Publications
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Attomolar analyte sensing techniques (AttoSens): A review on a decade of progress on chemical and biosensing nanoplatforms
Usha S.P., Manoharan H., Deshmukh R., Álvarez-Diduk R., Calucho E., Sai V.V.R., Merkoçi A. Chemical Society Reviews; 50 (23): 13012 - 13089. 2021. 10.1039/d1cs00137j. IF: 54.564
Detecting the ultra-low abundance of analytes in real-life samples, such as biological fluids, water, soil, and food, requires the design and development of high-performance biosensing modalities. The breakthrough efforts from the scientific community have led to the realization of sensing technologies that measure the analyte's ultra-trace level, with relevant sensitivity, selectivity, response time, and sampling efficiency, referred to as Attomolar Analyte Sensing Techniques (AttoSens) in this review. In an AttoSens platform, 1 aM detection corresponds to the quantification of 60 target analyte molecules in 100 μL of sample volume. Herein, we review the approaches listed for various sensor probe design, and their sensing strategies that paved the way for the detection of attomolar (aM: 10-18 M) concentration of analytes. A summary of the technological advances made by the diverse AttoSens trends from the past decade is presented. This journal is © The Royal Society of Chemistry.
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COVID-19 biosensing technologies
Merkoçi A., Li C.-Z., Lechuga L.M., Ozcan A. Biosensors and Bioelectronics; 178 (113046) 2021. 10.1016/j.bios.2021.113046. IF: 10.618
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Development of a Heavy Metal Sensing Boat for Automatic Analysis in Natural Waters Utilizing Anodic Stripping Voltammetry
Qiuyue Yang,Bhawna Nagar,Ruslán Alvarez-Diduk,Marc Balsells,Alessandro Farinelli,Domenico Bloisi, Lorenzo Proia, Carmen Espinosa, Marc Ordeix, Thorsten Knutz,Elisabetta De Vito-Francesco, Roza Allabashi, Arben Merkoçi Acs Es&t Water; 1 (12): 2470 - 2476. 2021. 10.1021/acsestwater.1c00192. IF: 0.000
Determination of the levels of heavy metal ions would support assessment of sources and pathways of water pollution. However, traditional spatial assessment by manual sampling and off-site detection in the laboratory is expensive and time-consuming and requires trained personnel. Aiming to fill the gap between on-site automatic approaches and laboratory techniques, we developed an autonomous sensing boat for on-site heavy metal detection using square-wave anodic stripping voltammetry. A fluidic sensing system was developed to integrate into the boat as the critical sensing component and could detect ≤1 μg/L Pb, ≤6 μg/L Cu, and ≤71 μg/L Cd simultaneously in the laboratory. Once its integration was completed, the autonomous sensing boat was tested in the field, demonstrating its ability to distinguish the highest concentration of Pb in an effluent of a galena-enriched mine compared to those at other sites in the stream (Osor Stream, Girona, Spain).
