Emerging water pollutants such as pharmaceutical contaminants are suspected to induce adverse effects to human health. These molecules became worrisome due to their increasingly high concentrations in surface waters. Despite this alarming situation, available data about actual concentrations in the environment is rather scarce, as it is not commonly monitored or regulated. This is aggravated even further by the absence of portable and reliable methods for their determination in the field. A promising way to tackle these issues is the use of enzyme-based and miniaturized biosensors for their electrochemical detection. Here, we present an overview of the latest developments in amperometric microfluidic biosensors that include, modeling and multiphysics simulation, design, manufacture, testing, and operation methods. Different types of biosensors are described, highlighting those based on oxidases/peroxidases and the integration with microfluidic platforms. Finally, issues regarding the stability of the biosensors and the enzyme molecules are discussed, as well as the most relevant approaches to address these obstacles.
Magnetite nanoparticles (MNPs) have attracted basic and applied research due to their immense potential to enable applications in fields as varied as drug delivery and bioremediation. Conventional synthesis schemes led to wide particle size distributions and inhomogeneous morphologies and crystalline structures. This has been attributed to the inability to control nucleation and growth processes under the conventional conditions of bulk batch processes. Here, we attempted to address these issues by scaling down the synthesis process aided by microfluidic devices, as they provide highly controlled and stable mixing patterns. Accordingly, we proposed three micromixers with different channel configurations, namely, serpentine, triangular, and a 3D arrangement with abrupt changes in fluid direction. The micromixers were first studied in silico, aided by Comsol Multiphysics® to investigate the obtained mixing patterns, and consequently, their potential for controlled growth and the nucleation processes required to form MNPs of uniform size and crystalline structure. The devices were then manufactured using a low-cost approach based on polymethyl methacrylate (PMMA) and laser cutting. Testing the micromixers in the synthesis of MNPs revealed homogeneous morphologies and particle size distributions, and the typical crystalline structure reported previously. A life cycle assessment (LCA) analysis for the devices was conducted in comparison with conventional batch co-precipitation synthesis to investigate the potential impacts on water and energy consumption. The obtained results revealed that such consumptions are higher than those of the conventional process. However, they can be reduced by conducting the synthesis with reused micromixers, as new PMMA is not needed for their assembly prior to operation. We are certain that the proposed approach represents an advantageous alternative to co-precipitation synthesis schemes, in terms of continuous production and more homogeneous physicochemical parameters of interest such as size, morphologies, and crystalline structure. Future work should be directed towards improving the sustainability indicators of the micromixers’ manufacturing process.
The use of micromixers and catalytically active nanocomposites can be an attractive alternative for the treatment of wastewaters from the textile industry, due to their high activity, low consumption of such nanocomposites, short reaction times and the possibility to work under continuous operation. In this study, 6 different designs of micromixers were modeled and evaluated for the treatment of wastewaters. Velocity profiles, pressure drops, and flows were analyzed and compared for the different devices under the same mixing conditions. In addition, Life cycle assessment (LCA) methodology was applied to determine their performance in terms of environmental impact. Considering the high environmental impact of water sources contaminated by dyes from the textile industry, it becomes critically important to determine when the proposed micromixers are a suitable alternative for their remediation. The LCA and operational efficiency studies results shown here provide a route for the design of novel wastewater treatment systems by coupling low-cost and high-performance micromixers.
