Constructing mesoporous CeO2 single-crystal particles in ionic liquids for enhancing the conversion of CO2 and alcohols to carbonates

Catalysts for CO2 value-added conversion have been extensively explored, but there is still a lack of systematic design for catalysts that achieve efficient CO2 conversion under mild conditions. Herein, we explored a mesoporous CeO2 single-crystal formed with the regulation of ionic liquids, which catalyzed the effective carbonylation reaction with CO2 under mild reaction conditions. By altering the synthetic environment, a series of uniform mesoporous CeO2 particles with atomically aligned single-crystal frameworks were constructed, which have different surface physicochemical properties and primary aggregation degree. The prepared mesoporous CeO2 single-crystal achieved efficient activation of CO2 and alcohols at 0.5 MPa CO2 and 100 degrees C, and the CeO2-IL-M catalyst shows optimal catalytic performance in the synthesis of ethylene carbonate with 46.22 mmol g -1 h-1, which was 50.6 times as high as that of the CeO2 obtained without ionic liquids. Subsequently, the catalytic pathway and mechanism of carbonylation reaction with CO2 on mesoporous CeO2 single-crystal were studied via React-IR spectra and C 18 O 2 labeling experiments. The research provides a new strategy for controllable nanoscale assembly of mesoporous single-crystal materials and expands the application range of single-crystal materials, aiming to develop novel catalytic materials to meet industrial needs. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.