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

Title: Adsorption of selected pharmaceuticals and an endocrine disrupting compound by granular activated carbon. 1. Adsorption capacity and kinetics

Abstract

The adsorption of two representative PhACs (naproxen and carbamazepine) and one EDC (nonylphenol) were evaluated on two granular activated carbons (GAC) namely coal-based Calgon Filtrasorb 400 and coconut shell-based PICA CTIF TE. The primary objective was to investigate preloading effects by natural organic matter (NOM) on adsorption capacity and kinetics under conditions and concentrations (i.e., ng/L) relevant for drinking water treatment. Isotherms demonstrated that all compounds were significantly negatively impacted by NOM fouling. Adsorption capacity reduction was most severe for the acidic naproxen, followed by the neutral carbamazepine and then the more hydrophobic nonylphenol. The GAC with the wider pore size distribution had considerably greater NOM loading, resulting in lower adsorption capacity. Different patterns for the change in Freundlich KF and 1/n with time revealed different competitive mechanisms for the different compounds. Mass transport coefficients determined by short fixed-bed (SFB) tests with virgin and preloaded GAC demonstrated that film diffusion primarily controls mass transfer on virgin and preloaded carbon. Naproxen suffered the greatest deteriorative effect on kinetic parameters due to preloading, followed by carbamazepine, and then nonylphenol. A type of surface NOM/biofilm, which appeared to add an additional mass transfer resistance layer and thus reduce film diffusion, was observed. Inmore » addition, electrostatic interactions between NOM/biofilm and the investigated compounds are proposed to contribute to the reduction of film diffusion. A companion paper building on this work describes treatability studies in pilot-scale GAC adsorbers and the effectiveness of a selected fixed-bed model. 32 refs., 3 figs., 2 tabs.« less

Authors:
; ;  [1]
  1. University of Waterloo, Waterloo, ON (Canada). NSERC Chair in Water Treatment
Publication Date:
OSTI Identifier:
21176783
Resource Type:
Journal Article
Resource Relation:
Journal Name: Environmental Science and Technology; Journal Volume: 43; Journal Issue: 5; Other Information: speldszu@uwaterloo.ca
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; 54 ENVIRONMENTAL SCIENCES; GRANULAR MATERIALS; ACTIVATED CARBON; COAL; ADSORPTION; SORPTIVE PROPERTIES; KINETICS; DRINKING WATER; WATER TREATMENT; ORGANIC MATTER; DECONTAMINATION; COCONUTS; DRUGS; PHENOLS; MASS TRANSFER; REMOVAL; PROPIONIC ACID

