Aptamer Selection and Application in Multivalent Binding-Based ElectricalImpedance Detection of Inactivated H1N1Virus Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-22 Chenjun Bai, Zhangwei Lu, Hua Jiang, Zihua Yang, Xuemei Liu, Hongmei Ding, Hui Li, Jie Dong, Aixue Huang, Tao Fang, Yongqiang Jiang, Lingling Zhu, Xinhui Lou, Shaohua Li, Ningsheng Shao
In-vitro model for assessing glucose diffusion through skin Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-22 Sana Ullah, Fadi Hammade, Urte Bubniene, Johan Engblom, Arunas Ramanvicius, Almira Ramanaviciene, Tautgirdas Ruzgas
Pig ear skin membrane-covered glucose biosensor based on oxygen electrode has been assessed as a tool to evaluate glucose penetration through skin in-vitro. For this, glucose oxidase (GOx) was immobilised on oxygen electrode and covered with the skin membrane. Exposing this electrode to the solution of glucose resulted in glucose penetration though skin membrane, its oxidation catalysed by GOx, consumption of O2 and decrease of the current of the oxygen electrode. By processing the biosensor responses to glucose, we found that glucose penetration through 250 µm thick skin membrane is slow; 90% of steady-state current response was reached in 32(±22) min. Apparent diffusion coefficient for glucose in skin was found to be equal to 0.15(±0.07)⁎10−6 cm2s−1. This value is 45 times lower than glucose diffusion coefficient in water. Tape-stripping of stratum corneum (SC) allows considerably faster glucose penetration. The electrodes covered with tape-stripped skin reached 90% of steady-state current response in 5.0(±2.7) min. The theoretical estimate of glucose flux through SC was considered exploiting four-pathway theory of transdermal penetration. Theoretical flux values were more that three orders lower than measured experimentally. This high discrepancy might indicate that glucose penetration through healthy human skin could be even slower, allowing much lower flux, than it was found in our study for skin membranes from pig ears.
Identification and characterisation of Staphylococcus aureus on low cost screen printed carbon electrodes using impedance spectroscopy Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-22 A.C. Ward, A.J. Hannah, S.L. Kendrick, N.P. Tucker, G. MacGregor, P. Connolly
Staphylococcus aureus infections are a cause of significant morbidity and mortality, in addition to representing a considerable economic burden. The aim of this study was to explore a low cost screen printed electrode as a sensor for the detection of S. aureus using impedance spectroscopy. S. aureus was incubated in chambers containing the electrodes and the results analysed using a novel normalisation approach. These results show that it is possible to detect the presence of S. aureus in LB media after 30 minutes incubation of a 1% growth culture, in addition to being able to see immediate cell concentration dependent changes in 0.9% NaCl. These observations imply that a number of electrochemical mechanisms cause a change in the impedance as a result of the presence of S. aureus, including adsorption to the electrode surface and the metabolism of the bacteria during growth. The study suggests that this detection approach would be useful in a number of clinical scenarios where S. aureus leads to difficult to treat infections.
Use of Torsional Resonators to Monitor Electroactive Biofilms Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-22 Phillipp Sievers, Christopher Moß, Uwe Schröder, Diethelm Johannsmann
Field-effect biosensor using virus particles as scaffolds for enzyme immobilization Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-21 Arshak Poghossian, Melanie Jablonski, Claudia Koch, Thomas S. Bronder, David Rolka, Christina Wege, Michael J. Schöning
A field-effect biosensor employing tobacco mosaic virus (TMV) particles as scaffolds for enzyme immobilization is presented. Nanotubular TMV scaffolds allow a dense immobilization of precisely positioned enzymes with retained activity. To demonstrate feasibility of this new strategy, a penicillin sensor has been developed by coupling a penicillinase with virus particles as a model system. The developed field-effect penicillin biosensor consists of an Al-p-Si-SiO2-Ta2O5-TMV structure and has been electrochemically characterized in buffer solutions containing different concentrations of penicillin G. In addition, the morphology of the biosensor surface with virus particles was characterized by scanning electron microscopy and atomic force microscopy methods. The sensors possessed a high penicillin sensitivity of ~92 mV/dec in a nearly-linear range from 0.1 mM to 10 mM, and a low detection limit of about 50 µM. The long-term stability of the penicillin biosensor was periodically tested over a time period of about one year without any significant loss of sensitivity. The biosensor has also been successfully applied for penicillin detection in bovine milk samples.
Electrochemical genoassays on gold-coated magnetic nanoparticles to quantify genetically modified organisms (GMOs) in food and feed as GMO percentage Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-21 Alexandra Plácido, Clara Pereira, Alexandra Guedes, M. Fátima Barroso, Rebeca Miranda-Castro, Noemí de-los-Santos-Álvarez, Cristina Delerue-Matos
The integration of nanomaterials in the field of (bio)sensors has allowed developing strategies with improved analytical performance. In this work, ultrasmall core-shell Fe3O4@Au magnetic nanoparticles (MNPs) were used as the platform for the immobilization of event-specific Roundup Ready (RR) soybean and taxon-specific DNA sequences. Firstly, monodisperse Fe3O4 MNPs were synthesized by thermal decomposition and subsequently coated with a gold shell through reduction of Au(III) precursor on the surface of the MNPs in the presence of an organic capping agent. This nanosupport exhibited high colloidal stability, average particle size of 10.2±1.3 nm, and spherical shape. The covalent immobilization of ssDNA probe onto the Au shell of the Fe3O4@Au MNPs was achieved through, a self-assembled monolayer (SAM) created from mixtures of alkane thiols (6-mercapto-1-hexanol and mercaptohexanoic acid). The influence of the thiols ratio on the electrochemical performance of the resulting electrochemical genoassays was studied, and remarkably, the best analytical performance was achieved for a pure mercaptohexanoic acid SAM. Two quantification assays were designed; one targeting an RR sequence and a second targeting a reference soybean gene, both with a sandwich format for hybridization, signaling probes labelled with fluorescein isothiocyanate (FITC), enzymatic amplification and chronoamperometric detection at screen-printed carbon electrodes (SPCE). The magnetogenoassays exhibited linear ranges from 0.1 to 10.0 nM and from 0.1 to 5.0 nM with similar detection limits of 0.02 nM and 0.05 nM for the event-specific (RR) and the taxon-specific (lectin) targets, respectively. The usefulness of the approach was demonstrated by its application to detect genetically modified organisms (GMOs) in feed and food.
Automatic Smartphone-based Microfluidic Biosensor System at the Point of Care Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-21 Dandan Xu, Xiwei Huang, Jinhong Guo, Xing Ma
Point-of-care testing technique is increasingly important for healthcare management in human being's daily life. However, traditional biosensor systems for health care are relatively expensive, bulky and hard-to-handle, which largely limits their use in point of care testing. The problems mentioned above are successfully addressed with the popularization of smartphone and the development of microfluidic technology for their applications of biosensor, which integrates smartphones, microfluidic components and sensory elements together, paving the way for wide application of smartphone-based microfluidic biomedical sensory system. According to the varieties of analytes, the most common sensing modalities of biosensor systems are divided into imaging analysis to detect cells and bacteria, biochemical analysis to detect blood sugar and blood fat, immunoassay to detect protein specifically bound to antibody, as well as molecular diagnosis to detect DNA and other biomolecules. Bsed on the most common analytical methods, this review article covers five types of smartphone-based microfluidic biosensor systems at the point-of-care detection, i.e., smartphone-based imaging biosensor, smartphone-based biochemical sensor, smartphone-based immune biosensor, smartphone-based hybrid biosensor with more than one sensing modality, and smartphone-based molecular sensor. We lay emphasis on reviewing the structures, analytical methods and sensing modalities about the four kinds of biosensor systems with detailed discussions on their application potentials, aiming at giving the audience an overview of the recent developments of automatic smartphone-based microfluidic biosensor systems, as well as their future prospective.
A Cell Viability Assessment Method Based on Area-Normalized Impedance Spectrum (ANIS) Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-21 Rongbiao Zhang, Mingji Wei, Shuohuan Chen, Guoxiao Li, Fei Zhang, Ning Yang, Linkui Huang
Impedance measurement of cells using electric cell-substrate impedance sensing (ECIS) is widely accepted as an effective method to assess cell status. However, the sensitive frequency drifts over time with the changes of culture condition according to the built circuit model and experimental results. The area-normalized impedance spectrum (ANIS) method, which uses normalized area of impedance spectrum in a certain interval to assess cell viability, was proposed in this paper to solve the problem. The certain interval is calculated due to the threshold Zth, which is determined by 2% decline of the maximum impedance. Stabilities of two methods were analyzed by normalizing the area and impedance, showing that the normalized impedance fluctuated like a wave, while the normalized area was smoother. In addition, Cell Count Kit-8 (CCK-8) assay was carried out proving that the correlation index of ANIS method increases by 2.4% compared with impedance sensing method, and the maximum error of ANIS method decreases by 4%. Comparison analysis of two methods with random measurement noise was also discussed in this paper, and the results showed that the ANIS method was less affected by measurement noise than impedance sensing method. It demonstrated that the ANIS method is a more stable and accurate method to assess cell viability.
