Editorial
Reviews
Sensing of Airborne Infochemicals for Green Pest Management: What Is the Challenge?
- Petra Ivaskovic ,
- Bedr'Eddine Ainseba ,
- Yohann Nicolas ,
- Thierry Toupance ,
- Pascal Tardy , and
- Denis Thiéry*
ACS Sensors 2021 , 6 , 11 , 3824-3840 (Review)
Publication Date (Web) : October 27, 2021
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ABSTRACT
One of the biggest global challenges for our societies is to provide natural resources to the rapidly expanding population while maintaining sustainable and ecologically friendly products. The increasing public concern about toxic insecticides has resulted in the rapid development of alternative techniques based on natural infochemicals (ICs). ICs (e.g., pheromones, allelochemicals, volatile organic compounds) are secondary metabolites produced by plants and animals and used as information vectors governing their interactions. Such chemical language is the primary focus of chemical ecology, where behavior-modifying chemicals are used as tools for green pest management. The success of ecological programs highly depends on several factors, including the amount of ICs that enclose the crop, the range of their diffusion, and the uniformity of their application, which makes precise detection and quantification of ICs essential for efficient and profitable pest control. However, the sensing of such molecules remains challenging, and the number of devices able to detect ICs in air is so far limited. In this review, we will present the advances in sensing of ICs including biochemical sensors mimicking the olfactory system, chemical sensors, and sensor arrays (e-noses). We will also present several mathematical models used in integrated pest management to describe how ICs diffuse in the ambient air and how the structure of the odor plume affects the pest dynamics.
Graphene Biodevices for Early Disease Diagnosis Based on Biomarker Detection
- Qingfang Han ,
- Jinbo Pang* ,
- Yufen Li ,
- Baojun Sun ,
- Bergoi Ibarlucea ,
- Xiaoyan Liu ,
- Thomas Gemming ,
- Qilin Cheng ,
- Shu Zhang ,
- Hong Liu* ,
- Jingang Wang ,
- Weijia Zhou ,
- Gianaurelio Cuniberti* , and
- Mark H. Rümmeli*
ACS Sensors 2021 , 6 , 11 , 3841-3881 (Review)
Publication Date (Web) : October 25, 2021
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ABSTRACT
The early diagnosis of diseases plays a vital role in healthcare and the extension of human life. Graphene-based biosensors have boosted the early diagnosis of diseases by detecting and monitoring related biomarkers, providing a better understanding of various physiological and pathological processes. They have generated tremendous interest, made significant advances, and offered promising application prospects. In this paper, we discuss the background of graphene and biosensors, including the properties and functionalization of graphene and biosensors. Second, the significant technologies adopted by biosensors are discussed, such as field-effect transistors and electrochemical and optical methods. Subsequently, we highlight biosensors for detecting various biomarkers, including ions, small molecules, macromolecules, viruses, bacteria, and living human cells. Finally, the opportunities and challenges of graphene-based biosensors and related broad research interests are discussed.
Recent Applications of Pillar[n]arene-Based Host–Guest Recognition in Chemosensing and Imaging
- Yutong Li ,
- Jia Wen* ,
- Jiangshan Li ,
- Zejia Wu ,
- Wei Li* , and
- Kui Yang*
ACS Sensors 2021 , 6 , 11 , 3882-3897 (Review)
Publication Date (Web) : October 19, 2021
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ABSTRACT
Pillar[n]arene is a novel kind of synthetic supramolecular macrocyclic host characterized by its particular pillar-shaped structure consisting of an electron-rich cavity and two finely adjustable rims. Benefiting from its rigid structure, facile synthesis, ease of functionalization, and outstanding host–guest chemistry, pillar[n]arene shows great potential for diverse applications. Significantly, the host–guest recognition of pillar[n]arene provides a novel approach for chemosensing and imaging. Herein, this Review critically and comprehensively reviews the applications of pillar[n]arene-based host–guest recognition in chemosensing and imaging. The sensing and imaging mechanisms as well as the unique roles and advantages of pillar[n]arene-based host–guest recognition are summarized. In addition, preparations of hybrid materials based on pillar[n]arene and inorganic materials are also introduced comprehensively in the light of chemosensing and imaging. Finally, current challenges and perspectives on pillar[n]arene-based host–guest recognition in chemosensing and imaging are outlined.
The Future in Sensing Technologies for Malaria Surveillance: A Review of Hemozoin-Based Diagnosis
- Vitória Baptista ,
- Mariana S. Costa ,
- Carla Calçada ,
- Miguel Silva ,
- José Pedro Gil ,
- Maria Isabel Veiga , and
- Susana O. Catarino*
ACS Sensors 2021 , 6 , 11 , 3898-3911 (Review)
Publication Date (Web) : November 4, 2021
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ABSTRACT
Early and effective malaria diagnosis is vital to control the disease spread and to prevent the emergence of severe cases and death. Currently, malaria diagnosis relies on optical microscopy and immuno-rapid tests; however, these require a drop of blood, are time-consuming, or are not specific and sensitive enough for reliable detection of low-level parasitaemia. Thus, there is an urge for simpler, prompt, and accurate alternative diagnostic methods. Particularly, hemozoin has been increasingly recognized as an attractive biomarker for malaria detection. As the disease proliferates, parasites digest host hemoglobin, in the process releasing toxic haem that is detoxified into an insoluble crystal, the hemozoin, which accumulates along with infection progression. Given its magnetic, optical, and acoustic unique features, hemozoin has been explored for new label-free diagnostic methods. Thereby, herein, we review the hemozoin-based malaria detection methods and critically discuss their challenges and potential for the development of an ideal diagnostic device.
Toward Sensitive and Reliable Surface-Enhanced Raman Scattering Imaging: From Rational Design to Biomedical Applications
- Shanshan Lin ,
- Ziyi Cheng ,
- Qifu Li* ,
- Rui Wang* , and
- Fabiao Yu*
ACS Sensors 2021 , 6 , 11 , 3912-3932 (Review)
Publication Date (Web) : November 2, 2021
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ABSTRACT
Early specific detection through indicative biomarkers and precise visualization of lesion sites are urgent requirements for clinical disease diagnosis. However, current detection and optical imaging methods are insufficient for these demands. Molecular imaging technologies are being intensely studied for reliable medical diagnosis. In the past several decades, molecular imaging with surface-enhanced Raman scattering (SERS) has significant advances from analytical chemistry to medical science. SERS is the inelastic scattering generated from the interaction between photons and substances, presenting molecular structure information. The outstanding SERS virtues of high sensitivity, high specificity, and resistance to biointerference are highly advantageous for biomarker detection in a complex biological matrix. In this work, we review recent progress on the applications of SERS imaging in clinical diagnostics. With the assistance of SERS imaging, the detection of disease-related proteins, nucleic acids, small molecules, and pH of the cellular microenvironment can be implemented for adjuvant medical diagnosis. Moreover, multimodal imaging integrates the high penetration and high speed of other imaging modalities and imaging precision of SERS imaging, resulting in final complete and accurate imaging outcomes and exhibiting robust potential in the discrimination of pathological tissues and surgical navigation. As a promising molecular imaging technology, SERS imaging has achieved remarkable performance in clinical diagnostics and the biomedical realm. It is expected that this review will provide insights for further development of SERS imaging and promote the rapid progress and successful translation of advanced molecular imaging with clinical diagnostics.
