Sanjeev Billa

Our research addresses the pressing need for environmental sensors capable of large-scale, on-site detection of a wide array of heavy metals with highly accurate sensor metrics. We present a novel approach using electrochemically polished (ECP) carbon screen-printed electrodes (cSPEs) for high-sensitivity detection of cadmium and lead. By applying a range of techniques, including scanning electron microscopy, energy-dispersive spectroscopy, Raman spectroscopy, electrochemical impedance spectroscopy, and cyclic voltammetry, we investigated the impact of the electrochemical potential scan range, scan rate, and the number of cycles on electrode response and its ability to detect cadmium and lead. Our findings reveal a 41 ± 1.2% increase in voltammogram currents and a 51 ± 1.6% decrease in potential separations (n = 3), indicating a significantly improved active electrode area and kinetics. The impedance model elucidates the microstructural and electrochemical property changes in the ECP-treated electrodes, showing an 88 ± 2% (n = 3) decrease in the charge transfer resistance, leading to enhanced electrode electrical conductivity. A bismuth-reduced graphene oxide nanocomposite-modified, ECP-treated electrode demonstrated a higher cadmium and lead sensitivity of up to 5 ± 0.1 μAppb⁻¹cm⁻² and 2.7 ± 0.1 μAppb⁻¹cm⁻² (n = 3), respectively, resulting in sub-ppb limits of detection in spiked deionized water samples. Our study underscores the potential of optimally ECP-activated electrodes as a foundation for designing ultrasensitive heavy metal sensors for a wide range of real-world heavy metal-contaminated waters.

Imbalances in levels of glutamate (GLU) and gamma-aminobutyric acid (GABA) and their sub-second signaling dynamics occur in several brain disorders including traumatic brain injury, epilepsy, and Alzheimer’s disease. The present work reports on the optimization and in vivo testing of a silicon (Si) multifunctional biosensor probe for sub-second simultaneous real-time detection of GLU and GABA. The Si probe features four surface-functionalized platinum ultramicroelectrodes (UMEs) for detection of GLU and GABA, a sentinel site, and integrated microfluidics for in-situ calibration. Optimal enzyme concentrations, size-exclusion phenylenediamine layer and micro spotting conditions were systematically investigated. The measured GLU sensitivity for the GLU and GABA sites were as high as 219 ± 8 nA μM⁻¹ cm⁻² (n = 3). The measured GABA sensitivity was as high as 10 ± 1 nA μM⁻¹ cm⁻² (n = 3). Baseline recordings (n = 18) in live rats demonstrated a useful probe life of at least 11 days with GLU and GABA concentrations changing at the levels of 100′s and 1000′s of μM and with expected periodic bursts or fluctuations during walking, teeth grinding and other activities and with a clear difference in the peak amplitude of the sensor fluctuations between rest (low) and activity (higher), or when the rat was surprised (a reaction with no movement). Importantly, the probe could improve methods for large-scale monitoring of neurochemical activity and network function in disease and injury, in live rodent brain.