Planar intercalated Copper (II) complex molecule as small molecule enzyme mimic combined with Fe3O4 nanozyme for bienzyme synergistic catalysis applied to the microRNA biosensor Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-21 Liang Tian, Jinxu Qi, Olayinka Oderinde, Chen Yao, Wei Song, Yihong Wang
Molybdenum Disulfide Field-Effect Transistor Biosensor for Ultrasensitive Detection of DNA by Employing Morpholino as Probe Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-20 Junchi Mei, Yu-Tao Li, Hong Zhang, Meng-Meng Xiao, Yong Ning, Zhi-Yong Zhang, Guo-Jun Zhang
This work reports on a molybdenum disulfide (MoS2) based field-effect transistor (FET) biosensor for ultrasensitive label-free detection of DNA via phosphorodiamidate morpholino oligos (PMO)-DNA hybridization. After the chip was fabricated and the sensing channel was modified with positive charges, the negatively charged MoS2 nanosheet was drop-casted onto the channel, enabling MoS2 to tightly bind to the sensing surface via electrostatic interactions. Meanwhile, DNA analogue, PMO, was immobilized on the MoS2 surface, and detection of PMO-DNA hybridization was conducted by the fabricated MoS2 FET biosensor. Due to the neutral character and high affinity of PMO, a limit of detection (LOD) down to 6 fM was obtained, which is lower than that of the previously reported MoS2 FET DNA biosensor based on DNA-DNA hybridization. In addition, the MoS2 FET biosensor also showed high sequence specificity capable of distinguishing the complementary DNA from one-base mismatched DNA, three-base mismatched DNA and noncomplementary DNA. Moreover, the unique FET biosensor was able to detect DNA in complex sample like serum, making the method potential in disease diagnostics.
Hand-held optical sensor using denatured antibody coated elctro-active polymer for ultra-trace detection of copper in blood serum and environmental samples Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-20 Sutapa Chandra, Arvind Dhawangale, Soumyo Mukherji
An optimun copper concentration in environment is highly desired for all forms of life. We have developed an ultrasensitive copper sensor which functions from femto to micro molar concentration accurately (R2=0.98). The sensor is based on denatured antibody immunoglobulin G (IgG), immobilized on polyaniline (PAni) which in turn is the coating on the core of an optical fiber. The sensing relies on changes in evanescent wave absorbance in the presence of the analyte. The sensor showed excellent selectivity towards Cu (II) ions over all other metal ions. The sensor was tested with lake and marine water samples to determine unknown concentrations of copper ions and the recovery results were within 90% to 115%, indicating reasonable accuracy. We further integrated the fiber-optic sensor with a miniaturized hand-held instrumentation platform to develop an accurate and field deployable device which can broadly be applicable to determine Cu (II) concentration in a wide range of systems – natural water bodies, soil as well as blood serum.
Aptamer-based biosensors and nanosensors for the detection of Vascular Endothelial Growth Factor (VEGF): A review Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-19 Sadegh Dehghani, Rahim Nosrati, Meysam Yousefi, Alireza Nezami, Fatemeh Soltani, Seyed Mohammad Taghdisi, Khalil Abnous, Mona Alibolandi, Mohammad Ramezani
Vascular endothelial growth factor (VEGF) is a key regulator of vascular formation and a predominant protein biomarker in cancer angiogenesis. Owing to its crucial roles in the cancer metastasis, VEGF detection and quantification is of great importance in clinical diagnostics. Today, there exist a wide variety of detection strategies for identifying many types of disease biomarkers, especially for VEGF. As artificial single-stranded DNA or RNA oligonucleotides with catalytic and receptor properties, aptamers have drawn lots of attention to be applied in biosensing platforms due to their target-induced conformational changes as well as high stability and target versatility. So far, various sensitivity-enhancement techniques in combination with a broad range of smart nanomaterials have integrated into the design of novel aptasensors to improve detection limit and sensitivity of analyte detection. This review article provides a brief classification and description of the research progresses of aptamer-based biosensors and nanobiosensors for the detection and quantitative determination of VEGF based on optical and electrochemical platforms.
A flexible and highly sensitive nonenzymatic glucose sensor based on DVD-laser scribed graphene substrate Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-17 Songyue Lin, Wendou Feng, Xiaofei Miao, Xiangxin Zhang, Sujing Chen, Yuanqiang Chen, Wei Wang, Yining Zhang
Isolation of HL-60 cancer cells from the human serum sample using MnO2-PEI/Ni/Au/aptamer as a novel nanomotor and electrochemical determination of thereof by aptamer/gold nanoparticles-poly(3,4-ethylene dioxythiophene) modified GC electrode Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-17 Mahmoud Amouzadeh Tabrizi, Mojtaba Shamsipur, Reza Saber, Saeed Sarkar
Photoelectrochemical TiO2 nanotube arrays biosensor for asulam determination based on in-situ generation of quantum dots Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-17 Jiuying Tian, Yan Li, Jingjiao Dong, Mingjuan Huang, Jusheng Lu
Inspired by the photoelectrochemical (PEC) properties of TiO2 nanotubes arrays (TNA) and their application as a super vessel for immobilizing biomolecules, we constructed an inhibition-effect PEC biosensor for determination of asulam based on the in-situ generation of CdS quantum dots (QDs) on TNA using an enzymatic reaction. Horseradish peroxidase (HRP) enzyme was covalently assembled on the inner-wall of TNAs, which exhibited good electrochemical and catalytic properties. In the mixture solution containing H2O2, CdY and S2O32-, HRP enzyme in TNAs catalyzed H2O2 reduce S2O32- to S2-. The generated S2- reacted with CdY to form CdS QDs in situ on the TNAs, improving the PEC performance of TNA under visible light irradiation. The photocurrent would decrease after addition of asulam due to its inhibitory effect towards HRP enzyme activity. Under the optimal experimental conditions, the constructed PEC TNA/HRP biosensor exhibited a satisfying linear range (0.02-2.0 ng mL−1), low limit of detection (4.1 pg mL−1) and good selectivity towards asulam determination, and has been successfully applied for the analysis of real environmental water samples with good accuracy of the recoveries ranged from 90 to 114%.
A chiral sensor based on weak measurement for the determination of Proline enantiomers in diverse measuring circumstances Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-16 Dongmei Li, Tian Guan, Yonghong He, Fang Liu, Anping Yang, Qinghua He, Zhiyuan Shen, Meiguo Xin
A new chiral sensor based on weak measurement to accurately measure the optical rotation (OR) has been developed for the estimation of a trace amount of chiral molecule. With the principle of optical weak measurement in frequency domain, the central wavelength shift of output spectra is quantitatively relative to the angle of preselected polarization. Hence, a chiral molecule (e.g., L-amino acid, or D-amino acid) can be enantioselectively determined by modifying the preselection angle with the OR, which will cause the rotation of a polarization plane. The concentration of the chiral sample, corresponding to its optical activity, is quantitatively analyzed with the central wavelength shift of output spectra, which can be collected in real time. Immune to the refractive index change, the proposed chiral sensor is valid in complicated measuring circumstance. The detections of Proline enantiomer concentration in different solvents were implemented. The results demonstrated that weak measurement acted as a reliable method to chiral recognition of Proline enantiomers in diverse circumstance with the merits of high precision and good robustness. In addition, this real-time monitoring approach plays a crucial part in asymmetric synthesis and biological systems.
Hybrid integration of scalable mechanical and magnetophoretic focusing for magnetic flow cytometry Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-15 Mathias Reisbeck, Lukas Richter, Michael Johannes Helou, Stephan Arlinghaus, Birgit Anton, Ignas van Dommelen, Mario Nitzsche, Michael Baßler, Barbara Kappes, Oliver Friedrich, Oliver Hayden
Time-of-flight (TOF) magnetic sensing of rolling immunomagnetically-labeled cells offers great potential for single cell function analysis at the bedside in even optically opaque media, such as whole blood. However, due to the spatial resolution of the sensor and the low flow rate regime required to observe the behavior of rolling cells, the concentration range of such a workflow is limited. Potential clinical applications, such as testing of leukocyte function, require a cytometer which can cover a cell concentration range of several orders of magnitude. This is a challenging task for an integrated dilution-free workflow, as for high cell concentrations coincidences need to be avoided, while for low cell concentrations sufficient statistics should be provided in a reasonable time-to-result. Here, we extend the spatial bandwidth of a magnetoresistive sensor with an adaptive and integratable workflow concept combining mechanical and magnetophoretic guiding of magnetically labeled targets for in-situ enrichment over a dynamic concentration range of 3 orders of magnitude. We achieve hybrid integration of the enrichment strategy in a cartridge mold and a giant-magnetoresistance (GMR) sensor in a functionalized Quad Flat No-Lead (QFN) package, which allows for miniaturization of the Si footprint for potential low-cost bedside testing. The enrichment results demonstrate that TOF magnetic flow cytometry with adaptive particle focusing can match the clinical requirements for a point-of-care (POC) cytometer and can potentially be of interest for other sheath-less methodologies requiring workflow integration.
