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7. Methylene Blue functionalized carbon nanodots combined with different shape gold nanostructures for sensitive and selective SARS-CoV-2 sensing

Author

Pina-Coronado, Clara, Martínez-Sobrino, Álvaro, Gutiérrez-Gálvez, Laura, Del Caño, Rafael, Martínez-Periñán, Emiliano, García-Nieto, Daniel, Rodríguez-Peña, Micaela, Luna, M., Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Somoza, Álvaro, García-Mendiola, Tania, Miranda, Rodolfo, and Lorenzo, Encarnación

Published
2022
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13. Compelling DNA intercalation through 'anion–anion' anti-coulombic interactions: boron cluster self-vehicles as promising anticancer agents.

Author

Gutiérrez-Gálvez, Laura, García-Mendiola, Tania, Lorenzo, Encarnación, Nuez-Martinez, Miquel, Ocal, Carmen, Yan, Shunya, Teixidor, Francesc, Pinheiro, Teresa, Marques, Fernanda, and Viñas, Clara

Abstract

Anticancer drugs inhibit DNA replication by intercalating between DNA base pairs, forming covalent bonds with nucleotide bases, or binding to the DNA groove. To develop safer drugs, novel molecular structures with alternative binding mechanisms are essential. Stable boron hydrides offer a promising alternative for cancer therapy, opening up additional options like boron neutron capture therapy based on 10B and thermal neutron beams or proton boron fusion therapy using 11B and proton beams. These therapies are more efficient when the boron compound is ideally located inside cancer cells, particularly in the nucleus. Current cancer treatments often utilize small, polycyclic, aromatic, planar molecules that intercalate between ds-DNA base pairs, requiring only a spacing of approximately 0.34 nm. In this paper, we demonstrate another type of intercalation. Notably, [3,3′-Fe(1,2-C2B9H11)2]−, ([o-FESAN]−), a compact 3D molecule measuring 1.1 nm × 0.6 nm, can as well intercalate by strong non-bonding interactions preferentially with guanine. Unlike known intercalators, which are positive or neutral, [o-FESAN]− is a negative species and when an [o-FESAN]− molecule approaches the negatively charged DNA phosphate chain an anion–anion interaction consistently anti-electrostatic via Ccluster–H⋯O–P bonds occurs. Then, when more molecules approach, an elongated outstandingly self-assembled structure of [o-FESAN]−–[o-FESAN]− forms moving anions towards the interthread region to interact with base pairs and form aggregates of four [o-FESAN]− anions per base pair. These aggregates, in this environment, are generated by Ccluster–H⋯O–C, N–H⋯H–B and Ccluster–H⋯H–B interactions. The ferrabis(dicarbollide) boron-rich small molecules not only effectively penetrate the nucleus but also intercalate with ds-DNA, making them promising for cancer treatment. This amphiphilic anionic molecule, used as a carrier-free drug, can enhance radiotherapy in a multimodal perspective, providing healthcare professionals with improved tools for cancer treatment. This work demonstrates these findings with a plethora of techniques. [ABSTRACT FROM AUTHOR]

Published
2024
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15. Amplification-free detection of SARS-CoV-2 using gold nanotriangles functionalized with oligonucleotides

Author

del Caño, Rafael, García-Mendiola, Tania, García-Nieto, Daniel, Álvaro, Raquel, Luna, Mónica, Iniesta, Hernán Alarcón, Coloma, Rocío, Diaz, Ciro Rodríguez, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Miranda, Rodolfo, Somoza, Álvaro, and Lorenzo, Encarnación

Published
2022
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16. Rapid and simple viral protein detection by functionalized 2D MoS2/graphene electrochemiluminescence aptasensor

Author

Agencia Estatal de Investigación (España), Ministerio de Ciencia, Innovación y Universidades (España), Comunidad de Madrid, Ministerio de Ciencia e Innovación (España), European Commission, Ministerio de Economía y Competitividad (España), López-Diego, David [0009-0003-0396-1077], Luna, Mónica [0000-0002-7104-0726], Gutiérrez-Gálvez, Laura, El Hajioui-El Ghalbzouri, Hanaa, Enebral-Romero, Estefanía, Garrido, Marina, Naranjo, Alicia, López-Diego, David, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, Lorenzo, Encarnación, Agencia Estatal de Investigación (España), Ministerio de Ciencia, Innovación y Universidades (España), Comunidad de Madrid, Ministerio de Ciencia e Innovación (España), European Commission, Ministerio de Economía y Competitividad (España), López-Diego, David [0009-0003-0396-1077], Luna, Mónica [0000-0002-7104-0726], Gutiérrez-Gálvez, Laura, El Hajioui-El Ghalbzouri, Hanaa, Enebral-Romero, Estefanía, Garrido, Marina, Naranjo, Alicia, López-Diego, David, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, and Lorenzo, Encarnación

