Responsive luminescent silver-based metal-organic frameworks for highly sensitive and selective detection of hydrogen...

As a highly toxic gas pollutant and also an endogenous gaseous signaling molecule existing in a variety of physiological processes, the rapid and accurate in-field detection of hydrogen sulfide is of great concern. Nevertheless, two drawbacks as for the optical probes for H₂S detection, taking about a long time to reach the optical signal balance or the low selectivity, always exist. Herein, by using a highly photoluminescent and H₂S-stimuli responsive silver-based metal-organic frameworks (MOFs): Ag-BDC (BDC = 1, 4-benzene dicarboxylate), we demonstrated that the luminescence intensity of Ag-BDC MOFs was inversely proportional to the concentration of H₂S due to the Ag-S coordination and the obstruction of ligand-to-metal charge transfer (LMCT) transition process, and there was a quick response time of below 3.0 min. Combined with a simple customized device to separate H₂S from the sample, the selectivity of the method for H₂S detection could be greatly improved, and no interference would be caused even if the other sulfur-containing species coexisted. The luminescence probe presented a favorable sensitivity within a linear range of 0.1-1000 μM along with a detection limit of 23.7 nM. When employed to assay the endogenous sulfide level in the human serum and mouse brain tissue, the approach showed recoveries from 96.3% to 102% with relative standard derivation (RSD) less than 2.0%. By the integration of the responsive luminescent silver-based MOFs with a simple self-assembled headspace separation device, obviously the present strategy could be beneficial to the development and design of the in-field fast H₂S measurement, possessing particular advantages in biological systems to eliminate the potential interferences.