Articles
Magnetoelastic Immunosensor via Antibody Immobilization for the Specific Detection of Lysozymes
- Xinru Huang ,
- Shengbo Sang ,
- Zhongyun Yuan* ,
- Qianqian Duan ,
- Xing Guo ,
- Hongpeng Zhang , and
- Chun Zhao*
ACS Sensors 2021 , 6 , 11 , 3933-3939 (Article)
Publication Date (Web) : October 22, 2021
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ABSTRACT
Lysozymes in human urine have crucial clinical significance as an indicator of renal tubular and glomerular diseases. Most lysozyme detection methods rely on the enzyme-linked immunosorbent assay (ELISA), which is usually a tedious procedure. Meanwhile, aptamer sensors and fluorescence-based techniques for lysozyme detection have emerged in recent studies. However, these methods are time-consuming and highly complex in operation, and some even require exorbitant reagents and instruments, which restricts real-time clinical monitoring as diagnostic approaches. Therefore, a rapid and low-cost lysozyme detection method with facile preparation is still in demand for modern precision medicine. Herein, we propose a magnetoelastic (ME) immunosensor for lysozyme detection by detecting changes in resonance frequency under a magnetostrictive effect. The detection system is composed of a magnetoelastic chip with an immobilized lysozyme antibody, a solenoid coil, and a vector network analyzer. Since the ME sensor is ultrasensitive to mass change, the frequency offset caused by mass change can be utilized to detect the content of lysozyme. The immunosensor is evaluated to possess superior sensitivity of 138 Hz/μg mL–1 in terms of the resonance frequency shift (RFS). In addition, our sensor displays an outstanding performance in specificity experiments and shows a relatively lower detection limit (1.26 ng/mL) than other conventional lysozyme detection methods (such as ELISA, chemiluminescence assay, fluorescence, and aptamer biosensors).
tdLanYFP, a Yellow, Bright, Photostable, and pH-Insensitive Fluorescent Protein for Live-Cell Imaging and Förster Resonance Energy Transfer-Based Sensing Strategies
- Yasmina Bousmah ,
- Hana Valenta ,
- Giulia Bertolin ,
- Utkarsh Singh ,
- Valérie Nicolas ,
- Hélène Pasquier ,
- Marc Tramier ,
- Fabienne Merola , and
- Marie Erard*
ACS Sensors 2021 , 6 , 11 , 3940-3947 (Article)
Publication Date (Web) : October 22, 2021
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ABSTRACT
Yellow fluorescent proteins (YFPs) are widely used as optical reporters in Förster resonance energy transfer (FRET)-based biosensors. Although great improvements have been done, the sensitivity of the biosensors is still limited by the low photostability and the poor fluorescence performances of YFPs at acidic pH values. Here, we characterize the yellow fluorescent protein tdLanYFP, derived from the tetrameric protein from the cephalochordate Branchiostoma lanceolatum, LanYFP. With a quantum yield of 0.92 and an extinction coefficient of 133,000 mol–1·L·cm–1, it is, to our knowledge, the brightest dimeric fluorescent protein available. Contrasting with EYFP and its derivatives, tdLanYFP has a very high photostability in vitro and in live cells. As a consequence, tdLanYFP allows imaging of cellular structures with subdiffraction resolution using STED nanoscopy and is compatible with the use of spectromicroscopies in single-molecule regimes. Its very low pK1/2 of 3.9 makes tdLanYFP an excellent tag even at acidic pH values. Finally, we show that tdLanYFP is a valuable FRET partner either as a donor or acceptor in different biosensing modalities. Altogether, these assets make tdLanYFP a very attractive yellow fluorescent protein for long-term or single-molecule live-cell imaging including FRET experiments at acidic pH.
Pentafluorosulfanyl (SF5) as a Superior 19F Magnetic Resonance Reporter Group: Signal Detection and Biological Activity of Teriflunomide Derivatives
- Christian Prinz ,
- Ludger Starke ,
- Tizian-Frank Ramspoth ,
- Janis Kerkering ,
- Vera Martos Riaño ,
- Jérôme Paul ,
- Martin Neuenschwander ,
- Andreas Oder ,
- Silke Radetzki ,
- Siegfried Adelhoefer ,
- Paula Ramos Delgado ,
- Mariya Aravina ,
- Jason M. Millward ,
- Ariane Fillmer ,
- Friedemann Paul ,
- Volker Siffrin ,
- Jens-Peter von Kries ,
- Thoralf Niendorf ,
- Marc Nazaré , and
- Sonia Waiczies*
ACS Sensors 2021 , 6 , 11 , 3948-3956 (Article)
Publication Date (Web) : October 19, 2021
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ABSTRACT
Fluorine (19F) magnetic resonance imaging (MRI) is severely limited by a low signal-to noise ratio (SNR), and tapping it for 19F drug detection in vivo still poses a significant challenge. However, it bears the potential for label-free theranostic imaging. Recently, we detected the fluorinated dihydroorotate dehydrogenase (DHODH) inhibitor teriflunomide (TF) noninvasively in an animal model of multiple sclerosis (MS) using 19F MR spectroscopy (MRS). In the present study, we probed distinct modifications to the CF3 group of TF to improve its SNR. This revealed SF5 as a superior alternative to the CF3 group. The value of the SF5 bioisostere as a 19F MRI reporter group within a biological or pharmacological context is by far underexplored. Here, we compared the biological and pharmacological activities of different TF derivatives and their 19F MR properties (chemical shift and relaxation times). The 19F MR SNR efficiency of three MRI methods revealed that SF5-substituted TF has the highest 19F MR SNR efficiency in combination with an ultrashort echo-time (UTE) MRI method. Chemical modifications did not reduce pharmacological or biological activity as shown in the in vitro dihydroorotate dehydrogenase enzyme and T cell proliferation assays. Instead, SF5-substituted TF showed an improved capacity to inhibit T cell proliferation, indicating better anti-inflammatory activity and its suitability as a viable bioisostere in this context. This study proposes SF5 as a novel superior 19F MR reporter group for the MS drug teriflunomide.
Development of a Rapid and Sensitive CasRx-Based Diagnostic Assay for SARS-CoV-2
- Daniel J. Brogan ,
- Duverney Chaverra-Rodriguez ,
- Calvin P. Lin ,
- Andrea L. Smidler ,
- Ting Yang ,
- Lenissa M. Alcantara ,
- Igor Antoshechkin ,
- Junru Liu ,
- Robyn R. Raban ,
- Pedro Belda-Ferre ,
- Rob Knight ,
- Elizabeth A. Komives , and
- Omar S. Akbari*
ACS Sensors 2021 , 6 , 11 , 3957-3966 (Article)
Publication Date (Web) : October 29, 2021
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ABSTRACT
The development of an extensive toolkit for potential point-of-care diagnostics that is expeditiously adaptable to new emerging pathogens is of critical public health importance. Recently, a number of novel CRISPR-based diagnostics have been developed to detect SARS-CoV-2. Herein, we outline the development of an alternative CRISPR nucleic acid diagnostic utilizing a Cas13d ribonuclease derived from Ruminococcus flavefaciens XPD3002 (CasRx) to detect SARS-CoV-2, an approach we term SENSR (sensitive enzymatic nucleic acid sequence reporter) that can detect attomolar concentrations of SARS-CoV-2. We demonstrate 100% sensitivity in patient-derived samples by lateral flow and fluorescence readout with a detection limit of 45 copy/μL. This technology expands the available nucleic acid diagnostic toolkit, which can be adapted to combat future pandemics.
Co-Polarized [1-13C]Pyruvate and [1,3-13C2]Acetoacetate Provide a Simultaneous View of Cytosolic and Mitochondrial Redox in a Single Experiment
- Gaurav Sharma ,
- Xiaodong Wen ,
- Nesmine R. Maptue ,
- Thomas Hever ,
- Craig R. Malloy ,
- A. Dean Sherry , and
- Chalermchai Khemtong*
ACS Sensors 2021 , 6 , 11 , 3967-3977 (Article)
Publication Date (Web) : November 11, 2021
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ABSTRACT
Cellular redox is intricately linked to energy production and normal cell function. Although the redox states of mitochondria and cytosol are connected by shuttle mechanisms, the redox state of mitochondria may differ from redox in the cytosol in response to stress. However, detecting these differences in functioning tissues is difficult. Here, we employed 13C magnetic resonance spectroscopy (MRS) and co-polarized [1-13C]pyruvate and [1,3-13C2]acetoacetate ([1,3-13C2]AcAc) to monitor production of hyperpolarized (HP) lactate and β-hydroxybutyrate as indicators of cytosolic and mitochondrial redox, respectively. Isolated rat hearts were examined under normoxic conditions, during low-flow ischemia, and after pretreatment with either aminooxyacetate (AOA) or rotenone. All interventions were associated with an increase in [Pi]/[ATP] measured by 31P NMR. In well-oxygenated untreated hearts, rapid conversion of HP [1-13C]pyruvate to [1-13C]lactate and [1,3-13C2]AcAc to [1,3-13C2]β-hydroxybutyrate ([1,3-13C2]β-HB) was readily detected. A significant increase in HP [1,3-13C2]β-HB but not [1-13C]lactate was observed in rotenone-treated and ischemic hearts, consistent with an increase in mitochondrial NADH but not cytosolic NADH. AOA treatments did not alter the productions of HP [1-13C]lactate or [1,3-13C2]β-HB. This study demonstrates that biomarkers of mitochondrial and cytosolic redox may be detected simultaneously in functioning tissues using co-polarized [1-13C]pyruvate and [1,3-13C2]AcAc and 13C MRS and that changes in mitochondrial redox may precede changes in cytosolic redox.