Hybridization conditions of oligonucleotide-capped gold nanoparticles for SPR sensing of microRNA Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-15 Long Hong, Mengdi Lu, Marie-Pier Dinel, Philippe Blain, Wei Peng, Hongya Gu, Jean-Francois Masson
MicroRNA (miRNA) sensing, especially the miRNA-200 family, is increasingly targeted for cancer diagnostics. As the sensing schemes often rely on nanoparticles functionalized with a specific oligonucleotide, we investigate the hydribization conditions using the common case of surface plasmon resonance (SPR) sensing of miRNA and a gold nanoparticle (Au NP) competitor. In this type of assays, the Au NPs compete with the microRNA to bind the capture probe immobilized on the gold surface. In our study, we simplify and improve the detection procedure by adopting 11-mercaptoundecanoic acid (11-MUA) as linker to the gold surface, not only omitting the blocking step of 6-mercapto-1-hexanol (MCH), but also increasing the probe density. We report that the response in our SPR sensing studies increased with the size of Au NPs according to the plasmon ruler equation, but the larger AuNPs of 32 nm lacked colloidal stability. In addition, decreasing the ratio of oligonucleotide to Au NPs and the addition of polyethylene glycol (PEG) to hybridization buffer also favored a better response in SPR sensing of miRNA. The optimization led to an improved detection sensitivity in our competition method and a detection limit as low as 500 pM for miRNA-200b without amplification of miRNA and use of other amplification schemes.
Performance comparison between multienzymes loaded single and dual electrodes for the simultaneous electrochemical detection of adenosine and metabolites in cancerous cells Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-15 Khalil K. Hussain, Mahmood H. Akhtar, Moo-Hyun Kim, Dong-Keun Jung, Yoon-Bo Shim
The analytical performance of the multi enzymes loaded single electrode sensor (SES) and dual electrode sensor (DES) was compared for the detection of adenosine and metabolites. The SES was fabricated by covalent binding of tri-enzymes, adenosine deaminase (ADA), purine nucleoside phosphorylase (PNP), and xanthine oxidase (XO) along with hydrazine (Hyd) onto a functionalized conducting polymer [2,2:5,2-terthiophene-3- (p-benzoic acid)] (pTTBA). The enzyme reaction electrode in DES was fabricated by covalent binding of ADA and PNP onto pTTBA coated on Au nanoparticles. The detection electrode in DES was constructed by covalent binding of XO and Hyd onto pTTBA coated on porous Au. Due to the higher amount (3.5 folds) of the immobilized enzymes and Hyd onto the DES than SES, and the lower Michaelis constant (Km) value for DES (28.7 µM) compared to SES (36.1 µM), the sensitivity was significantly enhanced for the DES (8.2 folds). The dynamic range obtained using DES was from 0.5 nM to 120.0 µM with a detection limit of 1.43 nM ±0.02, 0.76 nM ±0.02, and 0.48 nM ±0.01, for adenosine (AD), inosine (IN), and hypoxanthine (Hypo) respectively. Further, the DES was coupled with an electrochemical potential modulated microchannel for the separation and simultaneous detection of AD, IN, and Hypo in an extracellular matrix of cancerous (A549) and non-cancerous (Vero) cells. The sensor probe confirms a higher basal level of extracellular AD and its metabolites in cancer cells compared to normal cells. In addition, the effect of dipyridamole on released adenosine in A549 cells was investigated.
Electrochemically mediated polymerization for highly sensitive detection of protein kinase activity Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-15 Qiong Hu, Qiangwei Wang, Cuihua Jiang, Jian Zhang, Jinming Kong, Xueji Zhang
Protein kinases play a pivotal role in cellular regulation and signal transduction, the detection of protein kinase activity and inhibition is therefore of great importance to clinical diagnosis and drug discovery. In this work, a novel electrochemical platform using the electrochemically mediated polymerization as an efficient and cost-effective signal amplification strategy is described for the highly sensitive detection of protein kinase activity. This platform involves 1) the phosphorylation of substrate peptide by protein kinase, 2) the attachment of alkyl halide to the phosphorylated sites via the carboxylate-Zr4+-phosphate chemistry, and 3) the in situ grafting of electroactive polymers from the phosphorylated sites through the electrochemically mediated atom transfer radical polymerization (eATRP) at a negative potential, in the presence of the surface-attached alkyl halide as the initiator and the electroactive tag-conjugated acrylate as the monomer, respectively. Due to the electrochemically mediated polymerization, a large number of electroactive tags can be linked to each phosphorylated site, thereby greatly improving the detection sensitivity. This platform has been successfully applied to detect the activity of cAMP-dependent protein kinase (PKA) with a detection limit down to 1.63 mU mL−1. Results also demonstrate that it is highly selective and can be used for the screening of protein kinase inhibitors. The potential application of our platform for protein kinase activity detection in complex biological samples has been further verified using normal human serum and HepG2 cell lysate. Moreover, our platform is operationally simple, highly efficient and cost-effective, thus holding great potential in protein kinase detection and inhibitor screening.
Morphology-dependent Electrochemical Behavior of 18-facet Cu7S4 Nanocrystals Based Electrochemical Sensing Platform for Hydrogen Peroxide and Prostate Specific Antigen Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-15 Yuxue Dai, Xiaodong Zhu, Hao Liu, Yanna Lin, Weiyan Sun, Yuanling Sun, Chaofan Ding, Chuannan Luo, Qin Wei
18-facet polyhedron Cu7S4 nanocrystal and CuS sphere were prepared from Cu2O precursor, and CuS flower was synthesized through a simple solvothermal approach. Their electrochemical performances were investigated towards H2O2 and it was interesting to discover that Cu7S4 nanocrystal had the best electrochemical catalysis compared with CuS sphere and CuS flower. It can deduce that the special structure of Cu7S4 nanocrystal endowed it more exposed active points, higher surface area and higher Cu/S ratio. Therefore, Cu7S4 nanocrystal was firstly employed to prepare a nonenzymatic biosensor for H2O2. Satisfactory results were obtained. In addition, a label-free sensing platform for prostate specific antigen (PSA) was constructed based on electrochemical catalysis towards H2O2 of Cu7S4 nanocrystal. The label-free immunosenosr offered accurate PSA in the range of 0.001~15 ng/mL with the detection limit of 0.001 ng/mL. Besides, the immunosensor possessed good sensitivity, selectivity and stability and could detect PSA in real sample. More importantly, this work demonstrated that Cu7S4 nanocrystal hold great promising application in electrochemical sensors.
Biofunctionalization of PAMAM-montmorillonite decorated poly (Ɛ-caprolactone)-chitosan electrospun nanofibers for cell adhesion and electrochemical cytosensing Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-14 Fatma Ozturk Kirbay, Esra Evrim Yalcinkaya, Gozde Atik, Gizem Evren, Betul Unal, Dilek Odaci Demirkol, Suna Timur
Molecularly imprinted sensor based on Russian Matryoshka structured molecules for enhanced specific identification and double amplification in ultra-trace Tb3+ determination Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-14 Jianping Li, Bin Yang, Hongcheng Pan, Guobao Xu
The selective and sensitive detection of rare earth elements is thought to be difficult because the concentration of those elements in the sample is commonly at a low level and they normally have severe mutual interference which is caused by homologous chemical properties. In this study, a novel molecularly imprinted polymer (MIP) sensor was fabricated for highly sensitive and selective determination of ultra-trace Tb3+. The Tb3+-ethylenediaminetetraacetic acid complex (Tb-EDTA) as the template molecule was incorporated into mono-6-mercapto-β-cyclodextrin (mono-6-SH-β-CD) to form a Russian Matryoshka (RM)-structured molecule (CD/Tb-EDTA). Titanium isopropoxide was utilized in vapor sol–gel polymerization to construct MIP membrane. Moreover, the selectivity of the RM MIP sensor was remarkably enhanced by the “triple-selectivity” recognition of EDTA-to-Tb3+, β-CD-to-(Tb-EDTA), and 3D cavity-to-(CD/Tb-EDTA), while the sensitivity of the MIP sensor was significantly improved by ECL signal enhancement based on double amplification, in other words, the electrochemiluminescence resonance energy transfer (ECL-RET) between the ECL donor of CD/Tb-EDTA and the ECL acceptor of Ru(bpy)32+, and the ECL enhancement by the co-reactant of CD/Tb-EDTA on Ru(bpy)3Cl2. When the imprinted cavities were occupied by Tb-EDTA during rebinding, the host-guest inclusion structured complex was formed and the ECL intensities produced by the Ru(bpy)3Cl2 ECL system increased with increasing concentration of Tb-EDTA. The proposed sensor was used for quantitative analysis of Tb3+ with concentrations ranging from 8×10–13 mol/L to 4.00 × 10–9 mol/L and successfully applied to detect Tb3+ in seawater samples. The detection limit of the sensor was found to be 3.90×10–13 mol/L (DL=3δb/K), which is lower than previously reported values. Thus, the fabricated sensor is feasible for practical applications.
