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Highlights  Examining microstructured sensing areas of interferometric biosensors on silicon chip  Step-by-step surface modifications determined with biomolecular discrimination  Surface density of probe, blocking protein, primary and secondary antibody evaluated  Desorption upon primary immunoreaction depends on spotting concentration of probe  Binding stoichiometry evaluated more accurately than estimated from sensor response

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Estimation of glucose (GLU) levels in the human organism is very important in the diagnosis and monitoring of diabetes. Scientific advances in nanomaterials have led to the construction of new generations of enzymatic-free GLU sensors. In this work, an innovative 3D-printed device modified with a water-stable and non-toxic metal–organic framework of iron (Fe(II)-MOF), which serves as a nanozyme, has been developed for the voltammetric determination of GLU in artificial sweat. In contrast to existing MOF-based GLU sensors which exhibit electrocatalytic activity for the oxidation of GLU in alkaline media, the nanozyme Fe(II)-MOF/3D-printed device can operate in the acidic epidermal sweat environment. The enzymatic-free GLU sensor is composed of a 3-electrode 3D-printed device with the MOF nanozyme immobilized on the surface of the working electrode. GLU sensing is conducted by differential pulse voltammetry without interference from other co-existing metabolites in artificial sweat. The response is based on the oxidation of glucose to gluconolactone, induced by the redox activity of the Fe-centers of the MOF. GLU gives rise to an easily detectable and well-defined voltammetric peak at about − 1.2 V and the limit of detection is 17.6 μmol L-1. The synergy of a nanozyme with 3D printing technology results in an advanced, sensitive, and low-cost sensor, paving the way for on-skin applications. Graphical abstract

This work reports the development and optimization of a rapid and low-cost pen-on-paper plotting approach for the fabrication of paper-based analytical devices (PADs) using commercial writing stationery. The desired fluidic patterns were drawn on the paper substrate with commercial marker pens using an inexpensive computer-controlled x–y plotter. For the fabrication of electrochemical PADs, electrodes were further deposited on the devices using a second x–y plotting step with commercial writing pencils. The effect of the fabrication parameters (type of paper, type of marker pen, type of pencil, plotting speed, number of passes, single- vs. double-sided plotting), the chemical resistance of the plotted devices to different solvents and the structural rigidity to multiple loading cycles were assessed. The analytical utility of these devices is demonstrated through application in optical sensing of total phenols using reflectance calorimetry and in electrochemical sensing of paracetamol and ascorbic acid. The proposed manufacturing approach is simple, low cost, flexible, rapid and fit-for-purpose and enables the fabrication of sub-“one-dollar” PADs with satisfactory mechanical and chemical resistance and good analytical performance.

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