skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Automated portable analyzer for lead(II) based on sequential flow injection and nanostructured electrochemical sensors

Abstract

A fully-automated portable analyzer for toxic metal ion detection based on a combination of a nanostructured electrochemical sensor and a sequential flow injection system has been developed in this work. The sensor was fabricated from a carbon paste electrode modified with acetamide phosphonic acid self-assembled monolayer on mesoporous support (Ac-Phos SAMMS) which was embedded in a very small wall-jet (flow-onto) electrochemical cell. The electrode was solid-state and mercury-free. Samples and reagents were injected into the system and flowed through the electrochemical cell by a programmatic sequential flow technique which required minimal volume of samples and reagents and allowed the automation of the analyzer operation. The portable analyzer was evaluated for lead (Pb) detection due to the excellent binding affinity between lead and the functional groups of Ac-Phos SAMMS as well as the great concern for lead toxicity. Linear calibration curve was obtained in a low concentration range (1 to 25 ppb of Pb(II)). The reproducibility was excellent; the percent relative standard deviation was 2.5 for seven consecutive measurements of 10 ppb of Pb(II) solution. Excess concentrations of Ca, Ni, Co, Zn, and Mn ions in the solutions did not interfere with detection of lead, due to the specificity and themore » large number of the functional groups on the electrode surface. The electrode was reliable for at least 90 measurements over 5 days. This work is an important milestone in the development of the next-generation metal ion analyzers that are portable, fully-automated, and remotely-controllable.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
859979
Report Number(s):
PNNL-SA-45434
Journal ID: ISSN 0039-9140; TLNTA2; 11098; 9305; 6899; KP1301020; TRN: US200523%%16
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Talanta; Journal Volume: 68; Journal Issue: 2
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; LEAD; AUTOMATION; ELECTROCHEMICAL CELLS; ELECTRODES; ION DETECTION; PHOSPHONIC ACIDS; SPECIFICITY; ACETAMIDE; PORTABLE EQUIPMENT; MEASURING INSTRUMENTS; environmental molecular sciences laboratory