Facile Crosslinking of Polythiophenes by Polyethylenimine via Ester Aminolysis for Selective Cu(II) Detection in Water Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-14 Xuewei Wang, Chi Zhang, Yajie Zhang, Jian Sun, Leilei Cao, Jinkai Ji, Fude Feng
Functionalization of π-conjugated polymers is dispensable for solubilization of the rigid and hydrophobic backbones in water. However, polymer aggregation is always present and leads to issues with complication and reproducibility in spectral properties. Herein, we reported a simple and robust method to make a series of conjugated polymer nanostructures by a crosslinking strategy. In favor of multivalency effect, polythionenes with various chain lengths were functionalized with branched polyethylenimine (PEI) via ester aminolysis reaction under mild conditions. Photophysical studies revealed the conjugated backbones could be well stabilized and dispersed in water. By taking advantage of intermolecular recognition interaction between copper ions and cationic PEI, we applied crosslinked polythiophenes as a nano probe at very low concentration (0.01 mg/mL) to fluorescently detect copper ions with high sensitivity up to 10 nM and selectivity over other metal ions in aqueous solutions, without occurrence of detectable aggregates. The overall performance of our nano probes outperforms reported water-soluble polymers-based probes, particularly in probe availability and manipulation as well as selective copper detection capability.
One-step selective screening of bioactive molecules in living cells using sulfur-doped microporous carbon Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-14 Mohammed Y. Emran, Mohamed A. Shenashen, Hiromi Morita, Sherif A. El-Safty
A metal-free electrode using heteroatom-doped microporous carbon was fabricated for the ultrasensitive monitoring of mono-bioactive molecules and the selective signaling of dopamine (DA) secreted by living cells. The constructed electrode based on sulfur-doped microporous carbon (S-MC) shows a high surface area, a spherical construction, numerous carbon chain defects, and microporous structures, which are the key factors of the interactive signaling transducer, fast response, and active interfacial surfaces. The intrinsic features of S-MC with different %S-doping (S-MC-1, and S-MC-2) through the sp2-carbon chain create abundant catalytic active sites, facilitate molecular diffusion through the microporous structure, promote strong binding with the targeted molecules, and induce interactions at electrolyte–electrode interfaces. The S-MC-1 provides selective signaling in a tertiary mixture of DA, ascorbic acid (AA), and uric acid (UA) with a high sensitivity and a wide linear range of 0.01–5, 10–4000, and 1–2000 µM, respectively. The detection limits were set at 3 nM, 1.26 µM, and 0.23 µM for DA, AA, and UA respectively. The S-MC-1 demonstrated a selective screening of DA released from PC12 cells under a K+ ion- stimulator with high sensitivity and promoted high biocompatibility, low cytotoxicity, high stability, and reliable reproducibility (%RSD ranged from 1–2.7). Our findings indicated that the S-MC-1 can be utilized as an in-vitro model for simultaneously monitoring extracellular-DA secreted from living cells and sensing mono-bioactive molecules in biological samples.
Ultrasensitive Photoelectrochemical Biosensor for the Detection of HTLV-I DNA: A Cascade Signal Amplification Strategy Integrating λ-Exonuclease Aided Target Recycling with Hybridization Chain Reaction and Enzyme Catalysis Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-13 Xiao-Mei Shi, Gao-Chao Fan, Xueying Tang, Qingming Shen, Jun-Jie Zhu
Nanostructured silver fabric as a free-standing NanoZyme for colorimetric detection of glucose in urine Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-13 Md.N. Karim, Samuel R. Anderson, Sanjay Singh, Rajesh Ramanathan, Vipul Bansal
Enzyme-mimicking catalytic nanoparticles, more commonly known as NanoZymes, have been at the forefront for the development of new sensing platforms for the detection of a range of molecules. Although solution-based NanoZymes have shown promise in glucose detection, the ability to immobilize NanoZymes on highly absorbent surfaces, particularly on free-standing substrates that can be feasibly exposed and removed from the reaction medium, can offer significant benefits for a range of biosensing and catalysis applications. This work, for the first time, shows the ability of Ag nanoparticles embedded within the 3D matrix of a cotton fabric to act as a free-standing peroxidase-mimic NanoZyme for the rapid detection of glucose in complex biological fluids such as urine. The use of cotton fabric as a template not only allows high number of catalytically active sites to participate in the enzyme-mimic catalytic reaction, the absorbent property of the cotton fibres also helps in rapid absorption of biological molecules such as glucose during the sensing event. This, in turn, brings the target molecule of interest in close proximity of the NanoZyme catalyst allowing for the accurate detection of glucose in urine. Additionally, the ability to extract the free-standing cotton fabric-supported NanoZyme following the reaction overcomes the issue of potential interference from colloidal nanoparticles during the assay. Based on these unique characteristics, nanostructured silver fabrics offer remarkable promise for detection of glucose and other biomolecules in complex biological and environmental fluids.
Improved sandwich-format electrochemical immunosensor based on “smart” SiO2@polydopamine nanocarrier Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-13 Dongsheng Zhang, Weixiang Li, Zhanfang Ma
An improved sandwich-type electrochemical immunosensor based on the novel signal amplification strategy was developed. Methylene blue (MB) loaded mesoporous silica nanoparticles (MSN) with polydopamine coating (PDA) were employed as “smart” labels, while phytic acid doped polyaniline hydrogel (PANI) with high adsorption capacity was acted as substrate. In this strategy, amount of redox species (MB) encapsulated in MSN by PDA will be released under acidic condition and then absorbed stably by PANI. Meanwhile, the label tended to drop down due to the destruction of polydopamine coating and the disassociation of antibody-antigen composites. The advantages of as-prepared immunosensor are as follows: (1) Higher electron transfer efficiency was obtained because of the decrease of relative position between MB and the electrode; (2) Lower impedance was achieved due to the loss of the labels and the dissociation of antigen-antibody insulating layer; (3) Abundant MB molecules were loaded on MSN/PDA nanocarrier with large pore volume for signal amplification. Under optimum conditions, the proposed immunosensor exhibited a low detection limit of 1.25 fg mL−1 and a wide linear range from 10 fg mL−1 to 100 ng mL−1 for prostate specific antigen detection. Importantly, present method showed good stability, selectivity, and reproducibility, which possessed wide potential applications for the detection of other biomarkers.
Simultaneous Detection of Gastric Cancer-involved miR-106a and let-7a through a Dual-signal-marked Electrochemical Nanobiosensor Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-13 Maryam Daneshpour, Behzad Karimi, Kobra Omidfar
miRNAs are among the novel biomarkers that can be evaluated for sensitive and early cancer diagnosis. In the present study, an electrochemical nanobiosensor has been fabricated to detect two gastric cancer (GC) related miRNAs simultaneously. By employing Au nanoparticles- and CdSe@CdS quantum dots-contained magnetic nanocomposites as electrochemical labels along with the polythiophene/reduced graphene oxide-modified carbon electrodes, this dual signal nanobiosensor showed a considerable performance in quantifying miR-106a (a GC oncogenic miRNA) and let-7a (a GC tumor suppressor miRNA). Using cyclic voltammetry (CV) and differential pulse voltammetry (DPV), not only the accomplishment of desired biosensing platform construction was confirmed, but also its great specificity, appropriate selectivity, acceptable stability, and significant sensitivity were indicated. Through the combined analyses of the dual miRNAs, our nanobiosensor reached detection limit of 0.02 fM and 0.06 fM for let-7a and miR-106a, respectively. This multiplex PCR-free miRNA nanobiosensor demonstrates attractive potentials for promising applications in early diagnosis of GC and additionally the screen of any miRNA sequence.
