Thermoplastics have become attractive alternatives to glass/quartz for microfluidics, but the realization of thermoplastic nanofluidic devices has been slow in spite of the rather simple fabrication techniques that can be used to produce these devices. This slow transition has in part been attributed to insufficient understanding of surface charge effects on the transport properties of single molecules through thermoplastic nanochannels. We report the surface modification of thermoplastic nanochannels and an assessment of the associated surface charge density, zeta potential and electroosmotic flow (EOF). Mixed-scale fluidic networks were fabricated in poly(methylmethacrylate), PMMA. Oxygen plasma was used to generate surface-confined carboxylic acids with devices assembled using low temperature fusion bonding. Amination of the carboxylated surfaces using ethylenediamine (EDA) was accomplished via EDC coupling. XPS and ATR-FTIR revealed the presence of carboxyl and amine groups on the appropriately prepared surfaces. A modified conductance equation for nanochannels was developed to determine their surface conductance and was found to be in good agreement with our experimental results. The measured surface charge density and zeta potential of these devices were lower than glass nanofluidic devices and dependent on the surface modification adopted, as well as the size of the channel. This property, coupled to an apparent increase in fluid viscosity due to nanoconfinement, contributed to the suppression of the EOF in PMMA nanofluidic devices by an order of magnitude compared to the micro-scale devices. Carboxylated PMMA nanochannels were efficient for the transport and elongation of λ-DNA while these same DNA molecules were unable to translocate through aminated nanochannels.
Redox current amplification has been demonstrated using carbon interdigitated array ͑IDA͒ nanoelectrodes derived from precursor polymer microstructures through conventional photolithography and pyrolysis. This simple conversion process, also known as carbon-microelectromechanical systems, enables nanometer-level fabrication of carbon materials in a reproducible and an economic manner. We demonstrated that with carbon IDA nanoelectrodes fabricated in two mask processes a current amplification factor of 25 can be obtained. This high amplification factor is a result of the efficient recycling of redox species between the 1:1 aspect ratio carbon nanoelectrodes. This type of a current amplification value is hard to obtain when using more traditional flat nanometer level spaced noble metal IDA electrodes fabricated with more expensive nanopatterning processes such as E-beam lithography.
A batch fabrication process at the wafer-level integrating ring microelectrodes into atomic force microscopy (AFM) tips is presented. The fabrication process results in bifunctional scanning probes combining atomic force microscopy with scanning electrochemical microscopy (AFM-SECM) with a ring microelectrode integrated at a defined distance above the apex of the AFM tip. Silicon carbide is used as AFM tip material, resulting in reduced mechanical tip wear for extended usage. The presented approach for the probe fabrication is based on batch processing using standard microfabrication techniques, which provides bifunctional scanning probes at a wafer scale and at low cost. Additional benefits of batch fabrication include the high processing reproducibility, uniformity, and tuning of the physical properties of the cantilever for optimized AFM dynamic mode operation. The performance of batch-fabricated bifunctional probes was demonstrated by simultaneous imaging micropatterned platinum structures at a silicon dioxide substrate in intermittent (dynamic) and contact mode, respectively, and feedback mode SECM. In both, intermittent and contact mode, the bifunctional probes provided reliable correlated electrochemical and topographical data. In addition, simulations of the diffusion-limited steady-state currents at the integrated electrode using finite element methods were performed for characterizing the developed probes.
With the development of nanomaterial-based nanodevices, it became inevitable to develop cost-effective and simple nanofabrication technologies enabling the formation of nanomaterial assembly in a controllable manner. Herein, we present suspended monolithic carbon single nanowires and nanomeshes bridging two bulk carbon posts, fabricated in a designed manner using two successive UV exposure steps and a single pyrolysis step. The pyrolysis step is accompanied with a significant volume reduction, resulting in the shrinkage of micro-sized photoresist structures into nanoscale carbon structures. Even with the significant elongation of the suspended carbon nanowire induced by the volume reduction of the bulk carbon posts, the resultant tensional stress along the nanowire is not significant but grows along the wire thickness; this tensional stress gradient and the bent supports of the bridge-like carbon nanowire enhance structural robustness and alleviate the stiction problem that suspended nanostructures frequently experience. The feasibility of the suspended carbon nanostructures as a sensor platform was demonstrated by testing its electrochemical behavior, conductivity-temperature relationship, and hydrogen gas sensing capability.
We developed a versatile and highly sensitive biosensor platform. The platform is based on electrochemical-enzymatic redox cycling induced by selective enzyme immobilization on nano-sized carbon interdigitated electrodes (IDEs) decorated with gold nanoparticles (AuNPs). Without resorting to sophisticated nanofabrication technologies, we used batch wafer-level carbon microelectromechanical systems (C-MEMS) processes to fabricate 3D carbon IDEs reproducibly, simply, and cost effectively. In addition, AuNPs were selectively electrodeposited on specific carbon nanoelectrodes; the high surface-to-volume ratio and fast electron transfer ability of AuNPs enhanced the electrochemical signal across these carbon IDEs. Gold nanoparticle characteristics such as size and morphology were reproducibly controlled by modulating the step-potential and time period in the electrodeposition processes. To detect cholesterol selectively using AuNP/carbon IDEs, cholesterol oxidase (ChOx) was selectively immobilized via the electrochemical reduction of the diazonium cation. The sensitivity of the AuNP/carbon IDE-based biosensor was ensured by efficient amplification of the redox mediators, ferricyanide and ferrocyanide, between selectively immobilized enzyme sites and both of the combs of AuNP/carbon IDEs. The presented AuNP/carbon IDE-based cholesterol biosensor exhibited a wide sensing range (0.005–10 mM) and high sensitivity (~993.91 µA mM−1 cm−2; limit of detection (LOD) ~1.28 µM). In addition, the proposed cholesterol biosensor was found to be highly selective for the cholesterol detection.
Redox cycling is a commonly used electrochemical sensing scheme for enhancing faradaic current signals. This effect can be improved by either optimizing electrode geometries or restricting electrochemical reactions within a limited volume. Here, we demonstrate a simple batch fabrication of 1 : 1 aspect ratio carbon interdigitated array nanoelectrodes integrated in a polydimethylsiloxane microchannel that enables current amplification by up to 1116 times. We also examine the factors that influence the effect of redox cycling, including the electrode aspect ratio and channel height, by using experiments and simulations.
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