Tuning Selectivity of Fluorescent Carbon Nanotube-Based Neurotransmitter Sensors.
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ABSTRACT: Detection of neurotransmitters is an analytical challenge and essential to understand neuronal networks in the brain and associated diseases. However, most methods do not provide sufficient spatial, temporal, or chemical resolution. Near-infrared (NIR) fluorescent single-walled carbon nanotubes (SWCNTs) have been used as building blocks for sensors/probes that detect catecholamine neurotransmitters, including dopamine. This approach provides a high spatial and temporal resolution, but it is not understood if these sensors are able to distinguish dopamine from similar catecholamine neurotransmitters, such as epinephrine or norepinephrine. In this work, the organic phase (DNA sequence) around SWCNTs was varied to create sensors with different selectivity and sensitivity for catecholamine neurotransmitters. Most DNA-functionalized SWCNTs responded to catecholamine neurotransmitters, but both dissociation constants (Kd) and limits of detection were highly dependent on functionalization (sequence). Kd values span a range of 2.3 nM (SWCNT-(GC)15 + norepinephrine) to 9.4 μM (SWCNT-(AT)15 + dopamine) and limits of detection are mostly in the single-digit nM regime. Additionally, sensors of different SWCNT chirality show different fluorescence increases. Moreover, certain sensors (e.g., SWCNT-(GT)10) distinguish between different catecholamines, such as dopamine and norepinephrine at low concentrations (50 nM). These results show that SWCNTs functionalized with certain DNA sequences are able to discriminate between catecholamine neurotransmitters or to detect them in the presence of interfering substances of similar structure. Such sensors will be useful to measure and study neurotransmitter signaling in complex biological settings.
Project description:A scalable electrophoretic deposition (EPD) approach is used to create novel thin, flexible, and lightweight carbon nanotube-based textile pressure sensors. The pressure sensors can be produced using an extensive variety of natural and synthetic fibers. These piezoresistive sensors are sensitive to pressures ranging from the tactile range (<10 kPa), the body weight range (?500 kPa), and very high pressures (?40 MPa). The EPD technique enables the creation of a uniform carbon nanotube-based nanocomposite coating, in the range of 250-750 nm thick, of polyethyleneimine (PEI) functionalized carbon nanotubes on nonconductive fibers. In this work, nonwoven aramid fibers are coated by EPD onto a backing electrode followed by film formation onto the fibers creating a conductive network. The electrically conductive nanocomposite coating is firmly bonded to the fiber surface and shows piezoresistive electrical/mechanical coupling. The pressure sensor displays a large in-plane change in electrical conductivity with applied out-of-plane pressure. In-plane conductivity change results from fiber/fiber contact as well as the formation of a sponge-like piezoresistive nanocomposite "interphase" between the fibers. The resilience of the nanocomposite interphase enables sensing of high pressures without permanent changes to the sensor response, showing high repeatability.
Project description:A carbon nanotube (CNT) can be toxic to a living cell by binding to proteins and then impairing their functionalities; however, an efficient screening method that examines binding capability of a CNT to protein molecules in vitro is still unavailable. Here, we show that a nanopore-based sensor can be used to investigate CNT-protein interactions. With proof-of-principle molecular dynamics simulations, we have measured ionic currents in a nanopore when threading a CNT-protein complex through the pore, and demonstrated that CNT's binding capability, and thus potential nanotoxicity, can be inferred from current signals. We have then further investigated mechanics and energetics of CNT-protein interactions with the nanopore sensor. These findings indicate that solid-state nanopores have the potential to be ultra-sensitive and high-throughput sensors for nanotoxicity.