Citation Formats

Yu, Z., Peldszus, S., and Huck, P.M. Adsorption of selected pharmaceuticals and an endocrine disrupting compound by granular activated carbon. 1. Adsorption capacity and kinetics. United States: N. p., 2009. Web. doi:10.1021/es801961y.
Yu, Z., Peldszus, S., & Huck, P.M. Adsorption of selected pharmaceuticals and an endocrine disrupting compound by granular activated carbon. 1. Adsorption capacity and kinetics. United States. doi:10.1021/es801961y.
Yu, Z., Peldszus, S., and Huck, P.M. 2009. "Adsorption of selected pharmaceuticals and an endocrine disrupting compound by granular activated carbon. 1. Adsorption capacity and kinetics". United States. doi:10.1021/es801961y.
@article{osti_21176783,
title = {Adsorption of selected pharmaceuticals and an endocrine disrupting compound by granular activated carbon. 1. Adsorption capacity and kinetics},
author = {Yu, Z. and Peldszus, S. and Huck, P.M.},
abstractNote = {The adsorption of two representative PhACs (naproxen and carbamazepine) and one EDC (nonylphenol) were evaluated on two granular activated carbons (GAC) namely coal-based Calgon Filtrasorb 400 and coconut shell-based PICA CTIF TE. The primary objective was to investigate preloading effects by natural organic matter (NOM) on adsorption capacity and kinetics under conditions and concentrations (i.e., ng/L) relevant for drinking water treatment. Isotherms demonstrated that all compounds were significantly negatively impacted by NOM fouling. Adsorption capacity reduction was most severe for the acidic naproxen, followed by the neutral carbamazepine and then the more hydrophobic nonylphenol. The GAC with the wider pore size distribution had considerably greater NOM loading, resulting in lower adsorption capacity. Different patterns for the change in Freundlich KF and 1/n with time revealed different competitive mechanisms for the different compounds. Mass transport coefficients determined by short fixed-bed (SFB) tests with virgin and preloaded GAC demonstrated that film diffusion primarily controls mass transfer on virgin and preloaded carbon. Naproxen suffered the greatest deteriorative effect on kinetic parameters due to preloading, followed by carbamazepine, and then nonylphenol. A type of surface NOM/biofilm, which appeared to add an additional mass transfer resistance layer and thus reduce film diffusion, was observed. In addition, electrostatic interactions between NOM/biofilm and the investigated compounds are proposed to contribute to the reduction of film diffusion. A companion paper building on this work describes treatability studies in pilot-scale GAC adsorbers and the effectiveness of a selected fixed-bed model. 32 refs., 3 figs., 2 tabs.},
doi = {10.1021/es801961y},
journal = {Environmental Science and Technology},
number = 5,
volume = 43,
place = {United States},
year = 2009,
month = 3
}
  • The adsorption of two representative pharmaceutically active compounds (PhACs) naproxen and carbamazepine and one endocrine disrupting compound (EDC) nonylphenol was studied in pilot-scale granular activated carbon (GAC) adsorbers using post-sedimentation (PS) water from a full-scale drinking water treatment plant. The GAC adsorbents were coal-based Calgon Filtrasorb 400 and coconut shell-based PICA CTIF TE. Acidic naproxen broke through fastest while nonylphenol was removed best, which was consistent with the degree to which fouling affected compound removals. Model predictions and experimental data were generally in good agreement for all three compounds, which demonstrated the effectiveness and robustness of the pore and surfacemore » diffusion model (PSDM) used in combination with the time-variable parameter approach for predicting removals at environmentally relevant concentrations (i.e., ng/L range). Sensitivity analyses suggested that accurate determination of film diffusion coefficients was critical for predicting breakthrough for naproxen and carbamazepine, in particular when high removals are targeted. Model simulations demonstrated that GAC carbon usage rates (CURs) for naproxen were substantially influenced by the empty bed contact time (EBCT) at the investigated conditions. Model-based comparisons between GAC CURs and minimum CURs for powdered activated carbon (PAC) applications suggested that PAC would be most appropriate for achieving 90% removal of naproxen, whereas GAC would be more suitable for nonylphenol. 25 refs., 4 figs., 1 tab.« less
  • The properties of three different types of activated carbon, fibrous, powdered, and granular, were investigated theoretically and experimentally. The adsorption rate of the activated carbon fiber was found to be two orders of magnitude higher than that of the granular activated carbon, and one order of magnitude higher than that of the powdered activated carbon. Diffusion coefficients of methylene blue in the fibrous, powdered, and granular activated carbons were determined experimentally. A new method for estimating the meso- and macropore surface areas in these carbons was proposed.
  • Liquid-phase adsorption of organic compounds by granular activated carbon (GAC) and activated carbon fibers (ACFs) is investigated. Acetone, isopropyl alcohol (IPA), phenol, and tetrahydrofuran (THF) were employed as the model compounds for the present study. It is observed from the experimental results that adsorption of organic compounds by GAC and ACF is influenced by the BET (Brunauer-Emmett-Teller) surface area of adsorbent and the molecular weight, polarity, and solubility of the adsorbate. The adsorption characteristics of GAC and ACFs were found to differ rather significantly. In terms of the adsorption capacity of organic compounds, the time to reach equilibrium adsorption, andmore » the time for complete desorption, ACFs have been observed to be considerably better than GAC. For the organic compounds tested here, the GAC adsorptions were shown to be represented well by the Langmuir isotherm while the ACF adsorption could be adequately described by the Langmuir or the Freundlich isotherm. Column adsorption tests indicated that the exhausted ACFs can be effectively regenerated by static in situ thermal desorption at 150 C, but the same regeneration conditions do not do as well for the exhausted GAC.« less
  • The impact of anaerobic biological activity on the capacity of granular activated carbon (GAC) to adsorb organic compounds has not received much attention. In this study, the capacities of GAC for o-cresol obtained from bottle-point isotherm experiments were compared with the capacities measured in a completely mixed, biologically active, anaerobic GAC reactor treating a high-strength synthetic wastewater containing acetic acid, phenol, and o-cresol. O-cresol was not biodegraded in the reactors and was removed solely by adsorption. Because of the low concentrations of phenol measured in the effluents from the reactors, no competition for adsorption between phenol and o-cresol was observed.more » Also, the role of biological activity in the regeneration of GAC was demonstrated by preloading GAC with phenol and recovering the adsorbed phenol after the establishment of an active bacterial film on the GAC surface. 30 refs., 5 figs., 2 tabs.« less
  • The granular activated carbon adsorption unit process in drinking water treatment typically removes purgeable organic compounds for time periods on the order of a few weeks. Experimental evidence indicates that less volatile compounds of generally higher molecular weight than the purgeable fraction, but still detectable by gas chromatography, are efficiently removed for longer periods. Field data substantiate this. Explanatory mechanisms may include stronger adsorption affinities or biodegradation. Non-gas chromatographable, higher molecular weight materials such as humic acids, as measured by Total Organic Carbon (TOC) or trihalomethane formation potential, revert to lower removal efficiencies. Biodegradation may be responsible for a continuedmore » long term removal of a fraction of these materials.« less