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A detailed EIS study of boron doped diamond electrodes decorated with gold nanoparticles for high sensitivity mercury detection.

ABSTRACT: This work compares the electrochemical impedance response of polished and unpolished boron doped diamond (BDD) electrodes, during mercury detection measurements. For each substrate type both bare electrodes and electrodes decorated with average diameter 30 nm AuNPs were used, to investigate the role of AuNPs during mercury sensing with diamond electrodes. In square wave anodic stripping voltammetry (SWASV) measurements for mercury detection, the mercury ions in the electrolyte are deposited onto, then stripped from the diamond electrode surface. To investigate the different electrode performances during these steps, the EIS measurements were made at the deposition and stripping potentials, alongside scans at open circuit potential for comparison. The performance of the electrodes is assessed in terms of their electron transfer rate (k₀). The electrodes decorated with AuNPs are shown to have lower capacitance and higher reactivity than the bare pBDD and BDD electrodes, until the mercury concentration in the electrolyte is < 500 µM, when the sp²/sp³ carbon ratio at the surface of the electrodes has a greater influence on the sensitivity for mercury detection than the presence of AuNPs.

SUBMITTER: McLaughlin MHS

PROVIDER: S-EPMC8096807 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Fabrication of patterned boron-doped diamond (BDD) in an inexpensive and straightforward way is required for a variety of practical applications, including the development of BDD-based electrochemical sensors. This work describes a simplified and novel bottom-up fabrication approach for BDD-based three-electrode sensor chips utilizing direct inkjet printing of diamond nanoparticles on silicon-based substrates. The whole seeding process, accomplished by a commercial research inkjet printer with piezo-driven drop-on-demand printheads, was systematically examined. Optimized and continuous inkjet-printed features were obtained with glycerol-based diamond ink (0.4% vol/wt), silicon substrates pretreated by exposure to oxygen plasma and subsequently to air, and applying a dot density of 750 drops (volume 9 pL) per inch. Next, the dried micropatterned substrate was subjected to a chemical vapor deposition step to grow uniform thin-film BDD, which satisfied the function of both working and counter electrodes. Silver was inkjet-printed to complete the sensor chip with a reference electrode. Scanning electron micrographs showed a closed BDD layer with a typical polycrystalline structure and sharp and well-defined edges. Very good homogeneity in diamond layer composition and a high boron content (∼2 × 1021 atoms cm-3) was confirmed by Raman spectroscopy. Important electrochemical characteristics, including the width of the potential window (2.5 V) and double-layer capacitance (27 μF cm-2), were evaluated by cyclic voltammetry. Fast electron transfer kinetics was recognized for the [Ru(NH3)6]3+/2+ redox marker due to the high doping level, while somewhat hindered kinetics was observed for the surface-sensitive [Fe(CN)6]3-/4- probe. Furthermore, the ability to electrochemically detect organic compounds of different structural motifs, such as glucose, ascorbic acid, uric acid, tyrosine, and dopamine, was successfully verified and compared with commercially available screen-printed BDD electrodes. The newly developed chip-based manufacture method enables the rapid prototyping of different small-scale electrode designs and BDD microstructures, which can lead to enhanced sensor performance with capability of repeated use.

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A detailed EIS study of boron doped diamond electrodes decorated with gold nanoparticles for high sensitivity mercury detection.

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