Terpyridine Zn(II) Complexes with Azide Units for Visualization of Histone Deacetylation in Living Cells under STED Nanoscopy
- Wei Du ,
- Dayi Pan ,
- Pan Xiang ,
- Chaoya Xiong ,
- Mingzhu Zhang ,
- Qiong Zhang ,
- Yupeng Tian ,
- Zhongping Zhang ,
- Bo Chen* ,
- Kui Luo ,
- Qiyong Gong , and
- Xiaohe Tian*
ACS Sensors 2021 , 6 , 11 , 3978-3984 (Article)
Publication Date (Web) : September 9, 2021
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ABSTRACT
Histones are the alkali proteins in eukaryotic somatic chromatin cells which constitute the nucleosome structure together with DNA. Their abnormality is often associated with multiple tumorigenesis and other human diseases. Nevertheless, a simple and efficient super-resolution method to visualize histone distribution at the subcellular level is still unavailable. Herein, a Zn(II) terpyridine complex with rich-electronic azide units, namely, TpZnA–His, was designed and synthesized. The initial in vitro and in silico studies suggested that this complex is able to detect histones rapidly and selectively via charge–charge interactions with the histone H3 subunit. Its live cell nuclear localization, red-emission tail, and large Stokes shift allowed super-resolution evaluation of histone distributions with a clear distinction against nuclear DNA. We were able to quantitatively conclude three histone morphology alternations in live cells including condensation, aggregation, and cavity during activating histone acetylation. This work offers a better understanding as well as a versatile tool to study histone-involved gene transcription, signal transduction, and differentiation in cells.
Considerations of Thermodynamics and Kinetics for the Effects of Relative Humidity on the Electrolyte in Electrochemical Toxic Gas Sensors
- Michael L. Hitchman* and
- John R. Saffell
ACS Sensors 2021 , 6 , 11 , 3985-3993 (Article)
Publication Date (Web) : October 21, 2021
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ABSTRACT
In this paper, the physical chemistry of the absorption and desorption of water vapor for electrochemical gas sensors with commonly used sulfuric acid as the electrolyte is investigated. Electrochemical gas sensors are being increasingly used for monitoring toxic gases in the environment, and they are, in principle, simple devices, but in practice, their operation is complex. In particular, changes in atmospheric humidity and temperature can have significant effects on the sensor output. A model has been developed for the calculation of sensor weight changes as humidity varies, which are in good agreement with the analysis of experimental results. This then allows for the calculation of the rather more important electrolyte volume variations. Changes in acid molarity and physical characteristics of the electrolyte have also been determined. The effects on working electrode (WE) electrocatalytic activity are discussed, and potential problems with sensors for environmental monitoring are highlighted. In particular, changes in the electroactive area of the WE and, consequently, of the sensor output, and flooding of the WE catalyst aggregates which can lead to problems with electrolyte leakage from sensors are considered.
Immobilization of Recombinant Fluorescent Biosensors Permits Imaging of Extracellular Ion Signals
- Sandra Burgstaller ,
- Helmut Bischof ,
- Thomas Rauter ,
- Tony Schmidt ,
- Rainer Schindl ,
- Silke Patz ,
- Bernhard Groschup ,
- Severin Filser ,
- Lucas van den Boom ,
- Philipp Sasse ,
- Robert Lukowski ,
- Nikolaus Plesnila ,
- Wolfgang F. Graier , and
- Roland Malli*
ACS Sensors 2021 , 6 , 11 , 3994-4000 (Article)
Publication Date (Web) : November 9, 2021
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ABSTRACT
Given the importance of ion gradients and fluxes in biology, monitoring ions locally at the exterior of the plasma membrane of intact cells in a noninvasive manner is highly desirable but challenging. Classical targeting of genetically encoded biosensors at the exterior of cell surfaces would be a suitable approach; however, it often leads to intracellular accumulation of the tools in vesicular structures and adverse modifications, possibly impairing sensor functionality. To tackle these issues, we generated recombinant fluorescent ion biosensors fused to traptavidin (TAv) specifically coupled to a biotinylated AviTag expressed on the outer cell surface of cells. We show that purified chimeras of TAv and pH-Lemon or GEPII 1.0, Förster resonance energy transfer-based pH and K+ biosensors, can be immobilized directly and specifically on biotinylated surfaces including glass platelets and intact cells, thereby remaining fully functional for imaging of ion dynamics. The immobilization of recombinant TAv–GEPII 1.0 on the extracellular cell surface of primary cortical rat neurons allowed imaging of excitotoxic glutamate-induced K+ efflux in vitro. We also performed micropatterning of purified TAv biosensors using a microperfusion system to generate spatially separated TAv–pH-Lemon and TAv–GEPII 1.0 spots for simultaneous pH and K+ measurements on cell surfaces. Our results suggest that the approach can be greatly expanded by immobilizing various biosensors on extracellular surfaces to quantitatively visualize microenvironmental transport and signaling processes in different cell culture models and other experimental settings.
Fluorescent Sensor Array for Quantitative Determination of Saccharides
- Mariia Pushina ,
- Andrej Penavic ,
- Sepideh Farshbaf , and
- Pavel Anzenbacher Jr.*
ACS Sensors 2021 , 6 , 11 , 4001-4008 (Article)
Publication Date (Web) : October 20, 2021
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ABSTRACT
Accurate monitoring of sugar levels is essential for many fields from food industry to human health. Here, we developed FRET-based dual chromophore sensors for saccharides that form oxazolidine boronate and may be employed as a noninvasive method for monitoring of sugar levels in biological fluids, namely, urine. The saccharide-binding properties of the sensors were studied using fluorescence spectroscopy and utilized in the determination of saccharides in a high-throughput manner. Here, two fluorescent sensors were successful in the classification of nine different monosaccharides and disaccharides with 100% correct classification. Furthermore, the dual chromophore self-assembled sensors were successfully utilized for the quantitative determination of important carbohydrates such as glucose in the presence of competitive saccharides (fructose) and in complex media (urine) without sample pretreatment. The present fluorescent sensors allow for quantification of glucose in a concentration range of 0–60 mM, which matches the concentration range of frequently used urinalysis test strips.
Membrane-Activated Fluorescent Probe for High-Fidelity Imaging of Mitochondrial Membrane Potential
- Bo Lin ,
- Yunfan Liu ,
- Xiaoping Zhang ,
- Li Fan ,
- Yang Shu* , and
- Jianhua Wang*
ACS Sensors 2021 , 6 , 11 , 4009-4018 (Article)
Publication Date (Web) : November 10, 2021
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ABSTRACT
Mitochondrial membrane potential (ΔΨm) is a key indicator of cell health or injury due to its vital roles in adenosine 5′-triphosphate synthesis. Thus, monitoring ΔΨm is of great significance for the assessment of cell status, diagnosis of diseases, and medicament screening. Cationic fluorescent probes suffer from severe photobleaching or false positive signals due to the luminescence of the probe on non-mitochondria. Herein, we report a lipophilic cationic fluorescent probe [1-methyl-2-(4-(1,2,2-triphenylvinyl)styryl)-β-naphthothiazol-1-ium trifluoromethanesulfonate (TPE-NT)] with the features of aggregation-induced emission and intramolecular charge transfer for imaging ΔΨm in live cells. TPE-NT is enriched on the surface of the mitochondrial inner membrane due to the negative ΔΨm, and its fluorescence is activated in the high-viscosity microenvironment. The false positive signals of emission from TPE-NT on non-mitochondria are therefore effectively eliminated. Moreover, TPE-NT exhibits a Stokes shift of >200 nm, near-infrared (∼675 nm) emission, excellent photostability, and low cytotoxicity, which facilitate real-time imaging in live cells. Cell imaging confirmed that the probe can rapidly and reliably report mitochondrial depolarization (decrement of ΔΨm) during cell damage caused by CCCP and H2O2 as well as mitochondrial polarization (increment of ΔΨm) by oligomycin. Furthermore, the probe successfully detected the reduction of ΔΨm in these cell models of hypoxia, heat damage, acidification, aging, inflammation, mitophagy, and apoptosis caused by hypoxia, heatstroke, lactate/pyruvate, doxorubicin, lipopolysaccharide, rapamycin, monensin, and nystatin, respectively.