Signal Amplification Strategy for Biomarkers: Structural Origins of Epitaxial-Growth Twinned Nanocrystals and D–π–A Type Polymers Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-13 He Liu, Yue Gu, Tao Dong, Liuqing Yan, Xiaoyi Yan, Tingting Zhang, Nannan Lu, Zhiqian Xu, Haixin Xu, Zhiquan Zhang, Ting Bian
The combination of nanoparticles and biomarkers yields functional nanostructured biointerface, which is playing a notable role in biotechnology development. Due to the 5-fold twined structure in the Au-Pt star-shaped decahedra not only allowed it to act as efficient scaffold for immobilization of antibody, but it also exhibits superior electrocatalytic activity toward H2O2 reduction, the nanocrystal as the efficient signal transduction label is first employed to construct an electrochemical immunosensor. Donor–π–Acceptor (D–π–A) linking fashion generates a dipolar push-pull system and assures superior intramolecular charge transfer. It is considered as a suitable π-conjugated backbone for conducting polymer on biointerface application. Under a D–π–A architecture which imidazole as the π-bridge and amino phenyl/phenyl groups as peripheral electron-donating/withdrawing functional groups, 4-(2,4,5-triphenyl-1H-imidazol-1-yl) aniline (TPIDA) is designed and synthesized for good biocompatibility and high conductivity. In this proposal, we attempt to integrate the above-mentioned two features from nanobiotechnology and organic bioelectronics. Then, a novel nonenzymatic sandwich-type immunosensor is performed by Au-Pt core-shell with surface-engineered twinning as a label and π-conjugated D–π–A polymers as the signal amplification platform. Human IgG (HIgG) as the model target protein can be detected with a wide linear range from 0.1 pg mL−1 to 100 ng mL−1. The detection limit is down to 0.06 pg mL−1 (S/N = 3). Moreover, as a practical application, the prepared biosensor is used to monitor HIgG level in human serum with desirable results obtained.
Development of Cu nanoflowers modified the flexible needle-type microelectrode and its application in continuous monitoring glucose in vivo Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-13 Yuxin Fang, Shenjun Wang, Yangyang Liu, Zhifang Xu, Kuo Zhang, Yi Guo
A minimally invasive glucose microbiosensor based the flexibly integrated electrode for continuous monitoring glucose in vivo has been developed in this study. This was achieved by coating needle-type microelectrode with Cu nanoflowers, nafion, glucose oxidase (GOD) and polyurethane (PU) membranes, successfully prepared with layer-by-layer deposition. The Cu nanomaterials provided a large specific surface area and electrocatalytic activity for glucose detection. The PU layers as mass-transport limiting membranes significantly enhanced the linearity and stability of sensors. The resulting biosensor exhibited a wide linear range of 0 to 20 mM, with a good sensitivity of 42.38 nA mM−1 (correlation coefficient r2 was 0.99) and a fast response time of less than 15 s. In vivo implantable experiments using anesthetized rats showed excellent real-time response to the variation of blood glucose concentration. And the variation tendency of sensor output was consistent with that using the glucose meter. Overall, the results supported the suitability of this microsensor for measuring rapid changes of glucose in vivo. This work offers a promising approach in implantable device applications related to diabetes management as well as other medical diagnosis.
A Facile Synthesis of 3D NiFe2O4 Nanospheres Anchored on a Novel Ionic Liquid Modified Reduced Graphene Oxide for Electrochemical Sensing of Ledipasvir: Application to Human Pharmacokinetic Study Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-11 Mohamed M. El-Wekil, Ashraf M. Mahmoud, Saad A. Alkahtani, Adel A. Marzouk, Ramadan Ali
Wirelessly powered and remotely controlled valve-array for highly multiplexed analytical assay automation on a centrifugal microfluidic platform Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-10 Saraí M. Torres Delgado, David J. Kinahan, Lourdes Albina Nirupa Julius, Adam Mallette, David Sáenz Ardila, Rohit Mishra, Celina M. Miyazaki, Jan G. Korvink, Jens Ducrée, Dario Mager
In this paper we present a wirelessly powered array of 128 centrifugo-pneumatic valves that can be thermally actuated on demand during spinning. The valves can either be triggered by a predefined protocol, wireless signal transmission via Bluetooth, or in response to a sensor monitoring parameters like temperature or homogeneity of the dispersion. Upon activation of a resistive heater, a low-melting membrane (Parafilm™) is removed to vent an entrapped gas pocket, thus letting the incoming liquid wet an intermediate dissolvable film and thus open the valve. The proposed system allows up to 12 heaters to be activated in parallel with a response time below 3 seconds, potentially, resulting in 128 actuated valves in under 30 seconds. We demonstrate with three examples of common and standard procedures how the proposed technology could become a powerful tool for implementing diagnostic assays on Lab-on-a-Disc. First, we implement wireless actuation of 64 valves during rotation in a freely programmable sequence, or upon user input in real time. Then, we show a closed-loop centrifugal flow control sequence where the state of mixing between reagents evaluated from stroboscopically recorded images triggers the opening of valves. In our last experiment valving and closed-loop control are used to facilitate centrifugal processing of whole blood.
Fully 3D Printed Integrated Reactor Array for Point-of-Care Molecular Diagnostics Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-10 Karteek Kadimisetty, Jinzhao Song, Aoife M. Doto, Young Hwang, Jing Peng, Michael G. Mauk, Frederic D. Bushman, Robert Gross, Joseph N. Jarvis, Changchun Liu
Rapid Detection of Single E. coli Bacteria Using a Graphene-based Field-Effect Transistor Device Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-09 Bhawana Thakur, Guihua Zhou, Jingbo Chang, Haihui Pu, Bing Jin, Xiaoyu Sui, Xiaochen Yuan, Ching-Hong Yang, Matthew Magruder, Junhong Chen
Contamination of surface and drinking water due to the presence of Escherichia coli bacteria is a major cause of water-borne disease outbreak. To address unmet challenges for practical pathogen detection in contaminated samples, we report fabrication of thermally reduced graphene oxide-based field-effect transistor (rGO FET) passivated with an ultrathin layer of Al2O3 for real-time detection of E. coli bacteria. The sensor could detect a single E. coli cell within 50 s in a 1 µL sample volume. The ultrathin layer of Al2O3 acted as a barrier between rGO and potential interferents present in the sample. E. coli specific antibodies anchored on gold nanoparticles acted as probes for selective capture of E. coli. The high density of negative charge on the surface of E. coli cells strongly modulates the concentration of majority charge carriers in the rGO monolayer, thereby allowing real-time monitoring of E. coli concentration in a given sample. With a low detection limit of single cell, the FET sensor had a linear range of 1–100 CFU in 1 µL volume of sample (i.e., 103 to 105 CFU/ mL). The biosensor with good selectivity and rapid detection was further successfully demonstrated for E. coli sensing in river water. The rGO-based FET sensor provides a low cost and label-free approach, and can be mass produced for detection of a broad spectrum of pathogens in water or other liquid media.
Disposable electrochemical detection of breast cancer tumour marker CA 15-3 using poly(Toluidine Blue) as imprinted polymer receptor Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-08 J.A. Ribeiro, C.M. Pereira, A.F. Silva, M.Goreti F. Sales
In this work, electrically-conducting poly(Toludine Blue) was employed for the first time as synthetic receptor film, prepared by Molecular Imprinting strategies and using electrochemical methods, for the specific screening of breast cancer biomarker Carbohydrate Antigen 15-3 (CA 15-3). The protein imprinted poly(Toluidine Blue) film was grown in a pre-formed Toluidine Blue (TB) tailed SAM at the AuSPE surface, which greatly enhanced the stability against degradation of the Molecular Imprinted Polymer (MIP) film at the electrode surface. The MIP receptor film recognition ability towards the protein was investigated by fitting data to Freundlich isotherm. The binding affinity (KF) obtained for the MIP system was significantly higher (~12-fold) to that obtained for the NIP system, demonstrating the success of the approach in creating imprinted materials that specifically respond to CA 15-3 protein. The incubation of the MIP modified electrode with increasing concentration of protein (from 0.10 U mL−1 to 1000 U mL−1) resulted in a decrease of the ferro/ferricyanide redox current. The device displayed linear response from 0.10 U mL−1 to 100 U mL−1 and LODs below 0.10 U mL−1 were obtained from calibration curves built in neutral buffer and diluted artificial serum, using DPV technique, enabling the detection of the protein biomarker at clinically relevant levels. The developed MIP biosensor was applied to the determination of CA 15-3 in spiked serum samples with satisfactory results. The developed device provides a new strategy for sensitive, rapid, simple and cost-effective screening of CA 15-3 biomarker. Importantly, the overall approach seems suitable for point-of-care (PoC) use in clinical context.