Project description:Realization of advanced bio-interactive electronic devices requires mechanically compliant sensors with the ability to detect extremely large strain. Here, we design a new multifunctional carbon nanotube (CNT) based capacitive strain sensors which can detect strains up to 300% with excellent durability even after thousands of cycles. The CNT-based strain gauge devices exhibit deterministic and linear capacitive response throughout the whole strain range with a gauge factor very close to the predicted value (strictly 1), representing the highest sensitivity value. The strain tests reveal the presented strain gauge with excellent dynamic sensing ability without overshoot or relaxation, and ultrafast response at sub-second scale. Coupling these superior sensing capabilities to the high transparency, physical robustness and flexibility, we believe the designed stretchable multifunctional CNT-based strain gauge may have various potential applications in human friendly and wearable smart electronics, subsequently demonstrated by our prototypical data glove and respiration monitor.
Project description:In vitro simulators of the human gastrointestinal (GI) tract are remarkable technological platforms for studying the impact of food on the gut microbiota, enabling continuous and real-time monitoring of key biomarkers. However, comprehensive real-time monitoring of gaseous biomarkers in these systems is required with a cost-effective approach, which has been challenging to perform experimentally to date. In this work, we demonstrate the integration and in-line use of carbon nanotube (CNT)-based chemiresitive gas sensors coated with a thin polydimethylsiloxane (PDMS) membrane for the continuous monitoring of gases within the Simulator of the Human Microbial Ecosystem (SHIME). The findings demonstrate the ability of the gas sensor to continuously monitor the different phases of gas production in this harsh, anaerobic, highly humid, and acidic environment for a long exposure time (16 h) without saturation. This establishes our sensor platform as an effective tool for real-time monitoring of gaseous biomarkers in in vitro systems like SHIME.
Project description:The induction of autophagy by nanoparticles causes nanotoxicity, but appropriate modulation of autophagy by nanoparticles may have therapeutic potential. Multiwalled carbon nanotubes (MWCNTs) interact with cell membranes and membrane-associated molecules before and after internalization. These interactions alter cellular signaling and impact major cell functions such as cell cycle, apoptosis, and autophagy. In this work, we demonstrated that MWCNT-cell interactions can be modulated by varying densely distributed surface ligands on MWCNTs. Using a fluorescent autophagy-reporting cell line, we evaluated the autophagy induction capability of 81 surface-modified MWCNTs. We identified strong and moderate autophagy-inducing MWCNTs as well as those that did not induce autophagy. Variation of the surface ligand structure of strong autophagy nanoinducers led to the induction of different autophagy-activating signaling pathways, presumably through their different interactions with cell surface receptors.
Project description:This work describes the design and fabrication of free-standing carbon nanotube-palladium (CNT-Pd) composite sheets for hydrogen gas sensing. The CNT-Pd composites were made by electroplating palladium onto a solvent-densified and oxygen plasma-treated CNT sheet. The latter was prepared using high purity CNTs drawn from a dense, vertically aligned array grown by chemical vapor deposition on silicon substrates. The CNT-Pd sheets were characterized by energy-dispersive spectroscopy, scanning electron microscopy, and X-ray diffraction. The amount of palladium in the composite was 16.5 wt % as measured via thermogravimetric analysis. Thin strips of the CNT-Pd sheets were assembled as chemiresistor sensors and tested for hydrogen gas detection. The sensors demonstrated a limit of detection of 0.1 mol % and displayed signal reversibility without the need for oxygen removal or heat treatment. A decrease in signal reversibility was observed after multiple exposure cycles; however, redensification with ethanol significantly restored the original reversibility. The sensor showed the Freundlich adsorption isotherm behavior when exposed to hydrogen. The material's potential application toward a wearable, flexible sensor was demonstrated by integrating the chemiresistor onto a fabric material using hot-press processing and testing the composite for hydrogen sensitivity.