Abstract

In this work we present the development of an electrochemiluminescence aptasensor based on electrografting molybdenum disulphide nanosheets functionalized with diazonium salt (MoS2-N2+) upon screen-printed electrodes of graphene (SPEs GPH) for viral proteins detection. In brief, this aptasensor consists of SPEs GPH electrografted with MoS2-N2+ and modified with a thiolated aptamer, which can specifically recognize the target protein analyte. In this case, we have used SARS-CoV-2 spike protein as model protein. Electrochemiluminescence detection was performed by using the [Ru(bpy)3]2+/TPRA (tripropylamine) system, which allows the specific detection of the SARS-CoV-2 spike protein easily and rapidly with a detection limit of 9.74 fg/mL and a linear range from 32.5 fg/mL to 50.0 pg/mL. Moreover, the applicability of the aptasensor has been confirmed by the detection of the protein directly in human saliva samples. Comparing our device with a traditional saliva antigen test, our aptasensor can detect the spike protein even when the saliva antigen test gives a negative result.

Published
2024

20. Multiplex Portable Biosensor for Bacteria Detection

Author

Kaci, Karim, primary, Enebral-Romero, Estefanía, additional, Martínez-Periñán, Emiliano, additional, Garrido, Marina, additional, Pérez, Emilio M., additional, López-Diego, David, additional, Luna, Mónica, additional, González-de-Rivera, Guillermo, additional, García-Mendiola, Tania, additional, and Lorenzo, Encarnación, additional

Published
2023
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23. Multiplex Portable Biosensor for Bacteria Detection

Author

Enebral- Romero, Estefania, primary, Kaci, Karim, additional, Martinez-Periñan, Emiliano, additional, Garrido, Marina, additional, Pérez, Emilio, additional, López-Diego, David, additional, Luna, Monica, additional, González-de-Rivera, Guillermo, additional, García-Mendiola, Tania, additional, and Lorenzo, Encarnación, additional

Published
2023
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25. Electrochemiluminescent nanostructured DNA biosensor for SARS-CoV-2 detection

Author

Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Fundación Instituto Madrileño de Estudios Avanzados en Nanociencia, Banco Santander, Universidad Autónoma de Madrid, Conferencia de Rectores de las Universidades Españolas, Consejo Superior de Investigaciones Científicas (España), Caño, Rafael del [0000-0001-8762-8455], García-Nieto, Daniel [0000-0002-3006-0114], Luna, Mónica [0000-0002-7104-0726], García-Mendiola, Tania [0000-0002-7634-5844], Gutiérrez-Gálvez, Laura, Caño, Rafael del, Menéndez-Luque, Iris, García-Nieto, Daniel, Rodríguez-Peña, Micaela, Luna, Mónica, Pineda, Teresa, Pariente, Félix, García-Mendiola, Tania, Lorenzo, Encarnación, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Fundación Instituto Madrileño de Estudios Avanzados en Nanociencia, Banco Santander, Universidad Autónoma de Madrid, Conferencia de Rectores de las Universidades Españolas, Consejo Superior de Investigaciones Científicas (España), Caño, Rafael del [0000-0001-8762-8455], García-Nieto, Daniel [0000-0002-3006-0114], Luna, Mónica [0000-0002-7104-0726], García-Mendiola, Tania [0000-0002-7634-5844], Gutiérrez-Gálvez, Laura, Caño, Rafael del, Menéndez-Luque, Iris, García-Nieto, Daniel, Rodríguez-Peña, Micaela, Luna, Mónica, Pineda, Teresa, Pariente, Félix, García-Mendiola, Tania, and Lorenzo, Encarnación

Abstract

This work focuses on the development of an electrochemiluminescent nanostructured DNA biosensor for SARS-CoV-2 detection. Gold nanomaterials (AuNMs), specifically, a mixture of gold nanotriangles (AuNTs) and gold nanoparticles (AuNPs), are used to modified disposable electrodes that serve as an improved nanostructured electrochemiluminescent platform for DNA detection. Carbon nanodots (CDs), prepared by green chemistry, are used as coreactants agents in the [Ru(bpy)3]2+ anodic electrochemiluminescence (ECL) and the hybridization is detected by changes in the ECL signal of [Ru(bpy)3]2+/CDs in combination with AuNMs nanostructures. The biosensor is shown to detect a DNA sequence corresponding to SARS-CoV-2 with a detection limit of 514 aM.

