Persona: González Crevillén, Agustín
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0000-0002-4470-6502
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González Crevillén
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Publicación Disposable Passive Electrochemical Microfluidic Device for Diagnosis of Congenital Disorders of Glycosylation(European Chemical Societies Publishing, 2021-10-25) Sierra, Tania; Henry, Charles S.; González Crevillén, Agustín; Escarpa, AlbertoA disposable pump-free electrochemical microfluidic device made by using a multilayer lamination technique is proposed for diagnosis of glycosylation disorders. Thanks to the stacking of polyethylene terephthalate (PET) films and double adhesive layers, it is possible to create a geometry that allows the filling of the tailored channels in a fixed time. In the main channel of this passive microfluidic device, the necessary steps to perform the electrochemical determination of transferrin are performed: labeling of the protein with Os (VI) complex (electrochemical tag), washing with water of the osmium residues and electrochemical detection by adsorptive transfer stripping square wave voltammetry. Electrochemical detection released two electrochemical signals: one from Os (VI) complex due to carbohydrates at 0.9 V, and other from the intrinsic electrochemical signal of glycoprotein due to the amino acids at + 0.8 V. The ratio between them establishes an indicator of the degree of glycosylation (called electrochemical index of glycosylation). The method was successfully applied to the analysis of clinical samples from patients with congenital disorders of glycosylation.Publicación Electrochemically Reduced Graphene Oxide-Based Screen-Printed Electrodes for Total Tetracycline Determination by Adsorptive Transfer Stripping Differential Pulse Voltammetry(MDPI, 2019-12-21) S. Lorenzetti, Anabela; Sierra, Tania; Domini, Claudia E.; Lista, Adriana G.; González Crevillén, Agustín; Escarpa, AlbertoDisposable electrochemically reduced graphene oxide-based (ERGO) screen-printed electrodes (SPE) were developed for the determination of total tetracyclines as a sample screening approach. To this end, a selective adsorption-detection approach relied on adsorptive transfer stripping differential pulse voltammetry (AdTDPV) was devised, where the high adsorption capacity and the electrochemical properties of ERGO were simultaneously exploited. The approach was very simple, fast (6 min.), highly selective by combining the adsorptive and the electrochemical features of tetracyclines, and it used just 10 μL of the sample. The electrochemical sensor applicability was demonstrated in the analysis of environmental and food samples. The not-fully explored AdTDPV analytical possibilities on disposable nanostructured transducers become a new tool in food and environmental fields; drawing new horizons for “in-situ” analysis.Publicación Gold nanostructure-related non-plasmon resonance absorption band as a fingerprint of ortho-alkyl substituted phenolic compounds(Elsevier, 2021-08-29) Silvia Dortez; Maria Cristina González; González Crevillén, Agustín; Alberto EscarpaA systematic study for correlating the chemical structure of phenolic compounds with their capacity to form gold nanoparticles was carried out. Two groups of phenolic compounds were selected: one group with a substituent with different size at ortho position respect to hydroxyl group (phenol, o-cresol, 2-ethylphenol, 2-iso-propylphenol, 2-tert-butylphenol and 2-methoxyphenol); and the second group consists of phenolic compounds with the same substituent (methyl) at different positions respect to hydroxyl group (o-cresol, m-cresol and p-cresol). In addition to the characteristic gold nanoparticles (AuNPs) formation band at 550 nm obtained for all the structures of phenolic compounds studied, ortho-alkyl substituted yielded selectively a metastable band at 400 nm, due to gold nanoclusters (AuNCs) formation. We hypothesized that these specific phenolic compounds can temporally stabilize AuNCs with number of Au atoms ranging from 3 to 41. This new band was proposed for rapid screening of these phenolics with promising results, paving the way to new and more selective colorimetric assay for phenolic compounds determination.Publicación Cost-effective fully 3D-printed on-drop electrochemical sensor based on carbon black/polylactic acid: a comparative study with screen-printed sensors in food analysis(Springer, 2024) Monago Maraña, Olga; Aouladtayib-Boulakjar, Nadia; Zapardiel Palenzuela, Antonio; García Domínguez, Amabel; Ayllón Pérez, Jorge; Rodríguez Prieto, Álvaro; Claver Gil, Juan; Camacho López, Ana María; González Crevillén, Agustín3D-printing technology allows scientist to fabricate easily electrochemical sensors. Until now, these sensors were designed employing a large amount of material, which increases the cost and decreases manufacturing throughput. In this work, a low-cost 