Zirconium-Based Metal-Organic Frameworks for Oxygen Sensing
Received date: 2024-11-01
Online published: 2024-12-19
Supported by
National Natural Science Foundation of China(22175179)
Oxygen sensing plays a vital role in a variety of fields, including environmental monitoring, healthcare, industrial processes, and safety management. Metal-organic frameworks (MOFs), owing to their robust oxygen adsorption capacity and tunable structure, are anticipated to be applied in oxygen sensing to enhance response performance. In this work, we synthesized four common Zr-MOFs (MOF-808, UiO-66, NU-1000, NH2-UiO-66) using the solvothermal method and validated the interaction between the ligands and zirconium clusters by comparing their fluorescence emission and lifetime. Then, the fluorescence of these four MOFs were tested under vacuum, air, and oxygen atmospheres. The experiments demonstrate that oxygen is the main air component that effectively quenches the fluorescence of zirconium-based MOFs. Recirculation experiments and powder X-ray diffraction of MOFs before and after fluorescence quenching indicate that zirconium-based MOFs exhibit high photo-stability. Under vacuum and pure oxygen conditions, UiO-66 can quench 88% of its fluorescence, with response and recovery times as low as 13 s and 15 s, respectively. This rapid detection of O2 over multiple cycles suggests that UiO-66 possesses a high level of sensitivity. In contrast, the fluorescence of chromium-based MOFs with the same ligands is hardly affected. This may be related to the electronic structure of tetravalent zirconium being able to match the electronic structure of paramagnetic oxygen, allowing the fluorescence process of the MOF to be quenched under the action of oxygen. To explore the advantages of zirconium-based MOFs in oxygen sensing, density functional theory calculations are adopted to determine the adsorption energy of oxygen with MIL-100(Cr) and MOF-808(Zr), which have the same ligands, confirming that one of the reasons for the special sensitivity of zirconium-based MOFs to oxygen is the shorter collision radius between Zr metal clusters and O2 molecules. The reduction in fluorescence lifetime confirmed the interaction between oxygen and the MOF. These findings are expected to provide theoretical guidance for the development of sensitive oxygen sensors.
Yue Wang , Ying Zou , Yuan Zhang , Shujie Zheng , Hengyu Wang , Tianfu Liu , Renfu Li . Zirconium-Based Metal-Organic Frameworks for Oxygen Sensing[J]. Acta Chimica Sinica, 2025 , 83(1) : 45 -51 . DOI: 10.6023/A24110333
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