Electrochemical coupled immunosensing platform based on graphene oxide/gold nanocomposite for sensitive detection of Cronobacter sakazakii in powdered infant formula Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-08 Shruti Shukla, Yuvaraj Haldorai, Vivek K. Bajpai, Arunkumar Rengaraj, Seung Kyu Hwang, Xinjie Song, Myunghee Kim, Yun Suk Huh, Young-Kyu Han
Polymorphism genotyping based on loop-mediated isothermal amplification and smartphone detection Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-08 Eric Seiti Yamanaka, Luis A. Tortajada-Genaro, Nuria Pastor, Ángel Maquieira
A Robust, Magnetic, and Self-accelerated Electrochemiluminescent Nanosensor for Ultrasensitive Detection of Copper Ion Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-07 Yan-Mei Lei, Bai-Qi Xiao, Wen-Bin Liang, Ya-Qin Chai, Ruo Yuan, Ying Zhuo
A novel “modularized” optical sensor for pH monitoring in biological matrixes Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Xun Liu, Shang-Qing Zhang, Xing Wei, Ting Yang, Ming-Li Chen, Jian-Hua Wang
A novel core-shell structure optical pH sensor is developed with upconversion nanoparticles (UCNPs) serving as the core and silica as the shell, followed by grafting bovineserumalbumin (BSA) as another shell via glutaraldehyde cross-linking. The obtained core-shell-shell structure is shortly termed as UCNPs@SiO2@BSA, and its surface provides a platform for loading various pH sensitive dyes, which are alike “modules” to make it feasible for measuring pHs within different pH ranges by simply regulating the type of dyes. Generally, a single pH sensitive dye is adopted to respond within a certain pH range. This study employs bromothymol blue (BTB) and rhodamine B (RhB) to facilitate their responses to pH variations within two ranges, i.e., pH 5.99–8.09 and pH 4.98–6.40, respectively, with detection by ratio-fluorescence protocol. The core-shell-shell structure offers superior sensitivity, which is tens of times more sensitive than those achieved by ratio-fluorescence approaches based on various nanostructures, and favorable stability is achieved in high ionic strength medium. In addition, this sensor exhibits superior photostability under continuous excitation at 980 nm. Thanks to the near infrared excitation in the core-shell-shell structure, it effectively avoids the self-fluorescence from biological samples and thus facilitates accurate sensing of pH in various biological sample matrixes.
Culture-free, highly sensitive, quantitative detection of bacteria from minimally processed samples using fluorescence imaging by smartphone Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Sajal Shrivastava, Won-Il Lee, Nae-Eung Lee
Molecular Recognition by Synthetic Receptors: Application in field-effect transistor based chemosensing ☆ Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Zofia Iskierko, Krzysztof Noworyta, Piyush Sindhu Sharma
A novel electrochemical sensor based on silver/halloysite nanotube/molybdenum disulfide nanocomposite for efficient nitrite sensing Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Masoud Ghanei-Motlagh, Mohammad Ali Taher
In the present study, the silver/halloysite nanotube/molybdenum disulfide (Ag/HNT/MoS2) nanocomposite was successfully synthesized. For this purpose, the lumen of HNTs was firstly modified by silver to generate Ag nanorods via chemical process and then the MoS2 layers deposited on the Ag/HNT nanocomposite by hydrothermal method. The characterization of Ag/HNT/MoS2 nanocomposite were investigated by field emission scanning electron microscopy (FE-SEM), Fourier transform infrared (FT-IR) spectroscopy, transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS), energy dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD) analyses. The nanocomposite modified carbon paste electrode (CPE) was applied for the electrocatalytic detection of nitrite in aqueous solutions. It was demonstrated that the treatment of HNTs with Ag and MoS2 materials enhanced the catalytic performance of modified CPE. At optimal experimental conditions, the designed sensor displayed remarkable sensing ability toward nitrite oxidation, offering a good linearity from 2 to 425 µM. The limit of detection (LOD) of the proposed strategy was estimated to be 0.7 µM based S/N=3. The good reproducibility, acceptable stability, fast response time and anti-interference performance of the proposed assay suggests that the modified CPE has great potential working as a nitrite electrochemical sensor for environmental applications.
Application of antibody–nanogold–ionic liquid–carbon paste electrode for sensitive electrochemical immunoassay of thyroid-stimulating hormone Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Hadi Beitollahi, Susan Ghofrani Ivari, Masoud Torkzadeh-Mahani
A novel electrochemical immunosensor based on carbon paste electrode (CPE) composed of ionic liquid (IL) and graphite was constructed. It demonstrated good efficiency for quick (each test in 30 s) determination of thyroid stimulating hormone (TSH). Electrode surface was modified by gold nanoparticles in order to immobilize of the thyroid stimulating hormone antibody (anti-TSH) on the CPE. The immunoassay structure was established by sandwiching the antigen (TSH) between the thyroid stimulating hormone antibody on the CPE surface modified with gold nanoparticles and the secondary antibody, polyclonal anti-human-TSH labeled with horseradish peroxidase (HRP-labeled anti-TSH). The signal of differential pulse voltammetry (DPV) was used as a basis for the determination of TSH concentration. This signal is generated by the reaction between O-aminophenol (OAP) and H2O2 catalyzed by HRP. The proposed immunosensor is able to measure the concentration of TSH in a linear range between 0.2–90.0 ng/mL with a detection limit 0.1±0.02 ng/mL. In addition, high sensitivity and acceptable stability were achieved by this immunosensor which is promising in the clinical assay of TSH.
A Universal and Label-Free Impedimetric Biosensing Platform for Discrimination of Single Nucleotide Substitutions in Long Nucleic Acid Strands Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Dawn M. Mills, Christopher P. Martin, Stephanie Armas, Percy Calvo-Marzal, Dmitry M. Kolpashchikov, Karin Y. Chumbimuni-Torres
We report a label-free universal biosensing platform for highly selective detection of long nucleic acid strands. The sensor consists of an electrode-immobilized universal stem-loop (USL) probe and two adaptor strands that form a 4 J structure in the presence of a specific DNA/RNA analyte. The sensor was characterized by electrochemical impedance spectroscopy (EIS) using K3[Fe(CN)6]/K4[Fe(CN)6] redox couple in solution. An increase in charge transfer resistance (RCT) was observed upon 4 J structure formation, the value of which depends on the analyte length. Cyclic voltammetry (CV) was used to further characterize the sensor and monitor the electrochemical reaction in conjunction with thickness measurements of the mixed DNA monolayer obtained using spectroscopic ellipsometry. In addition, the electron transfer was calculated at the electrode/electrolyte interface using a rotating disc electrode. Limits of detection in the femtomolar range were achieved for nucleic acid targets of different lengths (22 nt, 60 nt, 200 nt). The sensor produced only a background signal in the presence of single base mismatched analytes, even in hundred times excess in concentration. This label-free and highly selective biosensing platform is versatile and can be used for universal detection of nucleic acids of varied lengths which could revolutionize point of care diagnostics for applications such as bacterial or cancer screening.
Recent progresses in DNA nanostructure-based biosensors for detection of tumor markers Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-06 Rongrong Huang, Nongyue He, Zhiyang Li
DNA has emerged as a promising biomaterial for assembling a variety of nanostructures based on its programmable base pairing. It also has other remarkable properties including stability, prominent biocompatibility, and can easily be modified with functional groups for further applications. In the past few decades, researchers have established various design rules and assembly technologies to improve the stability and complexity of DNA nanostructures. The detection of cancer-associated biomarkers has significant importance in identifying patients with different clinical stages and also in developing adaptive therapeutic strategies. Due to their unique advantages, DNA nanostructures can be designed to serve as universal units to form biosensors for the detection of tumor biomarkers. In this review, we first present a brief introduction of the development of structural DNA nanotechnology. Then we summarize recent strategies for DNA nanostructure-based optical, electrochemical and mass sensitive biosensors in cancer detection. Finally, we discuss the challenges and opportunities these technologies provide.
Single-molecule porphyrin-metal ion interaction and sensing application Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-05 Keke Wei, Fujun Yao, Xiao-feng Kang
It remains a significant challenge to study the interactions between metal ions and porphyrin molecules at single ion level. Here, we constructed a nanopore-based sensing for label-free and real-time analysis of the interaction between Cu2+ and 5,10,15,20-tetrakis(4-sulfonatophenyl)-porphyrin (TPPS). The results demonstrate that emerging electronic signatures of the Cu2+-TPPS complex that is completely different form the original free TPPS were observed in the α-hemolysin (α-HL) nanopore. Based on the distinctive electronic signal patterns between TPPS and Cu2+-TPPS complex, the unique nanopore sensor can achieve a highly sensitive detection of Cu2+ in aqueous media. The frequency of signature events showed a linear response toward the concentration of Cu2+ in the range of 0.03 µM – 1.0 μM, with a detection limit of 16 nM (S/N = 3). The sensing system also exhibited high selectivity against other metal ions, and the feasibility of this approach for practical applications was demonstrated with the determination of Cu2+ in running water.