Effects of Gas Adsorption Properties of an Au-Loaded Porous In2O3 Sensor on NO2-Sensing Properties
- Taro Ueda* ,
- Inci Boehme ,
- Takeo Hyodo ,
- Yasuhiro Shimizu ,
- Udo Weimar , and
- Nicolae Barsan
ACS Sensors 2021 , 6 , 11 , 4019-4028 (Article)
Publication Date (Web) : October 25, 2021
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ABSTRACT
Gas adsorption properties of semiconductor-type gas sensors using porous (pr-) In2O3 powders loaded with and without 0.5 wt % Au (Au/pr-In2O3 and pr-In2O3 sensors, respectively) at 100 °C were examined by using diffuse reflectance infrared Fourier transform spectroscopy, and the effect of the Au loading onto pr-In2O3 on the NO2-sensing properties were discussed in this study. We found the following: the resistance of the Au/pr-In2O3 sensor in dry air is lower than that of the pr-In2O3 sensor; the DRIFT spectra of both the sensors show a broad positive band between 1600 and 1000 cm–1 in dry air (reference: in dry N2 at 100 °C), which mainly originates from oxygen adsorbates and/or lattice oxygen, and that this band is much larger for the Au/pr-In2O3 sensor than for the pr-In2O3 sensor; the Au loading also increases the adsorption amount of H2O and the reactivity of NO2 on the pr-In2O3 surface; and the NO2 response of the Au/pr-In2O3 sensor in dry air is marginally higher than that of the pr-In2O3 sensor in the examined concentration range of NO2 (0.6–5 ppm) in dry air. The obtained results strongly support the enhancement of the NO2 adsorption onto the pr-In2O3 surface by Au loading, which contributed to the improvement of the NO2-sensing properties.
Stimuli-Induced Upgrade of Nuclease-Resistant DNA Nanostructure Composed of a Single Molecular Beacon for Detecting Mutant Genes
- Chang Xue ,
- Lei Wang ,
- Hong Huang ,
- Ruozhong Wang ,
- Pei Yuan* , and
- Zai-Sheng Wu*
ACS Sensors 2021 , 6 , 11 , 4029-4037 (Article)
Publication Date (Web) : November 3, 2021
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ABSTRACT
As a kind of cell-free DNA in the bloodstream liberated from tumor cells, circulating tumor DNAs (ctDNAs) have been recognized as promising biomarkers in the field of early cancer diagnosis. However, robust, sensitive, and accurate detection of ctDNA in serum remains extremely challenging, especially toward the mutant KRAS gene, one of the most frequently mutated genes. Although DNA oligonucleotides as emerging practical signaling materials have been developed as sensitive and accurate tools, some intrinsic defects need to be overcome, such as fragility in complex biological environments. In this work, on the basis of the hydrophilicity-promoted assembly, a core/shell DNA nanostructure (DNS-MB) probe is constructed from only one hairpin-shaped probe (cholesterol-modified palindromic molecular beacon, Chol-PMB) for the amplification detection of KRAS mutation in serum without the need for any auxiliary probe. Chol-PMB is designed to recognize target DNA and serve as a polymerization primer and template, and thus target species can initiate polymerization-based strand displacement amplification (SDA). Moreover, target DNA is able to induce further aggregation of DNS-MB particles due to the enzymatic cross-linking effect, leading to a structural upgrade. The DNS-MB probe exhibits a detection limit of 50 fM and a wide quantitative range (from 50 fM to 160 nM). In addition, single nucleotide polymorphisms can be discriminated, such as mutant KRAS G12D (KRAS-M), providing a desirable platform for screening ctDNAs. More excitingly, because the termini of DNA components are hidden inward from nuclease attack, DNS-MB circumvents a false-positive signal even in freshly sampled serum and is suitable for application in the complex biological milieu. As a proof of concept, the DNS-MB probe is expected to provide useful insight into the development of simple and degradation-resistant DNA probes for substantially amplified detection of ctDNAs in complex serum, showing potential applications in the field of early tumor diagnosis.
Programmable-Printing Paper-Based Device with a MoS2 NP and Gmp/Eu-Cit Fluorescence Couple for Ratiometric Tetracycline Analysis in Various Natural Samples
- Zongbao Sun ,
- Yunlong Gao ,
- Zeng Niu ,
- Haodong Pan ,
- Xuechao Xu ,
- Wen Zhang* , and
- Xiaobo Zou
ACS Sensors 2021 , 6 , 11 , 4038-4047 (Article)
Publication Date (Web) : October 21, 2021
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ABSTRACT
Paper-based fluorescence devices, with smartphone aids, bring considerable operation convenience for tetracycline (TC) sensing. Nevertheless, they must meet the challenge in real determination against complicated backgrounds. Considering that, we present a programmable-printing paper-based device and then apply it to TC determination for various natural samples. MoS2 NPs and Gmp/Eu-Cit are synthetized as composite probes. A static quenching process is found with MoS2 NP fluorescence at 430 nm, while significant magnification of Gmp/Eu-Cit emission is obtained at 617 nm, establishing a valuable ratiometric indicator. Remarkably, two-stage programmable printing maximizes the proposed sensing capability. A transitive device, containing a gradually changing amount of a certain probe, is prepared to sense TC. With a homemade smartphone application and 3D-printed measurement chamber, the corresponding signals are examined to explore optimal setups. These setups are automatically processed to prepare the final-version device, not requiring manual operations. Benefitting from this interesting feature, the proposed device gains many rewards in performances. It effectively senses TC in a wide range from 12.7 nM to 80 μM and simultaneously provides naked eye-legible signals and smartphone-based readouts with confident selectivity and stability. This device is consequently applied for various samples of soil, river water, milk, and serum and meets well with HPLC–MS and recovery tests.
Rotary Valve-Assisted Fluidic System Coupling with CRISPR/Cas12a for Fully Integrated Nucleic Acid Detection
- Hui Wu ,
- Siwenjie Qian ,
- Cheng Peng ,
- Xiaofu Wang ,
- Tingzhang Wang ,
- Xiaoping Zhong ,
- Yanju Chen ,
- Qunqing Yang ,
- Junfeng Xu* , and
- Jian Wu*
ACS Sensors 2021 , 6 , 11 , 4048-4056 (Article)
Publication Date (Web) : October 19, 2021
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ABSTRACT
Of late, many nucleic acid analysis platforms have been established, but there is still room for constructing integrated nucleic acid detection systems with high nucleic acid extraction efficiency, low detection cost, and convenient operation. In this work, a simple rotary valve-assisted fluidic chip coupling with CRISPR/Cas12a was established to achieve fully integrated nucleic acid detection. All of the detection reagents were prestored on the fluidic chip. With the aid of the rotary valve and syringe, the liquid flow and stirring can be precisely controlled. The nucleic acid extraction, loop-mediated isothermal amplification (LAMP) reaction, and CRISPR detection could be completed in 80 min. A clean reservoir and an air reservoir on the fluidic chip were designed to effectively remove the remaining ethanol. With Vibrio parahaemolyticus as the targets, the detection sensitivity of the fluidic chip could reach 3.1 × 101 copies of target DNA per reaction. A positive sample could be sensitively detected by CRISPR/Cas12a to produce a green fluorescent signal, while a negative sample generated no fluorescent signal. Further, the fluidic chip was successfully applied for detection of spiked shrimp samples, which showed the same detection sensitivity. A great feasibility for real-sample detection was showed by the fluidic chip. The proposed detection platform did not need expensive centrifugal instruments or pumps, which displayed its potential to become a powerful tool for food safety analysis and clinical diagnostics, especially in the resource-limited areas.
