This study quantitatively elucidates the role of metal clusters in the electrochemical activation of metal-oxide nanostructured electrodes. Through the deposition of nearly monodisperse Au x Pt1–x (x = 0, 0.5, 1) clusters, smaller than 3 nm, on the ZnO nanorod (NR) electrode surface, a controlled enhancement of charge transfer and activation of electrocatalytic processes was achieved. The interfacial electrical states of the hybrid electrodes were probed by electrochemical impedance spectroscopy (EIS). Analysis of the charge-transfer resistance and interface capacitance, estimated by modeling EIS curves in different bias regimes, indicated the presence of a large amount of active donor states (∼1020 cm–3) at the surface of the ZnO NRs. Decoration of the ZnO NRs with Au x Pt1–x clusters strongly increased the charge-transfer process at the cluster–ZnO/electrolyte interface. This induced a more effective depletion of the electron charge available in the donor states of the ZnO NRs, leading to the formation of a positively charged layer at the interface between ZnO and the clusters. These two effects, intrinsically linked with the alignment between the electronic states of the Au x Pt1–x clusters and ZnO, strongly enhance the interface reactivity of the ZnO NR electrodes toward the redox reaction of potassium ferricyanide. This is particularly relevant for understanding and improving the performance of electrochemical biosensors.
Perception, thoughts, and actions are encoded by the coordinated activity of large neuronal populations spread over large areas. Using thin film electrocorticography (ECoG) arrays, this cortical activity has been used to decode speech and individual finger movements, enabling neuroprosthetics, and to localize epileptic foci. However, the connectorization of these multi-thousand channel thin-film arrays to external circuitry is challenging; current state-of-the-art methods are complex, bulky, and unscalable. We address this shortcoming by developing an electrode connector based on an ultra-conformable thin film electrode array that self-assembles onto hard silicon chip sensors, such as microelectrode arrays (MEAs) or camera sensors enabling large channel counts at high density. The interconnects are formed using microfabricated electrode pads suspended by thin support arms, termed flex2chip. Capillary-assisted assembly drives the pads to deform towards the chip surface, and van der Waals forces maintain this deformation, establishing mechanical and Ohmic contact onto individual pixels. We demonstrate a 2200-channel array with a channel density of 272 channels / mm2 connected to the MEA through the flex2chip interconnection method. Thin film electrode arrays connected through the flex2chip successfully measured extracellular action potentials ex vivo. Furthermore, in a transgenic mouse model for absence epilepsy, Scn8a+/-, we observed highly variable propagation trajectories at micrometer scales, even across the duration of a single spike-and-wave discharge (SWD).
The development of in vivo, longitudinal, realtime monitoring devices is an essential step toward continuous, precision health monitoring. Molecularly imprinted polymers (MIPs) are popular sensor capture agents that are more robust than antibodies and have been used for sensors, drug delivery, affinity separations, assays, and solid-phase extraction. However, MIP sensors are typically limited to one-time use due to their high binding affinity (>10 7 M −1 ) and slow-release kinetics (<10 −4 μM/sec). To overcome this challenge, current research has focused on stimuli-responsive MIPs (SR-MIPs), which undergo a conformational change induced by external stimuli to reverse molecular binding, requiring additional chemicals or outside stimuli. Here, we demonstrate fully reversible MIP sensors based on electrostatic repulsion. Once the target analyte is bound within a thin film MIP on an electrode, a small electrical potential successfully releases the bound molecules, enabling repeated, accurate measurements. We demonstrate an electrostatically refreshed dopamine sensor with a 760 pM limit of detection, linear response profile, and accuracy even after 30 sensing−release cycles. These sensors could repeatedly detect <1 nM dopamine released from PC-12 cells in vitro, demonstrating they can longitudinally measure low concentrations in complex biological environments without clogging. Our work provides a simple and effective strategy for enhancing the use of MIPs-based biosensors for all charged molecules in continuous, real-time health monitoring and other sensing applications.
Due to the complexity of a chemo-electro-mechanical system and the need for a wet environment, to date, few devices fully integrate hydrogels with microelectromechanical systems. In this paper, we demonstrate the use of inkjet-printed gold electrodes integrated in microfluidic channels to alter the morphology of electroactive polymer hydrogels, cross-linked in situ. Microfluidics is a convenient platform for integrating hydrogels with microsystems as it provides a means for encapsulating electrolytic environments, while maintaining UV transparency. Printed electronics provide a new method for rapid prototyping of electrodes on flexible substrates for electrical control of electroactive polymer microsystems. We attribute the observed actuation to electrochemically-induced pH variations in the vicinity of the printed anode and cathode which diffuse into the hydrogel. Response to pH was verified by exposing the hydrogel to various pH conditions in control experiments without applied electrical bias. This work demonstrates a new, integrated, polymer-based, rapid prototyping approach to building flexible electroactive hydrogel systems which can benefit microfluidic valves, biomimetics, electrochemical sensors and artificial muscles.
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