Non-enzymatic electrochemical cholesterol sensor based on strong host-guest interactions with a polymer of intrinsic microporosity (PIM) with DFT study

Abstract

Advances in materials science has accelerated the development of diagnostic tools with the last decade witnessing the development of enzyme-free sensors, owing to the improved stability, low cost, and simple fabrication of component materials. However, the specificity of non-enzymatic sensors for certain analytes still represents a challenging task, for example, the determination of cholesterol level in blood is vital due to its medical relevance. In this work, a reagent displacement assay for cholesterol sensing in serum samples was developed. It is based on coating of a glassy carbon electrode with a polymer of intrinsic micro-porosity (PIM) that forms a host-guest complex with methylene blue (MB). In the presence of cholesterol, the MB electroactive probe was displaced due to the stronger association of cholesterol guest to the PIM host. The decrease in the oxidative current was proportional to the cholesterol concentration achieving a detection limit of approximately 0.1 nM.

PIM-1/Holey Graphene Oxide Mixed Matrix Membranes for Gas Separation: Unveiling the Role of Holes

“…Hence, physical aging is the main limitation for their use in industrial separations . Apart from gas separation membranes, PIMs and PIMs-based composite materials also have a strong potential for a large number of applications, among many others water treatment, energy storage, redox flow batteries, fuel cells, H 2 storage, breathable materials, and sensors . More specifically, PIM-1/graphene materials have been reported for membrane pervaporation, , hydrogels for environmental remediation, and substrates/promoters for catalysis and for sensing …”

“…14 Apart from gas separation membranes, PIMs and PIMs-based composite materials also have a strong potential for a large number of applications, among many others water treatment, 15 energy storage, 16 redox flow batteries, 16 fuel cells, 16 H 2 storage, 17 breathable materials, 18 and sensors. 19 More specifically, PIM-1/graphene materials have been reported for membrane pervaporation, 20,21 hydrogels for environmental remediation, 22 and substrates/promoters for catalysis and for sensing. 23 A common strategy to enhance the gas separation performance of PIM-1 membranes is the use of fillers and the formation of what is known as mixed-matrix membranes (MMMs).…”

Polymers of Intrinsic Microporosity Based on Dibenzodioxin Linkage: Design, Synthesis, Properties, and Applications

“…[19] Apart from fluorometric and colorimetric changes, electrochemical sensing of cholesterol, an important molecule in biology, has been performed by utilizing the guest inclusion property of PIM-1. [126] In this approach, PIM-1 coated glassy carbon electrode was used as the sensor, and the change in electrochemical response in the electrode was recorded as a function of change in host-guest chemistry of the PIM. Upon exposing the electrode to a solution of cationic dye MB, the dye gets adsorbed on the PIM surface.…”

“…Because of rapid and efficient sensing ability, this method has been adopted for industrial application as well [19] . Apart from fluorometric and colorimetric changes, electrochemical sensing of cholesterol, an important molecule in biology, has been performed by utilizing the guest inclusion property of PIM‐1 [126] . In this approach, PIM‐1 coated glassy carbon electrode was used as the sensor, and the change in electrochemical response in the electrode was recorded as a function of change in host–guest chemistry of the PIM.…”

Polymers of intrinsic microporosity (PIMs) in sensing and in electroanalysis

“…Molecular electrocatalysts (water-insoluble TEMPO derivatives) as guest species in PIM-EA-TB deposited onto carbon electrodes [30] were shown to oxidise aliphatic and aromatic alcohols (Figure 3). Recently, films of PIM-1 deposited onto a carbon electrode were studied for cholesterol detection [31]. The electrochemical response was induced by methylene blue adsorbed to the microporous polymer surface.…”