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Bifunctional Au@UiO-67-bpy-Cu Plasmonic Nanostructures for the Solar-Driven CO2 Reduction to Methanol
Summary:
The authors from the Universidade de Vigo, Spain, developed a bifunctional Au@UiO-67-bpy-Cu plasmonic nanostructure material, achieving significant results in the solar-driven CO2 reduction to methanol.
Background:
1. To address the problem of sustainable methanol production from CO2, previous researchers have explored various photocatalysts, achieving certain success. However, challenges remain in developing highly efficient, selective, and stable photocatalysts that operate without the need for hole scavengers.
2. The authors in this study proposed an innovative method of synthesizing a hybrid photocatalyst by integrating plasmonic Au nanospheres and Cu active centers into UiO-67-bpy MOFs, obtaining high methanol yield and selectivity under solar irradiation.
Research Content:
1. Synthesis:
The authors synthesized the Au@UiO-67-bpy-Cu material using a two-step method. First, Au@UiO-67-bpy core-shell structures were prepared by growing UiO-67-bpy MOFs on Au nanospheres. Then, the bpy ligands were functionalized with Cu ions.
2. Characterizations:
1) The BET surface area of the pristine UiO-67-bpy was 1806.5 m²/g, which decreased to 518.1 m²/g after Cu functionalization.
2) SEM/TEM tests show the particle size of the UiO-67-bpy-Cu and Au@UiO-67-bpy-Cu materials to be around 126.3 nm and 21.3 nm for the Au nanospheres, respectively.
3) UV-Vis DRS, XPS, and TRPL tests indicate the successful coordination of Cu ions and the enhanced light absorption and charge carrier lifetime of the hybrid material.
3. Application:
The material was tested in photocatalytic CO2 reduction under visible light irradiation. The Au@UiO-67-bpy-Cu sample demonstrated a methanol formation rate of 118.4 μmol h−1 gcat−1 and 96% selectivity to methanol, which remained stable during four consecutive cycles.
4. Mechanism:
The analysis of the experimental results suggests that the synergistic effect of the excitation of the bpy-Cu complex and the intraband transitions of Au nanospheres under visible light conditions generates hot electrons at the bpy-Cu states, enhancing CO2 reduction efficiency. The hot holes at the UiO-67-bpy valence band can oxidize water to close the charge circulation cycle.
Outlook:
This research provides a novel and efficient approach to developing plasmonic-MOF hybrid photocatalysts for sustainable CO2 reduction to methanol, offering significant potential for future renewable energy applications.
Bifunctional Au@UiO-67-bpy-Cu Plasmonic Nanostructures for the Solar-Driven CO2 Reduction to Methanol
Authors: Elizabeth Cepero-Rodríguez, Ana Sousa-Castillo, Lucas V. Besteiro, Begoña Puértolas, Margarita Vázquez-González, M.A Correa-Duarte
DOI：10.1002/aenm.202401887
Link：https://onlinelibrary.wiley.com/doi/10.1002/aenm.202401887
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