Increased level of low-density lipoprotein (LDL) strongly correlates with incidence of coronary heart disease. We synthesized novel molecularly imprinted polymers (MIP) as biomimetic specific receptors to establish rapid analysis of LDL levels. For that purpose the ratios of monomers acrylic acid (AA), methacrylic acid (MAA), and N-vinylpyrrolidone (VP), respectively, were screened on 10 MHz dual-electrode quartz crystal microbalances (QCM). Mixing MAA and VP in the ratio 3:2 (m/m) revealed linear sensor characteristic to LDL cholesterol (LDL-C) from 4 to 400 mg/dL or 0.10-10.34 mmol/L in 100 mM phosphate-buffered saline (PBS) without significant interference: high-density lipoprotein (HDL) yields 4-6% of the LDL signal, very-low-density-lipoprotein (VLDL) yields 1-3%, and human serum albumin (HSA) yields 0-2%. The LDL-MIP sensor reveals analytical accuracy of 95-96% at the 95% confidence interval with precision at 6-15%, respectively. Human serum diluted 1:2 with PBS buffer was analyzed by LDL-MIP sensors to demonstrate applicability to real-life samples. The sensor responses are excellently correlated to the results of the standard technique, namely, a homogeneous enzymatic assay (R(2) = 0.97). This demonstrates that the system can be successfully applied to human serum samples for determining LDL concentrations.

This work presents a simple hydrothermal synthesis of nitrogen-doped carbon dots (N-CDs), fabrication of microfluidic paper-based analytical device (μPAD), and their joint application for colorimetric determination of total cholesterol (TC) in human blood. The N-CDs were characterized by various techniques including transmission electron microscopy (TEM), Xray photoelectron spectroscopy (XPS), and X-ray powder diffraction (XRD), and the optical and electronic properties of computational models were studied using the time-dependent density functional theory (TD-DFT). The characterization results confirmed the successful doping of nitrogen on the surface of carbon dots. The N-CDs exhibited high affinity toward 2,2′-azinobis(3-ethylbenzothiazoline-6-sulfonic acid)-diammonium salt (ABTS) with the Michaelis−Menten constant (K M ) of 0.018 mM in a test for their peroxidase-like activity. Particularly, since hydrogen peroxide (H 2 O 2 ) is the oxidative product of cholesterol in the presence of cholesterol oxidase, a sensitive and selective method of cholesterol detection was developed. Overall, the obtained results from TD-DFT confirm the strong adsorption of H 2 O 2 on the graphitic N positions of the N-CDs. The laminated three-dimensional (3D)-μPAD featuring a 6 mm circular detection zone was fabricated using a simple wax screen printing technique. Classification of TC according to the clinically relevant criteria (healthy, <5.2 mM; borderline, 5.2−6.2 mM; and high risk, >6.2 mM) could be determined by the naked eye within 10 min by simple comparison using a color chart. Overall, the proposed colorimetric device serves as a low-cost, rapid, simple, sensitive, and selective alternative for TC detection in whole blood samples that is friendly to unskilled end users.

Decreased blood level of high-density lipoprotein (HDL) is one of the essential criteria in diagnosing metabolic syndrome associated with the development of atherosclerosis and coronary heart disease. Herein, we report the synthesis of a molecularly imprinted polymer (MIP) that selectively binds HDL, namely, HDL-MIP, and thus serves as an artificial, biomimetic sensor layer. The optimized polymer contains methacrylic acid and N-vinylpyrrolidone in the ratio of 2:3, cross-linked with ethylene glycol dimethacrylate. On 10 MHz dual electrode quartz crystal microbalances (QCM), such HDL-MIP revealed dynamic detection range toward HDL standards in the clinically relevant ranges of 2–250 mg/dL HDL cholesterol (HDL-C) in 10 mM phosphate-buffered saline (PBS, pH = 7.4) without significant interference: low-density lipoprotein (LDL) yields 5% of the HDL signal, and both very-low-density lipoprotein (VLDL) and human serum albumin (HSA) yield 0%. The sensor reveals recovery rates between 94 and 104% at 95% confidence interval with precision of 2.3–7.7% and shows appreciable correlation (R 2 = 0.97) with enzymatic colorimetric assay, the standard in clinical tests. In contrast to the latter, it achieves rapid results (10 min) during one-step analysis without the need for sample preparation. Graphical Abstractᅟ

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Graphene oxide-molecularly imprinted polymer composites (GO-MIP) have attracted significant attention as recognition materials in sensing due to their outstanding properties in terms of electrical and thermal conductivity, high mechanical modulus, and the comparably straightforward way to functionalize them. The aim of this study was to design a MIP-based sensor recognition material and enhance its sensitivity by blending it with GO for sensing a harmful dengue hemorrhagic fever pathogen, namely the dengue type 1 virus (DENV-1). Polymer composites comprising GO incorporated to an acrylamide (AAM)/methacrylic acid (MAA)/methyl methacrylate (MMA)/N-vinylpyrrolidone (VP) copolymer were synthesized and compared to the “pure” MIP, i.e., the copolymer without GO. The pure polymer revealed a zeta potential of + 9.9 ± 0.5 mV, whereas GO sheets prepared have a zeta potential of − 60.3 ± 2.7 mV. This results in an overall zeta potential of − 11.2 ± 0.2 mV of the composite. Such polymer composites seem appropriate to bind the positively charged DENV-1 particle (+ 42.2 ± 2.8 mV). GO-MIP coated onto 10-MHz quartz crystal microbalance (QCM) sensors indeed revealed two times sensitivity compared to sensors based on the pure MIP. Furthermore, GO-polymer composites revealed imprinting factors of up to 21, compared to 3 of the pure MIP. When plotting the sensor characteristic in a semilogarithmic way, the composite sensor shows the linear response to DENV-1 in the concentration range from 100 to 103 pfu mL−1. The corresponding limits of detection (S/N = 3) and quantification (S/N = 10) are 0.58 and 1.94 pfu mL−1, respectively. Furthermore, imprinted polymer composites selectively bind DENV-1 without significant interference: DENV-2, DENV-3, DENV-4, respectively, yield 13–16% of DENV-1 signal. The sensor requires only about 15–20 min to obtain a result. Graphical abstract