3D-printed on-drop electrochemical sensor (3D-PES) was fully manufactured by fused filament fabrication, minimizing the number of printing layers. Carbon black/polylactic acid filament was employed, and the design and several printing parameters were optimized to yield the maximum electroanalytical performance using the minimal amount of material. Print speed and extrusion width showed a critical influence on the electroanalytical performance of 3D-PES. Under optimized conditions, the fabrication procedure offered excellent reproducibility (RSD 1.3% in working electrode diameter), speed (< 3 min/unit), and costs (< 0.01 $ in material cost). The 3D-PES was successfully applied to the determination of phloridzin in apple juice. The analytical performance of 3D-PES was compared with an equivalent commercial on-drop screen-printed electrode, yielding similar precision and accuracy but lower sensitivity. However, 3D-PES provides interesting features such as recyclability, biodegradability, low-cost, and the possibility of being manufactured near the point of need, some of which meets several demands of Green Chemistry. This cost-effective printing approach is a green and promising alternative for manufacturing disposable and portable electroanalytical devices, opening new possibilities not only in on-site food analysis but also in point-of-care testing.Publicación Effect of nanocellulose polymorphism on electrochemical analytical performance in hybrid nanocomposites with non‑oxidized single‑walled carbon nanotubes(Springer, 2022-06-14) Dortez, Silvia; Sierra, Tania; Álvarez‑Sánchez, Miguel Á.; González‑Domínguez, José M.; Benito, Ana M.; Maser, Wolfgang K.; González Crevillén, Agustín; Escarpa, AlbertoTwo cellulose nanocrystals/single-walled carbon nanotube (CNC/SW) hybrids, using two cellulose polymorphs, were evaluated as electrochemical transducers: CNC type I (CNC-I/SW) and CNC type II (CNC-II/SW). They were synthesized and fully characterized, and their analytical performance as electrochemical sensors was carefully studied. In comparison with SWCNT-based and screen-printed carbon electrodes, CNC/SW sensors showed superior electroanalytical performance in terms of sensitivity and selectivity, not only in the detection of small metabolites (uric acid, dopamine, and tyrosine) but also in the detection of complex glycoproteins (alpha-1-acid glycoprotein (AGP)). More importantly, CNC-II/SW exhibited 20 times higher sensitivity than CNC-I/SW for AGP determination, yielding a LOD of 7 mg L −1 .These results demonstrate the critical role played by nanocellulose polymorphism in the electrochemical performance of CNC/SW hybrid materials, opening new directions in the electrochemical sensing of these complex molecules. In general, these high-active-surface hybrids smartly exploited the preserved non-oxidized SW conductivity with the high aqueous dispersibility of the CNC, avoiding the use of organic solvents or the incorporation of toxic surfactants during their processing, making the CNC/SW hybrids promising nanomaterials for electrochemical detection following greener approaches.Publicación Disposable electrochemical sensor combined with molecularly imprinted solid-phase extraction for catabolites detection of flavan-3-ol in urine samples(Elsevier, 2021-07-26) Mora-Granados, M.; González Crevillén, Agustín; González-Gómez D.; Gallego-Picó, A.; https://orcid.org/0000-0002-6167-6106; https://orcid.org/0000-0002-3321-9290Polyphenols are bioactive substances of vegetal origin with a significant impact on human health. The assessment of polyphenol intake and excretion is therefore important. In this work, a new electrochemical approach based on molecularly imprinted polymer extraction and preconcentration, combined with a disposable carbon screen-printed sensor and adsorptive transfer differential pulse voltammetry detection has been proposed for quantifying of 4-hydroxyphenylacetic acid (4-HPA), which is a biomarker of flavan-3-ols intake, and other phenolic acids. The simple experimental performance has allowed the rapid data collection with relevant information about the profile of catabolites extracted. The method was validated over a concentration range of 10–200 mg L−1, R2 > 0.999. In the optimized conditions, the recovery value was 94% with RSD 8%. The limits of detection and quantification were 2.38 mg L−1 and 7.21 mg L−1, respectively. The method was validated by means of a chromatographic method, being the differences between the values of the 4-HPA concentrations obtained by both methods under 1%. The proposed method showed high recoveries, low detection limit, and good accuracy, providing a fast, reliable, and cheap procedure to quantify phenolic metabolites in urine, and representing therefore a good and interesting alternative method. Also, the procedure offers other advantages, including the miniaturization, the low use of organic solvents, the ability to analyse small volumes of samples, in