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Electrochromism: An emerging and promising approach in (bio)sensing technology
Farahmand Nejad M.A., Ranjbar S., Parolo C., Nguyen E.P., Álvarez-Diduk R., Hormozi-Nezhad M.R., Merkoçi A. Materials Today; 50: 476 - 498. 2021. 10.1016/j.mattod.2021.06.015. IF: 31.041
Electrochromism (EC) is a unique property of certain materials that undergo an electrochemical-induced change in colouration. During the last decades, electrochromic materials (ECMs) have been applied in a variety of technologies ranging from smart windows to information displays and energy storage devices. More recently, ECMs have attracted the attention of the (bio)sensing community thanks to their ability to combine the sensitivity of electrochemical methods with the intuitive readout of optical sensors. Although still a nascent technology, EC-based sensors are on the rise with several targets (e.g. cancer biomarkers, bacteria, metabolites and pesticides), which have already been detected by (bio)sensors using ECMs as transducers. In this review, we provide the reader with all the information to understand EC and its use in the development of EC-based biosensors. © 2021 Elsevier Ltd
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Improved Aliivibrio fischeri based-toxicity assay: Graphene-oxide as a sensitivity booster with a mobile-phone application
Bergua J.F., Álvarez-Diduk R., Hu L., Hassan A.H.A., Merkoçi A. Journal of Hazardous Materials; 406 (124434) 2021. 10.1016/j.jhazmat.2020.124434. IF: 10.588
Recently, many bioluminescence-based applications have arisen in several fields, such as biosensing, bioimaging, molecular biology, and human health diagnosis. Among all bioluminescent organisms, Aliivibrio fischeri (A. fischeri) is a bioluminescent bacterium used to carry out water toxicity assays since the late 1970s. Since then, several commercial A. fischeri-based products have been launched to the market, as these bacteria are considered as a gold standard for water toxicity assessment worldwide. However, the aforementioned commercial products rely on expensive equipment, requiring several reagents and working steps, as well as high-trained personnel to perform the assays and analyze the output data. For these reasons, in this work, we have developed for the first time a mobile-phone-based sensing platform for water toxicity assessment in just 5 min using two widespread pesticides as model analytes. To accomplish this, we have established new methodologies to enhance the bioluminescent signal of A. fischeri based on the bacterial culture in a solid media and/or using graphene oxide. Finally, we have addressed the biocompatibility of graphene oxide to A. fischeri, boosting the sensitivity of the toxicity assays and the bacterial growth of the lyophilized bacterial cultures for more user-friendly storage. © 2020 Elsevier B.V.
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Integrated Devices for Non-Invasive Diagnostics
Ates H.C., Brunauer A., von Stetten F., Urban G.A., Güder F., Merkoçi A., Früh S.M., Dincer C. Advanced Functional Materials; 31 (15, 2010388) 2021. 10.1002/adfm.202010388. IF: 18.808
“Sample-in-answer-out” type integrated diagnostic devices have been widely recognized as the ultimate solution to simplify testing across healthcare systems. Such systems are equipped with advanced fluidic, mechanical, chemical, biological, and electronic components to handle patient samples without any manual steps therefore have the potential to accelerate intervention and improve patient outcomes. In this regard, the combination of integrated devices and non-invasive sampling has gained a substantial interest to further improve the comfort and safety of patients. In this Review, the pioneering developments in integrated diagnostics are covered and their potential in non-invasive sampling is discussed. The key properties of possible sample types are highlighted by addressing their relevance for the clinical practice. Last, the factors affecting the transition of integrated devices from academia to the market are identified by analyzing the technology readiness levels of selected examples and alternative remedies are explored to increase the rate of survival during this transition. © 2020 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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Integrating gold nanoclusters, folic acid and reduced graphene oxide for nanosensing of glutathione based on “turn-off” fluorescence
Wong X.Y., Quesada-González D., Manickam S., New S.Y., Muthoosamy K., Merkoçi A. Scientific Reports; 11 (1, 2375) 2021. 10.1038/s41598-021-81677-8. IF: 4.380
Glutathione (GSH) is a useful biomarker in the development, diagnosis and treatment of cancer. However, most of the reported GSH biosensors are expensive, time-consuming and often require complex sample treatment, which limit its biological applications. Herein, a nanobiosensor for the detection of GSH using folic acid-functionalized reduced graphene oxide-modified BSA gold nanoclusters (FA-rGO-BSA/AuNCs) based on the fluorescence quenching interactions is presented. Firstly, a facile and optimized protocol for the fabrication of BSA/AuNCs is developed. Functionalization of rGO with folic acid is performed using EDC/NHS cross-linking reagents, and their interaction after loading with BSA/AuNCs is demonstrated. The formation of FA-rGO, BSA/AuNCs and FA-rGO-BSA/AuNCs are confirmed by the state-of-art characterization techniques. Finally, a fluorescence turn-off sensing strategy is developed using the as-synthesized FA-rGO-BSA/AuNCs for the detection of GSH. The nanobiosensor revealed an excellent sensing performance for the detection of GSH with high sensitivity and desirable selectivity over other potential interfering species. The fluorescence quenching is linearly proportional to the concentration of GSH between 0 and 1.75 µM, with a limit of detection of 0.1 µM under the physiological pH conditions (pH 7.4). Such a sensitive nanobiosensor paves the way to fabricate a “turn-on” or “turn-off” fluorescent sensor for important biomarkers in cancer cells, presenting potential nanotheranostic applications in biological detection and clinical diagnosis. © 2021, The Author(s).
