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Ultratrace Antibiotic Sensing Using Aptamer/Graphene-based Field-effect Transistors
Abstract
Antibiotic residue, as emerging pollution resulting from antibiotic abuse, poses a serious threat on ecosystem and human health. Conventional methods for antibiotic detection, e.g., liquid/gas chromatography, are based on complicated instruments and time-consuming; therefore, efforts have been made to realize in situ and real-time monitoring of antibiotics. Here, a miniaturized and integratable electronic antibiotic sensor based on field-effect transistor (FET) is reported. The reduced graphene oxide (rGO) nanosheet is used as the channel material and the aptamer RNA for tobramycin is modified onto rGO as the probe. A novel sensor design with 6-mercapto-1-hexanol (MCH)/1-pyrenebutanol (PBA) blocking layer (BL) for structure optimization is applied to enhance the sensor reliability and specificity. This rGO/aptamer/BL sensor shows an ultra-sensitivity to tobramycin with a lower detection limit of 0.3 nM and a quick response within 5 s, as well as a high specificity over other antibiotics such as kanamycin, streptomycin, ciprofloxacin, and tetracycline. The sensing mechanism based on the deformation of the charged aptamer probe is proposed via an in-depth analysis of the interactions between aptamer, tobramycin and rGO. In addition, sensing test performed under controlled microfluidic flow conditions demonstrates a great potential of the sensors in practical applications.
... One of the specific features in the use of graphene sensor for small molecule detection is the large intrinsic charge of molecules that provide reasonably high shift in the graphene channel's conductivity. GFETs have previously been used for the highly sensitive detection of various antibiotics (Chen et al., 2019), small antigens (Kanai et al., 2020), and small-molecule drugs (Xu et al., 2021). While sensitivity and response times are mainly defined by the physical nature of the graphene channel, selectivity is provided by the specific recognition elements, i.e., bioreceptors such as enzymes, antibodies, and aptamers. ...
... Aptamers are oligonucleotides in a typical size range of 20-70 nucleic bases that form a specific three-dimensional structure during analyte capture. The oligonucleotides have intrinsic charges distributed over their backbone, and their deformation can bring charges closer to or further from the graphene surface, providing the sensing signal (Chen et al., 2019;Kanai et al., 2020). Different sensing principles based on aptamers have been demonstrated for mycotoxin detection, such as fluorescence (Liu et al., 2018), surface plasmon resonance (Zhu et al., 2015), spectral-phase interferometry (Nekrasov et al., 2021), chemiluminescence (Wang et al., 2019), and electrochemistry . ...
... In this work, we report on an array of optimized GFET-based aptasensors on a single chip used to detect mycotoxins that can provide better statistical data analysis generated by the sensors. Since the size of an aptamer is larger than the size of a small molecule, such as MT, the main influence on charge carriers in graphene is the transformation of the aptamer's 3D configuration due to the binding of small molecules (Chen et al., 2019). We verified this assumption by demonstrating that buffer's ionic strength dramatically affects the overall sensitivity of the reported GFET aptasensors. ...
Mycotoxins comprise a frequent type of toxins present in food and feed. The problem of mycotoxin contamination has been recently aggravated due to the increased complexity of the farm-to-fork chains, resulting in negative effects on human and animal health and, consequently, economics. The easy-to-use, on-site, on-demand, and rapid monitoring of mycotoxins in food/feed is highly desired. In this work, we report on an advanced mycotoxin biosensor based on an array of graphene field-effect transistors integrated on a single silicon chip. A specifically designed aptamer against Ochratoxin A (OTA) was used as a recognition element, where it was covalently attached to graphene surface via pyrenebutanoic acid, succinimidyl ester (PBASE) chemistry. Namely, an electric field stimulation was used to promote more efficient π-π stacking of PBASE to graphene. The specific G-rich aptamer strand suggest its π-π stacking on graphene in free-standing regime and reconfiguration in G-quadruplex during binding an OTA molecule. This realistic behavior of the aptamer is sensitive to the ionic strength of the analyte solution, demonstrating a 10-fold increase in sensitivity at low ionic strengths. The graphene-aptamer sensors reported here demonstrate fast assay with the lowest detection limit of 1.4 pM for OTA within a response time as low as 10 s, which is more than 30 times faster compared to any other reported aptamer-based methods for mycotoxin detection. The sensors hold comparable performance when operated in real-time within a complex matrix of wine without additional time-consuming pre-treatment.
... FETs have been used in pharmaceutical applications such as detection of i) antibiotics, like kanamycin A [69], kanamycin, tobramycin [70] tenofovir [71] and penicillin G [72]; ii) antiinflammatory drugs, like lupeol [31] and β-cyclodextrin [73,74], iii) anticoagulant drug, like heparin [75] and iv) vasopressor, inotropic drug, like dopamine [31]. Representatives of these drug families exhibited in this review were chosen according to their relevance in the literature and in the recently published works in which FETs were involved. ...
... Inhaled antibiotic like Tobramycin is highly effective and improves delivery to the infection site, giving more than 1000 times higher drug levels in the sputum than in serum [108,109]. Chen et al. [70] fabricated a FET reduced graphene oxide (rGO) and RNA-APT for tobramycin / blocking layer (BL) detection in static water samples ( Table 2). Given the chemical and morphological complementarity of tobramycin and the aptamer, a stable three-dimensional "hairpin" structure was formed. ...
... At low concentrations, tobramycin molecules were captured thanks to the specific affinity to the aptamer by hydrophobic interactions rather than by the physical adsorption on rGO. At high concentrations, there is an accumulation of tobramycin molecules, a saturation of the aptamer probes, a decrease in the rGO holes' density, a positive charge of the rGO's surface and a diffusion effect on the rGO generating a reduction in the mobility of carriers [70]. The analytical performance of FET with rGO / aptamer / BL is characterized by an LR ranging from 0 to 4.675 mg/L and a LoD 0.14 mg/L. ...
Field-effect transistors (FETs) are one of the most widely-used electronic sensors for continuous monitoring and detection of contaminants such as pharmaceuticals and endocrine-disrupting compounds at low concentrations. FETs have been successfully utilized for the rapid analysis of these environmental pollutants due to their advantageous material properties like the disposability, rapid responses and simplicity. This paper presented an up-to-date overview of applied strategies with different bio-based materials in order to enhance the analytical performances of the designed sensors. Comparison and discussion were made between characteristics of recently engineered FET bio-sensors used for the detection of famous and selected pharmaceutical compounds in the literature. The recent progress in environmental research applications, comments on interesting trends, current challenge for future research in endocrine-disrupting chemicals’ (EDCs) detection using FETs biosensors were highlighted.
... One of the specific features in the use of graphene sensor for small molecule detection is the large intrinsic charges of molecules that could provide higher sensitivity in the conductivity change of the graphene channel. GFETs have previously been used for the highly sensitive detection of various antibiotics [8], small antigens [9], and small molecule drugs [10]. While sensitivity and response time are mainly defined by the physical nature of the graphene channel, selectivity is provided by the specific recognition elements, i.e., bioreceptors such as enzymes, antibodies and aptamers. ...
... Aptamers are oligonucleotides in a typical size range of 20 to 70 nucleic bases that form a specific three-dimensional structure during analyte capture. The oligonucleotides have intrinsic charges distributed over their backbone, and their deformation can bring charges closer to or further from the graphene surface, providing the sensing signal [8,9]. Different sensing principles based on aptamers have been demonstrated for mycotoxin detection, such as fluorescence [12], surface plasmon resonance [13], spectral-phase interferometry [14], chemiluminescence [15], and electrochemistry [16]. ...
... In this work, we report on an array of optimized GFET-based aptasensors on a single chip used to detect mycotoxins that can provide better statistical data analysis generated by the sensors. Since the size of an aptamer is larger than the size of a small molecule, such as MT, the main influence on charge carriers in graphene is the transformation of the aptamer's 3D configuration due to the binding of small molecules [8]. Such advanced technology allowed us to track the processes of mycotoxin binding in real time. ...