Microfluidic Biosensor for Rapid Nucleic Acid Quantitation Based on Hyperspectral Interferometric Amplicon-Complex Analysis
- Rongxin Fu ,
- Wenli Du ,
- Xiangyu Jin ,
- Ruliang Wang ,
- Xue Lin ,
- Ya Su ,
- Han Yang ,
- Xiaohui Shan ,
- Wenqi Lv ,
- Zhi Zheng* , and
- Guoliang Huang*
ACS Sensors 2021 , 6 , 11 , 4057-4066 (Article)
Publication Date (Web) : October 25, 2021
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ABSTRACT
Nucleic acid detection plays a vital role in both biomedical research and clinical medicine. The temperature circulation changes of the widely used polymerase chain reaction technique are time-consuming and technically challenging for system development. Recombinase polymerase amplification (RPA) is an isothermal method for rapid nucleic acid detection. However, current RPA amplicon detection methods are complicated and expensive and easily generate false positives, restricting the promotion of RPA techniques. In this work, a hyperspectral interferometric amplicon-complex quantitation method is presented, combined with asymmetric dipole complex strategy optical scattering analysis. GelRed dye was utilized to form amplicon-complex particles, and the Fourier domain spectrum computation contributed to complex scattering quantitation. With this method, a supporting microfluidic chip and automatic system were developed to achieve integrated, rapid, quantitative, and miniscule nucleic acid detection. The Plasmodium falciparum dhfr gene was utilized as an example for targeted nucleic acid quantitation and single nucleotide polymorphism detection. The total reaction time was decreased to merely 20 min, and the limit of detection was only 3.17 ng/μL. The minimum measurable concentration of target was 1.68 copies/μL, 31.67 times more sensitive than turbidity detection, and the single reaction chamber was only 9.33 μL. No scattering increase occurred for template-free control, and thus, false positives caused by primer dimers and nonspecific products could be avoided. The experimental results prove that the provided method and system can detect single-base mutations in the dhfr gene and is a reasonable technique for rapid, automatic, and low-cost nucleic acid detection.
Electrochemical Capillary-Flow Immunoassay for Detecting Anti-SARS-CoV-2 Nucleocapsid Protein Antibodies at the Point of Care
- Isabelle C. Samper ,
- Ana Sánchez-Cano ,
- Wisarut Khamcharoen ,
- Ilhoon Jang ,
- Weena Siangproh ,
- Eva Baldrich ,
- Brian J. Geiss ,
- David S. Dandy , and
- Charles S. Henry*
ACS Sensors 2021 , 6 , 11 , 4067-4075 (Article)
Publication Date (Web) : October 25, 2021
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ABSTRACT
Rapid and inexpensive serological tests for SARS-CoV-2 antibodies are needed to conduct population-level seroprevalence surveillance studies and can improve diagnostic reliability when used in combination with viral tests. Here, we report a novel low-cost electrochemical capillary-flow device to quantify IgG antibodies targeting SARS-CoV-2 nucleocapsid proteins (anti-N antibody) down to 5 ng/mL in low-volume (10 μL) human whole blood samples in under 20 min. No sample preparation is needed as the device integrates a blood-filtration membrane for on-board plasma extraction. The device is made of stacked layers of a hydrophilic polyester and double-sided adhesive films, which create a passive microfluidic circuit that automates the steps of an enzyme-linked immunosorbent assay (ELISA). The sample and reagents are sequentially delivered to a nitrocellulose membrane that is modified with a recombinant SARS-CoV-2 nucleocapsid protein. When present in the sample, anti-N antibodies are captured on the nitrocellulose membrane and detected via chronoamperometry performed on a screen-printed carbon electrode. As a result of this quantitative electrochemical readout, no result interpretation is required, making the device ideal for point-of-care (POC) use by non-trained users. Moreover, we show that the device can be coupled to a near-field communication potentiostat operated from a smartphone, confirming its true POC potential. The novelty of this work resides in the integration of sensitive electrochemical detection with capillary-flow immunoassay, providing accuracy at the point of care. This novel electrochemical capillary-flow device has the potential to aid the diagnosis of infectious diseases at the point of care.
Subcellular Dynamic Immunopatterning of Cytosolic Protein Complexes on Microstructured Polymer Substrates
- Roland Hager ,
- Ulrike Müller ,
- Nicole Ollinger ,
- Julian Weghuber* , and
- Peter Lanzerstorfer*
ACS Sensors 2021 , 6 , 11 , 4076-4088 (Article)
Publication Date (Web) : October 15, 2021
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ABSTRACT
Analysis of protein–protein interactions in living cells by protein micropatterning is currently limited to the spatial arrangement of transmembrane proteins and their corresponding downstream molecules. Here, we present a robust and straightforward method for dynamic immunopatterning of cytosolic protein complexes by use of an artificial transmembrane bait construct in combination with microstructured antibody arrays on cyclic olefin polymer substrates. As a proof, the method was used to characterize Grb2-mediated signaling pathways downstream of the epidermal growth factor receptor (EGFR). Ternary protein complexes (Shc1:Grb2:SOS1 and Grb2:Gab1:PI3K) were identified, and we found that EGFR downstream signaling is based on constitutively bound (Grb2:SOS1 and Grb2:Gab1) as well as on agonist-dependent protein associations with transient interaction properties (Grb2:Shc1 and Grb2:PI3K). Spatiotemporal analysis further revealed significant differences in stability and exchange kinetics of protein interactions. Furthermore, we could show that this approach is well suited to study the efficacy and specificity of SH2 and SH3 protein domain inhibitors in a live cell context. Altogether, this method represents a significant enhancement of quantitative subcellular micropatterning approaches as an alternative to standard biochemical analyses.
Development of an Electrochemical Dual H2S/Ca2+ Microsensor and Its In Vivo Application to a Rat Seizure Model
- Jaeyoung Lee ,
- Yoonyi Jeong ,
- Subin Park ,
- Minah Suh* , and
- Youngmi Lee*
ACS Sensors 2021 , 6 , 11 , 4089-4097 (Article)
Publication Date (Web) : October 14, 2021
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ABSTRACT
A dual electrochemical microsensor was fabricated for concurrent monitoring of hydrogen sulfide (H2S) and calcium ions (Ca2+), which are closely linked important signaling species involved in various physiological processes. The dual sensor was prepared using a dual recessed electrode consisting of two platinum (Pt) microdisks (50 μm in diameter). Each electrode was individually optimized for the best sensing ability toward a target analyte. One electrode (WE1, amperometric H2S sensor) was modified with electrodeposition of Au and electropolymerized polyaniline coating. The other electrode (WE2, all-solid-state Ca2+-selective electrode) was composed of Ag/AgCl onto the recessed Pt disk formed via electrodeposition/chloridation, followed by silanization and Ca2+-selective membrane loading. The current of WE1 and the potential of WE2 in a dual sensor responded linearly to H2S concentration and logarithm of Ca2+ concentration, respectively, without a crosstalk between the sensing signals. Both WE1 and WE2 presented excellent sensitivity, selectivity (logKH2S,iAmp≤−3.5, i = CO, NO, O2, NO2–, AP, AA, DA, and GABA; and logKCa2+,jPot≤−3.2, j = Na+, K+, and Mg2+), and fast response time with reasonable stability (during ca. 6 h in vivo experiment). Particularly, WE2 prepared using a mixture of two ionophores (ETH1001 and ETH129) and two plasticizers (2-nitrophenyl octyl ether and bis(2-ethylhexyl) sebacate) showed a very shortened response time (tR to attain the ΔE/Δt slope of 0.6 mV/min = 3.0 ± 0.2 s, n ≥ 10), a critically required factor for real-time analysis. The developed sensor was utilized for simultaneous real-time monitoring of H2S and Ca2+ changes at the brain cortex surface of a living rat during spontaneous epileptic seizures induced by a cortical 4-aminopyridine injection. The dynamic changes of H2S and Ca2+ were clearly observed in an intimate correlation with the electrophysiological recording of seizures, demonstrating the sensor feasibility of in vivo and real-time simultaneous measurements of H2S and Ca2+.
SARS-CoV-2-Impedimetric Biosensor: Virus-Imprinted Chips for Early and Rapid Diagnosis
- Heba A. Hussein ,
- Ahmed Kandeil ,
- Mokhtar Gomaa ,
- Rasha Mohamed El Nashar ,
- Ibrahim M. El-Sherbiny , and
- Rabeay Y. A. Hassan*
ACS Sensors 2021 , 6 , 11 , 4098-4107 (Article)
Publication Date (Web) : November 10, 2021
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ABSTRACT
Due to the current global SARS-CoV-2 pandemic, rapid and accurate diagnostic tools are needed to prevent the spread of COVID-19 across the globe. An electrochemical sensing platform was constructed using CNTs/WO3-screen printed electrodes for imprinting the complete virus particles (SARS-CoV-2 particles) within the polymeric matrix to create viral complementary binding sites. The sensor provided high selectivity toward the target virus over other tested human corona and influenza respiratory interference viruses. The sensitivity performance of the sensor chips was evaluated using different viral concentrations, while the limits of detection and quantification were 57 and 175 pg/mL, respectively. Reaching this satisfied low detection limit (almost 27-fold more sensitive than the RT-PCR), the sensor was applied in clinical specimens obtained from SARS-CoV-2 suspected cases. Thus, dealing directly with clinical samples on the chip could be provided as a portable device for instantaneous and simple point of care in hospitals, airports, and hotspots.