Published
2022

28. Supplementary Material MoS2-Carbon Nanodots as New Electrochemiluminescence Platform for Breast Cancer Biomarker Detection

Author

Gutiérrez-Gálvez, Laura, Vázquez Sulleiro, Manuel, Gutiérrez-Sánchez, Cristina, García-Nieto, Daniel, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, Lorenzo, Encarnación, Gutiérrez-Gálvez, Laura, Vázquez Sulleiro, Manuel, Gutiérrez-Sánchez, Cristina, García-Nieto, Daniel, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, and Lorenzo, Encarnación

Published
2023

29. Multiplex Portable Biosensor for Bacteria Detection

Author

Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Ciencia e Innovación (España), Comunidad de Madrid, Ministerio de Economía y Competitividad (España), European Commission, Kaci, Karim, Enebral-Romero, Estefanía, Martínez-Periñán, Emiliano, Garrido, Marina, Pérez, Emilio M., López-Diego, David, Luna, Mónica, González de Rivera, Guillermo, García-Mendiola, Tania, Lorenzo, Encarnación, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Ciencia e Innovación (España), Comunidad de Madrid, Ministerio de Economía y Competitividad (España), European Commission, Kaci, Karim, Enebral-Romero, Estefanía, Martínez-Periñán, Emiliano, Garrido, Marina, Pérez, Emilio M., López-Diego, David, Luna, Mónica, González de Rivera, Guillermo, García-Mendiola, Tania, and Lorenzo, Encarnación

Abstract

An advanced, cost-effective, and portable DNA biosensor capable of detecting multiple bacteria simultaneously has been developed. The biosensor comprises a fast and inexpensive potentiostat that controls the applied potential to a screen-printed electrochemical array platform functionalized with MoS2 flakes and bacterial DNA probes. The current response obtained by à la carte thionine functionalized carbon nanodots (Ty-CDs) is monitored as an electrochemical indicator of the hybridization event. The design of the potentiostat prioritizes achieving an optimal signal-to-noise ratio and incorporates a user-friendly interface compatible with various devices, including computers, mobile phones, and tablets. The device is compact, lightweight, and manufactured at a low cost. The key components of the potentiostat include a data acquisition board capable of analyzing multiple samples simultaneously and a controller board. The results of this study confirm the ability of the multiplex portable biosensor to successfully detect specific bacterial DNA sequences, demonstrating its reliability and superior performance compared with a traditional, more complex, and laboratory-oriented potentiostat.

Published
2023

30. MoS2-Carbon nanodots as a new electrochemiluminescence platform for breast cancer biomarker detection

Author

Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Comunidad de Madrid, Consejo Superior de Investigaciones Científicas (España), European Commission, Ministerio de Ciencia e Innovación (España), Gutiérrez-Gálvez, Laura, Vázquez Sulleiro, Manuel, Gutiérrez-Sánchez, Cristina, García-Nieto, Daniel, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, Lorenzo, Encarnación, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Comunidad de Madrid, Consejo Superior de Investigaciones Científicas (España), European Commission, Ministerio de Ciencia e Innovación (España), Gutiérrez-Gálvez, Laura, Vázquez Sulleiro, Manuel, Gutiérrez-Sánchez, Cristina, García-Nieto, Daniel, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, and Lorenzo, Encarnación

Abstract

In this work, we present the combination of two different types of nanomaterials, 2D molybdenum disulfide nanosheets (MoS2-NS) and zero-dimensional carbon nanodots (CDs), for the development of a new electrochemiluminescence (ECL) platform for the early detection and quantification of the biomarker human epidermal growth factor receptor 2 (HER2), whose overexpression is associated with breast cancer. MoS2-NS are used as an immobilization platform for the thiolated aptamer, which can recognize the HER2 epitope peptide with high affinity, and CDs act as coreactants of the anodic oxidation of the luminophore [Ru(bpy)3]2+. The HER2 biomarker is detected by changes in the ECL signal of the [Ru(bpy)3]2+/CD system, with a low detection limit of 1.84 fg/mL and a wide linear range. The proposed method has been successfully applied to detect the HER2 biomarker in human serum samples.

Published
2023

31. Pathogen sensing device based on 2D MoS2/graphene heterostructure

Author

Enebral Romero, Estefanía, Gutiérrez Gálvez, Laura, Del Caño Ochoa, Rafael, Vázquez Sulleiro, Manuel, Naranjo, Alicia, Gómez, I. Jénnifer, Pariente Alonso, Félix, Pérez, Emilio M., García Mendiola, Tania, Lorenzo Abad, Encarnación, and UAM. Departamento de Química Analítica y Análisis Instrumental

Subjects
SARS-CoV-2, Electrografting, Covalent heterostructures, Aptasensor, Química, f-MoS 2
Abstract