Mycotoxins comprise a frequent type of toxins present in food and feed. The problem of mycotoxin contamination has been recently aggravated due to the increased complexity of the farm-to-fork chains, resulting in negative effects on human and animal health and, consequently, economics. The easy-to-use, on-site, on-demand, and rapid monitoring of mycotoxins in food/feed is highly desired. In this work, we report on an advanced bioelectronic mycotoxin sensor based on graphene field-effect transistors integrated on a silicon chip. A specific aptamer for Ochratoxin A (OTA) was attached to graphene through covalent bonding with the pyrene-based linker, which was deposited with an electric field stimulation to increase the surface coverage. This graphene/aptamer sensor demonstrates high sensitivity to OTA with the lowest detection limit of 1.4 pM within a response time of 10 s which is superior to any other reported aptamer-based methods.
... With the continuous improvement of breeding industry, numerous antibiotics have been used in livestock and poultry in the pursuit of economic benefits, resulting in the abuse of antibiotics and a great threat to human health [1,2]. ...
To explore the adsorption performance of antibiotics in different amphoteric clays loaded with magnesium (Mg) and dodecyl dimethyl betaine (BS) was used to modify bentonite (B), kaolin (K), and diatomite (D) to obtain different amphoteric clays (named as BS-B, BS-K, and BS-D, respectively). Then, Mg-loaded amphotropic clays (abbreviated as Mg-BS-B, Mg-BS-K, and Mg-BS-D, respectively) were obtained by loading Mg ions on BS-B, BS-K, and BS-D. The isother-mal adsorption characteristics of tetracycline (TC), chlortetracycline (CTC), and oxytetracycline (OTC) were studied by batch treatment with B, K, and D as the controls, and the adsorption differences under different environmental factors (i.e., temperature, pH, and ionic strength) were compared. The results show that the following. (1) The TC, CTC, and OTC adsorptions of the tested samples were all suitable for Langmuir isothermal adsorption model, and the maximum adsorption capacities (q m) were 1.70-5.21 mol/kg (TC), 1.80-5.94 mol/kg (CTC), and 1.81-6.28 mol/ kg (OTC). Under the same modification conditions, the q m of TC, CTC, and OTC followed the order Mg-BS-B > Mg-BS-K > Mg-BS-D. (2) When the temperature changed from 25°C to 45°C, the adsorption amount of TC, CTC, and OTC on the tested samples increased, exhibiting a positive temperature effect. The thermodynamic parameters showed that the adsorption of TC, CTC, and OTC was spontaneous, endothermic, and entropic-_increasing processes. (3) In the pH range of 2-10, the adsorption amount of TC, CTC, and OTC on each soil sample increased first and then decreased and reached the peak value at pH = 6. With the increase of the ionic strength, the adsorption amount of the three antibiotics decreased, and the decrease ranges were 15.17%-84.17% (TC), 16.07%-68.07% (CTC) and 16.30%-76.54% (OTC).
... Similarly, another study demonstrated the development of a multicolor aptasensor for simultaneous detection of inorganic (Hg 2+ ) and organic mercury (CH 3 Hg + and C 2 H 5 Hg + ) using T rich DNA probe and gold nanorods (X. Chen et al., 2019a). The method showed 2 ppm and 10 ppm detection limits for Hg 2+ and organic mercury, respectively. ...
Chemical and biological contaminants are of primary concern in ensuring seafood safety. Rapid detection of such contaminants is needed to keep us safe from being affected. For over three decades, immunoassay (IA) technology has been used for the detection of contaminants in seafood products. However, limitations inherent to antibody generation against small molecular targets that cannot elicit an immune response, along with the instability of antibodies under ambient conditions greatly limit their wider application for developing robust detection and monitoring tools, particularly for non-biomedical applications. As an alternative, aptamer-based biosensors (aptasensors) have emerged as a powerful yet robust analytical tool for detection of a wide range of analytes. Due to the high specificity of aptamers in recognising targets ranging from small molecules to large proteins and even whole cells, these have been suggested to be viable molecular recognition elements (MREs) in the development of new diagnostic and biosensing tools for detecting a wide range of contaminants including heavy metals, antibiotics, pesticides, pathogens and biotoxins. In this review, we discuss the recent progress made in the field of aptasensors for detection of contaminants in seafood products with a view of effectively managing their potential human health hazards. A critical outlook is also provided to facilitate translation of aptasensors from academic laboratories to the mainstream seafood industry and consumer applications.
... For example, monolayer graphene FETs have been used sensing for heavy metal cations, small molecules like acetylcholine or antibiotics, and larger proteins like virus antigen. [17][18][19][20][21][22] These examples rely on aptamers or proteins to facilitate molecular recognition and capture but depend on structural confirmation to retain binding function. Solutal variables influence biomolecular structure and function. ...
Electrical detection of messenger ribonucleic acid (mRNA) is a promising approach to enhancing transcriptomics and disease diagnostics because of its sensitivity, rapidity, and modularity. Reported here is a fast SARS-CoV-2 mRNA biosensor (<1 minute) with a limit of detection of 1 aM, and dynamic range of 4 orders of magnitude and a linear sensitivity of 22 mV per molar decade. These figures of merit were obtained on photoresistlessly patterned monolayer graphene field-effect transistors (FETs) derived from commercial four-inch graphene on 90 nm of silicon dioxide on p-type silicon. Then, to facilitate mRNA hybridization, graphene sensing mesa were coated with an ultrathin sub-percolation threshold gold film for bonding 3'-thiolated single-stranded deoxyribonucleic acid (ssDNA) probes complementary to SARS-CoV-2 nucleocapsid phosphoprotein (N) gene. Sub-percolated gold was used to minimize the distance between the graphene material and surface hybridization events. The liquid-transfer characteristics of the graphene FETs repeatedly shows correlation between the Dirac voltage and the copy number of polynucleotide. Ultrathin percolated gold films on graphene FETs facilitate two-dimensional electron gas (2DEG) mRNA biosensors for transcriptomic profiling.
... El principio de funcionamiento de los biosensores, se basa en el cambio de la distribución de cargas a lo largo de la superficie del grafeno y del potencial eléctrico al unirse con las moléculas diana. Posteriormente, se recoge la señal del transductor al medir las variaciones en conductancia, corriente, resistencia o voltaje(Yüce et al., 2021;Chen et al., 2019).El proceso de caracterización de los sensores es un paso fundamental en los artículos estudiados, mediante técnicas instrumentales como: voltamperometría de pulsos (dvp), espectroscopía de impedancia electroquímica, amperometría, voltamperometría cíclica, espectroscopía Raman, xps, sem, entre otras, se comprueba si las funcionalizaciones del grafeno con los enlazadores de detección están correctamente ensambladas. De manera que se mida, y verifique la fiabilidad y rendimiento de los biosensores.En todos los casos las caracterizaciones se dieron en 3 etapas, las superficies de grafeno sin funcionalización, superficies funcionalizadas con biorreceptores, y finalmente la respuesta a la unión con los analitos, de esta manera se fue corroborando y comprobando los cambios en el voltaje y la conductancia que se fueron produciendo al añadir al grafeno, las sondas y las moléculas diana.Principio de funcionamiento físico-químico Debido a la naturaleza hidrofóbica del grafeno monocapa, muchas de las reacciones biológicas no podrían llevarse a cabo, de ahí que es necesario añadir enlazadores como, por ejemplo, el ácido pirenobutírico (pba) o éster succinimidílico del ácido 1-pirenobutanoico (pbase) que constan de un grupo pireno y carboxílico, donde una vez funcionalizados con la capa de grafeno se unen mediante interacciones hidrófobas y de apilamiento π(Hinnemo et al., 2017).Las capas de grafeno interactúan fuertemente con las unidades de pireno del pba y pbase, gracias a la afinidad de la unión covalente entre los grupos carboxilos de los enlazadores y los grupos amino receptores de captura(Hinnemo et al., 2017), de esta forma sus propiedades se mantienen excelentemente conservadas. ...
