Room Temperature design of Ce(IV)-MOFs: from photocatalytic HER and OER to overall water splitting under simulated sunlight irradiation - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Chemical Science Année : 2023

Room Temperature design of Ce(IV)-MOFs: from photocatalytic HER and OER to overall water splitting under simulated sunlight irradiation

Shan Dai
Eva Montero-Lanzuela
  • Fonction : Auteur
Antoine Tissot
Herme Baldoví
Hermenegildo García
Sergio Navalón
  • Fonction : Auteur
Christian Serre

Résumé

The development of MOF-based efficient and reusable catalysts for hydrogen production under simulated sunlight irradiation, especially through overall water splitting, remains challenging. This is mainly due to either the inappropriate optical features or poor chemical stability of the given MOFs. Room temperature synthesis (RTS) of tetravalent MOFs is a promising strategy to design robust MOFs and their related (nano)composites. By employing these mild conditions, herein, we report for the first time that RTS lead to the efficient formation of highly redox active Ce(IV)-MOFs that are inaccessible at elevated temperatures. Consequently, not only highly crystalline Ce-UiO-66-NH2 is synthesized, but also many other derivatives and topologies (8 and 6-connected phases) without compromise in space-time yield. Their photocatalytic HER and OER activity under simulated sunlight irradiation are in good agreement with their energy level diagrams: Ce-UiO-66-NH2 and Ce-UiO-66-NO2 are the most active photocatalysts for the HER and OER, respectively, with a higher activity than other metals-based UiO-type MOFs. Combining Ce-UiO-66-NH2 with supported Pt NPs results finally in one of the most active and reusable photocatalysts for the overall water splitting into H2 and O2 under simulated sunlight irradiation, due to its efficient photoinduced charge separation evidenced by laser flash photolysis and photoluminescence spectroscopies.
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Dates et versions

hal-04283016 , version 1 (13-11-2023)

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Shan Dai, Eva Montero-Lanzuela, Antoine Tissot, Herme Baldoví, Hermenegildo García, et al.. Room Temperature design of Ce(IV)-MOFs: from photocatalytic HER and OER to overall water splitting under simulated sunlight irradiation. Chemical Science, 2023, 14 (13), pp.3451-3461. ⟨10.1039/D2SC05161C⟩. ⟨hal-04283016⟩
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