In this work we propose a new methodology for selective and sensitive pathogen detection based on a 2D layered heterostructured biosensing platform. As a proof of concept, we have chosen SARS-CoV-2 virus because the availability of new methods to detect this virus is still a great deal of interest. The prepared platform is based on the covalent immobilization of molybdenum disulphide functionalized with a diazonium salt (f-MoS2) onto graphene screen-printed electrodes (GPH SPE) by electrografting of the diazonium salt. This chemistry-based method generates an improved heterostructured biosensing platform for aptamer immobilization and aptasensor development. Electrochemical impedance spectroscopy (EIS) is used to obtain the signal response of the device, proving the ability of the sensor platform to detect the virus. SARS-CoV-2 spike RBD recombinant protein (SARS-CoV-2 S1 protein) has been detected and quantified with a low detection limit of 2.10 fg/mL. The selectivity of the developed biosensor has been confirmed after detecting the S1 protein even in presence of other interfering proteins. Moreover, the ability of the device to detect SARS-CoV-2 S1 protein has been also tested in nasopharyngeal swab samples, This work has been financially supported by the Spanish Ministry of Economy and Competitiveness (PID2020-116728RB-I00, PID2020- 116661RB-I00, CTQ2015-71955-REDT (ELECTROBIONET)) and Community of Madrid (TRANSNANOAVANSENS, S2018/NMT-4349, and PhotoArt P2018/NMT-4367). E. Enebral thank the financial support of “Nanotecnología para detección del SARS-CoV-2 y sus variantes. NANOCOV” project. IMDEA Nanociencia receives support from the “Severo Ochoa” Programme for Centres of Excellence in R&D (MINECO, Grant CEX2020-001039-S). We also thank the Spanish Ministry of Universities for supporting Laura Gutiérrez-Galvez with the Formación del Profesorado Universitario (FPU) grant (FPU19/06309)

Published
2023

33. Paving the way to Point of Care (POC) devices for SARS-CoV-2 detection [Dataset]

Author

Kaci, Karim, Caño, Rafael del, Luna, Mónica, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Somoza, Álvaro, Miranda, Rodolfo, González de Rivera, Guillermo, García-Mendiola, Tania, Lorenzo, Encarnación, Kaci, Karim, Caño, Rafael del, Luna, Mónica, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Somoza, Álvaro, Miranda, Rodolfo, González de Rivera, Guillermo, García-Mendiola, Tania, and Lorenzo, Encarnación

Published
2022

34. Electronic Supplementary Material Amplification-Free Detection of SARS-CoV-2 using Gold Nanotriangles Functionalized with Oligonucleotides

Author

Caño, Rafael del, García-Mendiola, Tania, García-Nieto, Daniel, Álvaro Bruna, Raquel, Luna, Mónica, Alarcón Iniesta, Hernán, Coloma, Rocío, Rodríguez Diaz, Ciro, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Miranda, Rodolfo, Somoza, Álvaro, Lorenzo, Encarnación, Caño, Rafael del, García-Mendiola, Tania, García-Nieto, Daniel, Álvaro Bruna, Raquel, Luna, Mónica, Alarcón Iniesta, Hernán, Coloma, Rocío, Rodríguez Diaz, Ciro, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Miranda, Rodolfo, Somoza, Álvaro, and Lorenzo, Encarnación

Published
2022

35. Paving the way to point of care (POC) devices for SARS-CoV-2 detection

Author

Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Comunidad de Madrid, European Commission, Fundación Instituto Madrileño de Estudios Avanzados en Nanociencia, Universidad Autónoma de Madrid, Banco Santander, Conferencia de Rectores de las Universidades Españolas, Consejo Superior de Investigaciones Científicas (España), Kaci, Karim, Caño, Rafael del, Luna, Mónica, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Somoza, Álvaro, Miranda, Rodolfo, González de Rivera, Guillermo, García-Mendiola, Tania, Lorenzo, Encarnación, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), Comunidad de Madrid, European Commission, Fundación Instituto Madrileño de Estudios Avanzados en Nanociencia, Universidad Autónoma de Madrid, Banco Santander, Conferencia de Rectores de las Universidades Españolas, Consejo Superior de Investigaciones Científicas (España), Kaci, Karim, Caño, Rafael del, Luna, Mónica, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Somoza, Álvaro, Miranda, Rodolfo, González de Rivera, Guillermo, García-Mendiola, Tania, and Lorenzo, Encarnación

Abstract

In this work we present a powerful, affordable, and portable biosensor to develop Point of care (POC) SARS-CoV-2 virus detection. It is constructed from a fast, low cost, portable and electronically automatized potentiostat that controls the potential applied to a disposable screen-printed electrochemical platform and the current response. The potentiostat was designed to get the best signal-to-noise ratio, a very simple user interface offering the possibility to be used by any device (computer, mobile phone or tablet), to have a small and portable size, and a cheap manufacturing cost. Furthermore, the device includes as main components, a data acquisition board, a controller board and a hybridization chamber with a final size of 10 × 8 × 4 cm. The device has been tested by detecting specific SARS-CoV-2 virus sequences, reaching a detection limit of 22.1 fM. Results agree well with those obtained using a conventional potentiostat, which validate the device and pave the way to the development of POC biosensors. In this sense, the device has finally applied to directly detect the presence of the virus in nasopharyngeal samples of COVID-19 patients and results confirm its utility for the rapid detection infected samples avoiding any amplification process.

