Integrated paper/graphene 3D pop-up device for the quantitative sensing of carbaryl

Abstract

A completely lab-made paper/graphene-based 3D pop-up device (3D-PP) for the analysis of carbaryl (CBR), a pesticide widely used in crop production, is proposed. The device is composed of a nitrocellulose sensor equipped with reduced graphene oxide (rGO) and a foldable 3D paper pop-up. The rationale of the device is based on 3D and 2D configurations to allow the whole analytical procedure. In the 3D arrangement sample pre-concentration and hydrolysis occur; after folding (2D), contact with the complementary nitrocellulose-based sensor is ensured. The sensor, constituted by nanostructured graphene film, allows to obtain the necessary electroanalytical performance. 3D-PP has been shaped and nanostructured using a CO2-laser plotter and finished using low-cost benchtop instruments, ensuring in-series manufacturing of the device modules. 3D-PP includes the main steps required for CBR determination, i.e. (i) pre-concentration/purification, (ii) hydrolysis, (iii) medium neutralization, and (iv) electrochemical detection. 3D-PP was challenged for CBR quantification in model solutions and different grain samples. The response linearity (1.5–33 μM) and LOD (0.4 μM) obtained ensures CBR determination at the European-law admitted maximum residue levels (MRL). As proof of applicability, to simulate contaminates samples, different grains (i.e. soft and durum wheat, kamut, and barley) were spiked, before extraction, with CBR at three concentration levels corresponding to 0.5x, 1x, and 1.5x MRL; in all cases, quantitative and reproducible recoveries were obtained (93–109%; RSD ≤ 6%, n = 3). 3D-PP is produced using cellulosic components and solvent-free approaches, includes all CBR analysis steps, and returns reliable results in 15 min, resulting portable and usable with a smartphone