This thesis work aims to develop electrochemical sensors for sub-ppb level detection of inorganic and organic pollutants in drinking water with environmentally benign materials and processes. While traditional laboratory-based methods such as mass spectroscopy, and chromatography have been used to analyze the concentration of contaminants in drinking water, miniaturized electrochemical sensors offer a compelling alternative to those methods, enabling rapid on-site cost-effective detection of low concentrations of pollutants. In this research, a set of three-electrode sensors was designed and fabricated on a flexible substrate using a screen-printing technique. Additionally, an in-situ electrochlorination process was implemented to create the reference electrode. These sensors were utilized to precisely detect lead ions and perfluorooctane sulfonate (PFOS) in drinking water. The first set of sensors was fabricated to measure the concentration of lead ions, a toxic inorganic pollutant, in potable water. The novelty of the proposed research lies in using non-toxic, biodegradable sodium alginate grafted with 2- acrylamido-2-methyl propane sulfonic acid (AMPS) and conductive fillers for trace-level lead ion detection in water. The principle of square wave anodic square wave stripping voltammetry (SWASV) was used to determine the trace level lead ion concentration. Employing a similar approach with a different material, a PFOS sensor was developed. Utilizing chitosan, one of the sustainable and biodegradable biopolymers found in crustacean shells, rapid parts-per-trillion (ppt) level PFOS detection by electrochemical impedance spectroscopy (EIS) was demonstrated. The proposed sensors made low-cost electrochemical detection of contaminants such as lead ions and PFOS possible with eco-friendly materials and processes.

Lead (Pb) levels in tap water below the established water safety guideline are now considered harmful, thus detecting sub-parts-per-billion level Pb is important. This thesis reports on a miniaturized Copper (Cu)−based electrochemical sensor fabricated from thick film electrodes for their superior sensing performance. These thick film electrodes are based on highly conductive rolled-annealed Cu foil that has a compact bulk structure, but these advantages are often offset by the fact that RA Cu foil is difficult to bond to a substrate due to poor film-adhesion property and lack of mechanical interlocks. For this reason, we develop a direct bonding process for Cu/polymer. An integrated three-electrode planar configuration is then fabricated on the bonded specimen to achieve a fully-functional sensor that can detect 0.2 μg/L (0.2 ppb) Pb2+ ions from a 100 μL sample in only 30 s. This is the most rapid detection of Pb featured to date by an all Cu-based sensor. This thesis first focuses on improving substrate adhesion of RA Cu foil to liquid crystal polymer (LCP). This is achieved by a surface activated bonding process where Cu and LCP surfaces are treated with low-power reactive ion etching oxygen plasma followed by low-pressure contact at 230 °C. This treatment produces hydroxyl (OH−) groups on Cu and LCP surfaces making them highly hydrophilic. When Cu and LCP are contacted and heated, the OH− chains condense by dehydration and form an intermediate oxide layer. This layer mainly develops as Cu2O nanoparticles from the plasma-treated Cu side due to thermal oxidation in air. These nanoparticles diffuse into the polymer substrate when heated under mechanical pressure, resulting in a strongly bonded flexible specimen for the sensor. A simple, inexpensive, and production-friendly fabrication process is then developed for these sensors. Following direct bonding, flexible Cu/LCP is fed into a LaserJet printer for a one-step transfer of polyester resin−based electrode mask on Cu. This is followed by etching, packaging, and a chlorinating process to achieve a fully-functional integrated sensor. The sensing performance of directly bonded Cu/LCP is comparable to that of commercially available Cu/polyimide (PI) laminate. Our approach holds promise towards realizing low-cost integrated water quality monitoring systems. / Thesis / Master of Applied Science (MASc) / Lead contamination in tap water has major health risks for which monitoring of its levels is important. In this thesis, we develop a low-cost copper/polymer-based lead sensor. The sensor is fabricated from high-quality metal foil electrodes that are integrated to a polymer substrate by a direct bonding process. This enables strong adhesion of foil-based electrodes to the substrate that is crucial to the sensor performance and packaging integrity. We investigate the bonding mechanism between copper and polymer to understand the fundamentals of materials integration. These findings will lead to the development of polymer-based sensors and integrated systems. The bonded sensor bases are mechanically flexible, which facilitates a rapid and low-cost fabrication process using a laser printer. The developed sensor has a fast response time (30 s) and can detect very low levels of lead, thus making it suitable for water quality monitoring applications in under-developed and developed countries with legacy water systems that have not been upgraded yet.