Flexible Tongue Electrode Array System for In Vivo Mapping of Electrical Signals of Taste Sensation
- Shuang Huang ,
- Tao Zhang ,
- Hongbo Li ,
- Mingyue Zhang ,
- Xingxing Liu ,
- Dongxin Xu ,
- Hao Wang ,
- Zhiran Shen ,
- Qianni Wu ,
- Jun Tao ,
- Wenhao Xia* ,
- Xi Xie* , and
- Fanmao Liu*
ACS Sensors 2021 , 6 , 11 , 4108-4117 (Article)
Publication Date (Web) : November 10, 2021
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ABSTRACT
Tongue is a unique organ that senses tastes, and the scientific puzzle about whether electricity can evoke taste sensations and how the sensations have been distributed on the tongue has not been solved. Investigations on tongue stimulation by electricity might benefit the developments of techniques for clinical neuromodulation, tissue activation, and a brain–tongue–machine interface. To solve the scientific puzzle of whether electrical stimulation induces taste-related sensations, a portable flexible tongue electrode array system (FTEAS) was developed, which can synchronously provide electrical stimulation and signal mapping at each zone of the tongue. Utilizing the FTEAS to perform tests on the rat tongue in vivo, specific electrical signals were observed to be evoked by chemical and electrical stimulations. The features and distributions of the electric signals evoked during the rat tongue tests were systematically studied and comprehensively analyzed. The results show that an appropriate electrical stimulation can induce multiple sensations simultaneously, while the distribution of each sensation was not significantly distinguished among different zones of the tongue, and at the same time, this taste-related electrical signal can be recorded by the FTEAS. This work establishes a promising platform to solve the scientific puzzle of how sensations are activated chemically and electrically on the tongue and may provide advanced noninvasive oral-electrotherapy and a brain–tongue–machine interface.
Crystalline-to-Amorphous Phase Transformation in CuO Nanowires for Gaseous Ionization and Sensing Application
- Hai Liu ,
- Haoyu Zhang ,
- Wenhuan Zhu ,
- Maolin Bo , and
- Tingting Zhao*
ACS Sensors 2021 , 6 , 11 , 4118-4125 (Article)
Publication Date (Web) : October 27, 2021
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ABSTRACT
We report a dramatic reduction of operation voltage of a CuO nanowire-based ionization gas sensor due to the crystalline-to-amorphous phase transformation. The structural change is attributed to the ion bombardment and heating effect during the initial discharge, which brings about the formation of abundant nanocrystallites and surface states favoring gaseous ionization. The gas-sensing properties of the CuO nanowire sensor are confirmed by differentiating various types or concentrations of volatile organic compounds diluted in nitrogen, with a low detection limit at the ppm level. Moreover, a sensing mechanism is proposed on the basis of charge redistribution by electron-gas collision related to the specific ionization energy. The insightful study of the electrode microstructure delivers an exploratory investigation to the effect of gas ionization toward the discharge system, which provides new approaches to develop advanced ionization gas sensors.
Dense Packed Drivable Optrode Array for Precise Optical Stimulation and Neural Recording in Multiple-Brain Regions
- Longchun Wang ,
- Chaofan Ge ,
- Fang Wang ,
- Zhejun Guo ,
- Wen Hong ,
- Chunpeng Jiang ,
- Bowen Ji ,
- Minghao Wang ,
- Chengyu Li ,
- Bomin Sun , and
- Jingquan Liu*
ACS Sensors 2021 , 6 , 11 , 4126-4135 (Article)
Publication Date (Web) : November 15, 2021
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ABSTRACT
The input–output function of neural networks is complicated due to the huge number of neurons and synapses, and some high-density implantable electrophysiology recording tools with a plane structure have been developed for neural circuit studies in recent years. However, traditional plane probes are limited by the record-only function and inability to monitor multiple-brain regions simultaneously, and the complete cognition of neural networks still has a long way away. Herein, we develop a three-dimensional (3D) high-density drivable optrode array for multiple-brain recording and precise optical stimulation simultaneously. The optrode array contains four-layer probes with 1024 microelectrodes and two thinned optical fibers assembled into a 3D-printed drivable module. The recording performance of microelectrodes is optimized by electrochemical modification, and precise implantation depth control of drivable optrodes is verified in agar. Moreover, in vivo experiments indicate neural activities from CA1 and dentate gyrus regions are monitored, and a tracking of the neuron firing for 2 weeks is achieved. The suppression of neuron firing by blue light has been realized through high-density optrodes during optogenetics experiments. With the feature of large-scale recording, optoelectronic integration, and 3D assembly, the high-density drivable optrode array possesses an important value in the research of brain diseases and neural networks.
On-Chip Optical Anodic Stripping with Closed Bipolar Cells and Cathodic Electrochemiluminescence Reporting
- Jeronimo Miranda ,
- Nicholas Humphrey ,
- Rowan Kinney ,
- Riley O'Sullivan ,
- Bradley Thomas ,
- Ivan Elias Mondaca Medina ,
- Ryan Freedman , and
- Eli Fahrenkrug*
ACS Sensors 2021 , 6 , 11 , 4136-4144 (Article)
Publication Date (Web) : October 26, 2021
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ABSTRACT
The aim of this work was to develop a simple, accessible, and point-of-use sensor to measure heavy metal ions in water in low-resource areas that cannot accommodate expensive or technical solutions. This report describes a new bipolar electrochemical sensor platform that reimagines conventional anodic stripping voltammetry in a wireless bipolar format with an optical electrochemiluminescent readout that can be quantified with any simple optical sensor like that found on most modern cell phone cameras. We call this technique as optical anodic stripping. Using a new nonlithographic fabrication process, devices could be produced rapidly and simply at <$1/sensor. The sensing scheme was developed, characterized, and optimized using electrochemical and optical methods. Quantitation of Pb2+ in both lab and natural water samples was rapid (2–3 min), accurate, precise, and highly linear in the 25–1000 ppb range and was shown to be sufficiently selective in the presence of other common heavy metal ions such as Cu2+, Cd2+, and Zn2+.
An Analysis of a Highly Sensitive and Selective Hydrogen Gas Sensor Based on a 3D Cu-Doped SnO2 Sensing Material by Efficient Electronic Sensor Interface
- Sihyeok Kim ,
- Gurpreet Singh ,
- Mintaek oh , and
- Keekeun Lee*
ACS Sensors 2021 , 6 , 11 , 4145-4155 (Article)
Publication Date (Web) : November 4, 2021
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ABSTRACT
In this research, a highly sensitive and selective hydrogen gas sensor was developed based on Cu-doped SnO2. Sensing characteristics were compared based on SnO2 doped with different concentrations of Cu, and the highest sensitivity and fastest response time were shown when 3% Cu was contained. A 3D structure was formed using a polystyrene to increase the surface-to-volume ratio, which allows more oxygen molecules to bond with the surface of the SnO2 sensing material. Extremely increased sensitivity was observed as compared to the planar structure. A temperature sensor and micro-heater were integrated into the sensor, and the surface temperature was maintained constant regardless of external influences. In addition, an electronic sensor interface was developed for the efficient analysis of real-time data. The developed sensor was wire-bonded to the flexible printed circuit board (FPCB) cable and connected with the sensor interface. Sensitivity and linearity measured based on the developed sensor and interface system were analyzed as 0.286%/ppm and 0.98, respectively, which were almost similar to the results observed by a digital multimeter (DMM). This indicates that our developed sensor system can be a very promising candidate for real-time measurement and can be applied in various fields. The enhanced sensitivity of 3% doped SnO2 toward hydrogen is attributed to the huge number of oxygen vacancies in the doped sample.
