Abstract
Identification on catalytic sites of heterogeneous catalysts at atomic level is important to understand catalytic mechanism. Surface engineering on defects of metal oxides can construct new active sites and regulate catalytic activity and selectivity. Here we outline the strategy by controlling surface defects of nanoceria to create the solid frustrated Lewis pair (FLP) metal oxide for efficient hydrogenation of alkenes and alkynes. Porous nanorods of ceria (PN-CeO2) with a high concentration of surface defects construct new Lewis acidic sites by two adjacent surface Ce3+. The neighbouring surface lattice oxygen as Lewis base and constructed Lewis acid create solid FLP site due to the rigid lattice of ceria, which can easily dissociate H–H bond with low activation energy of 0.17 eV.
Highlights
Identification on catalytic sites of heterogeneous catalysts at atomic level is important to understand catalytic mechanism
Ozin and colleagues[33,34,35,36,37] has reported that the surface frustrated Lewis pair (FLP) sites of In2O3-x(OH)y created by a Lewis acidic coordinately unsaturated surface indium site proximal to an oxygen vacancy and a Lewis basic surface hydroxide site showed the catalytic activity for the CO2 reduction by H2 in both experimental results and theoretical predictions
Porous nanorods of ceria (PN-CeO2) with a large surface Ce3 þ fraction of 30.8% associated with a high concentration of oxygen vacancy have been demonstrated as the solid metal oxide FLP catalyst with a low activation barrier of 0.17 eV for H2 dissociation
Summary
Identification on catalytic sites of heterogeneous catalysts at atomic level is important to understand catalytic mechanism. Solid FLP sites on CeO2 surface, which deliver a very high catalytic activity for hydrogenation of alkenes and alkynes with a wide scope under mild conditions (T 1⁄4 100 °C and P(H2) 1⁄4 1.0 MPa), have been successfully created by regulating their surface defects.
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