Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 283, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119626
Keywords
Metal-organic frameworks; Photocatalysis; Hydrogen evolution; Charge separation; Ligand tuning
Funding
- China Scholarship Council (CSC)
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The study found that the combination of MIL-125-Ti with methanol exhibited higher activity in photocatalysis due to the effective scavenging of holes in the metal-oxo cluster by methanol and prevention of charge recombination, while holes in NH2 groups were detrimental to photocatalytic performance. Mixed-ligand MOFs follow a dual-excitation pathway, introducing new states and transitions.
We synthesized a series of isostructural MIL-125-Ti with various terephthalic: amino-terephthalic acid ratios and evaluated their photostability and performance for photocatalytic hydrogen evolution in aqueous solutions with different hole scavengers. We demonstrate that the commonly used triethanolamine corroded the MOFs under photocatalytic conditions, in contrast to methanol. The combination of MIL-125-Ti and methanol outperformed the photocatalytic activity of NH2-MIL-125-Ti by 45 times under broad UV irradiation. Photoluminescence spectroscopy under simulated photocatalytic conditions and in solid-state as well as time-resolved emission studies reveal that the holes residing in the metal-oxo cluster can be effectively scavenged by methanol, leading to high HER activity, while the holes residing in the NH2-groups in the ligand favour charge recombination and are thus detrimental to the photocatalytic performance. The mixed-ligand MOFs follow a dual-excitation pathway, introducing new states and transitions. These results are expected to advance our understanding of MOF-based photocatalysis.
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