Porous graphite: a facile synthesis from ferrous gluconate and excellent performance as anode electrocatalyst of microbial fuel cell Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-05 Juan Xiong, Meihua Hu, Xiaoping Li, Hongying Li, Xin Li, Xiang Liu, Guozhong Cao, Weishan Li
A porous graphite (PG) is proposed as anode electrocatalyst of microbial fuel cell (MFC), which is synthesized by thermally decomposing ferrous gluconate followed by leaching iron. The physical characterizations from scanning electron microscopy, Brunauer-Emmeet-Teller, X-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy, indicate that the resulting PG is mesopore-rich and exhibits high graphitization with oxygen-containing functional groups. When evaluated on a naked carbon felt (NCF) anode, the resulting PG provides the MFC based on Escherichia coli with excellent power output. The MFC using the carbon felt anode loaded with 3.0 mg cm−2 PG delivers a maximum power density of 2.6 W m−2, compared to the 0.2 W m−2 for the MFCs using NCF anode. This excellent performance is attributed to the electronically conductive graphite and porous structure of the resulting PG. The former provides the anode with high activity towards redox reactions of c-type cytochromes in bacteria, the latter stimulates bacteria to produce their flagella that help bacteria to firmly bond each other.
Ce(III, IV)-MOF electrocatalyst as signal-amplifying tag for sensitive electrochemical aptasensing Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-05 Hua Yu, Jing Han, Shangjie An, Gang Xie, Sanping Chen
Metal–organic frameworks (MOFs) as a new class of porous materials have attracted increasing attention in the field of biomimetic catalysis. This study firstly reports a mixed valence state Ce-MOF possessing intrinsic catalytic activity towards thionine (Thi), and its application in constructing an amplified electrochemical aptasensor for thrombin detection. As noticed, the novel catalytic process combines the advantages of 3D infinite extension of the Ce(III, IV)-MOF skeleton containing large amounts of catalytic sites and spontaneous recycling of the Ce(III)/Ce(IV) for electrochemical reduction of Thi, thereby presenting amplified electrochemical signals. To further improve the aptasensor performance, the high selectivity of proximity binding-induced DNA strand displacement and high efficiency of exonuclease III-assisted recycling amplification were incorporated into the assay. The aptasensor was employed to detect thrombin in complex serum samples, which shows high sensitivity, specificity, stability and reproducibility. This work offers an opportunity to develop MOF-based electrocatalyst as signal-amplifying tag for versatile bioassays and catalytic applications.
The importance of antibody orientation in the electrochemical detection of ferritin Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-05 Edyta Matysiak-Brynda, Barbara Wagner, Michał Bystrzejewski, Ireneusz P. Grudzinski, Anna M. Nowicka
The way of immobilization of the monoclonal antibody (type IgG) on the electrode surface has a significant effect on the amount of the immobilized protein and in consequence on current signal of protein. Herein, we demonstrate that the application of appropriately functionalized phenyl film allowed us to control the orientation of the antibody (Ab) molecules on the electrode surface. The influence of Ab orientation on the efficiency of antigen-antibody interaction was tested with an example blood plasma protein (ferritin; Ft). To control the orientation of Ab molecules the phenyl films containing –COOH or –NH2 groups were applied. Contrary to aminoethylophenyl layer, the carboxyphenyl film guaranteed the shortest distance between the redox center of the protein and the electrode surface. Additionally, the application of an external magnetic field together with magnetic nanoparticles allowed achieving the best orientation to observe well-defined ferritin current signals. The proposed method of ferritin detection can be successfully used in the concentration range of Ft between 0.1 and 30 µg·dL−1. The detection limit for a carboxyphenyl film was estimated as 0.40 ± 0.04 and 0.13 ± 0.04 µg·dL−1 for impedance and voltammetric measurements, respectively. In turn, for an aminoethylophenyl film the detection limit was 0.03 ± 0.002 (electrochemical impedance spectroscopy; EIS) and 0.02 ± 0.002 µg·dL−1 (differential pulse voltammetry, DPV). The interday precision (reproducibility) was calculated (4.10÷9.10% RSD) together with the intraday precision /repeatability (3.20÷8.0% RSD) for the studied samples. The functionality of the sensor has been tested on rat blood samples. Based on the performed investigations it can be stated that the developed sensor was characterized by high selectivity and good sensitivity.
Novel photoluminescence enzyme immunoassay based on supramolecular host-guest recognition using L-arginine/6-aza-2-thiothymine-stabilized gold nanocluster Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-05 Youmei Wang, Minghua Lu, Dianping Tang
A new photoluminescence (PL) enzyme immunoassay was designed for sensitive detection of aflatoxin B1 (AFB1) via an innovative enzyme substrate, 6-aza-2-thiothymine-stabilized gold nanocluster (AAT-AuNC) with L-arginine. The enzyme substrate with strong PL intensity was formed through supramolecular host-guest assembly between guanidine group of L-arginine and AAT capped on the surface of AuNC. Upon arginase introduction, the captured L-arginine was hydrolyzed into ornithine and urea, thus resulting in the decreasing PL intensity. Based on this principle, a novel competitive-type immunoreaction was first carried out on AFB1-bovine serum albumin (AFB1-BSA) conjugate-coated microplate, using arginase-labeled anti-AFB1 antibody as the competitor. Under the optimum conditions, the PL intensity increased with the increment of target AFB1, and allowed the detection of the analyte at concentrations as low as 3.2 pg mL−1 (ppt). Moreover, L-arginine-AAT-AuNC-based PL enzyme immunoassay afforded good reproducibility and acceptable specificity. In addition, the accuracy of this methodology, referring to commercial AFB1 ELISA kit, was evaluated to analyze naturally contaminated or spiked peanut samples, giving well-matched results between two methods, thus representing a useful scheme for practical application in quantitative monitoring of mycotoxins in foodstuff.
Sensitive electrogenerated chemiluminescence biosensors for protein kinase activity analysis based on bimetallic catalysis signal amplification and recognition of Au and Pt loaded metal-organic frameworks nanocomposites Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-05 Zhiyong Yan, Feng Wang, Pingye Deng, Yu Wang, Kai Cai, Yanhui Chen, Zonghua Wang, Yang Liu
In this work, a novel and sensitive electrogenerated chemiluminescence (ECL) biosensor for protein kinase A (PKA) activity analysis and relevant inhibitor screening was proposed based on bimetallic catalysis signal amplification and recognition of Au and Pt nanoparticles loaded metal-organic frameworks (Au&Pt@UiO-66) nanocomposite. After being phosphorylated by PKA in the presence of ATP, Au&Pt@UiO-66 probes were specifically chelated to the modified electrode by forming Zr-O-P bonds between the surface defects of UiO-66 and the phosphorylated kemptide. Due to the high synergistic catalysis of Au&Pt@UiO-66 nanocomposites to the luminol-H2O2 reaction, the ECL signal of luminol was greatly enhanced. Moreover, UiO-66 afford numerous Zr defect sites for high efficient phosphate group recognition, and can also prevent the nanoparticles from aggregating during catalytic reactions. Thus, the excellent performance of the ECL biosensor with high sensitivity and superior stability was obtained. Under the optimized conditions, the detection limit for PKA activity was 0.009 UmL−1 (S/N=3). Meanwhile, the ECL biosensor was successfully applied in inhibitor screening and cell lysates PKA activity analysis, showing great promise in kinase related research.
Study of Inflammatory Factors’ Effect on the Endothelial Barrier Using Piezoelectric Biosensor Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-03-02 Junliang Han, Feifei Tong, Ping Chen, Xiancai Zeng, Zhengyong Duan
This paper used piezoelectric sensor to study the dysfunction of endothelial cell monolayer barrier caused by inflammatory factors. The biocompatible conductive polymer membrane of pPy[pGlu]-pLys was prepared on the surface of the ITO work electrode to improve the interface between the endothelial cell and the electrode. Both the impedance analysis data and the stable plateau stage of sensor's frequency shift indicated that endothelial cells formed a good monolayer barrier on this polymer surface. The response frequency shifts of lipopolysaccharide (LPS)- and histamine-induced endothelial barrier dysfunction were different, which distinguished their different stimulation mechanism. It provided a valuable analysis method for detecting the endothelial barrier function affected by inflammatory factor, and could further promote the application of piezoelectric sensor in cell biology and toxicology research.