In this work, the design, manufacture, and testing of three different magnetic microreactors based on torus geometries (i.e., one-loop, two-horizontal-loop, and two-vertical-loop) is explored to increase the enzyme-based transformation of dyes by laccase bio-nanocomposites, improve the particle suspension, and promote the interaction of reagents. The laccase enzyme was covalently immobilized on amino-terminated silanized magnetite nanoparticles (laccase-magnetite). The optimal configuration for the torus microreactor and the applied magnetic field was evaluated in silico with the aid of the CFD and particle tracing modules of Comsol Multiphysics®. Eriochrome Black T (EBt) dye was tested as a biotransformation model at three different concentrations, i.e., 5 mg/L, 10 mg/L, and 20 mg/L. Phenol oxidation/removal was evaluated on artificial wastewater and real wastewater. The optimal catalytic performance of the bionanocomposite was achieved in the range of pH 4 to 4.5. A parabolic movement on the particles along the microchannels was induced by the magnetic field, which led to breaking the stability of the laminar flow and improving the mixing processes. Based on the simulation and experiments conducted with the three geometries, the two-vertical-loop microreactor demonstrated a better performance mainly due to larger dead zones and a longer residence time. Additionally, the overall dye removal efficiencies for this microreactor and the laccase-magnetite bionanocomposite were 98.05%, 93.87%, and 92.74% for the three evaluated concentrations. The maximum phenol oxidation with the laccase-magnetite treatment at low concentration for the artificial wastewater was 79.89%, while its phenol removal efficiency for a large volume of real wastewater was 17.86%. Treatments with real wastewater were carried out with a larger volume, equivalent to 200 biotransformation (oxidation) operating cycles of those carried out with dyes or phenol. Taken together, our results indicate that the novel microreactors introduced here have the potential to process wastewaters rich in contaminant dyes in continuous mode with efficiencies that are attractive for a potential large-scale operation. In this regard, future work will focus on finding the requirements for scaling-up the processes and evaluating the involved environmental impact indexes, economic performance, and different device geometries and processing schemes.
Magnetite-based nanocomposites are used for biomedical, industrial, and environmental applications. In this study, we evaluated their effects on survival, malformation, reproduction, and behavior in a zebrafish animal model. Nanoparticles were synthesized by chemical coprecipitation and were surface-functionalized with (3-aminopropyl) triethoxysilane (APTES), L-cysteine (Cys), and 3-(triethoxysilyl) propylsuccinic anhydride (CAS). All these nanocomposites were designed for the treatment of wastewater. Zebrafish embryos at 8 h post-fertilization (hpf) and larvae at 4 days post-fertilization (dpf) were exposed to the magnetic nanocomposites Fe3O4 MNP (magnetite), MNP+APTES, MNP+Cys, MNP+APTES+Cys, and MNP+CAS, at concentrations of 1, 10, 100, and 1000 µg/mL. Zebrafish were observed until 13 dpf, registering daily hatching, survival, and malformations. Behavior was tested at 10 dpf for larvae, and reproduction was analyzed later in adulthood. The results showed that the toxicity of the nanocomposites used were relatively low. Exploratory behavior tests showed no significant changes. Reproduction in adults treated during development was not affected, even at concentrations above the OECD recommendation. Given the slight effects observed so far, these results suggest that nanocomposites at the concentrations evaluated here could be a viable alternative for water remediation because they do not affect the long-term survival and welfare of the animals.
This work studied the feasibility of using a novel microreactor based on torus geometry to carry out a sample pretreatment before its analysis by graphite furnace atomic absorption. The miniaturized retention of total arsenic was performed on the surface of a magnetic sorbent material consisting of 6 mg of magnetite (Fe3O4) confined in a very small space inside (20.1 µL) a polyacrylate device filling an internal lumen (inside space). Using this geometric design, a simulation theoretical study demonstrated a notable improvement in the analyte adsorption process on the solid extractant surface. Compared to single-layer geometries, the torus microreactor geometry brought on flow turbulence within the liquid along the curvatures inside the device channels, improving the efficiency of analyte–extractant contact and therefore leading to a high preconcentration factor. According to this design, the magnetic solid phase was held internally as a surface bed with the use of an 8 mm-diameter cylindric neodymium magnet, allowing the pass of a fixed volume of an arsenic aqueous standard solution. A preconcentration factor of up to 60 was found to reduce the typical “characteristic mass” (as sensitivity parameter) determined by direct measurement from 53.66 pg to 0.88 pg, showing an essential improvement in the arsenic signal sensitivity by absorption atomic spectrometry. This methodology emulates a miniaturized micro-solid-phase extraction system for flow-through water pretreatment samples in chemical analysis before coupling to techniques that employ reduced sample volumes, such as graphite furnace atomic absorption spectroscopy.
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