Cu-Mg-Al layered double hydroxides (LDHs) with amine modification were prepared by an organic combination of an anionic surfactant-mediated method and an ultrasonic spalling method using N-aminoethyl-γ-aminopropyltrimethoxysilane as a grafting agent. The materials were characterized by elemental analysis, XRD, SEM, FTIR, TGA, and XPS. The effects of the Cu2+ content on the surface morphology and the CO2 adsorption of Cu-Mg-Al LDHs were investigated, and the kinetics of the CO2 adsorption and the photocatalytic reduction of CO2 were further analyzed. The results indicated that the amine-modified method and appropriate Cu2+ contents can improve the surface morphology, the increase amine loading and the free-amino functional groups of the materials, which were beneficial to CO2 capture and adsorption. The CO2 adsorption capacity of Cu-Mg-Al N was 1.82 mmol·g−1 at 30 °C and a 0.1 MPa pure CO2 atmosphere. The kinetic model confirmed that CO2 adsorption was governed by both the physical and chemical adsorption, which could be enhanced with the increase of the Cu2+ content. The chemical adsorption was suppressed, when the Cu2+ content was too high. Cu-Mg-Al N can photocatalytically reduce CO2 to methanol with Cu2+ as an active site, which can significantly improve the CO2 adsorption and photocatalytic conversion.

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