Project description:Four-dimensional (4D) printing has attracted significant attention, because it enables structures to be reconfigured based on an external stimulus, realizing complex architectures that are useful for different applications. Nevertheless, most previously reported 4D-printed components have focused on actuators, which are just one part of a full soft robotic system. In this study, toward achieving fully 4D-printed systems, the design and direct ink writing of sensors with a straining mechanism that mimics the 4D effect are explored. Solution-processable carbon nanotubes (CNTs) were used as the sensing medium, and the effect of a heat-shrinkable shape-memory polymer-based substrate (i.e., potential 4D effect) on the electronic and structural properties of CNTs was assessed, followed by their application in various sensing devices. Herein, we reveal that substrate shrinking affords a more porous yet more conductive film owing to the compressive strain experienced by CNTs, leading to an increase in the carrier concentration. Furthermore, it improves the sensitivity of the devices without the need for chemical functionalization. Interestingly, the results show that, by engineering the potential 4D effect, the selectivity of the sensor can be tuned. Finally, the sensors were integrated into a fully 4D-printed flower structure, exhibiting their potential for different soft robotic applications.
Project description:The dielectrophoresis (DEP) method is used to fabricate sensor devices by assembling and aligning carbon nanotubes (CNTs) across electrode structures. The challenges of the method increase as the gap width between the electrodes increases. In this work, a novel DEP setup is proposed to reduce the resistance mismatch in manufacturing carbon nanotube-based sensors. The proposed setup utilizes hot airflow and thermal annealing to fabricate long-aligned multi-walled carbon nanotube (MWCNT) bridges across transparent electrodes with a gap width up to 75 μm. The best alignment results were obtained at airflow velocities between 1.5 m s-1 and 2.5 m s-1. The minimum variation in the resistance of the aligned bridges was 1.81% observed at a MWCNT concentration of 0.005 wt% and deposition time of 10 min. Long MWCNT bridges have many contact points that link MWCNTs to each other, making the contact resistance a robust indicator of the variation in the ambient temperature. The characteristics of the MWCNT bridges as a temperature sensor, including the response, sensitivity, and recovery, were investigated.
Project description:A novel strategy to fabricate a hydrogen peroxide (H₂O₂) sensor was developed by using platinum (Pt) electrodes modified with multi-wall carbon nanotube-platinum nanoparticle nanohybrids (MWCNTs/Pt nanohybrids). The process to synthesize MWCNTs/Pt nanohybrids was simple and effective. Pt nanoparticles (Pt NPs) were generated in situ in a potassium chloroplatinate aqueous solution in the presence of multi-wall carbon nanotubes (MWCNTs), and readily attached to the MWCNTs convex surfaces without any additional reducing reagents or irradiation treatment. The MWCNT/Pt nanohybrids were characterized by transmission electron microscope (TEM), and the redox properties of MWCNTs/Pt nanohybrids-modified Pt electrode were studied by electrochemical measurements. The MWCNTs/Pt-modified electrodes exhibited a favorable catalytic ability in the reduction of H₂O₂. The modified electrodes can be used to detect H₂O₂ in the range of 0.01-2 mM with a lower detection limit of 0.3 μM at a signal-to-noise ratio of 3. The sensitivity of the electrode to H₂O₂ was calculated to be 205.80 μA mM-1 cm-2 at working potential of 0 mV. In addition, the electrodes exhibited an excellent reusability and long-term stability as well as negligible interference from ascorbic acid, uric acid, and acetaminophen.
Project description:Point-functionalized carbon nanotube field-effect transistors can serve as highly sensitive detectors for biomolecules. With a probe molecule covalently bound to a defect in the nanotube sidewall, two-level random telegraph noise (RTN) in the conductance of the device is observed as a result of a charged target biomolecule binding and unbinding at the defect site. Charge in proximity to the defect modulates the potential (and transmission) of the conductance-limiting barrier created by the defect. In this Letter, we study how these single-molecule electronic sensors are affected by ionic screening. Both charge in proximity to the defect site and buffer concentration are found to affect RTN amplitude in a manner that follows from simple Debye length considerations. RTN amplitude is also dependent on the potential of the electrolyte gate as applied to the reference electrode; at high enough gate potentials, the target DNA is completely repelled and RTN is suppressed.