Published
2022

36. Methylene Blue functionalized carbon nanodots combined with different shape gold nanostructures for sensitive and selective SARS-CoV-2 sensing

Author

Comunidad de Madrid, Ministerio de Economía y Competitividad (España), Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Conferencia de Rectores de las Universidades Españolas, Banco Santander, Consejo Superior de Investigaciones Científicas (España), Pina-Coronado, Clara, Martínez-Sobrino, Álvaro, Gutiérrez-Gálvez, Laura, Caño, Rafael del, Martínez-Periñán, Emiliano, García-Nieto, Daniel, Rodríguez-Peña, Micaela, Luna, Mónica, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Somoza, Álvaro, García-Mendiola, Tania, Miranda, Rodolfo, Lorenzo, Encarnación, Comunidad de Madrid, Ministerio de Economía y Competitividad (España), Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Conferencia de Rectores de las Universidades Españolas, Banco Santander, Consejo Superior de Investigaciones Científicas (España), Pina-Coronado, Clara, Martínez-Sobrino, Álvaro, Gutiérrez-Gálvez, Laura, Caño, Rafael del, Martínez-Periñán, Emiliano, García-Nieto, Daniel, Rodríguez-Peña, Micaela, Luna, Mónica, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Somoza, Álvaro, García-Mendiola, Tania, Miranda, Rodolfo, and Lorenzo, Encarnación

Abstract

The development of DNA-sensing platforms based on new synthetized Methylene Blue functionalized carbon nanodots combined with different shape gold nanostructures (AuNs), as a new pathway to develop a selective and sensitive methodology for SARS-CoV-2 detection is presented. A mixture of gold nanoparticles and gold nanotriangles have been synthetized to modify disposable electrodes that act as an enhanced nanostructured electrochemical surface for DNA probe immobilization. On the other hand, modified carbon nanodots prepared a la carte to contain Methylene Blue (MB-CDs) are used as electrochemical indicators of the hybridization event. These MB-CDs, due to their structure, are able to interact differently with double and single-stranded DNA molecules. Based on this strategy, target sequences of the SARS-CoV-2 virus have been detected in a straightforward way and rapidly with a detection limit of 2.00 aM. Moreover, this platform allows the detection of the SARS-CoV-2 sequence in the presence of other viruses, and also a single nucleotide polymorphism (SNPs). The developed approach has been tested directly on RNA obtained from nasopharyngeal samples from COVID-19 patients, avoiding any amplification process. The results agree well with those obtained by RT-qPCR or reverse transcription quantitative polymerase chain reaction technique.

Published
2022

37. Potential application of metallacarboranes as an internal reference: an electrochemical comparative study to ferrocene

Author

Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, European Commission, Comunidad de Madrid, Xavier, Jewel Ann Maria, Viñas, Clara, Lorenzo, Encarnación, García Mendiola, Tania, Teixidor, Francesc, Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, European Commission, Comunidad de Madrid, Xavier, Jewel Ann Maria, Viñas, Clara, Lorenzo, Encarnación, García Mendiola, Tania, and Teixidor, Francesc

Abstract

Ferrocene and its derivatives have been extensively used as an internal reference in electrochemical processes. Yet, they possess limitations such as solvent restrictions that require chemical modifications. In this regard, we have studied the use of metallacarboranes [3,3'-M(1,2-C2B9H11)2]- (M = Co, Fe) as general internal reference systems and have proven their suitability by thoroughly investigating their electrochemical properties in both aqueous and organic electrolytes without any derivatization.

Published
2022

38. Amplification-free detection of SARS-CoV-2 using gold nanotriangles functionalized with oligonucleotides

Author

Consejo Superior de Investigaciones Científicas (España), Conferencia de Rectores de las Universidades Españolas, Comunidad de Madrid, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), European Commission, Banco Santander, Instituto de Salud Carlos III, Caño, Rafael del, García-Mendiola, Tania, García-Nieto, Daniel, Álvaro Bruna, Raquel, Luna, Mónica, Alarcón Iniesta, Hernán, Coloma, Rocío, Rodríguez Diaz, Ciro, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Miranda, Rodolfo, Somoza, Álvaro, Lorenzo, Encarnación, Consejo Superior de Investigaciones Científicas (España), Conferencia de Rectores de las Universidades Españolas, Comunidad de Madrid, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Ministerio de Economía y Competitividad (España), European Commission, Banco Santander, Instituto de Salud Carlos III, Caño, Rafael del, García-Mendiola, Tania, García-Nieto, Daniel, Álvaro Bruna, Raquel, Luna, Mónica, Alarcón Iniesta, Hernán, Coloma, Rocío, Rodríguez Diaz, Ciro, Milán-Rois, Paula, Castellanos, Milagros, Abreu, Melanie, Cantón, Rafael, Galán, Juan Carlos, Pineda, Teresa, Pariente, Félix, Miranda, Rodolfo, Somoza, Álvaro, and Lorenzo, Encarnación