facultad de ingeniería en geología, minas, petRóleos y ambiental universidad central del ecuador figempa: Investigación y Desarrollo 2021, vol 12(2), diciembre, pp. 70-84 abstract Due to the health emergency produced by SARS-CoV-2, which has generated a pandemic, this work proposes a review on developed methods for the detection of covid-19 based on graphene biosensors, considering their physicochemical properties. This research includes a compilation and analysis of information on this type of biosensors published in high-impact journals in recent years. For the development of the study, parameters such as detection time, detection limit, type of sensor, proteins that the biosensor detects, type of graphene, and cost were chosen to verify its effectiveness. The analyzed results demonstrate that most biosensors functionalizing the antibody of S, N protein or recombination of both, and some biosensors allow the detection of up to 4 types of proteins (C-reactive protein, IgG, IgM, and nucleapside). Several of the analyzed studies show a specific sequence detection of the virus and a low limit of detection (LOD) ranging from 0.1 fg/mL to 1 fg/mL, which allows detecting SARS-CoV-2 at low concentrations. In conclusion, the analysis indicates a feasible option for the implementation of graphe-ne-based biosensors as an alternative to traditional test. resumen Debido a la emergencia sanitaria producida por el SARS-CoV-2, que ha generado una pandemia, en este trabajo se propone una revisión sobre métodos desarrollados para la detección de covid-19 basados en biosensores de grafeno, considerando sus propiedades fisicoquímicas. Esta investigación abarca una recopilación y análisis de información sobre biosensores en revistas de alto impacto en los últimos dos años. Para el desarrollo del estudio, se escogieron parámetros como: tiempo de detección, límite de de-tección, tipo de sensor, proteínas que detectan el biosensor, tipo de grafeno y costo, a fin de comprobar su efectividad. Los resultados analizados demuestran que la mayoría de biosensores funcionalizan el anticuerpo de la proteína S, N, o una recombinación de ambas, y algunos biosensores permiten la detec-ción de hasta 4 tipos de proteínas (proteína reactiva C, IgG, IgM y nucleapside). Varios de los estudios analizados muestran una detección de secuencia específica del virus y un bajo límite de detección (LOD) que va desde 0,1 fg/mL hasta a 1 fg/mL, lo que permite detectar SARS-CoV-2 a bajas concentraciones. El análisis indica una opción factible para la implementación de biosensores basados en grafeno como alternativa a las pruebas tradicionales introducción Desde diciembre de 2019 en la ciudad de Wuhan, China , se reportaron los primeros casos del nuevo coronavi-rus, conocido como sars-cov-2, mucho más contagioso que el mers del 2012 y el sars del 2002, que presentaba una tasa de transmisión muy elevada, el cual se propagó rápidamente por todo el planeta, provocando una pan-demia de carácter mundial. Según la Organización Mundial de la Salud (oms), una de las principales acciones para contener tanto el conta-gio como la propagación se centra en el aislamiento de las personas infectadas, quienes deben permanecer en cuarentena quince días. Los pacientes que han sido diag-nosticados con el nuevo virus presentan sintomatologías como: tos, fiebre, opresión en el pecho, dolor de cabeza, entre otros síntomas agudos. Sin embargo, lo más grave historial del artículo Recepción
... El principio de funcionamiento de los biosensores, se basa en el cambio de la distribución de cargas a lo largo de la superficie del grafeno y del potencial eléctrico al unirse con las moléculas diana. Posteriormente, se recoge la señal del transductor al medir las variaciones en conductancia, corriente, resistencia o voltaje (Yüce et al., 2021;Chen et al., 2019). ...
En una época densa, sinuosa, llena de trampas, se entrecruzan, se interrumpen y se corresponden y terminarán uniéndose al infinito como experiencia límite la sobrevivencia de la especie y de su entorno, por tanto, de nuestra casa, nuestro planeta. Tratemos de ver la luz al final del túnel y no solo como una forma discursiva sino como algo nuevo con perspectivas que generen un eco hacia la vida, la innovación, el humanismo y poder escapar a los estereotipos y cadenas, tal vez nos causen vértigo, pero es un camino que nos lleva a encontrarnos a nosotros mismos en la vida cotidiana con un aprendizaje nuevo que no esté sujeto al azar en el destino de los hombres. Somos afortunados, entendido en el sentido de suerte, pero sabemos que para el inconsciente nada es imprevisible y para la filosofía no hay casualidades.
... El principio de funcionamiento de los biosensores, se basa en el cambio de la distribución de cargas a lo largo de la superficie del grafeno y del potencial eléctrico al unirse con las moléculas diana. Posteriormente, se recoge la señal del transductor al medir las variaciones en conductancia, corriente, resistencia o voltaje(Yüce et al., 2021;Chen et al., 2019).El proceso de caracterización de los sensores es un paso fundamental en los artículos estudiados, mediante técnicas instrumentales como: voltamperometría de pulsos (dvp), espectroscopía de impedancia electroquímica, amperometría, voltamperometría cíclica, espectroscopía Raman, xps, sem, entre otras, se comprueba si las funcionalizaciones del grafeno con los enlazadores de detección están correctamente ensambladas. De manera que se mida, y verifique la fiabilidad y rendimiento de los biosensores.En todos los casos las caracterizaciones se dieron en 3 etapas, las superficies de grafeno sin funcionalización, superficies funcionalizadas con biorreceptores, y finalmente la respuesta a la unión con los analitos, de esta manera se fue corroborando y comprobando los cambios en el voltaje y la conductancia que se fueron produciendo al añadir al grafeno, las sondas y las moléculas diana.Principio de funcionamiento físico-químico Debido a la naturaleza hidrofóbica del grafeno monocapa, muchas de las reacciones biológicas no podrían llevarse a cabo, de ahí que es necesario añadir enlazadores como, por ejemplo, el ácido pirenobutírico (pba) o éster succinimidílico del ácido 1-pirenobutanoico (pbase) que constan de un grupo pireno y carboxílico, donde una vez funcionalizados con la capa de grafeno se unen mediante interacciones hidrófobas y de apilamiento π(Hinnemo et al., 2017).Las capas de grafeno interactúan fuertemente con las unidades de pireno del pba y pbase, gracias a la afinidad de la unión covalente entre los grupos carboxilos de los enlazadores y los grupos amino receptores de captura(Hinnemo et al., 2017), de esta forma sus propiedades se mantienen excelentemente conservadas. ...
Debido a la emergencia sanitaria producida por el SARS-CoV-2 que ha generado una pandemia, en este trabajo se propone una revisión sobre métodos desarrollados para la detección de Covid-19 basados en biosensores de grafeno, considerando sus propiedades fisicoquímicas. Esta investigación abarca una recopilación y análisis de información sobre biosensores en revistas de alto impacto en los últimos dos años. Para el desarrollo del estudio, se escogieron parámetros como: tiempo de detección, límite de detección, tipo de sensor, proteínas que detecta el biosensor, tipo de grafeno y costo, a fin de comprobar su efectividad. Los resultados analizados demuestran que la mayoría de biosensores funcionalizan el anticuerpo de la proteína S, N o una recombinación de ambas, y, algunos biosensores permiten la detección de hasta 4 tipos de proteínas (proteína reactiva C, IgG, IgM y nucleapside). Varios de los estudios analizados muestran una detección de secuencia especifica del virus y un bajo límite de detección (LOD) que va desde 0,1 fg/mL hasta a 1 fg/mL, lo que permite detectar SARS-CoV-2 a bajas concentraciones. El análisis indica una opción factible para la implementación de biosensores basados en grafeno como alternativa a las pruebas tradicionales.
... Hence, constructing an electrochemical sensor to see CIP level with quick response, highly selective, and sensitive detection is much needed. Various techniques have been employed to determine CIP concentration, such as electrochemical technique [7,8], field-effect transistor (FET) sensor [9], capillary electrophoreses [10], fluorimetry [11], immunoassays [12], spectrophotometry [13], and highperformance liquid chromatography (HPLC) [14,15]. Among all techniques, the electrochemical technique is viable because of several advantages: low-cost, facile miniaturization, easy handle, quick response, high sensitivity, and selectivity in detecting the target analyte [16,17]. ...
Ciprofloxacin (CIP) electrochemical sensor was constructed using cobalt-iron Prussian blue analogs decorated on carbon nitride (Co-Fe-PBA@CN). Co-Fe-PBA decorated on CN was fabricated using a simple sonication-assisted hydrothermal method to prepare the composite to obtain a cube-shaped structure decorated on CN sheets. The fabricated Co-Fe-PBA@CN was physically characterized using XRD and SEM analysis. Then, the fabricated composite was electrochemically studied to sense antibiotic drug ciprofloxacin (CIP). The electrochemical behavior was investigated using tools such as cyclic voltammetry (CV) and amperometric I-t studies. The Co-Fe-PBA@CN modified electrode displays a wide linear range (0.005–300 and 325–741 μM) with a low detection limit (0.7389 and 1.0313 nM) and good sensitivity (0.3157 and 0.2263 μA.μM⁻¹cm⁻²) toward CIP. The Co-Fe-PBA@CN modified electrode also exhibits good selectivity, reproducibility, and repeatability toward CIP. The proposed sensor was validated with real sample analysis, biological samples like urine and blood serum containing commercially available ciprofloxacin tablets were studied, and the results demonstrate good viability.
