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Advanced Designs of Materials, Devices and Techniques for Biosensing

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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (30 June 2022) | Viewed by 29869

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Special Issue Editors

Prof. Dr. Eugen Gheorghiu

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Guest Editor

1. International Centre of Biodynamics, Bucharest, Romania
2. Faculty of Physics, University of Bucharest, Bucharest, Romania
Interests: analysis of the dynamics of living cells and biointerfaces; rapid antibacterial and antifungal susceptibility testing based on (coupled) optical (including optical waveguides); electrical and magnetic assays

Dr. Mihaela Gheorghiu

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Guest Editor

1. International Centre of Biodynamics, Bucharest, Romania
2. Faculty of Biology, University of Bucharest, Bucharest, Romania
Interests: cell-based biosensing platforms; surface functionalization; nanostructuring and new materials for electro-optical biosensing

Special Issue Information

Dear Colleagues,

Development of functional materials featuring exquisite electrochemical, magnetic and/or plasmonic properties in conjunction with the related analytical techniques, deployed either per se or in combination, are expected to boost the sensitivity of biosensing platforms.

Research in this area could support novel sensing concepts as well as promising biosensing applications in healthcare, early diagnosis, and environmental monitoring.

Sensing approaches at the cutting edge of the chemistry, physics, and biology of functional materials involve either affinity assays with ligands of the target analyte, live cells, or biomimetic structures immobilized onto tailored sensor chips, in 2D or 3D arrangements, or alternatively, coupled with functional materials integrated within the transducing layer(s) of the sensor. Thus, the aim of this Special Issue is to publish and disseminate original research data, review articles, communications, and short notes that focus on new (experimental or theoretical) advances, challenges, and outlooks concerning the design, construction, and characterization of sensing chips/devices and of related analytical techniques for biosensor development.

We invite contributions on topics that include but are not limited to various state-of-the-art biosensing technologies. As Guest Editors, we warmly invite you to submit manuscripts for this Special Issue entitled “Advanced Designs of Materials, Devices and Techniques for Biosensing”.

Prof. Eugen Gheorghiu
Prof. Mihaela Gheorghiu
Guest Editors

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Keywords

advancing sensor structure and related analytic techniques for increased biosensing capabilities
plasmonic materials, nanostructures, functional interfaces, biopolymers, graphene

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Published Papers (10 papers)

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Research

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20 pages, 5870 KiB

Open AccessArticle

Direct, Rapid Detection of Pathogens from Urine Samples

by Sorin David, Raluca-Elena Munteanu, Ana-Maria Tițoiu, Ionela-Cristina Petcu, Ioana-Cristina Cernat, Corina Leancu, Mihaela Gheorghiu and Eugen Gheorghiu

Materials 2022, 15(21), 7640; https://doi.org/10.3390/ma15217640 - 31 Oct 2022

Cited by 3 | Viewed by 2572

Abstract

The problem of rapidly detecting pathogens directly from clinical samples poses significant analytical challenges. Addressing this issue in relation to urinary tract infections, we propose an effective protocol and related immunomagnetic test kits enabling versatile screening for the presence of pathogenic bacteria in unprocessed urine samples. To achieve this, the components of a typical immunomagnetic separation protocol were optimized towards the sensitive assessment of the aggregates formed out of immunomagnetically tagged target pathogens collected from clinical samples. Specifically, a dedicated immunomagnetic material was developed via the functionalization of standardized, micron-sized magnetic beads with generic antibodies against gram-specific bacterial constituents with mannan binding lectin. As such, we demonstrate efficient procedures for achieving the enhanced, specific, and pathogen-mediated cluster formation of these tailored affinity-coated magnetic beads in complex samples. We further show how cluster analysis, in conjunction with the use of nonspecific, inexpensive fluorescent dye, allows for a straightforward optical assessment of the bacterial load directly from urine samples. The optimized sensing protocol and related kits provide, in less than 60 min, qualitative (positive/negative) information on the bacterial load with 85% specificity and 96% sensitivity, which is appropriate to empower clinical microscopy with a new analytic dimension. The procedure is prone to automation, can be conveniently used in clinical microbiology laboratories and, since it preserves the viability of the captured bacteria, can be interfaced with downstream analyses and antimicrobial susceptibility testing. Moreover, the study emphasizes a suite of practical validation assays that are useful for bringing the tool-box of immunomagnetic materials outside the academic laboratory and into real-life applications. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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11 pages, 4756 KiB

Open AccessArticle

Effect of Electrode Modification with Chitosan and Nafion^® on the Efficiency of Real-Time Enzyme Glucose Biosensors Based on ZnO Tetrapods

by Valerii Myndrul, Igor Iatsunskyi, Nataliya Babayevska, Marcin Jarek and Teofil Jesionowski