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Lateral flow device for water fecal pollution assessment: From troubleshooting of its microfluidics using bioluminescence to colorimetric monitoring of genericEscherichia coli
Bergua J.F., Hu L., Fuentes-Chust C., Álvarez-Diduk R., Hassan A.H.A., Parolo C., Merkoçi A. Lab on a Chip; 21 (12): 2417 - 2426. 2021. 10.1039/d1lc00090j. IF: 6.799
Water is the most important ingredient of life. Water fecal pollution threatens water quality worldwide and has direct detrimental effects on human health and the global economy. Nowadays, assessment of water fecal pollution relies on time-consuming techniques that often require well-trained personnel and highly-equipped laboratories. Therefore, faster, cheaper, and easily-used systems are needed toin situmonitor water fecal pollution. Herein, we have developed colorimetric lateral flow strips (LFS) able to detect and quantifyEscherichia colispecies in tap, river, and sewage water samples as an indicator of fecal pollution. The combination of LFS with a simple water filtration unit and a commercially available colorimetric reader enhanced the assay sensitivity and enabled more accurate quantification of bacteria concentration down to 104CFU mL−1in 10 minutes, yielding recovery percentages between 80% and 90% for all water samples analyzed. Overall, this system allows for monitoring and assessing water quality based onE. colispecies as a standard microbiological indicator of fecal pollution. Furthermore, we have developed a novel bioluminescent, bacteria-based method to quickly characterize the performance of a great variety of LFS materials. This new method allows evaluating the flow rate of big analytes such as bacteria through the LFS materials, as a suggestive means for selecting the appropriate materials for fabricating LFS targeting big analytes (≈2 μm). As a whole, the proposed approach can accelerate and reduce the costs of water quality monitoring and pave the way for further improvement of fecal pollution detection systems. © The Royal Society of Chemistry 2021.
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Nanodiagnostics to Face SARS-CoV-2 and Future Pandemics: From an Idea to the Market and beyond
Rosati G., Idili A., Parolo C., Fuentes-Chust C., Calucho E., Hu L., Castro E Silva C.D.C., Rivas L., Nguyen E.P., Bergua J.F., Alvárez-Diduk R., Muñoz J., Junot C., Penon O., Monferrer D., Delamarche E., Merkoçi A. ACS Nano; 15 (11): 17137 - 17149. 2021. 10.1021/acsnano.1c06839. IF: 15.881
The COVID-19 pandemic made clear how our society requires quickly available tools to address emerging healthcare issues. Diagnostic assays and devices are used every day to screen for COVID-19 positive patients, with the aim to decide the appropriate treatment and containment measures. In this context, we would have expected to see the use of the most recent diagnostic technologies worldwide, including the advanced ones such as nano-biosensors capable to provide faster, more sensitive, cheaper, and high-throughput results than the standard polymerase chain reaction and lateral flow assays. Here we discuss why that has not been the case and why all the exciting diagnostic strategies published on a daily basis in peer-reviewed journals are not yet successful in reaching the market and being implemented in the clinical practice. ©
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Paper-based electrophoretic bioassay: Biosensing in whole blood operating via smartphone
Merkoçi A., Sena-Torralba A., Alvarez-Diduk R., Parolo C., Torné-Morató H., Müller A. Analytical Chemistry; 93 (6): 3112 - 3121. 2021. 10.1021/acs.analchem.0c04330. IF: 6.986