Graphical abstract
... Although these methods are sensitive and selective for detection of tetracycline, the methods are expensive and require intricate sample preparation. Aptamers are small sequences of single stranded oligonucleotide of RNA or DNA able of good binding affinity toward the various targets such as ions, toxins, viruses, bacteria, enzymes, proteins, antibiotics, and so on, owing to their three-dimensional structures [17,18]. Compared to antibodies, aptamers have prominent features including low cost, binding affinity to specific targets, reusability, hight stability in the different temperature and pH conditions, ease of production and modification, low immunogenicity. ...
In this research, a screening procedure was applied for designing new aptamers with the enhanced binding affinity for tetracycline detection through a common theoretical and experimental study. In the first step, among the specific aptamers introduced from the experimental studies, the 8-mer aptamer was chosen toward tetracycline with a low limit of detection. The different mutants were designed by changing the nucleotides of the native sequence and, their MD simulations were performed in the presence of tetracycline. The conformational factor (Pi) was computed as a parameter that indicates the affinity of each aptamer nucleotides to target. To calculate the ΔGbind as a suitable factor for the specificity of aptamer toward the target, the umbrella sampling simulation was applied. Theoretical results proved that some of the mutants, such as the M-5T and M-5C mutants possess enhanced binding affinity toward tetracycline compared to the native aptamer. In the next step, the enhanced selective detection of designed mutants toward tetracycline was investigated by utilizing an easy colorimetric test relying on the gold nanoparticles (AuNPs). Based on the experimental outcomes, the limit of detection values of 159, 1.2 and, 0.1 pM were determined for the native, M-5T and, M-5C aptamers, respectively. The results of colorimetric showed that the designed mutants have good selectivity to tetracycline compared to other antibiotics. Besides, the designed mutants were successfully applied to detect tetracycline in milk samples. The agreement among the theoretical and experimental results proves the ability of theoretical approaches for designing the new aptamers with enhanced binding affinity to identify different targets.
... For example, GFETs functionalization with aptamers has been reported for human thrombin proteins [223] and interferongamma detection [190]. Similarly, RNA aptamers have also been used for small molecule detection, such as antibiotic tobramycin [224]. ...
Ever since the more than decade-old discovery of the mechanical exfoliation method for graphene isolation, this miraculous 2-dimensional material is still widely used in various applications because of its exceptional electron mobility and thermal conductivity. Graphene, commonly grown on a metallic substrate using chemical vapor deposition (CVD), needs to be transferred onto dielectric substrates compatible with complementary metal oxideesemiconductor (CMOS) technology for various electronic and optical applications. However, the ultra-clean transfer of graphene with defect-free is still crucial for large-area graphene devices' efficiency. This review introduces a comprehensive and up-to-date account of the transfer of the most attention kinds of CVD-grown graphene on copper substrates. The advances and main challenges of both wet and dry transfer methods are also carefully described. Particular emphasis is also given on graphene-based BioFET devices, revising their sensing mechanism and the optimum operational conditions toward high specificity and sensitivity. The authors have been convinced that upgrading the transfer process to accomplish the cleanest graphene surface and exploiting the optimum operating conditions will undoubtedly be of considerable significance to fabricate graphene-based devices.
... Localized surface plasmon resonance (LSPR) sensor detects the SARS-CoV-2 nucleic acid with combined use of photo-thermal effect and plasmon sensing [42]. In FET-based biosensors, biological molecules modify the charge distribution of the surface, or they generate a surface potential by binding to the surface, which is further measured as a conductance value [43]. For mass screening of such pandemic, we need a global e-platform to control the spread of the virus which is now possible with emergence of data science and advancement in mobile telecommunications. ...
In December 2019, an unexpected outbreak was caused by novel corona virus, severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). The lung disease caused by SARS-CoV-2 was given the name of the novel coronavirus disease 2019 (COVID-19) by the World Health Organization (WHO) on February 11, 2020. Since its origin in the Hubei province of Wuhan city in China, now it has spread to 218 countries worldwide. Panic situation created by COVID-19 has compelled researchers and doctors to work collaboratively. To combat with the disease, every control measures are under consideration from drug discovery to vaccine development. In the management of disease, rapid diagnosis is equally important as development of vaccine and drug. At present, various diagnostic kits are available for COVID-19. With the disease progression, global demand for diagnostics is raising. So, this chapter will include the updates on efficient diagnostic assays and future of diagnostic.
... With the development of FET-based biosensors, they have been applied to diagnosing the viral disease, point-of-care testing, on-site detection, and detecting small molecules [98]. FET-based biosensors are based on semiconductor materials such as graphene, titanium oxide, etc., which can increase the efficacy and sensitivity in different device [101]. Recently, Changkyun Park and Seung Il Kim groups reported a FET-based biosensor device applied to detecting clinical samples infected with SARS-CoV-2. ...
The outbreak of severe pneumonia at the end of 2019 was proved to be caused by the SARS-CoV-2 virus spreading out the world. And COVID-19 spread rapidly through a terrible transmission way by human-to-human, which led to many suspected cases waiting to be diagnosed and huge daily samples needed to be tested by an effective and rapid detection method. With an increasing number of COVID-19 infections, medical pressure is severe. Therefore, more efficient and accurate diagnosis methods were keen urgently established. In this review, we summarized several methods that can rapidly and sensitively identify COVID-19; some of them are widely used as the diagnostic techniques for SARS-CoV-2 in various countries, some diagnostic technologies refer to SARS (Severe Acute Respiratory Syndrome) or/and MERS (Middle East Respiratory Syndrome) detection, which may provide potential diagnosis ideas.
... These devices present high sensitivity for various analytes and operate at low gate potentials due to the nanosized electrical double layer (EDL) at the graphene/solution interface [8]. There is a broad range of applications of rGO as FET-based sensors including: (i) the detection of new analytes such as biomarkers for diagnosis [9], (ii) the use of new receptors for (bio) molecular recognition, aiming to increase selectivity [10], and (iii) innovations in the method of manufacturing the transistors [11]. ...
In this study, graphene oxide (GO) has been reduced in two different ways for the production of oppositely charged reduced graphene oxide (rGO) sheets. One reduction route consisted of the covalent modification of GO with (3-aminopropyl) triethoxysilane and subsequent chemical reduction to produce positively charged rGO. In the second route employed, GO was reduced in a domestic microwave oven, in which the presence of urea doped the material with nitrogen, increasing its electrical conductivity considerably. Multilayers of oppositely charged rGO were manufactured using a layer-by-layer (LbL) assembly technique. The kinetics and growth of multilayers were monitored by UV-Vis absorption spectroscopy and quartz crystal microbalance. rGO multilayers on the interdigitated gold electrodes originate high conductive films, in which the number of deposited layers controls the conductivity. As a solution-gated field-effect transistor, the devices presented high transconductance; (90 µS and 55 µS for holes and electrons, respectively). Upon modification of the LbL films with papain, used as a biological recognition element, the devices were capable of detecting Cystatin C protein (a chronic renal disease biomarker) in synthetic urine in concentrations as low as 5 ng.mL⁻¹. Therefore, the proposed transistors proposed here represent interesting alternatives as novel sensors and biosensors platforms.
Adenosine triphosphate (ATP) is closely related to the pathogenesis of certain diseases, so the detection of trace ATP is of great significance to disease diagnosis and drug development. Graphene field-effect transistors (GFETs) have been proven to be a promising platform for the rapid and accurate detection of small molecules, while the Debye shielding limits the sensitive detection in real samples. Here, a three-dimensional wrinkled graphene field-effect transistor (3D WG-FET) biosensor for ultra-sensitive detection of ATP is demonstrated. The lowest detection limit of 3D WG-FET for analyzing ATP is down to 3.01 aM, which is much lower than the reported results. In addition, the 3D WG-FET biosensor shows a good linear electrical response to ATP concentrations in a broad range of detection from 10 aM to 10 pM. Meanwhile, we achieved ultra-sensitive (LOD: 10 aM) and quantitative (range from 10 aM to 100 fM) measurements of ATP in human serum. The 3D WG-FET also exhibits high specificity. This work may provide a novel approach to improve the sensitivity for the detection of ATP in complex biological matrix, showing a broad application value for early clinical diagnosis and food health monitoring.