Hybrid-Flexible Bimodal Sensing Wearable Glove System for Complex Hand Gesture Recognition
- Jieming Pan* ,
- Yida Li ,
- Yuxuan Luo ,
- Xiangyu Zhang ,
- Xinghua Wang ,
- David Liang Tai Wong ,
- Chun-Huat Heng ,
- Chen-Khong Tham , and
- Aaron Voon-Yew Thean*
ACS Sensors 2021 , 6 , 11 , 4156-4166 (Article)
Publication Date (Web) : November 2, 2021
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ABSTRACT
As 5G communication technology allows for speedier access to extended information and knowledge, a more sophisticated human–machine interface beyond touchscreens and keyboards is necessary to improve the communication bandwidth and overcome the interfacing barrier. However, the full extent of human interaction beyond operation dexterity, spatial awareness, sensory feedback, and collaborative capability to be replicated completely remains a challenge. Here, we demonstrate a hybrid-flexible wearable system, consisting of simple bimodal capacitive sensors and a customized low power interface circuit integrated with machine learning algorithms, to accurately recognize complex gestures. The 16 channel sensor array extracts spatial and temporal information of the finger movement (deformation) and hand location (proximity) simultaneously. Using machine learning, over 99 and 91% accuracy are achieved for user-independent static and dynamic gesture recognition, respectively. Our approach proves that an extremely simple bimodal sensing platform that identifies local interactions and perceives spatial context concurrently, is crucial in the field of sign communication, remote robotics, and smart manufacturing.
Discriminating BTX Molecules by the Nonselective Metal Oxide Sensor-Based Smart Sensing System
- Hongyu Liu ,
- Gang Meng* ,
- Zanhong Deng ,
- Kazuki Nagashima ,
- Shimao Wang ,
- Tiantian Dai ,
- Liang Li* ,
- Takeshi Yanagida , and
- Xiaodong Fang*
ACS Sensors 2021 , 6 , 11 , 4167-4175 (Article)
Publication Date (Web) : November 4, 2021
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ABSTRACT
Discriminating structurally similar volatile organic compounds (VOCs) molecules, such as benzene, toluene, and three xylene isomers (BTX), remains a significant challenge, especially, for metal oxide semiconductor (MOS) sensors, in which selectivity is a long-standing challenge. Recent progress indicates that temperature modulation of a single MOS sensor offers a powerful route in extracting the features of adsorbed gas analytes than conventional isothermal operation. Herein, a rectangular heating waveform is applied on NiO-, WO3-, and SnO2-based sensors to gradually activate the specific gas/oxide interfacial redox reaction and generate rich (electrical) features of adsorbed BTX molecules. Upon several signal preprocessing steps, the intrinsic feature of BTX molecules can be extracted by the linear discrimination analysis (LDA) or convolutional neural network (CNN) analysis. The combination of three distinct MOS sensors noticeably benefits the recognition accuracy (with a reduced number of training iterations). Finally, a prototype of a smart BTX recognition system (including sensing electronics, sensors, Wi-Fi module, UI, PC, etc.) based on temperature modulation has been explored, which enables a prompt, accurate, and stable identification of xylene isomers in the ambient air background and raises the hope of innovating the future advanced machine olfactory system.
A Valve-Enabled Sample Preparation Device with Isothermal Amplification for Multiplexed Virus Detection at the Point-of-Care
- Carlos Manzanas ,
- Md. Mahbubul Alam ,
- Julia C. Loeb ,
- John A. Lednicky ,
- Chang-Yu Wu , and
- Z. Hugh Fan*
ACS Sensors 2021 , 6 , 11 , 4176-4184 (Article)
Publication Date (Web) : November 12, 2021
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ABSTRACT
Early and accurate detection of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) and influenza viruses at the point-of-care is crucial for reducing disease transmission during the current pandemic and future flu seasons. To prepare for potential cocirculation of these two viruses, we report a valve-enabled, paper-based sample preparation device integrated with isothermal amplification for their simultaneous detection. The device incorporates (1) virus lysis and RNA enrichment, enabled by ball-based valves for sequential delivery of reagents with no pipet requirement, (2) reverse transcription loop-mediated isothermal amplification, carried out in a coffee mug, and (3) colorimetric detection. We have used the device for simultaneously detecting inactivated SARS-CoV-2 and influenza A H1N1 viruses in 50 min, with limits of detection at 2 and 6 genome equivalents, respectively. The device was further demonstrated to detect both viruses in environmental samples.
Extremely Sensitive Molecularly Imprinted ECL Sensor with Multiple Probes Released from Liposomes Immobilized by a Light-Triggered Click Reaction
- Guangyan Liu ,
- Jun Ling , and
- Jianping Li*
ACS Sensors 2021 , 6 , 11 , 4185-4192 (Article)
Publication Date (Web) : October 18, 2021
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ABSTRACT
A molecularly imprinted electrochemiluminescence sensor was prepared for sensitive and selective determination of aminotriazole via a novel strategy of multiple Ru(bpy)3Cl2 probes released from liposomes immobilized by a light-triggered click reaction. This sensing strategy provides a platform for trace detection of amino-containing pesticides. The target on the molecularly imprinted membrane connected to the Ru(bpy)3Cl2-encapsulated liposomes via the click reaction. After the destabilizing agent Triton X-100 was added, numerous Ru(bpy)3Cl2 molecules were released by liposomes on the molecularly imprinted polymer electrode. The ECL response of the sensor was linearly proportional to the logarithm of the aminotriazole concentration ranging from 5.00 × 10–18 to 1.00 × 10–12 mol/L, and the detection limit was 1.15 × 10–18 mol/L. The sensitivity of the detection was significantly improved, and the analysis process was simplified.
A Rationally and Computationally Designed Fluorescent Biosensor for d-Serine
- Vanessa Vongsouthi ,
- Jason H. Whitfield ,
- Petr Unichenko ,
- Joshua A. Mitchell ,
- Björn Breithausen ,
- Olga Khersonsky ,
- Leon Kremers ,
- Harald Janovjak ,
- Hiromu Monai ,
- Hajime Hirase ,
- Sarel J. Fleishman ,
- Christian Henneberger* , and
- Colin J. Jackson*
ACS Sensors 2021 , 6 , 11 , 4193-4205 (Article)
Publication Date (Web) : November 16, 2021
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ABSTRACT
Solute-binding proteins (SBPs) have evolved to balance the demands of ligand affinity, thermostability, and conformational change to accomplish diverse functions in small molecule transport, sensing, and chemotaxis. Although the ligand-induced conformational changes that occur in SBPs make them useful components in biosensors, they are challenging targets for protein engineering and design. Here, we have engineered a d-alanine-specific SBP into a fluorescence biosensor with specificity for the signaling molecule d-serine (D-serFS). This was achieved through binding site and remote mutations that improved affinity (KD = 6.7 ± 0.5 μM), specificity (40-fold increase vs glycine), thermostability (Tm = 79 °C), and dynamic range (∼14%). This sensor allowed measurement of physiologically relevant changes in d-serine concentration using two-photon excitation fluorescence microscopy in rat brain hippocampal slices. This work illustrates the functional trade-offs between protein dynamics, ligand affinity, and thermostability and how these must be balanced to achieve desirable activities in the engineering of complex, dynamic proteins.
Real-Time 3D Framework Tracing of Extracellular Polymeric Substances by an AIE-Active Nanoprobe
- Neng Yan ,
- Yubing Hu ,
- Ben Zhong Tang* , and
- Wen-Xiong Wang*
ACS Sensors 2021 , 6 , 11 , 4206-4216 (Article)
Publication Date (Web) : November 5, 2021
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ABSTRACT
Extracellular polymeric substances (EPS) are produced by many microorganisms and play an essential role in physiological systems such as nutrient storage and stress resistance. Besides, EPS show great potential in biomedical and therapeutic applications due to their biocompatibility and biodegradability. In situ noninvasive monitoring of the EPS produced by microorganisms is thus critical but has not yet been achieved. Herein, we developed a novel aggregation-induced emission (AIE) active nanoprobe enabling in situ visualization of the EPS distribution produced by various microorganisms (cyanobacteria, yeast, freshwater, and marine phytoplankton). The synthesized AIE-active nanoprobe displayed excellent specificity and precision for the staining of EPS, as well as strong photostability, showing great advantage in sensing the EPS in living organisms. With the application of this novel probe, the three-dimensional (3D) framework of EPS distribution was visualized under different environmental conditions (temperature, light intensity, nutrition, and pH). The EPS distribution was found to correlate significantly with the metal tolerance and cyanobacterial photosynthesis capability. Collectively, this study proposed an AIE-active nanoprobe for visualizing the EPS distribution and quantifying the EPS thickness/volume, and has significant implications in understanding the physiological functions of microorganisms.