situ analysis and simple instrumentation requirement.Publicación Electrochemical sensor for the assessment of carbohydrate deficient transferrin: Application to diagnosis of congenital disorders of glycosilation(Elsevier, 2021-05) Tania Sierra; González Crevillén, Agustín; Escarpa Miguel, Jesús Alberto; https://orcid.org/0000-0002-7302-0948Carbohydrate deficient transferrin (CDT) is used as biomarker of different health problems as, for example, congenital disorders of glycosylation (CDG). We propose a screen-printed-based electrochemical sensor for the determination of carbohydrate deficient transferrin using an Os (VI) tag-based electrochemistry. When transferrin is labeled with Os (VI) complex, it generates two voltammetric signals: one from carbohydrates (electrochemical signal of osmium (VI) complex at -0.9 V/Ag) and one from the amino acids present in glycoprotein (intrinsic electrochemical signal of glycoprotein at +0.8 V/Ag). The relationship between the two analytical signals (carbohydrate signal/protein signal) is an indicator of the degree of glycosylation (electrochemical index of glycosylation), which has shown an excellent correlation (r = 0.990) with the official parameter %CDT obtained by CE-UV. The suitability of this approach was demonstrated by analyzing serum samples from CDG patients.Publicación 3D-printed Transmembrane Glycoprotein Cancer Biomarker Aptasensor(Elsevier, 2021-08-21) González Crevillén, Agustín; Mayorga Martinez, Carmen C.; Zelenka, Jaroslav; Rimpelová, Silvie; Ruml, Tomáš; Pumera, MartinPoint-of-care, easy to manufacture, and low cost detection of cancer biomarkers is crucial for fighting the early stage disease. 3D printing allows delocalized printing at remote locations with updates/upgrades available globally via electronic files. Mucin 1 (MUC1) is a protein that is overexpressed in a number of epithelial cancers and is a key factor in advancement of the disease. Here we show the simple point-of-care 3D printing fabrication of a MUC1 aptasensor using a nanocarbon/polymer filament. Efficacy of the 3D-printed aptasensor is demonstrated by monitoring the expression and release of MUC1 in breast cancer cell cultures. Such a simple, low cost, and easy to locally fabricate cancer biosensor will have a large impact on the field of cancer diagnostics.Publicación 3D-Printed SARS-CoV-2 RNA Genosensing Microfluidic System(Wiley, 2022-02-05) González Crevillén, Agustín; Mayorga-Martinez, Carmen C.; Vaghasiya, Jayraj V.; Martin PumeraAdditive manufacturing technology, referred as 3D printing technology, is a growing research field with broad applications from nanosensors fabrication to 3D printing of buildings. Nowadays, the world is dealing with a pandemic and requires the use of simple sensing systems. Here, the strengths of fast screening by a lab-on-a-chip device through electrochemical detection using 3D printing technology for SARS-CoV-2 sensing are combined. This system comprises a PDMS microfluidic channel integrated with an electrochemical cell fully 3D-printed by a 3D printing pen (3D-PP). The 3D-PP genosensor is modified with an ssDNA probe that targeted the N gene sequence of SARS-CoV-2. The sensing mechanism relies on the electro-oxidation of adenines present in ssDNA when in contact with SARS-CoV-2 RNA. The hybridization between ssDNA and target RNA takes a place and ssDNA is desorbed from the genosensor surface, causing a decrease of the sensor signal. The developed SARS-CoV-2/3D-PP genosensor shows high sensitivity and fast response.Publicación Pump-Free Microfluidic Device for the Electrochemical Detection of α1-Acid Glycoprotein(American Chemical Society Publications, 2021-07-05) Tania, Sierra; Jang, Ilhoon; Noviana, Eka; González Crevillén, Agustín; Escarpa, Alberto; S. Henry, Charlesα1-Acid glycoprotein (AGP) is a glycoprotein present in serum, which is associated with the modulation of the immune system in response to stress or injuries, and a biomarker for inflammatory diseases and cancers. Here, we propose a pump-free microfluidic device for the electrochemical determination of AGP. The microfluidic device utilizes capillary-driven flow and a passive mixing system to label the AGP with the Os (VI) complex (an electrochemical tag) inside the main channel, before delivering the products to the electrode surface. Furthermore, thanks to the resulting geometry, all the analytical steps can be carried out inside the device: labeling, washing, and detection by adsorptive transfer stripping square wave voltammetry. The microfluidic device exhibited a linear range from 500 to 2000 mg L–1 (R2 = 0.990) and adequate limit of detection (LOD = 231 mg L–1). Commercial serum samples were analyzed to demonstrate the success of the method, yielding recoveries around 83%. Due to its simplicity, low sample consumption, low cost, short analysis time, disposability, and portability, the proposed method can serve as a point-of-care/need testing device for AGP.