Probes such as carbon dots (C-dots) have extensive and important applications in the quantitative analysis of complex biological and environmental systems. However, the development of probes is often hindered by incomplete selectivity, i.e., a probe that responds to one substance is also prone to respond to coexisting structurally similar substances. Therefore, the above dilemma often leads to be developed as semi-selective probes, so that the development of probes is abandoned halfway. This work shows how a semi-selective probe can enhance selectivity by combining a proper multivariate calibration model. Primarily, we developed a semi-selective fluorescent probe that responded to tetracyclines (TCs) with discarded tobacco leaves. Then, we introduced the multivariate quantitative fluorescence model (QFM) to enhance its selectivity and solve the problem of fluorescence spectral shift. For the determination of chlortetracycline (CTC) with this semi-selective C-dots probe in mineral and lake water samples and compared to the traditional quantitative model, the introduced QFM resulted in an average relative predictive error (ARPE) in mineral water spiked samples decreased from 57.1 to 5.6%, which reduced the ARPE in the lake water spiked samples from 18.1 to 4.7%. The above results show that the QFM-assisted semi-selective probe C-dots strategy (QFMC-dots) can enhance selectivity, and QFMC-dots achieved high-selective and accurate determination of CTC in interfering mineral and lake water samples, with the limit of detection and limit of quantitation of 0.55 and 1.66 μM, respectively. The proposed strategy of enhancing selectivity by introducing a proper multivariate calibration model can reduce the difficulty and increase success rate of developing probes, which can be expected to provide an interesting alternative for the development of probes, especially when encountering semi-selective problems.
Molybdenum disulfide (MoS2) nanolayers are one of the most promising two-dimensional (2D) nanomaterials for constructing next-generation field-effect transistor (FET) biosensors. In this article, we report an ultrasensitive FET biosensor that integrates a novel format of 2D MoS2, vertically-aligned MoS2 nanolayers (VAMNs), as the channel material for label-free detection of the prostate-specific antigen (PSA). The developed VAMNs-based FET biosensor shows two distinctive advantages. First, the VAMNs can be facilely grown using the conventional chemical vapor deposition (CVD) method, permitting easy fabrication and potential mass device production. Second, the unique advantage of the VAMNs for biosensor development lies in its abundant surface-exposed active edge sites that possess a high binding affinity with thiol-based linkers, which overcomes the challenge of molecule functionalization on the conventional planar MoS2 nanolayers. The high binding affinity between 11-mercaptoundecanoic acid and the VAMNs was demonstrated through experimental surface characterization and theoretical calculations via density functional theory. The FET biosensor allows rapid (within 20 min) and ultrasensitive PSA detection in human serum with simple operations (limit of detection: 800 fg mL-1). This FET biosensor offers excellent features such as ultrahigh sensitivity, ease of fabrication, and short assay time, and thereby possesses significant potential for early-stage diagnosis of life-threatening diseases.
Two-dimensional (2D) black phosphorus (BP) has been reported to have appealing semiconducting properties as the sensing channel in field-effect transistor (FET) sensors. However, the intrinsic instability of BP in water greatly hinders its application, and little is known about its sensing performance and mechanism in aqueous medium. Herein, a water-stable BP FET sensor for antibiotic detection is reported. A novel surface engineering strategy with Ag+ coordination and melamine cyanurate (MC) supramolecular passivation is utilized to enhance the stability and transistor performance of BP. With molecularly imprinted polymers (MIPs) as the detection probe for tetracycline, the BPAg(+)/MC/MIPs sensor shows high sensitivity to tetracycline with a detection limit of 7.94 nM and a quick response within 6 s as well as high selectivity against other antibiotics with similar molecular structures. A new sensing mechanism relying on the conjugation effect of the probe structure is proposed, and new knowledge about alkalinity-enhanced and ionic strength-related response from the electrostatic gating effect is given based on the solution chemistry impact study. This work offers an efficient surface engineering strategy to enable the application of 2D BP for antibiotic detection in aqueous medium and presents a new sensing mechanism in chemical analysis by FET sensors.
Paraquat (PQ) is a nonselective contact herbicide used in agriculture for the control of broad leaf weeds, which would cause irreversible damage to human organs even at very low concentrations. Therefore, the trace residue detection of PQ in the environment is of vital importance. Here, a novel graphene electrochemical transistor (GECT) for PQ detection is reported for the first time. The key to the device design is the application of a layer of Ag nanoparticle (Ag NP) modified monolayer graphene as the channel layer. Due to the good electrochemical activity of Ag NPs for PQ detection, the device exhibits excellent sensitivity for PQ with the detection limit of 0.068 nM and a wide linear range from 0.1 nM to 5 mM. The GECT sensor also reveals good selectivity toward several common interferents and exhibits satisfactory recoveries for PQ detection when using Chinese cabbage as a simulant to deduce the real detection situation. The GECT sensor not only provides an efficient method for the detection of PQ residues, but also provides an effective grafting platform for the construction of novel high-sensitivity electrochemical sensors.
Oxacillin sodium (OXS) is a typical antibiotic contaminant in water and belongs to the semi-synthetic penicillin category. OXS is toxic to human cells and may damage the immune system when it enters the human body. In this study, we propose an optical fiber sensor to detect antibiotic pollutants in water based on the photothermal effect of OXS with a polydimethylsiloxane (PDMS) /Ti
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CN MXene composite-coated microfiber. The interaction between the evanescent field and OXS can be enhanced by the coated microfiber, which improves the sensor performance. Moreover, the coated microfiber can enhance the detection sensitivity owing to the high thermo-optic coefficient of PDMS and the strong molecular adsorption of Ti
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CN MXene. The results show that using the PDMS/Ti
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CN MXene composite-coated microfiber, detection in the linear range of 0.02–0.1 mg/ml with a sensitivity of -761.39 nm/(mg/ml), and a detection limit of 26 ng/ml are achieved. Compared to that of an uncoated microfiber, the sensitivity of the composited-coated microfiber is improved by a factor of 6. The proposed sensor does not require solvent extraction or complex antibody preparation; therefore, it is easy to operate and exhibits a high sensitivity. Furthermore, the sensor has potential applications in food safety and environmental pollutant detection.
In order to effectively monitor a wide variety of sulfonamides residues in the environment, group-targeting immunoassay based on the group-specific antibodies has attracted great attentions, which can realize the detection of a group of contaminants in environment as many as possible even the unrecognized ones. Indirect competitive immunoassay is generally adopted for small molecule detection however the rational design of immobilized coating antigen for improved recognition capability on the solid surface is far from enough. To cover the research gap, we proposed the design criteria of coating antigen for surface-based indirect competitive immunoassay based on the molecular docking. Taking the group-specific antibodies against sulfonamides (SA) as a proof-of-concept, a hapten with a linking arm with 3 methyl groups was selected to synthesize the coating antigen. Through surface immobilization of coating antigen, a portable biosensor for group-targeting immunoassay of sulfonamides was developed and demonstrated excellent performance with detection limits lower than 0.6 μg/L for four SA variants, and the cross-reactivities of 148–215 % relative to sulfadiazine. The recovery rates of SAs in liquid milk ranges from 87 to 97 %, which confirmed the application potential of this method in the determination of SAs. Its capability to measure total SAs in a simple and low-cost way would pave the way for a variety of application fields.
In recent years, the significance of biosensors has increased rapidly due to the growing demand for rapid detection of various biomarkers with high selectivity and sensitivity. Among different biosensors, Graphene Field Effect Transistor (Gr-FET) based biosensors has emerged as a promising device and exhibited wide range of application prospects. Gr-FET biosensors are ideal for ultra-sensitive immunological diagnosis applications as it can sense surrounding changes on their surface with low noise. Recently Gr-FET based biosensors have gained profound research interest among scientific community because of its ability in detection of SARS-CoV-2 (corona virus-2). This review article highlights the sensing performance and characteristics of different Gr-FET biosensors like DNA sensor, RNA sensor, glucose sensor, lactose sensor, protein sensor, pH sensor, various bacteria and virus detecting sensors etc.This article also critically reviews the recent progress in Gr-FET based SARS- CoV-2 covid-19 virus detection bio-sensors.