Materials 2022, 15(13), 4672; https://doi.org/10.3390/ma15134672 - 3 Jul 2022

Cited by 11 | Viewed by 2283

Abstract

Noninvasive, continuous glucose detection can provide some insights into daily fluctuations in blood glucose levels, which can help us balance diet, exercise, and medication. Since current commercially available glucose sensors can barely provide real-time glucose monitoring and usually imply different invasive sampling, there is an extraordinary need to develop new harmless methods for detecting glucose in non-invasive body fluids. Therefore, it is crucial to design (bio)sensors that can detect very low levels of glucose (down to tens of µM) normally found in sweat or tears. Apart from the selection of materials with high catalytic activity for glucose oxidation, it is also important to pay considerable attention to the electrode functionalization process, as it significantly contributes to the overall detection efficiency. In this study, the (ZnO tetrapods) ZnO TPs-based electrodes were functionalized with Nafion and chitosan polymers to compare their glucose detection efficiency. Cyclic voltammetry (CV) measurements have shown that chitosan-modified ZnO TPs require a lower applied potential for glucose oxidation, which may be due to the larger size of chitosan micelles (compared to Nafion micelles), and thus easier penetration of glucose through the chitosan membrane. However, despite this, both ZnO TPs modified with chitosan and Nafion membranes, provided quite similar glucose detection parameters (sensitivities, 7.5 µA mM⁻¹ cm⁻¹ and 19.2 µA mM⁻¹ cm⁻¹, and limits of detection, 24.4 µM and 22.2 µM, respectively). Our results show that both electrodes have a high potential for accurate real-time sweat/tears glucose detection. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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13 pages, 2823 KiB

Open AccessArticle

Real Time SPR Assessment of the Structural Changes of Adaptive Dynamic Constitutional Frameworks as a New Route for Sensing

by Sorin David, Mihaela Gheorghiu, Sanaa Daakour, Raluca-Elena Munteanu, Cristina Polonschii, Szilveszter Gáspár, Mihail Barboiu and Eugen Gheorghiu

Materials 2022, 15(2), 483; https://doi.org/10.3390/ma15020483 - 9 Jan 2022

Cited by 2 | Viewed by 2322

Abstract

Cross linked gold-dynamic constitutional frameworks (DCFs) are functional materials of potential relevance for biosensing applications, given their adaptivity and high responsivity against various external stimuli (such as pH, temperature) or specific interactions with biomolecules (enzymes or DNA) via internal constitutional dynamics. However, characterization and assessment of their dynamic conformational changes in response to external stimuli has never been reported. This study proves the capability of Surface Plasmon Resonance (SPR) assays to analyse the adaptive structural modulation of a functional matrix encompassing 3D gold-dynamic constitutional frameworks (Au-DCFs) when exposed to pH variations, as external stimuli. We analyse Au-DCFs formed from Au nanoparticles, (AuNP) connected through constitutionally dynamic polymers, dynamers, with multiple functionalities. For increased generality of this proof-of-concept assay, Au-DCFs, involving DCFs designed from 1,3,5-benzene-tricarbaldehyde (BTA) connecting centres and polyethylene glycol (PEG) connectors, are covalently attached to standard SPR sensing chips (Au nanolayers, carboxyl terminated or with carboxymethyl dextran, CMD top-layer) and analysed using state-of-the art SPR instrumentation. The SPR effects of the distance from the Au-DCFs matrix to the Au nanolayer of the sensing chip, as well as of Au-DCFs thickness were investigated. This study reveals the SPR response, augmented by the AuNP, to the conformational change, i.e., shrinkage, of the dynamer and AuNP matrix when decreasing the pH, and provides an unexplored insight into the sensing applicability of SPR real-time analysis of adaptive functional materials. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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15 pages, 31217 KiB

Open AccessArticle

Electrochemically Synthesized Poly(3-hexylthiophene) Nanowires as Photosensitive Neuronal Interfaces

by Szilveszter Gáspár, Tiziana Ravasenga, Raluca-Elena Munteanu, Sorin David, Fabio Benfenati and Elisabetta Colombo