Point-of-care (PoC) tests are practical and effective diagnostic solutions for major clinical problems, ranging from the monitoring of a pandemic to recurrent or simple measurements. Although, in recent years, a great improvement in the analytical performance of such sensors has been observed, there is still a major issue that has not been properly solved: The ability to perform adequate sample treatments. The main reason is that normally sample treatments require complicated or long procedures not adequate for deployment at the PoC. In response, a sensing platform, called paperbased electrophoretic bioassay (PEB), that combines the key characteristics of a lateral flow assay (LFA) with the sample treatment capabilities of electrophoresis is developed. In particular, the ability of PEB to separate different types of particles and to detect human antibodies in untreated spiked whole blood is demonstrated. Finally, to make the platform suitable for PoC, PEB is coupled with a smartphone that controls the electrophoresis and reads the optical signal generated. It is believed that the PEB platform represents a much-needed solution for the detection of low target concentrations in complex media, solving one of the major limitations of LFA and opening opportunities for point-of-care sensors. © 2021 American Chemical Society.
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Rapid and Efficient Detection of the SARS-CoV-2 Spike Protein Using an Electrochemical Aptamer-Based Sensor
Idili A., Parolo C., Alvarez-Diduk R., Merkoçi A. ACS Sensors; 6 (8): 3093 - 3101. 2021. 10.1021/acssensors.1c01222. IF: 7.711
The availability of sensors able to rapidly detect SARS-CoV-2 directly in biological fluids in a single step would allow performing massive diagnostic testing to track in real time and contain the spread of COVID-19. Motivated by this, here, we developed an electrochemical aptamer-based (EAB) sensor able to achieve the rapid, reagentless, and quantitative measurement of the SARS-CoV-2 spike (S) protein. First, we demonstrated the ability of the selected aptamer to undergo a binding-induced conformational change in the presence of its target using fluorescence spectroscopy. Then, we engineered the aptamer to work as a bioreceptor in the EAB platform and we demonstrated its sensitivity and specificity. Finally, to demonstrate the clinical potential of the sensor, we tested it directly in biological fluids (serum and artificial saliva), achieving the rapid (minutes) and single-step detection of the S protein in its clinical range. © 2021 American Chemical Society.
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Smart nanobiosensors in agriculture
Merkoçi A. Nature Food; 2 (12): 920 - 921. 2021. 10.1038/s43016-021-00426-2. IF: 0.000
[No abstract available]
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The Microbiome Meets Nanotechnology: Opportunities and Challenges in Developing New Diagnostic Devices
Fuentes-Chust C., Parolo C., Rosati G., Rivas L., Perez-Toralla K., Simon S., de Lecuona I., Junot C., Trebicka J., Merkoçi A. Advanced Materials; 33 (18, 2006104) 2021. 10.1002/adma.202006104. IF: 30.849
Monitoring of the human microbiome is an emerging area of diagnostics for personalized medicine. Here, the potential of different nanomaterials and nanobiosensing technologies is reviewed for the development of novel diagnostic devices for the detection and measurement of microbiome-related biomarkers. Moreover, the current and future landscape of microbiome-based diagnostics is defined by exploring the advantages and disadvantages of current nanotechnology-based approaches, especially in the context of developing point-of-care (PoC) devices that would meet the international guidelines known as REASSURED (Real-time connectivity; Ease of specimen collection; Affordability; Sensitivity; Specificity; User-friendliness; Rapid & robust operation; Equipment-free; and Deliverability). Finally, the strategies of the latest international scientific consortia working in this field are analyzed, the current microbiome diagnostics market are reported and the principal ethical, legal, and societal issues related to microbiome R&D and innovation are discussed. © 2021 Wiley-VCH GmbH