The large-scale use of antibiotics and the resulting drug residues poses a significant threat to global human health. Waste discharge and biological chain transmission are closely linked to residual antibiotic pollution in the fields of medicine, environmental monitoring, and food safety. Monitoring drug dosage in medicines and the detection of trace antibiotic residues in environmental and food matrices is therefore especially important. Microfluidic technology allows manipulation and flexible design of micro/nanofluids and is thus an essential means of antibiotic detection and analysis. Herein, we review recent progress in the design and applications of microfluidic chips as biosensors for the analysis of antibiotic residue analysis over the past five years. The types of chip materials and combination of microfluidic chips with essential technologies involving optics, electrochemistry, and mass spectrometry are introduced, and the critical principles of antibiotic microfluidic analysis and its application in the three aforementioned fields are summarized.
Antibiotics are powerful tools to treat bacterial infections, but antibiotic pollution is becoming a severe threat to the effective treatment of human bacterial infections. The detection of antibiotics in water has been a crucial research area for bioassays in recent years. There is still an urgent need for a simple ultrasensitive detection approach to achieve accurate antibiotic detection at low concentrations. Herein, a field-effect transistor (FET)-based biosensor was developed using ultraclean graphene and an aptamer for ultrasensitive tetracycline detection. Using a newly designed camphor-rosin clean transfer (CRCT) scheme to prepare ultraclean graphene, the carrier mobility of the FET is found to be improved by more than 10 times compared with the FET prepared by the conventional PMMA transfer (CPT) method. Based on the FET, aptamer-functionalized transistor antibiotic biosensors were constructed and characterized. A dynamic detection range of 5 orders of magnitude, a sensitivity of 21.7 mV/decade, and a low detection limit of 100 fM are achieved for the CRCT-FET biosensors with good stability, which are much improved compared with the biosensor prepared by the CPT method. The antibiotic sensing and sensing performance enhancement mechanisms for the CRCT-FET biosensor were studied and analyzed based on experimental results and a biosensing model. Finally, the CRCT-FET biosensor was verified by detecting antibiotics in actual samples obtained from the entrances of Bohai Bay.
Performing sensitive and selective detection in a mixture is challenging for terahertz (THz) sensors. In light of this, many methods have been developed to detect molecules in complex samples using THz technology. Here we demonstrate a defect-rich monolayer graphene-coated metamaterial operating in the THz regime for pesticide sensing in a mixture through strong local interactions between graphene and external molecules. The monolayer graphene induces a 50% change in the resonant peak excited by the metamaterial absorber that could be easily distinguished by THz imaging. We experimentally show that the Fermi level of the graphene can be tuned by the addition of molecules, which agrees well with our simulation results. Taking chlorpyrifos methyl in the lixivium of rice as a sample, we further show the molecular sensing potential of this device, regardless of whether the target is in a mixture or not.
The discharge and migration of antibiotics in the environment become a threat to human health and pose long term impact on ecological security, which leads to a great need for efficient analytical methods for antibiotic monitoring. To tackle this demand, various strategies for antibiotics detection have been developed in the past decades. This review article comprehensively summarizes recent progress in antibiotic monitoring with an emphasis on antibiotic analysis in environmental samples including food, biological sample, water and wastewater, soil, manure, and solid waste. The working principles and detection performances of these methods are introduced. The existing challenges and future directions for antibiotic monitoring are discussed, which is instructive for the development of advanced antibiotic analysis techniques for efficient monitoring and control of antibiotic pollution in the environment.
Antibiotics are often used in human and veterinary medicine for the treatment of bacterial diseases. However, extensive use of antibiotics in agriculture can result in the contamination of common food staples such as milk. Consumption of contaminated products can cause serious illness and a rise in antibiotic resistance. Conventional methods of antibiotics detection such are microbiological assays chromatographic and mass spectroscopy methods are sensitive; however, they require qualified personnel, expensive instruments, and sample pretreatment. Biosensor technology can overcome these drawbacks. This review is focused on the recent achievements in the electrochemical biosensors based on nucleic acid aptamers for antibiotic detection. A brief explanation of conventional methods of antibiotic detection is also provided. The methods of the aptamer selection are explained, together with the approach used for the improvement of aptamer affinity by post-SELEX modification and computer modeling. The substantial focus of this review is on the explanation of the principles of the electrochemical detection of antibiotics by aptasensors and on recent achievements in the development of electrochemical aptasensors. The current trends and problems in practical applications of aptasensors are also discussed.
Despite significant eradication efforts, malaria remains a persistent infectious disease with high mortality due to the lack of efficient point-of-care (PoC) screening solutions required to manage low-density asymptomatic parasitemia. In response, we demonstrate a quantitative electrical biosensor based on system-integrated two-dimensional field-effect transistors (2DBioFETs) of reduced graphene oxide (rGO) as transducer for high sensitivity screening of the main malaria biomarker, Plasmodium falciparum lactate dehydrogenase (PfLDH). The 2DBioFETs were biofunctionalized with pyrene-modified 2008s aptamers as specific PfLDH receptors. While we systematically optimize biosensor interface for optimal performance, aptamer-protein transduction at 2DBioFETs is elucidated based on delineation of charge and capacitance in an updated analytical model for two-dimensional rGO/biofunctional layer/electrolyte (2DiBLE) interfaces. Our 2DBioFET-aptasensors display a limit-of-detection down to 0.78 fM (0.11 pg/mL), dynamic ranges over 9 orders of magnitude (subfemto to submicromolar), and high sensitivity and selectivity in human serum validating their diagnostic potential as rapid PoC tests for malarial management.
Antibiotics residue in food is a big threat to human being health and life. Development of simple and fast detection techniques targeting residual antibiotics are urgently needed for food safety. Many analytical techniques have been used for the detection of antibiotic residues in food. Among these analytical techniques, microfluidic analysis gains increasing attention due to its advantages of low-cost, easy to carry, high integration, simple operation, and fast detection. In this review, we summarized the microfluidic devices applied in the analysis of antibiotic residues in food, mainly focusing on their detection techniques (including fluorescence, chemiluminescence, surface enhanced Raman spectroscopy, colorimetric method, electrochemical technique, and mass spectrometry), molecular recognition materials (such as antibodies, aptamers and molecularly imprinted polymers) and fabrication materials. Prospects and challenges of the microfluidic analysis platforms for practical applications were discussed in this review.
Graphene has received intensive research interest due to its remarkable charge mobility, and the efforts in the use of graphene-based field effect transistors (GFETs) for the sensing of biological biomarkers is on the rise. Because of the high non-specific protein adsorption on graphene, well-defined surface modification strategies have to be implemented to benefit from the excellent electronic transfer characteristics of GFET devices for specific detection of biomarkers. Surprisingly, while pyrene-based ligands are the most widely used graphene surface anchors for sensing-related applications, no systematic investigation on the reaction conditions employed and the influence of pyrene functionalities has been reported so far. As this is one of the essential steps for efficient receptor integration and sensitive sensing, by using GFET-based analysis of cardiac troponin I (cTnI) as the model compound we will show that an optimized pyrene–maleimide ligand incubation time on graphene of 2 h gives the best sensing performance. This study not only will be a guideline for researchers interested in GFET biosensors but also will hopefully allow industrial GFET development in a faster path.
The pollution and damages caused by antibiotics in water have aroused serious concerns. Metal-organic frameworks (MOF), which are hotly investigated as a novel kind of sensing materials, are tentatively applied...
Four coordination polymers have been synthesized by using Zn(II)/Cd(II) salt and bis(imidazole) ligand in the presence of the different flexible phenylenediacetate isomers under hydrothermal conditions. The flexible trans-conformation pda and biyb ligands in complexes 1, 3, 4 afford the 2D (4,4)-connected layer, which are further stacked in an offset fashion with an ABAB sequence to propagate into a 3D supramolecular architecture through strong C–H···π and C–H⋯O interactions. Differently, the flexible cis-conformation pda and biyb ligands in 2 can be seen as “V” type building block, linking Zn(II) atoms to form a 3D helix network. The structural diversity of these complexes is mainly attributed to the different coordination modes and isomer conformations of the flexible phenylenediacetic acids and bis(imidazole) ligand. The fluorescence property application and mechanisms of four complexes for detecting antibiotic cefixime (CEF) have been researched. Compared with 1, 3, 4 complex 2 has higher quenching percentage, this may be because 2 is a 3D structure with a large hole (18.99 × 20.02 Å window). The detection limits of complexes 1–4 have been measured to be 0.23 μΜ, 0.34 μΜ, 0.37 μΜ, 0.38 μΜ, respectively. The theoretic calculation and UV–vis absorption experiments confirmed that the fluorescence quenching of complexes 1–4 toward cefixime (CEF) should be attributed to the electron transfer and the fluorescence inner filter effect between the fluorescent matter and the analyte.