Abstract

Gold nanotriangles (AuNTs) functionalized with dithiolated oligonucleotides have been employed to develop an amplification-free electrochemical biosensor for SARS-CoV-2 in patient samples. Gold nanotriangles, prepared through a seed-mediated growth method and exhaustively characterized by different techniques, serve as an improved electrochemical platform and for DNA probe immobilization. Azure A is used as an electrochemical indicator of the hybridization event. The biosensor detects either single stranded DNA or RNA sequences of SARS-CoV-2 of different lengths, with a low detection limit of 22.2 fM. In addition, it allows to detect point mutations in SARS-CoV-2 genome with the aim to detect more infective SARS-CoV-2 variants such as Alpha, Beta, Gamma, Delta, and Omicron. Results obtained with the biosensor in nasopharyngeal swab samples from COVID-19 patients show the possibility to clearly discriminate between non-infected and infected patient samples as well as patient samples with different viral load. Furthermore, the results correlate well with those obtained by the gold standard technique RT-qPCR, with the advantage of avoiding the amplification process and the need of sophisticated equipment.

Published
2022

39. Neutral Red-carbon nanodots for selective fluorescent DNA sensing

Author

Martínez Periñán, Emiliano, Martínez Sobrino, Álvaro, Bravo Segura, Iria, García Mendiola, Tania, Mateo Martí, Eva, Pariente Alonso, Félix, Lorenzo Abad, Encarnación, and UAM. Departamento de Química Analítica y Análisis Instrumental

Subjects
Spectrometry, Fluorescence, Neutral Red, Quantum Dots, Fluorescence DNA assay, Escherichia coli, DNA, Química, Carbon nanodots, Biochemistry, Carbon, Analytical Chemistry, Fluorescent Dyes
Abstract

Carbon nanodots modified with Neutral Red covalently inserted in the nanostructure (NR-CDs) have been prepared by a simple synthesis method based on microwave irradiation under controlled temperature and pressure. The synthetized NR-CDs have been characterized by different techniques, demonstrating the covalent bonding of Neutral Red molecules to the carbon dots nanostructure. Fluorescence activity of the prepare NR-CDs has been explored showing different interaction pathways with singled and doubled stranded DNA. These studies have been successfully applied to develop a new fluorescence DNA hybridization assay to the detection of a specific DNA sequence of Escherichia coli bacteria. Graphical abstract: [Figure not available: see fulltext.], Open Access funding provided thanks to the CRUE-CSIC agreement with Springer Nature. This work has been supported by the Spanish Ministerio de Ciencia, Innovación y Universidades (CTQ2017- 84309-C2-1-R; RED2018-102412-T) and Comunidad Autónoma de Madrid (SI3/PJI/2021–00341, P2018/NMT-4349 TRANSNANOAVANSENS Program)

Published
2022

40. MoS 2 -Carbon Nanodots as a New Electrochemiluminescence Platform for Breast Cancer Biomarker Detection.

Author

Gutiérrez-Gálvez, Laura, Sulleiro, Manuel Vázquez, Gutiérrez-Sánchez, Cristina, García-Nieto, Daniel, Luna, Mónica, Pérez, Emilio M., García-Mendiola, Tania, and Lorenzo, Encarnación

Subjects
ELECTROCHEMILUMINESCENCE, APTAMERS, EPIDERMAL growth factor receptors, EARLY detection of cancer, BREAST cancer, MOLYBDENUM disulfide
Abstract

In this work, we present the combination of two different types of nanomaterials, 2D molybdenum disulfide nanosheets (MoS2-NS) and zero-dimensional carbon nanodots (CDs), for the development of a new electrochemiluminescence (ECL) platform for the early detection and quantification of the biomarker human epidermal growth factor receptor 2 (HER2), whose overexpression is associated with breast cancer. MoS2-NS are used as an immobilization platform for the thiolated aptamer, which can recognize the HER2 epitope peptide with high affinity, and CDs act as coreactants of the anodic oxidation of the luminophore [Ru(bpy)3]2+. The HER2 biomarker is detected by changes in the ECL signal of the [Ru(bpy)3]2+/CD system, with a low detection limit of 1.84 fg/mL and a wide linear range. The proposed method has been successfully applied to detect the HER2 biomarker in human serum samples. [ABSTRACT FROM AUTHOR]

Published
2023
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42. Potential application of metallacarboranes as an internal reference: an electrochemical comparative study to ferrocene.

