Titanium-based metal-organic framework, NH-MIL-125(Ti), has been widely investigated for photocatalytic applications but has low activity in the hydrogen evolution reaction (HER). In this work, we show a one-step low-cost postmodification of NH-MIL-125(Ti) via impregnation of Co(NO). The resulting Co@NH-MIL-125(Ti) with embedded single-site Co species, confirmed by XPS and XAS measurements, shows enhanced activity under visible light exposure. The increased H production is likely triggered by the presence of active Co transient sites detected upon collection of pump-flow-probe XANES spectra. Furthermore, both photocatalysts demonstrated a drastic increase in HER performance after consecutive reuse while maintaining their structural integrity and consistent H production. Via thorough characterization, we revealed two mechanisms for the formation of highly active proton reduction sites: nondestructive linker elimination resulting in coordinatively unsaturated Ti sites and restructuring of single Co sites. Overall, this straightforward manner of confinement of Co cocatalysts within NH-MIL-125(Ti) offers a highly stable visible-light-responsive photocatalyst.
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| http://dx.doi.org/10.1021/acsami.3c15490 | DOI Listing |
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