Heavy metal ions are highly toxic for living organisms especially after bioaccumulation and biomagnification, which possess a serious threat to human health and ecological environment. The rapid, portable, and efficient analytical methods are urgently needed for the determination of heavy metals in different media. Due to the unique advantages of field‐effect transistor (FET) sensors including fast response, easy manipulation, small size, and high sensitivity, FET sensor has become a novel strategy for heavy metal ion monitoring and numerous attempts have been made for the analysis of various heavy metal ions (e.g., mercury, lead, arsenic, copper, cadmium, iron, and silver) in the past decade. Thus, it is of urgent need to systematically summarize recent advances of FET sensing strategies in fast and highly efficient detection of heavy metal ions. In this review, the representative FET sensing platforms for heavy metal ions are introduced with a focus on their working principle and sensing performance. Moreover, the limitations of current FET sensors as well as the gap between the research achievements and practical application requirements are also discussed. At last, future directions of FET sensors in heavy metal ion analysis are proposed, which provides guidance to the further development of FET sensors for monitoring heavy metal ions as well as other chemicals. Representative field‐effect transistor sensing platforms with 2D nanomaterial‐based channels for heavy metal ion analysis.
This work demonstrates the high-performance hydrogen peroxide (H
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) sensing field-effect transistor (FET) using reduced graphene oxide - polypyrrole (rGO/PPy) nanocomposites. The SiO
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trench type FET is fabricated using lithography and etching techniques. The fabricated SiO
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trench structure was used not only for holding H
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but also for sensing purpose. The morphology and structure of the rGO/PPy nanocomposites were analyzed and confirmed their bonding. The output electrical signal changes as the concentration of H
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increases. The device shows a fast response of 5 s and is highly stable with excellent sensitivity. The detection limit obtained is 10 pM at appropriate signal-to-noise ratio (S/N) of the sensing electrical signal. The device is high selectivity towards H
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. The device structure may be employed for other liquid sensing applications.
A fluorescent probe based on single metal-organic framework material without additional fluorophores and active sites can significantly improve the stability of the probe for detection, and has very important application value in environmental analysis and detection. In this paper, a simple and rapid fluorescence detection method was established with Zn-MOF, which realized the highly sensitive detection of tetracycline antibiotics and NH4+ in water. The prepared Zn-MOF has abundant pores and can exist stably in water. When tetracycline antibiotics are present in Zn-MOF aqueous solution, based on the unique coordination ability between Zn and N, tetracycline antibiotics rich in N will be adsorbed into the pore canals of MOF, and aggregation-induced luminescence will occur. The original non-fluorescent Zn-MOF will immediately produce yellow fluorescence, realizing the detection of tetracycline antibiotics in water, with the limit of detection reaching 0.017 μM in a linear range of 0.02-13 μM. Zn-MOF is further used for the detection of tetracycline antibiotics in actual samples of milk and honey. Oxytetracycline (OTC) with the best fluorescence response of tetracycline antibiotics was coated on Zn-MOF to synthesize OTC@Zn-MOF fluorescent probe. NH4+ will replace the original ligand of Zn-MOF, which will disintegrate MOF and release OTC, resulting in a fluorescence decrease. Therefore, NH4+ can be detected with low limit of detection (0.038 μM) in a linear range of 0 to 3 mM. The probe is expected to be able to detect ammonia in the environment.
In general, nanoscience technology can be best described as a medium of design, fabrication, and application of nanostructured materials, as well as a fundamental understanding of physicochemical properties and phenomena of nanomaterials and nanostructures. Owing to the fact they offer a plethora of perspectives for modern living and fascinating technological advancements, sensors that are based on different types of nanostructured materials have uplifted the technology to greater heights of late. Nanostructure-based sensors can detect biologically as well as environmentally pertinent target species with high exactitude. The recognition of the targeted species, which usually befalls through a controlled binding affair, is then communicated as a readable signal. In addition, the surface-functionalized nanostructured materials, comprising both inorganic and organic components, have recently been inspected as potential platforms for sensing applications and have huge advantages over other materials. In this extensive tutorial review, we have focused on the current development of functionalized and non-functionalized nanostructured materials that can be used in environmental and biological applications, in which these chromofluorogenic chemosensors can selectively and sensitively detect specific analytes of interest through different principles and mechanisms. Additionally, few pieces of literature on the fabrication of nanostructured materials-based sensor devices are also listed out.
Field-effect transistors (FETs) receive growing attention for gas detection owing to their superior sensing performance over traditional techniques. The sensitivity and selectivity of FET sensors can be enhanced by tuning the structure of channel materialsviadoping, surface functionalization, hybridization,etc.However, the intrinsic semiconductor characteristics of the channel material and its gas adsorption capacity largely determine the sensing performance. In this work, we compared the room-temperature sensing performance of FET sensors with few-layer graphene, black phosphorous (BP), and MoS2with mixed polymorphic phases (metallic 1T phase and semiconducting 2H phase), and 2H-MoS2as a channel material for formaldehyde. The sensing results indicate that 1T/2H-MoS2exhibits the best sensitivity, response time as well as selectivity for formaldehyde detection. The theoretical calculation demonstrates that 1T/2H-MoS2yields the optimum semiconducting properties and gas adsorption capability for formaldehyde over other 2D channels. Moreover, by investigating the sensing performance under humid conditions, it was discovered that high humidity enhances the sensing response. This study demonstrates that the regulation of the intrinsic electronic structures of the 2D semiconducting channel directly affects the gas detection performance.
The detection of dopamine, one of the neurotransmitters in cerebral physiology, is critical in studying brain activities and understanding brain functions. However, regenerative biosensor for monitoring dopamine in the progress of physiological and pathological events is still challenging, due to lack of the platform for repetitive on-line detection-regeneration cycle. Herein, we have developed a regenerated field effect transistor (FET) combined with in vivo monitoring system. In this biosensor, gold-coated magnetic nanoparticles (Fe3O4@AuNPs) acts as a regenerated recognition unit for dopamine. Just by simple removal of a permanent magnet, dopamine on the biosensor interface are catalyzed by tyrosinase, thus achieving the regeneration of the biosensor. As a result, this FET biosensor not only reveals high sensitivity and selectivity, but also exhibits excellent stability after 15 regeneration processing. This biosensor is capable of monitor dopamine with a linear range between 1 μmol L⁻¹ and 120 μmol L⁻¹ and low detection limit (DL) of 3.3 nmol L⁻¹. Then, the platform has been successfully applied in dopamine analysis in fish brain under global cerebral cortical neurons. This FET biosensor is the first to on-line and remote control the sensitivity and DL by permanent magnet. It opens the door to reusable, inexpensive and large-scale productions.
Antibiotics are widely used in the prevention and treatment of infectious diseases in animals due to its bactericidal or bacteriostatic action. Residual antibiotics and their metabolites pose great threats to human and animal health, such as potential carcinogenic and mutagenic effects, and bacterial resistances. Therefore, it is necessary and urgent to accurately monitor trace amounts of antibiotics in food samples. Up to now, many analytical methods have been reported for the determination of antibiotics. Biosensors with the advantages of high sensitivity, rapid response, easy miniaturization, and low price have been widely applied to the detection of antibiotics residues in past decades. This review offered an in-depth evaluation of recognition elements for antibiotic residues in diverse food matrices. In addition, it presented a systematical and critical review on signal amplification via various materials, focusing on recently developed nanomaterials. Finally, the review provided an outlook on the future concepts to help upgrade the sensing techniques for antibiotics in food.
