in many catalytic reactions. Here we create well‐defined surface by directly growing porous CeO2 single crystals at 2 cm scale and confining Pt in lattice to construct isolated Pt1/CeO2 sites at a continuously twisted surface in a monolith. We demonstrate significantly enhanced activation of lattice oxygen linked to Pt ions in contrast to Ce ions in local structures. We show complete CO oxidation with air at 67 °C without degradation being observed after operation of 300 hours. The isolated Pt1/CeO2 sites at twisted surfaces not only contribute to the chemisorption of CO but also effectively activate the lattice oxygen linked to Pt ion for CO oxidation. The current work would open a new route to activate lattice oxygen by incorporating well‐defined active structures confined at the surfaces. Well‐defined active sites are created at the surface in mesoporous CeO2 single crystals at the 2 cm scale. Complete CO oxidation with air at 67 °C is demonstrated with no degradation observed after operation of 300 hours.