Dawson-type polyoxometalate nanoclusters confined in a carbon nanotube matrix as efficient redox mediators for enzymatic glucose biofuel cell anodes and glucose biosensors Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-28 Feriel Boussema, Andrew J. Gross, Fatma Hmida, Brahim Ayed, Hatem Majdoub, Serge Cosnier, Abderrazak Maaref, Michael Holzinger
Two new inorganic-organic hybrid materials based on heteropolyoxometalates (POMs): (C4H10N)6[P2Mo18O62]. 4H2O (P2Mo18) and (C6H8NO)4[H2P2W18O62]. 6H2O (P2W18) are reported as mediators for electron transfer between FAD-dependent glucose dehydrogenase (FAD-GDH) and a multiwalled carbon nanotube (MWCNT) matrix for glucose biofuel cell and biosensor applications. These polyoxometalates were chosen due to their promising redox behavior in a potential range for mediated electron transfer with the glucose oxidizing enzyme, FAD-GDH. P2Mo18 and P2W18 were immobilized on 1-pyrenemethylamine (PMA) functionalized MWCNT deposits. After immobilization of FAD-GDH, the P2W18-modified MWCNT electrode demonstrated mediated electron transfer and provided a catalytic current density of 0.34 mAcm-2 at 0.2 V vs SCE with an open circuit potential (OCP) of −0.08 V vs SCE. A 10-fold increase in catalytic current to 4.7 mAcm-2 at 0.2 V vs SCE and a slightly lower OCP of −0.10 V vs SCE was observed for an equivalent electrode modified with P2Mo18.The apparent superiority of P2Mo18 is related, at least in part, to its improved incorporation in the MWCNT matrix compared to P2W18. Both POM-modified bioanodes showed exceptional stabilities with 45% of their initial performances remaining after 15 days. The mediated electron transfer capacities of the POMs were also evaluated in a glucose sensor setup and showed very satisfying performances for glucose detection, including a sensitivity of 0.198 mAmolL-1cm-2, a satisfying linear range between 1 mmolL-1 and 20 mmolL-1, and good reproducibility for the P2Mo18 electrode.
Glucose biosensor based on disposable electrochemical paper-based transducers fully fabricated by screen-printing Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-28 P.J. Lamas-Ardisana, G. Martínez-Paredes, L. Añorga, H.J. Grande
This paper describes a new approach for the massive production of electrochemical paper-based analytical devices (ePADs). These devices are fully fabricated by screen-printing technology and consist of a lineal microfluidic channel delimited by hydrophobic walls (patterned with diluted ultraviolet screen-printing ink in chromatographic paper grade 4) and a three-electrode system (printed with carbon and/or Ag/AgCl conductive inks). The printing process was characterised and optimised for pattern each layer with only one squeeze sweep. These ePADs were used as transducers to develop a glucose biosensor. Ionic strength/pH buffering salts, electrochemical mediator (ferricyanide) and enzyme (glucose dehydrogenase FAD-dependent) were separately stored along the microfluidic channel in order to be successively dissolved and mixed after the sample dropping at the entrance. The analyses required only 10 µl and the biosensors showed good reproducibility (RSD = 6.2%, n = 10) and sensitivity (0.426 C/M·cm2), wide linear range (0.5–50 mM; r2 = 0.999) and low limit of detection (0.33 mM). Furthermore, the new biosensor was applied for glucose determination in five commercial soft-drinks without any sample treatment before the analysis. These samples were also analysed with a commercial enzymatic-kit assay. The results indicated that both methods provide accurate results.
Dual-signal amplified photoelectrochemical biosensor for detection of N6-methyladenosine based on BiVO4–110-TiO2 heterojunction, Ag+-mediated cytosine pairs Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-27 Haiyan Wang, Huanshun Yin, Hua Huang, Kelin Li, Yunlei Zhou, Geoffrey I.N. Waterhouse, Hai Lin, Shiyun Ai
A Wearable Electrochemical Glucose Sensor based on Simple and Low-Cost Fabrication Supported Micro-Patterned Reduced Graphene Oxide Nanocomposite Electrode on Flexible Substrate Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-27 Xing Xuan, Hyo S. Yoon, Jae Y. Park
In this study, a reduced graphene oxide (rGO)-based nanostructured composite working electrode of high quality was successfully microfabricated and micro-patterned on a flexible polyimide substrate using simple low-cost fabrication processes. Gold and platinum alloy nanoparticles were electrochemically deposited onto the microfabricated rGO surface and chitosan-glucose oxidase composites were integrated onto the modified surface of the working electrode to develop a human sweat-based wearable glucose sensor application. The fabricated biosensor exhibited excellent amperometric response to glucose at a detection range of 0–2.4 mM (covers the glucose range in sweat), with a sensitivity of 48 μA/mMcm2, a short response time (20 sec), and high linearity (0.99). The detection limit for glucose was calculated as 5 µm. The human sweat/mixing glucose samples initially used for testing indicated acceptable detection performance and stability for low glucose concentrations. These results confirm that the proposed nanostructured composite flexible working electrode and fabrication process are highly promising for application as human sweat-based electrochemical glucose sensors.
Highly Sensitive and Specific On-Site Detection of Serum Cocaine by a Low Cost Aptasensor Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-27 Rania Oueslati, Cheng Cheng, Jayne Wu, Jiangang Chen
Cocaine is one of the most used illegal recreational drugs. Developing an on-site test for cocaine use detection has been a focus of research effort, since it is essential to the control and legal action against drug abuse. Currently most of cocaine detection methods are time-consuming and require special or expensive equipment, and the detection often suffers from high cross-reactivity with cocaine metabolites and relative low sensitivity with the best limit of detection reported at sub nanomolar (nM) level. In this work, an aptasensor has been developed using capacitive monitoring of sensor surface incorporating alternating current electrokinetics effects to speed up molecular transport and minimize matrix effects. The aptasensor is rapid, low cost, highly sensitive and specific as well as simple-to-use for the detection of cocaine from serum. The assay has a sample-to-result time of 30 seconds, a limit of detection of 7.8 fM, and a linear response for cocaine ranging from 14.5fM to 14.5pM in standard buffer, which are great improvements from other reported cocaine sensors. Special buffer is used for serum cocaine detection, and a limit of detection of 13.4 fM is experimentally demonstrated for cocaine spiked in human serum (equivalent to 1.34 pM cocaine in neat serum). The specificity of the biosensor is also demonstrated with structurally similar chemicals, ecgonine ethyl ester and methylecgonidine. This biosensor shows high promise in detection of low levels of cocaine from complex matrices.
Development of a SPR aptasensor containing oriented aptamer for direct capture and detection of tetracycline in multiple honey samples Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-27 Sai Wang, Yiyang Dong, Xingguo Liang
Although surface plasmon resonance (SPR) technique and aptamer technology shows great potential in analytical and biological chemistry, direct capture and analysis of small molecules using SPR remains tough. Detection sensitivity of aptasensor and recognition ability of aptamer is limited, because direct immobilization of aptamer causes large steric hindrance and strand entanglement. Herein, we chose a typical small molecule-tetracycline (Mw.444.4 g/mol) as a model, and combined aptamer technology, DNA nanostructure, and commercial Biacore T200 SPR instrument to develop a straightforward format SPR aptasensor. Anti-tetracycline aptamer (Apt76) was fabricated on the top of a tetrahedron nanostructure to provide a better accessibility to tetracycline than the single-stranded Apt76 (ss-Apt76), and thus to improve sensitivity of the SPR aptasensor. The aptasensor was then validated in real world application for tetracycline screening in multiple honey samples, achieving good recovery rates of 80.20%~114.3%, intuitive sensorgrams indicating the binding kinetic properties, and high specificity towards tetracycline. LOD of the tetrahedron-based SPR aptasensor was obtained using the real honey sample and calculated to be 0.0069 μg/kg, which was 10-fold range lower than that of the ss-Apt76-based aptasensor. The proof-of-concept demonstrated that aptamers of small molecules can be oriented immobilized on the SPR surface in a uniform nanoscale distance in both lateral and vertical direction, so as to achieve better conformational folding and better accessibility to small molecules. The concept is promising to be a universal and powerful tool for other ligand immobilization and SPR studies for both real world detection and molecular interaction.
Silver Decahedral Nanoparticles Empowered SPR Imaging-SELEX for High Throughput Screening of Aptamers with Real-Time Assessment Biosens. Bioelectron. (IF 7.780) Pub Date : 2018-02-23 Wenchao Jia, Hui Li, Thomas Wilkop, Xiaohui Liu, Xiaodong Yu, Quan Cheng, Danke Xu, Hong-Yuan Chen
A highly efficient method for aptamer screening with real-time monitoring of the SELEX process was described by silver decahedra nanoparticles (Ag10-NPs) enhanced surface plasmon resonance imaging (SPRI). A microarray chip was developed by immobilization of target protein (Lactoferrin (Lac)) and control proteins (α-lactalbumin (α), β-lactoglobulin (β), casein, and bovine serum albumin (BSA)) on the biochip surface. Ag10-NPs were conjugated with an ssDNA library (lib) (Ag10-NPs-library) that consisted of a central 40 nt randomized sequence and a 20 nt fixed primer sequence. Introduction of the Ag10-NPs-library to the SPRI flow channels drastically increased the sensitivity of SPRI signal for real-time monitoring of SELEX. The work allows rapid screening of potential targets, and yields nine aptamers with high affinity (nanomolar range) for Lac after only six-rounds of selection. The aptamer Lac 13–26 was then further tested by SPRI, and the results demonstrated that the aptamer had the capacity to be ultra-sensitive for specific detection of Lac. The novel SPRI-SELEX method demonstrated here showed many advantages of real-time evaluation, high throughput, and high efficiency.
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