Author

Xavier, Jewel Ann Maria, Viñas, Clara, Lorenzo, Encarnación, García-Mendiola, Tania, and Teixidor, Francesc

Subjects
AQUEOUS electrolytes, FERROCENE derivatives, COMPARATIVE studies, DERIVATIZATION, SOLVENTS
Abstract

Ferrocene and its derivatives have been extensively used as an internal reference in electrochemical processes. Yet, they possess limitations such as solvent restrictions that require chemical modifications. In this regard, we have studied the use of metallacarboranes [3,3′-M(1,2-C2B9H11)2]− (M = Co, Fe) as general internal reference systems and have proven their suitability by thoroughly investigating their electrochemical properties in both aqueous and organic electrolytes without any derivatization. [ABSTRACT FROM AUTHOR]

Published
2022
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43. Breast cancer biomarker detection through the photoluminescence of epitaxial monolayer MoS2 flakes

Author

Ministerio de Economía y Competitividad (España), Comunidad de Madrid, Catalán-Gómez, Sergio, Briones, María, Cortijo-Campos, Sandra, García-Mendiola, Tania, Andrés, Alicia de, Garg, Sourav, Kung, Patrick, Lorenzo, Encarnación, Pau, José Luis, Redondo-Cubero, Andrés, Ministerio de Economía y Competitividad (España), Comunidad de Madrid, Catalán-Gómez, Sergio, Briones, María, Cortijo-Campos, Sandra, García-Mendiola, Tania, Andrés, Alicia de, Garg, Sourav, Kung, Patrick, Lorenzo, Encarnación, Pau, José Luis, and Redondo-Cubero, Andrés

Abstract

In this work we report on the characterization and biological functionalization of 2D MoS flakes, epitaxially grown on sapphire, to develop an optical biosensor for the breast cancer biomarker miRNA21. The MoS flakes were modified with a thiolated DNA probe complementary to the target biomarker. Based on the photoluminescence of MoS, the hybridization events were analyzed for the target (miRNA21c) and the control non-complementary sequence (miRNA21nc). A specific redshift was observed for the hybridization with miRNA21c, but not for the control, demonstrating the biomarker recognition via PL. The homogeneity of these MoS platforms was verified with microscopic maps. The detailed spectroscopic analysis of the spectra reveals changes in the trion to excitation ratio, being the redshift after the hybridization ascribed to both peaks. The results demonstrate the benefits of optical biosensors based on MoS monolayer for future commercial devices.

Published
2020

44. Metallacarboranes as tunable redox potential electrochemical indicators for screening of gene mutation† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c6sc01567k

Author

García-Mendiola, Tania, Bayon-Pizarro, Victoria, Zaulet, Adnana, Fuentes, Isabel, Pariente, Félix, Teixidor, Francesc, Viñas, Clara, and Lorenzo, Encarnación

Subjects
Chemistry
Abstract

The electrochemical behaviour of metallocarborane sodium salts and their interactions with DNA have been studied. They are shown to be selective redox indicators with wide-ranging potential as electrochemical indicators in DNA biosensors., The substitution of hydrogen with chlorine in the metallacarborane [3,3-Fe(1,2-closo-C2B9H11)2]– cluster modulates the formal potential of the Fe3+/Fe2+ redox couple, shifting it to a more positive value. Hence, very similar redox probes with a wide range of formal potentials, ranging from negative to positive values, are available. Thus, we have achieved the synthesis and studied the electrochemical behaviour of the sodium salt of [3,3-Fe(8,9,12-Cl3-1,2-closo-C2B9H8)2]– in aqueous media. This strategy allows tuning of the redox potential of the [3,3-Fe(1,2-closo-C2B9H11)2]– framework with a minor change in its shape and dimensions. We also describe the interaction of the prepared [3,3-Fe(8,9,12-Cl3-1,2-closo-C2B9H8)2]– and the pristine [3,3-Fe(1,2-closo-C2B9H11)2]– with DNA. These studies have been carried out not only with DNA in solution but also with DNA immobilized on screen-printed gold electrodes. The results obtained point to a strong interaction between the metallacarboranes and DNA, to a different extent with single stranded DNA (ssDNA) compared to double stranded DNA (dsDNA). This property makes them selective and wide-ranging potential electrochemical indicators of hybridization. The suitability of these new redox indicators for selective DNA biosensor development has been probed by the direct detection of two different mutations associated with cystic fibrosis in PCR amplicons extracted from blood cells.

Published
2016

49. Metallacarboranes on the Road to Anticancer Therapies: Cellular Uptake, DNA Interaction, and Biological Evaluation of Cobaltabisdicarbollide [COSAN]−.

Author

Fuentes, Isabel, García‐Mendiola, Tania, Sato, Shinichi, Pita, Marcos, Nakamura, Hiroyuki, Lorenzo, Encarnación, Teixidor, Francesc, Marques, Fernanda, and Viñas, Clara

Subjects
*CARBORANES, *ANTINEOPLASTIC agents, *CELL-mediated cytotoxicity, *OXIDATION-reduction reaction, *CARBON electrodes
Abstract