Advanced Recovery and High-Sensitive Properties of Memristor-Based Gas Sensor Devices Operated at Room Temperature
- Doowon Lee ,
- Min Ju Yun ,
- Kyeong Heon Kim ,
- Sungho kim , and
- Hee-Dong Kim*
ACS Sensors 2021 , 6 , 11 , 4217-4224 (Article)
Publication Date (Web) : November 16, 2021
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ABSTRACT
Fast recovery, high sensitivity, high selectivity, and room temperature (RT) sensing characteristics of NO gas sensors are essential for environmental monitoring, artificial intelligence, and inflammatory diagnosis of asthma patients. However, the conventional semiconductor-type gas sensors have poor sensing characteristics that need to be solved, such as slow recovery speeds (>360 s), low sensitivity (3.8), and high operating temperatures (>300 °C). We propose here a memristor-based NO gas sensor as a gasistor (gas sensor + memory resistor) with SnO2, Ta2O5, and HfO2 films, which successfully demonstrated the feasibility of fast reaction/recovery (<1 s/90 ns) and high sensitivities such as 11.66 and 5.22 in Ta2O5 and HfO2 gasistors for NO gas, at RT. Furthermore, so as to reinforce the selectivity in multigas ambient, we suggest a parallel circuit using three kinds of gasistors having different sensitivities for NO, O2, and C2H6 gases, which results in an improvement of selectivity for the selected gas at RT.
A Dual-Control Strategy by Phosphate Ions and Local Microviscosity for Tracking Adenosine Triphosphate Metabolism in Mitochondria and Cellular Activity Dynamically
- Peng Zhang ,
- Xinjie Guo ,
- Jian Gao ,
- Haihong Liu ,
- Chenyang Wan ,
- Jiajia Li ,
- Qian Zhang* ,
- Yuqing Song , and
- Caifeng Ding*
ACS Sensors 2021 , 6 , 11 , 4225-4233 (Article)
Publication Date (Web) : October 28, 2021
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ABSTRACT
Adenosine triphosphate (ATP) acts as the main energy source for growth and development in organisms, and the disorder reflects the mitochondrial damage to a large extent. Therefore, an efficient tool for the evaluation of the ATP metabolic level is important to track mitochondrial health, providing an additional perspective for an in-depth long-term study on living activities. Herein, a twisted intramolecular charge transfer (TICT) framework is utilized to build up a sensitive receptor, Mito-VP, with a negligible background to target mitochondrial ATP metabolism by monitoring the phosphate ion (Pi) level upon ATP hydrolysis under the overall consideration of the structural and functional features of mitochondria. The responsive fluorescence could be lighted on under the dual control of Pi and local microviscosity, and the two steps of ATP hydrolysis could be captured through fluorescence. In addition to the well-behaved mitochondrial targeting, the energy metabolism at cellular and organism levels has been clarified via mitosis and zebrafish development, respectively.
Three-Dimensional Tracking of Tethered Particles for Probing Nanometer-Scale Single-Molecule Dynamics Using a Plasmonic Microscope
- Guangzhong Ma ,
- Zijian Wan ,
- Yunze Yang ,
- Wenwen Jing , and
- Shaopeng Wang*
ACS Sensors 2021 , 6 , 11 , 4234-4243 (Article)
Publication Date (Web) : November 17, 2021
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Three-dimensional (3D) tracking of surface-tethered single particles reveals the dynamics of the molecular tether. However, most 3D tracking techniques lack precision, especially in the axial direction, for measuring the dynamics of biomolecules with a spatial scale of several nanometers. Here, we present a plasmonic imaging technique that can track the motion of ∼100 tethered particles in 3D simultaneously with sub-nanometer axial precision and single-digit nanometer lateral precision at millisecond time resolution. By tracking the 3D coordinates of a tethered particle with high spatial resolution, we are able to determine the dynamics of single short DNA and study its interaction with enzymes. We further show that the particle motion pattern can be used to identify specific and nonspecific interactions in immunoassays. We anticipate that our 3D tracking technique can contribute to the understanding of molecular dynamics and interactions at the single-molecule level.
Label-Free Imaging of Nanoscale Displacements and Free-Energy Profiles of Focal Adhesions with Plasmonic Scattering Microscopy
- Pengfei Zhang ,
- Xinyu Zhou ,
- Rui Wang ,
- Jiapei Jiang ,
- Zijian Wan , and
- Shaopeng Wang*
ACS Sensors 2021 , 6 , 11 , 4244-4254 (Article)
Publication Date (Web) : October 28, 2021
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ABSTRACT
Cell adhesion plays a critical role in cell communication, cell migration, cell proliferation, and integration of medical implants with tissues. Focal adhesions physically link the cell cytoskeleton to the extracellular matrix, but it remains challenging to image single focal adhesions directly. Here, we show that plasmonic scattering microscopy (PSM) can directly image the single focal adhesions in a label-free, real-time, and non-invasive manner with sub-micrometer spatial resolution. PSM is developed based on surface plasmon resonance (SPR) microscopy, and the evanescent illumination makes it immune to the interference of intracellular structures. Unlike the conventional SPR microscopy, PSM can provide a high signal-to-noise ratio and sub-micrometer spatial resolution for imaging the analytes with size down to a single-molecule level, thus allowing both the super-resolution lateral localization for measuring the nanoscale displacement and precise tracking of vertical distances between the analyte centroid and the sensor surface for analysis of free-energy profiles. PSM imaging of the RBL-2H3 cell with temporal resolution down to microseconds shows that the focal adhesions have random diffusion behaviors in addition to their directional movements during the antibody-mediated activation process. The free-energy mapping also shows a similar movement tendency, indicating that the cell may change its morphology upon varying the binding conditions of adhesive structures. PSM provides insights into the individual focal adhesion activities and can also serve as a promising tool for investigating the cell/surface interactions, such as cell capture and detection and tissue adhesive materials screening.
Bimodal Multiplexed Detection of Tumor Markers in Non-Small Cell Lung Cancer with Polymer Dot-Based Immunoassay
- Yu-Chi Yang ,
- Ming-Ho Liu ,
- Shun-Mao Yang* , and
- Yang-Hsiang Chan*
ACS Sensors 2021 , 6 , 11 , 4255-4264 (Article)
Publication Date (Web) : November 17, 2021
- Abstract
- Full text
ABSTRACT
Semiconducting polymer nanoparticles (Pdots) have been demonstrated to be a promising class of probes for use in fluorometric immunochromatographic test strips (ICTS). The advantages of Pdots in ICTSs include ultrahigh brightness, minimal nonspecific adsorption, and multicolor availability, which together contribute to the high sensitivity, good specificity, and multiplexing ability. These unique properties can therefore circumvent several significant challenges of commercial ICTSs, including insufficient specificity/sensitivity and difficulty in quantitative and multiplexed detection. Here, we developed a colorimetric and fluorescent bimodal readout ICTS based on gold-Pdot nanohybrids for the determination of carcinoembryonic antigen (CEA) and cytokeratin 19 fragment (CYFRA 21-1) expressed abnormally in human blood of non-small-cell lung cancer (NSCLS). The vivid color from Au nanomaterials can be used for rapid qualitative screening (colorimetry) in 15 min, while the bright fluorescence of Pdots is ideal for the advanced quantitative measurements of CEA and CYFRA21-1 concentrations in whole blood samples. This bimodal ICTS platform possesses phenomenal detection sensitivity of 0.07 and 0.12 ng/mL for CYFRA21-1 and CEA, respectively. The accuracy and reliability of this ICTS platform were further evaluated with clinical serum samples from NSCLS patients at different stages, showing good consistency with the results from electrochemiluminescence immunoassay.
Additions & Corrections
Correction to "Devices for Nanoscale Guiding of DNA through a 2D Nanopore"
- David J. Niedzwiecki* ,
- Brian DiPaolo ,
- Chih-Yuan Lin ,
- Alice Castan ,
- Rachael Keneipp ,
- Dimitri Monos , and
- Marija Drndić*
ACS Sensors 2021 , 6 , 11 , 4265 (Addition/Correction)
Publication Date (Web) : October 15, 2021
- Full text
Mastheads
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Source: https://pubs.acs.org/toc/ascefj/6/11
