Highly efficient preconcentration using anodically generated shrinking gas bubbles for per- and polyfluoroalkyl substances (PFAS) detection
Authors:
- 21 June 2022
- journal article
- research article
- Published by Springer Nature in Analytical and Bioanalytical Chemistry
- Vol. 415 (18) , 4153-4162
Abstract
Here we report a highly efficient PFAS preconcentration method that uses anodically generated shrinking gas bubbles to preconcentrate PFAS via aerosol formation, achieving ~ 1400-fold enrichment of PFOS and PFOA—the two most common PFAS—in 20 min. This new method improves the enrichment factor by 15 to 105% relative to the previous method that uses cathodically generated H2 bubbles. The shrinking gas bubbles are in situ electrogenerated by oxidizing water in an NH4HCO3 solution. H+ produced by water oxidation reacts with HCO3− to generate CO2 gas, forming gas bubbles containing a mixture of O2 and CO2. Due to the high solubility of CO2 in aqueous solutions, the CO2/O2 bubbles start shrinking when they leave the electrode surface region. A mechanistic study reveals two reasons for the improvement: (1) shrinking bubbles increase the enrichment rate, and (2) the attractive interactions between the positively charged anode and negatively charged PFAS provide high enrichment at zero bubble path length. Based on this preconcentration method, we demonstrate the detection of ≥ 70 ng/L PFOA and PFOS in water in ~ 20 min by coupling it with our bubble-nucleation-based detection method, fulfilling the need of the US Environmental Protection Agency. Graphical abstractKeywords
Funding Information
- National Science Foundation (CHE-1943737)
- Engineer Research and Development Center (W912HZ2220002)
This publication has 30 references indexed in Scilit:
- Molecularly imprinted polymer modified TiO2 nanotube arrays for photoelectrochemical determination of perfluorooctane sulfonate (PFOS)Sensors and Actuators B: Chemical, 2014
- Quaternary Ammonium Bromide Surfactant Adsorption on Low-Index Surfaces of Gold. 2. Au(100) and the Role of Crystallographic-Dependent Adsorption in the Formation of Anisotropic NanoparticlesLangmuir, 2012
- Potential controlled surface aggregation of surfactants at electrode surfaces – A molecular viewSurface Science, 2009
- In Situ STM Study of Potential-Driven Transitions in the Film of a Cationic Surfactant Adsorbed on a Au(111) Electrode SurfaceLangmuir, 2007
- Bench-Top Method for Fabricating Glass-Sealed Nanodisk Electrodes, Glass Nanopore Electrodes, and Glass Nanopore Membranes of Controlled SizeAnalytical Chemistry, 2007
- Adsorption of N-Decyl-N,N,N-trimethylammonium Triflate (DeTATf), a Cationic Surfactant, on the Au(111) Electrode SurfaceLangmuir, 2006
- Electrochemical and Neutron Reflectivity Characterization of Dodecyl Sulfate Adsorption and Aggregation at the Gold−Water InterfaceLangmuir, 2001
- Direct Visualization of the Potential-Controlled Transformation of Hemimicellar Aggregates of Dodecyl Sulfate into a Condensed Monolayer at the Au(111) Electrode SurfaceLangmuir, 1999
- Carbon dioxide in water and seawater: the solubility of a non-ideal gasMarine Chemistry, 1974
- Photographic Investigation of the Projection of Droplets by Bubbles Bursting at a Water SurfaceTellus, 1954