After uptake by U87 MG and A375 cancer cells, cobaltabisdicarbollide [COSAN]− distributes between membrane and nucleus and presents no relevant cytotoxicity against both cell lines even for long incubation times. The cytotoxicity of Na[COSAN] was also tested towards one normal cell line, the V79 fibroblasts, in order to ascertain the noncytotoxic profile of the compound. As the cell's nucleus contains DNA, the interaction between [COSAN]− and double‐stranded calf thymus DNA (CT‐dsDNA) has been investigated. There is a strong interaction between both molecules forming a nanohybrid CT‐dsDNA‐[COSAN] biomaterial, which was fully characterized. Moreover, Na[COSAN] shows characteristic redox peaks ascribed to the oxidation/reduction of Co3+/2+ at a formal potential of −1.444 V and it can be accumulated at a surface‐immobilized DNA layer of glassy carbon electrodes. The equilibrium surface‐binding constants (Kox/Kred), which confirm that [COSAN]− interacts with DNA by an intercalative or electrostatic mode, depending on the ionic strength of the solution, were estimated. In addition, high binding affinity of Na[COSAN] to proteins was observed by 11B{1H} NMR and confirmed in vivo. Finally, biodistribution studies of [COSAN]− in normal mice were run. After administration, Na[COSAN] was distributed into many organs but mainly accumulated in the reticuloendothelial system (RES), including liver and spleen. After 1 h, the formation of aggregates by plasma protein interaction plays a role in the biodistribution profile; the aggregates accumulate mostly in the lungs. Na[COSAN], which displays low toxicity and high uptake by relevant cancer cells accumulating boron within the nucleus, could act as a suitable compound for further developments as boron neutron capture therapy (BNCT) agents. Bioactive metallacarborane: The noncytotoxic profile of Na[3,3′‐M(1,2‐closo‐C2B9H11)2], [COSAN]−, has been demonstrated on V79 fibroblast cells and its biodistribution in normal mice reported. Pristine [COSAN]− molecules enter the cytoplasm of the cell and reach the nucleus. The strong interaction between Na[COSAN] and double‐stranded calf thymus DNA (CT‐dsDNA) has been revealed (see graphic) and the formed nanohybrid biomaterial fully characterized. [ABSTRACT FROM AUTHOR]

Published
2018
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50. Metallacarboranes on the Road to Anticancer Therapies: Cellular Uptake, DNA Interaction, and Biological Evaluation of Cobaltabisdicarbollide [COSAN]−.

Author

Fuentes, Isabel, García‐Mendiola, Tania, Sato, Shinichi, Pita, Marcos, Nakamura, Hiroyuki, Lorenzo, Encarnación, Teixidor, Francesc, Marques, Fernanda, and Viñas, Clara

Subjects
CARBORANES, ANTINEOPLASTIC agents, CELL-mediated cytotoxicity, OXIDATION-reduction reaction, CARBON electrodes
Abstract

After uptake by U87 MG and A375 cancer cells, cobaltabisdicarbollide [COSAN]− distributes between membrane and nucleus and presents no relevant cytotoxicity against both cell lines even for long incubation times. The cytotoxicity of Na[COSAN] was also tested towards one normal cell line, the V79 fibroblasts, in order to ascertain the noncytotoxic profile of the compound. As the cell's nucleus contains DNA, the interaction between [COSAN]− and double‐stranded calf thymus DNA (CT‐dsDNA) has been investigated. There is a strong interaction between both molecules forming a nanohybrid CT‐dsDNA‐[COSAN] biomaterial, which was fully characterized. Moreover, Na[COSAN] shows characteristic redox peaks ascribed to the oxidation/reduction of Co3+/2+ at a formal potential of −1.444 V and it can be accumulated at a surface‐immobilized DNA layer of glassy carbon electrodes. The equilibrium surface‐binding constants (Kox/Kred), which confirm that [COSAN]− interacts with DNA by an intercalative or electrostatic mode, depending on the ionic strength of the solution, were estimated. In addition, high binding affinity of Na[COSAN] to proteins was observed by 11B{1H} NMR and confirmed in vivo. Finally, biodistribution studies of [COSAN]− in normal mice were run. After administration, Na[COSAN] was distributed into many organs but mainly accumulated in the reticuloendothelial system (RES), including liver and spleen. After 1 h, the formation of aggregates by plasma protein interaction plays a role in the biodistribution profile; the aggregates accumulate mostly in the lungs. Na[COSAN], which displays low toxicity and high uptake by relevant cancer cells accumulating boron within the nucleus, could act as a suitable compound for further developments as boron neutron capture therapy (BNCT) agents. Bioactive metallacarborane: The noncytotoxic profile of Na[3,3′‐M(1,2‐closo‐C2B9H11)2], [COSAN]−, has been demonstrated on V79 fibroblast cells and its biodistribution in normal mice reported. Pristine [COSAN]− molecules enter the cytoplasm of the cell and reach the nucleus. The strong interaction between Na[COSAN] and double‐stranded calf thymus DNA (CT‐dsDNA) has been revealed (see graphic) and the formed nanohybrid biomaterial fully characterized. [ABSTRACT FROM AUTHOR]

Published
2018
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