Materials 2021, 14(16), 4761; https://doi.org/10.3390/ma14164761 - 23 Aug 2021

Cited by 1 | Viewed by 2455

Abstract

Poly(3-hexylthiophene) (P3HT) is a hole-conducting polymer that has been intensively used to develop organic optoelectronic devices (e.g., organic solar cells). Recently, P3HT films and nanoparticles have also been used to restore the photosensitivity of retinal neurons. The template-assisted electrochemical synthesis of polymer nanowires advantageously combines polymerization and polymer nanostructuring into one, relatively simple, procedure. However, obtaining P3HT nanowires through this procedure was rarely investigated. Therefore, this study aimed to investigate the template-assisted electrochemical synthesis of P3HT nanowires doped with tetrabutylammonium hexafluorophosphate (TBAHFP) and their biocompatibility with primary neurons. We show that template-assisted electrochemical synthesis can relatively easily turn 3-hexylthiophene (3HT) into longer (e.g., 17 ± 3 µm) or shorter (e.g., 1.5 ± 0.4 µm) P3HT nanowires with an average diameter of 196 ± 55 nm (determined by the used template). The nanowires produce measurable photocurrents following illumination. Finally, we show that primary cortical neurons can be grown onto P3HT nanowires drop-casted on a glass substrate without relevant changes in their viability and electrophysiological properties, indicating that P3HT nanowires obtained by template-assisted electrochemical synthesis represent a promising neuronal interface for photostimulation. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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8 pages, 981 KiB

Open AccessCommunication

Surface Adsorption of the Cancer Biomarker Lysophosphatidic Acid in Serum Studied by Acoustic Wave Biosensor

by Brian De La Franier and Michael Thompson

Materials 2021, 14(15), 4158; https://doi.org/10.3390/ma14154158 - 27 Jul 2021

Cited by 1 | Viewed by 2113

Abstract

The thickness shear mode acoustic wave device is of interest for the sensing of biomarkers for diseases in various biological fluids, but suffers from the issue of non-specific adsorption of compounds other than those of interest to the electrode surface, thus affecting the device’s output. The aim of this present study was to determine the level of non-specific adsorption on gold electrodes from serum samples with added ovarian cancer biomarker lysophosphatidic acid in the presence of a surface anti-fouling layer. The latter was an oligoethylene molecule with thiol group for attachment to the electrode surface. It was found that the anti-fouling layer had a minimal effect on the level of both adsorption of components from serum and the marker. This result stands in sharp contrast to the analogous monolayer employed for anti-fouling reduction on silica. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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12 pages, 3663 KiB

Open AccessArticle

The Potential Use of a Thin Film Gold Electrode Modified with Laccases for the Electrochemical Detection of Pyrethroid Metabolite 3-Phenoxybenzaldehyde

by Verónica Aglaeé Esquivel-Blanco, Gabriela Elizabeth Quintanilla-Villanueva, Juan Francisco Villarreal-Chiu , José Manuel Rodríguez-Delgado and Melissa Marlene Rodríguez-Delgado

Materials 2021, 14(8), 1992; https://doi.org/10.3390/ma14081992 - 15 Apr 2021

Cited by 4 | Viewed by 2395

Abstract

There is increasing interest in developing portable technologies to detect human health threats through hybrid materials that integrate specific bioreceptors. This work proposes an electrochemical approach for detecting 3-Phenoxybenzaldehyde (3-PBD), a biomarker for monitoring human exposure to pyrethroid pesticides. The biosensor uses laccase enzymes as an alternative recognition element by direct oxidation of 3-PBD catalysts by the enzyme onto thin-film gold electrodes. The thin-film gold electrode modified by the immobilized laccase was characterized by Fourier-transform infrared spectrometry and scanning electron microscopy. The detection method’s electrochemical parameters were established, obtaining a linear range of 5 t 50 μM, the limit of detection, and quantification of 0.061 and 2.02 μM, respectively. The proposed biosensor’s analytical performance meets the concentration of pyrethroids detected in natural environments, reflecting its potential as an alternative analytical tool for monitoring the pyrethroid insecticide’s presence. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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15 pages, 2199 KiB

Open AccessArticle

Assembling Surface Linker Chemistry with Minimization of Non-Specific Adsorption on Biosensor Materials

by Jack Chih-Chieh Sheng, Brian De La Franier and Michael Thompson

Materials 2021, 14(2), 472; https://doi.org/10.3390/ma14020472 - 19 Jan 2021

Cited by 10 | Viewed by 2763

Abstract

The operation of biosensors requires surfaces that are both highly specific towards the target analyte and that are minimally subject to fouling by species present in a biological fluid. In this work, we further examined the thiosulfonate-based linker in order to construct robust and durable self-assembling monolayers (SAMs) onto hydroxylated surfaces such as silica. These SAMs are capable of the chemoselective immobilization of thiol-containing probes (for analytes) under aqueous conditions in a single, straightforward, reliable, and coupling-free manner. The efficacy of the method was assessed through implementation as a biosensing interface for an ultra-high frequency acoustic wave device dedicated to the detection of avidin via attached biotin. Fouling was assessed via introduction of interfering bovine serum albumin (BSA), IgG antibody, or goat serum. Improvements were investigated systematically through the incorporation of an oligoethylene glycol backbone employed together with a self-assembling diluent without a functional distal group. This work demonstrates that the incorporation of a diluent of relatively short length is crucial for the reduction of fouling. Included in this work is a comparison of the surface attachment of the linker to Si₃N₄ and AlN, both materials used in sensor technology. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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18 pages, 4931 KiB

