Dataset Information

Carbon-Based Solid-State Calcium Ion-Selective Microelectrode and Scanning Electrochemical Microscopy: A Quantitative Study of pH-Dependent Release of Calcium Ions from Bioactive Glass.

ABSTRACT: Solid-state ion-selective electrodes are used as scanning electrochemical microscope (SECM) probes because of their inherent fast response time and ease of miniaturization. In this study, we report the development of a solid-state, low-poly(vinyl chloride), carbon-based calcium ion-selective microelectrode (Ca(2+)-ISME), 25 ?m in diameter, capable of performing an amperometric approach curve and serving as a potentiometric sensor. The Ca(2+)-ISME has a broad linear response range of 5 ?M to 200 mM with a near Nernstian slope of 28 mV/log[a(Ca(2+))]. The calculated detection limit for Ca(2+)-ISME is 1 ?M. The selectivity coefficients of this Ca(2+)-ISME are log K(Ca(2+),A) = -5.88, -5.54, and -6.31 for Mg(2+), Na(+), and K(+), respectively. We used this new type of Ca(2+)-ISME as an SECM probe to quantitatively map the chemical microenvironment produced by a model substrate, bioactive glass (BAG). In acidic conditions (pH 4.5), BAG was found to increase the calcium ion concentration from 0.7 mM ([Ca(2+)] in artificial saliva) to 1.4 mM at 20 ?m above the surface. In addition, a solid-state dual SECM pH probe was used to correlate the release of calcium ions with the change in local pH. Three-dimensional pH and calcium ion distribution mapping were also obtained by using these solid-state probes. The quantitative mapping of pH and Ca(2+) above the BAG elucidates the effectiveness of BAG in neutralizing and releasing calcium ions in acidic conditions.

SUBMITTER: Ummadi JG

PROVIDER: S-EPMC4873256 | biostudies-literature | 2016 Mar

REPOSITORIES: biostudies-literature

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Publications

Carbon-Based Solid-State Calcium Ion-Selective Microelectrode and Scanning Electrochemical Microscopy: A Quantitative Study of pH-Dependent Release of Calcium Ions from Bioactive Glass.

Ummadi Jyothir Ganesh JG Downs Corey J CJ Joshi Vrushali S VS Ferracane Jack L JL Koley Dipankar D

Analytical chemistry 20160223 6

Solid-state ion-selective electrodes are used as scanning electrochemical microscope (SECM) probes because of their inherent fast response time and ease of miniaturization. In this study, we report the development of a solid-state, low-poly(vinyl chloride), carbon-based calcium ion-selective microelectrode (Ca(2+)-ISME), 25 μm in diameter, capable of performing an amperometric approach curve and serving as a potentiometric sensor. The Ca(2+)-ISME has a broad linear response range of 5 μM to 200 ...[more]

PMID: 26861499

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Project description:The electrochemical reduction of CO2 is widely studied as a sustainable alternative for the production of fuels and chemicals. The electrolyte's bulk pH and composition play an important role in the reaction activity and selectivity and can affect the extent of the buildup of pH gradients between the electrode surface and the bulk of the electrolyte. Quantifying the local pH and how it is affected by the solution species is desirable to gain a better understanding of the CO2 reduction reaction. Local pH measurements can be realized using Scanning Electrochemical Microscopy (SECM); however, finding a pH probe that is stable and selective under CO2 reduction reaction conditions is challenging. Here, we have used our recently developed voltammetric pH sensor to perform pH measurements in the diffusion layer during CO2 reduction using SECM, with high time resolution. Using a 4-hydroxylaminothiophenol (4-HATP)/4-nitrosothiophenol (4-NSTP) functionalized gold ultramicroelectrode, we compare the local pH developed above a gold substrate in an argon atmosphere, when only hydrogen evolution is taking place, to the pH developed in a CO2 atmosphere. The pH is monitored at a fixed distance from the surface, and the sample potential is varied in time. In argon, we observe a gradual increase of pH, while a plateau region is present in CO2 atmosphere due to the formation of HCO3 - buffering the reaction interface. By analyzing the diffusion layer dynamics once the sample reaction is turned "off", we gain insightful information on the time scale of the homogeneous reactions happening in solution and on the time required for the diffusion layer to fully recover to the initial bulk concentration of species. In order to account for the effect of the presence of the SECM tip on the measured pH, we performed finite element method simulations of the fluid and reaction dynamics. The results show the significant localized diffusion hindrance caused by the tip, so that in its absence, the pH values are more acidic than when the tip is present. Nonetheless, through the simulation, we can account for this effect and estimate the real local pH values across the diffusion layer.

Dataset Information

Carbon-Based Solid-State Calcium Ion-Selective Microelectrode and Scanning Electrochemical Microscopy: A Quantitative Study of pH-Dependent Release of Calcium Ions from Bioactive Glass.

Publications

Carbon-Based Solid-State Calcium Ion-Selective Microelectrode and Scanning Electrochemical Microscopy: A Quantitative Study of pH-Dependent Release of Calcium Ions from Bioactive Glass.

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