Abstract
The dynamic pore systems and high surface areas of flexible metal–organic framework materials make them excellent candidates to be used in different kinds of adsorption processes. However, the adsorption and desorption behaviors of therapeutic drugs on metal–organic frameworks in solution are not fully developed. Here, we systematically investigated the adsorption and desorption behaviors of a typical therapeutic drug, verapamil, over several Zr-based metal–organic frameworks [e.g., Zr-FUM, UiO-66(Zr), UiO-66(Zr)-NH2 and UiO-66(Zr)-2COOH] as well as ZrO2 in an acetonitrile solution by using paper spray mass spectrometry. In contrast to other materials, UiO-66(Zr)-2COOH demonstrated a superior adsorption performance to verapamil due to their strong acid-base and/or hydrogen-bond interactions, and the adsorption process fitted well with the pseudo-second-order kinetic model. As verapamil-adsorbed materials were used for desorption experiments, ZrO2 demonstrated the most favorable desorption performance, whereas UiO-66(Zr)-2COOH yielded the poorest desorption capability. These Zr-based materials had also been coated at the surface with filter papers for the analysis of various drugs and proteins in the process of paper spray mass spectrometry. The results demonstrated that among the studied materials, ZrO2-coated paper gave the most favorable desorption performance as a pure drug solution, whereas the paper from UiO-66(Zr) demonstrated the optimal capability in the analyses of therapeutic drugs in a complex matrix (e.g., blood) and a protein (e.g., myoglobin).
Highlights
To expand the application of Metal–organic frameworks (MOFs) in a mass spectrometric analysis, more recently we explored the capabilities of three types of MOFs [e.g., MIL-53(Al), ZIF-8 and UiO-66(Zr)] as substrates for paper spray Mass spectrometry (MS), in which analyte transport was achieved by wicking a porous paper substrate into a high electric field [53], by coating them on the surfaces of filter paper
The adsorption capacity of verapamil on different MOFs is calculated by q = (C − C ) V/m, t t in which qt is the adsorption capacity, C0 and Ct are the concentrations of verapamil before and after adsorption, V is the volume of solution (L), and m is the mass of the used ZrO2 or MOFs (g)
The surface areas of different MOFs are extremely higher than that of ZrO2, the adsorption feature of the less porous ZrO2 is comparable to some, such as UiO-66(Zr) and UiO-66(Zr)-NH2 (Figure 1a). This case could be attributed to their various surface properties, leading to different interactions between verapamil and those materials
Summary
Metal–organic frameworks (MOFs) [1,2] have received considerable attention over the past decades and have been applied in diverse fields including gas storage [3,4], clean energy [5,6,7], purification [8,9], adsorption and separation [10,11,12,13,14,15,16], catalysis [17,18,19], sensors [20], supercapacitors [21]. Numerous important advances have been made in the investigation of the adsorption and desorption properties of various compounds on MOFs, but those studies are mainly focused on volatile compounds including H2 [25,26], CO and CO2 [27,28,29,30], NO [31], H2 O [32], benzene [33], toluene [34], 1,2-dichloroethane [35], and methanol [36] The performances of different MOFs with coated paper substrates have been compared in the elution or desorption of different therapeutic drugs and protein samples
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