Open AccessArticle

Low-Cost Method and Biochip for Measuring the Trans-Epithelial Electrical Resistance (TEER) of Esophageal Epithelium

by Daniel Puiu Poenar, Guang Yang, Wei Keat Wan and Shilun Feng

Materials 2020, 13(10), 2354; https://doi.org/10.3390/ma13102354 - 20 May 2020

Cited by 14 | Viewed by 4073

Abstract

Trans-epithelial electrical resistance (TEER) is a good indicator of the barrier integrity of epithelial tissues and is often employed in biomedical research as an effective tool to assess ion transport and permeability of tight junctions. The Ussing chamber is the gold standard for measuring TEER of tissue specimens, but it has major drawbacks: it is a macroscopic method that requires a careful and labor intensive sample mounting protocol, allows a very limited viability for the mounted sample, has large parasitic components and low throughput as it cannot perform multiple simultaneous measurements, and this sophisticated and delicate apparatus has a relatively high cost. This paper demonstrates a low-cost home-made “sandwich ring” method which was used to measure the TEER of tissue specimens effectively. This method inspired the subsequent design of a biochip fabricated using standard soft lithography and laser engraving technologies, with which the TEER of pig epithelial tissues was measured. Moreover, it was possible to temporarily preserve the tissue specimens for days in the biochip and monitor the TEER continuously. Tissue responses after exposure tests to media of various pH values were also successfully recorded using the biochip. All these demonstrate that this biochip could be an effective, cheaper, and easier to use Ussing chamber substitute that may have relevant applications in clinical practice. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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27 pages, 5979 KiB

Open AccessReview

Recent Advances in Materials for Wearable Thermoelectric Generators and Biosensing Devices

by Maria Sattar and Woon-Hong Yeo

Materials 2022, 15(12), 4315; https://doi.org/10.3390/ma15124315 - 18 Jun 2022

Cited by 24 | Viewed by 4471

Abstract

Recently, self-powered health monitoring systems using a wearable thermoelectric generator (WTEG) have been rapidly developed since no battery is needed for continuous signal monitoring, and there is no need to worry about battery leakage. However, the existing materials and devices have limitations in rigid form factors and small-scale manufacturing. Moreover, the conventional bulky WTEG is not compatible with soft and deformable tissues, including human skins or internal organs. These limitations restrict the WTEG from stabilizing the thermoelectric gradient that is necessary to harvest the maximum body heat and generate valuable electrical energy. This paper summarizes recent advances in soft, flexible materials and device designs to overcome the existing challenges. Specifically, we discuss various organic and inorganic thermoelectric materials with their properties for manufacturing flexible devices. In addition, this review discusses energy budgets required for effective integration of WTEGs with wearable biomedical systems, which is the main contribution of this article compared to previous articles. Lastly, the key challenges of the existing WTEGs are discussed, followed by describing future perspectives for self-powered health monitoring systems. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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27 pages, 2325 KiB

Open AccessReview

Advanced Optogenetic-Based Biosensing and Related Biomaterials

by Mihaela Gheorghiu, Cristina Polonschii, Octavian Popescu and Eugen Gheorghiu

Materials 2021, 14(15), 4151; https://doi.org/10.3390/ma14154151 - 26 Jul 2021

Cited by 5 | Viewed by 3199

Abstract

The ability to stimulate mammalian cells with light, brought along by optogenetic control, has significantly broadened our understanding of electrically excitable tissues. Backed by advanced (bio)materials, it has recently paved the way towards novel biosensing concepts supporting bio-analytics applications transversal to the main biomedical stream. The advancements concerning enabling biomaterials and related novel biosensing concepts involving optogenetics are reviewed with particular focus on the use of engineered cells for cell-based sensing platforms and the available toolbox (from mere actuators and reporters to novel multifunctional opto-chemogenetic tools) for optogenetic-enabled real-time cellular diagnostics and biosensor development. The key advantages of these modified cell-based biosensors concern both significantly faster (minutes instead of hours) and higher sensitivity detection of low concentrations of bioactive/toxic analytes (below the threshold concentrations in classical cellular sensors) as well as improved standardization as warranted by unified analytic platforms. These novel multimodal functional electro-optical label-free assays are reviewed among the key elements for optogenetic-based biosensing standardization. This focused review is a potential guide for materials researchers interested in biosensing based on light-responsive biomaterials and related analytic tools. Full article

(This article belongs to the Special Issue Advanced Designs of Materials, Devices and Techniques for Biosensing)

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