A catalyst in which Pd nanoparticles are supported on triangle‐shaped La2O2CO3 nanosheets exposing predominantly the (001) planes (Pd/La2O2CO3‐TNS; where TNS denotes triangular nanosheets) was prepared by a facile solvothermal method. The Pd/La2O2CO3‐TNS catalysts exhibited excellent catalytic activity and recycling stability for hydrogenation of cinnamaldehyde to hydrocinnamaldehyde with turnover frequency of up to 41 238 h−1. This enhanced activity of Pd/La2O2CO3‐TNS results from strong metal–support interactions. Structure analysis and characterization demonstrated that surface‐oxygen‐enriched La2O2CO3‐TNS supports exposing (001) planes are beneficial to charge transfer between the Pd nanoparticles and triangle‐shaped La2O2CO3 nanosheets and increase the electron density of Pd. Moreover, the modulated electronic states of the Pd/La2O2CO3‐TNS catalysts can enhance the adsorption and activation of hydrogen to enhance the hydrogenation activity.
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