Citation Formats

Yantasee, Wassana, Timchalk, Chuck, Fryxell, Glen E., Dockendorff, Brian P., and Lin, Yuehe. Automated portable analyzer for lead(II) based on sequential flow injection and nanostructured electrochemical sensors. United States: N. p., 2005. Web. doi:10.1016/j.talanta.2005.07.013.
Yantasee, Wassana, Timchalk, Chuck, Fryxell, Glen E., Dockendorff, Brian P., & Lin, Yuehe. Automated portable analyzer for lead(II) based on sequential flow injection and nanostructured electrochemical sensors. United States. doi:10.1016/j.talanta.2005.07.013.
Yantasee, Wassana, Timchalk, Chuck, Fryxell, Glen E., Dockendorff, Brian P., and Lin, Yuehe. Thu . "Automated portable analyzer for lead(II) based on sequential flow injection and nanostructured electrochemical sensors". United States. doi:10.1016/j.talanta.2005.07.013.
@article{osti_859979,
title = {Automated portable analyzer for lead(II) based on sequential flow injection and nanostructured electrochemical sensors},
author = {Yantasee, Wassana and Timchalk, Chuck and Fryxell, Glen E. and Dockendorff, Brian P. and Lin, Yuehe},
abstractNote = {A fully-automated portable analyzer for toxic metal ion detection based on a combination of a nanostructured electrochemical sensor and a sequential flow injection system has been developed in this work. The sensor was fabricated from a carbon paste electrode modified with acetamide phosphonic acid self-assembled monolayer on mesoporous support (Ac-Phos SAMMS) which was embedded in a very small wall-jet (flow-onto) electrochemical cell. The electrode was solid-state and mercury-free. Samples and reagents were injected into the system and flowed through the electrochemical cell by a programmatic sequential flow technique which required minimal volume of samples and reagents and allowed the automation of the analyzer operation. The portable analyzer was evaluated for lead (Pb) detection due to the excellent binding affinity between lead and the functional groups of Ac-Phos SAMMS as well as the great concern for lead toxicity. Linear calibration curve was obtained in a low concentration range (1 to 25 ppb of Pb(II)). The reproducibility was excellent; the percent relative standard deviation was 2.5 for seven consecutive measurements of 10 ppb of Pb(II) solution. Excess concentrations of Ca, Ni, Co, Zn, and Mn ions in the solutions did not interfere with detection of lead, due to the specificity and the large number of the functional groups on the electrode surface. The electrode was reliable for at least 90 measurements over 5 days. This work is an important milestone in the development of the next-generation metal ion analyzers that are portable, fully-automated, and remotely-controllable.},
doi = {10.1016/j.talanta.2005.07.013},
journal = {Talanta},
number = 2,
volume = 68,
place = {United States},
year = {Thu Dec 15 00:00:00 EST 2005},
month = {Thu Dec 15 00:00:00 EST 2005}
}
  • We have successfully developed electrochemical sensors based on functionalized nanostructured materials for voltammetric analysis of toxic metal ions. Glycinyl-urea self-assembled monolayers on mesoporous silica (Gly-UR SAMMS) was incorporated in carbon paste electrodes for the detection of toxic metal ions such as lead, copper, and mercury based on adsorptive stripping voltammetry (AdSV). The electrochemical sensor yields a linear response at low ppb level of Pb2+ (i.e., 2.5 to 50 ppb) after a 2 minute preconcentration period, with reproducible measurements (%RSD = 3.5, N = 6), and excellent detection limits (at few ppb). By exploiting the interfacial functionality of Gly-UR SAMMS, themore » sensor is selective for the target species, does not require the use of a mercury film, and can be easily regenerated in dilute acid solution. The rigid, open, parallel pore structure, combined with suitable interfacial chemistry of SAMMS, also results in fast analysis times (2-3 minutes). The nanostructured SAMMS materials enable the development of miniature sensing devices that are compact and low-cost, have low-energy-consumption, and are easily integrated into field-deployable units. Keywords: electrochemical sensor, glycinyl-urea, self-assembled monolayer, mesoporous silica, lead, mercury, copper, adsorptive stripping voltammetry.« less
  • Required characterizations of the DOE's transuranic (TRU) and mixed wastes (MW) before disposing and treatment of the wastes are currently costly and have lengthy turnaround. Research toward developing faster and more sensitive characterization and analysis tools to reduce costs and accelerate throughputs is therefore desirable. This project is aimed at the development of electrochemical sensors, specific to toxic transition metals, uranium, and technetium, that can be integrated into the portable sensor systems. This system development will include fabrication and performance evaluation of electrodes as well as understanding of electrochemically active sites on the electrodes specifically designed for toxic metals, uraniummore » and technetium detection. Subsequently, these advanced measurement units will be incorporated into a microfluidic prototype specifically designed and fabricated for field-deployable characterizations of such species. The electrochemical sensors being invest igated are based on a new class of nanoengineered sorbents, Self-Assembled Monolayer on Mesoporous Supports (SAMMS). SAMMS are highly efficient sorbents due to their interfacial chemistry that can be fine-tuned to selectively sequester a specific target species. Adsorptive stripping voltammetry (AdSV) will be performed on two classes of electrodes: the SAMMS modified carbon paste electrodes, and the SAMMS thin film immobilized on microelectrode arrays. Interfacial chemistry and electrochemistry of metal species on the surfaces of SAMMS-based electrodes will be studied. This fundamental knowledge is required for predicting how the sensors will perform in the real wastes which consist of many interferences/ligands and a spectrum of pH levels. The best electrode for each specific waste constituent will be integrated onto the portable microfluidic platform. Efforts will also be focused on testing the portable microfluidics/electrochemical sensor systems with the selected MW and T RU waste samples at the Hanford site. The outcome of this project will lead to the development of a portable analytical system for in-situ characterization of MW and TRU wastes. The technology will greatly reduce costs and accelerate throughputs for characterizations of MW and TRU wastes.« less
  • Required characterizations of the DOE's transuranic (TRU) and mixed wastes (MW) before disposing and treatment of the wastes are currently costly and have lengthy turnaround. Research toward developing faster and more sensitive characterization and analysis tools to reduce costs and accelerate throughputs is therefore desirable. This project is aimed at the development of electrochemical sensors, specific to toxic transition metals, uranium, and technetium, that can be integrated into the portable sensor systems. This system development will include fabrication and performance evaluation of electrodes as well as understanding of electrochemically active sites on the electrodes specifically designed for toxic metals, uraniummore » and technetium detection. Subsequently, these advanced measurement units will be incorporated into a microfluidic prototype specifically designed and fabricated for field-deployable characterizations of such species. The electrochemical sensors being invest igated are based on a new class of nanoengineered sorbents, Self-Assembled Monolayer on Mesoporous Supports (SAMMS). SAMMS are highly efficient sorbents due to their interfacial chemistry that can be fine-tuned to selectively sequester a specific target species. Adsorptive stripping voltammetry (AdSV) will be performed on two classes of electrodes: the SAMMS modified carbon paste electrodes, and the SAMMS thin film immobilized on microelectrode arrays. Interfacial chemistry and electrochemistry of metal species on the surfaces of SAMMS-based electrodes will be studied. This fundamental knowledge is required for predicting how the sensors will perform in the real wastes which consist of many interferences/ligands and a spectrum of pH levels. The best electrode for each specific waste constituent will be integrated onto the portable microfluidic platform. Efforts will also be focused on testing the portable microfluidics/electrochemical sensor systems with the selected MW and T RU waste samples at the Hanford site. The outcome of this project will lead to the development of a portable analytical system for in-situ characterization of MW and TRU wastes. The technology will greatly reduce costs and accelerate throughputs for characterizations of MW and TRU wastes.« less
  • This report summarizes the NMSU activity over the first year of the project (i.e., the 11/03-8/04 period). This research effort aims at developing a portable analytical system for fast, sensitive, and inexpensive, on-site monitoring of toxic transition metals and radionuclides in contaminated DOE Sites. In accordance to our original objectives our studies have focused on various fundamental and practical aspects of microchip devices for monitoring metal contaminants. As described in this section, we have made a substantial progress, and introduced effective routes for improving the reliability of devices for field screening of toxic metals. This 11-mos activity has already resultedmore » in 2 research papers (published or in press in major journals), and several invited presentations in major meetings. (Several more publications are expected in the late part of 2004.) The electrochemical sensors being investigated rely on the highly sensitive adsorptive stripping voltammetry (AdSV) technique to detect metal ions of interest to the DOE, particularly uranium and chromium.« less
  • This research effort aims at developing a portable analytical system for fast, sensitive, and inexpensive, on-site monitoring of toxic transition metals and radionuclides in contaminated DOE Sites. The portable devices will be based on Microscale Total Analytical systems ( -TAS) or ''Lab-on-a-chip'' in combination with electrochemical (stripping-voltammetric) sensors. The resulting microfluidics/electrochemical sensor system would allow testing for toxic metals to be performed more rapidly, inexpensively, and reliably in a field setting. Progress Summary/Accomplishments: This report summarizes the ASU activity over the second year of the project. In accordance to our original objectives our studies have focused on various fundamental andmore » practical aspects of sensing and microchip devices for monitoring metal contaminants. As described in this section, we have made a substantial progress, and introduced effective routes for improving the on-site detection of toxic metals and for interfacing microchips with the real world.« less