In recent years, the abuse of antibiotics has led to the pollution of soil and water environment, not only poultry husbandry and food manufacturing will be influenced to different degree, but also the human body will produce antibody. The detection of antibiotic content in production and life is imperative. In this review, we provide comprehensive information about chemical sensors and biosensors for antibiotic detection. We classify the currently reported antibiotic detection technologies into chromatography, mass spectrometry, capillary electrophoresis, optical detection, and electrochemistry, introduce some representative examples for each technology, and conclude the advantages and limitations. In particular, the optical and electrochemical methods based on nanomaterials are discussed and evaluated in detail. In addition, the latest research in the detection of antibiotics by photosensitive materials is discussed. Finally, we summarize the pros and cons of various antibiotic detection methods and present a discussion and outlook on the expansion of cross-scientific areas. The synthesis and application of optoelectronic nanomaterials and aptamer screening are discussed and prospected, and the future trends and potential impact of biosensors in antibiotic detection are outlined.
Graphical abstract
Single-walled carbon nanotube-based field effect transistors (SWCNT-FETs) are ideal candidates for fabricating sensors and have been widely used for chemical sensing applications. SWCNT-FETs have low selectivity because of the environmentally sensitive electronic properties of SWCNTs, and SWCNT-FETs also show a high noise signal and poor sensitivity because of charge trapping from Si-OH hydration of the SiO2/Si substrate on the SWCNTs. Herein, poly (4-vinylpyridine) (P4VP) was used for noncovalent attachment to SWCNTs and selective binding to copper ions (Cu²⁺). Importantly, the introduction of a hafnium-oxide (HfO2) layer through atomic layer deposition (ALD) overcame the charge trapping by SiO2 hydration and remarkably decreased the interference signal. The sensitivity of the P4VP/SWCNT/HfO2-FET sensor for Cu²⁺ was 7.9 μA μM⁻¹, which was approximately 100 times higher than that of the P4VP/SWCNT/SiO2-FET sensor, and its limit of detection (LOD) was as low as 33 pmol L⁻¹. Thus, the P4VP/SWCNT/HfO2-FET sensor is a promising candidate for the development of Cu²⁺-selective sensors and can be designed for the large-scale manufacturing of custom-made sensors in the future.
Field-effect transistor (FET) is a very promising platform for biosensor applications due to its magnificent properties, including label-free detection, high sensitivity, fast response, real-time measurement capability, low running power, and the feasibility to miniaturize to a portable device. 1D (e.g. carbon nanotubes, Si nanowires, conductive polymer nanowires, 1D metal oxides, and others) and 2D (e.g. graphene materials, transition metal dichalcogenides, black phosphorus, and 2D metal oxides) materials, with their unique structural and electronic properties that are unavailable in bulk materials, have helped improve the sensitivity of FET biosensors and enabled detection down to single molecule. In this review, we give insights into the rapidly evolving field of 1D and 2D materials-based FET biosensors, with an emphasis on structure and electronic properties, synthesis, and biofunctionalization approaches of these nanomaterials. In addition, the progress in the 1D/2D-FET biosensors in North America, in the last decade, is summarized in tables. Moreover, challenges and future perspectives of 1D/2D-FET biosensors are covered.
Herein, a high-efficiency photoactive material, hollow ZnIn2S4 nanocages (ZIS-HNCs) composed of ultrathin nanosheets were creatively synthesized via a metal-organic framework (MOF) derived solvothermal method. It had been specified the underlying mechanism of the ZIS-HNCs evolution under the MOF templated surface. Subsequently, the obtained ZIS-HNCs combined with annealing TiO2 modified electrode ([email protected]2), and the [email protected]2 exhibited intense transient photocurrent. The enhanced photocurrent signal benefited from the multiple light capture effect of ZIS-HNCs, ultrathin nanosheet subunits of ZIS-HNCs, and typical type Ⅱ heterojunction, which could effectively retard the photoexcited electron-hole pairs recombination, and accelerated charge separation and transfer. Taking antibiotic lincomycin (Lin) as a model, a signal-off photoelectrochemical (PEC) aptasensor based on the [email protected]2 was established and manifested a high sensitive detection for Lin with a linear response range from 0.0001 to 0.1 nM as well as an ultralow detection limit of 0.084 pM. Additionally, the proposed PEC aptasensor showed acceptable stability and remarkable selectivity. Therefore, this study provides a promising strategy to design nanomaterials with superior photoelectric activity for PEC sensing applications.
Graphene field-effect transistors (GFETs) are emerging as bioanalytical sensors, in which their responsive electrical conductance is used to perform quantitative analyses of biologically-relevant molecules such as DNA, proteins, ions and small molecules. This review provides a detailed evaluation of reported approaches in the design, operation and performance assessment of GFET biosensors. We first dissect key design elements of these devices, along with most common approaches for their fabrication. We compare possible modes of operation of GFETs as sensors, including transfer curves, output curves and time series as well as their integration in real-time or a posteriori protocols. Finally, we review performance metrics reported for the detection and quantification of bioanalytes, and discuss limitations and best practices to optimize the use of GFETs as bioanalytical sensors.
Subinhibitory levels of antibiotics in reservoirs highly affected by anthropogenic activity, e.g. wastewater treatment plants, have a profound impact on the development and spread of resistant bacteria in the biosphere. As an aid, advanced oxidation processes (AOP) have been suggested to eliminate the antibacterial activity of several antibiotics, this activity has been followed using conventional antibiotic susceptibility tests. While the antibacterial activity can hardly be monitored below the minimum inhibitory concentration (MIC) with these assays, the selective pressure on a bacterial population might still remain in this concentration range. To assess the applicability of AOP for eliminating the subinhibitory effects of antibiotics on selection of resistant bacteria, a microbiological assay is introduced. The test is based on the dynamics of a mixed bacterial population in response to the presence of antibiotics in a concentration range well below the MIC in a synthetic wastewater matrix. Sensitive and resistant subtypes of Staphylococcus aureus in 1:1 ratio are added to the test medium and the fraction of resistant mutants is determined after 24 h incubation time by simple colony counting. By using electron beam irradiation as an AOP we show that the assay provides a simple tool to find the optimum treatment stage.
Aminoglycoside antibiotics are known to target ribosomal, retroviral and catalytic RNAs with high affinity and specificity. Recently, in vitro selection experiments have identified RNA aptamers that bind to aminoglycoside antibiotics with nanomolar affinity and stringent specificity, allowing discrimination between closely related family members. There has, to date, been limited structural information on the molecular basis of such saccharide-RNA recognition.
We describe a solution-structure determination of the tobramycin-RNA aptamer complex, obtained using NMR and molecular dynamics. The structure gives insight into the molecular features associated with saccharide-RNA recognition. Tobramycin adopts a defined alignment and binds to the RNA major groove centered about a stem-loop junction site. A portion of the bound tobramycin is encapsulated between the floor of the major groove and a looped-out cytosine residue that forms a flap over the binding site in the complex.
The emergence of antibiotic-resistant pathogens and their impact on human health continues to be a major concern in the medical community. Rational modification of existing antibiotics aimed at improving their efficacy requires a molecular view of their receptor-binding sites. We have provided such a molecular view for a member of the aminoglycoside antibiotic family that targets RNA.
Novel features of RNA structure, recognition and discrimination have been recently elucidated through the solution structural characterization of RNA aptamers that bind cofactors, aminoglycoside antibiotics, amino acids and peptides with high affinity and specificity. This review presents the solution structures of RNA aptamer complexes with adenosine monophosphate, flavin mononucleotide, arginine/citrulline and tobramycin together with an example of hydrogen exchange measurements of the base-pair kinetics for the AMP-RNA aptamer complex. A comparative analysis of the structures of these RNA aptamer complexes yields the principles, patterns and diversity associated with RNA architecture, molecular recognition and adaptive binding associated with complex formation.
A packed column GC-electron-capture detection method for the analysis of the aminoglycoside antibiotics kanamycin and gentamicin was adapted to capillary GC-MS. The analytes were derivatised using a two-step procedure involving trimethylsilylation of the hydroxyl groups with trimethylsilylimidazole and acylation of the amino groups with heptafluorobutyrylimidazole. Electron impact mass spectra of the resulting derivatives of kanamycin A and gentamicins C1, C1a and C2 are given and interpreted. The derivatisation procedure was optimised using experimental design. This chemometrical approach considers main effects as well as interactions of the influential parameters, thus conducting a more thorough investigation of the method than the common step-by-step approach. Optimisation using fractional factorial and Box Behnken Designs produced a derivatisation method featuring better yield than previously published methods while in many cases requiring less reagents and shorter reaction times.
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