Powdered activated carbon (PAC) for organic micro-pollutant (OMP) removal can be applied effectively on wastewater treatment plant (WWTP) effluents by using re-circulation schemes, accumulating the PAC in the system. This technique is complex because several factors are unknown: (i) the PAC concentration in the system, (ii) specific and average contact times of PAC particles, and (iii) PAC particle loadings with target compounds/competing water constituents. Thus, performance projections (e.g. in the lab) are very challenging. We sampled large-scale PAC plants with PAC sludge re-circulation on eight different WWTPs. The PAC plant-induced OMP removals were notably different, even when considering PAC concentrations in proportion to background organic sum parameters. The variability is likely caused by differing PAC products, varying water composition, differently effective plant/re-circulation operation, and variable biodegradation. Plant PAC samples and parts of the PAC plant influent samples were used in laboratory tests, applying multiples (0.5, 1, 2, 4) of the respective large-scale "fresh" PAC doses, and several fixed contact times (0.5, 1, 2, 4, 48 h). The aim was to empirically identify suitable combinations of lab PAC dose (as multiples of the plant PAC dose) and contact time, which represent the PAC plant performances in removing OMPs (for specific OMPs at single locations, and for averages of different OMPs at all locations). E.g., for five well adsorbing, little biodegradable OMPs, plant performances can be projected by using a lab PAC dose of twice the respective full-scale PAC dose and 4 h lab contact time (standard deviation of 13 %-points).
Adsorption onto powdered activated carbon (PAC) is a promising technique for the removal of organic micropollutants (OMPs) from treated wastewater. To enhance the adsorption efficiency, PAC is recycled back into the adsorption stage. This technique was examined in pilot scale in comparison to a reference without recirculation. Coagulation with Fe(3+) was carried out simultaneously to adsorption. Extensive OMP measurements showed that recirculation significantly increased OMP eliminations. Thus, significant PAC savings were feasible. The PAC concentration in the contact reactor proved to be an important operating parameter that can be surrogated by the easily measurable total suspended solids (TSS) concentration. OMP eliminations increased with increasing TSS concentrations. At 20 mg PAC L(-1) and 2.8 g TSS L(-1) in the contact reactor, well-adsorbable carbamazepine was eliminated by 97%, moderately adsorbable diclofenac was eliminated by 92% and poorly-adsorbable acesulfame was eliminated by 54% in comparison to 49%, 35% and 18%, respectively, without recirculation. The recirculation system represents an efficient technique, as the PAC's adsorption capacity is practically completely used. Small PAC dosages yield high OMP eliminations. Poorly-adsorbable gabapentin was eliminated to an unexpectedly high degree. A laboratory-scale biomass inhibition study showed that aerobic biodegradation removed gabapentin in addition to adsorption.
PAC adsorption is a widespread option for the removal of organic micropollutants (OMP) from secondary effluent. For an optimal exploitation of the adsorption capacity, PAC recirculation is nowadays a common practice, although the mechanistic interrelations of the complex recirculation process are not fully resolved. In this work, extensive multi-stage batch adsorption testing with repeated PAC and coagulant dosage was performed to evaluate the continuous-flow recirculation system. Partly loaded PAC showed a distinct amount of remaining capacity, as OMP and DOC removals considerably increased with each additional adsorption stage. At a low PAC dose of 10 mg PAC L−1, removals of benzotriazole and carbamazepine were shown to rise from <40% in the first stage up to >80% in the 11th stage at 30 min adsorption time per stage. At a high PAC dose of 30 mg PAC L−1, OMP and DOC removals were significantly higher and reached 98% (for benzotriazole and carbamazepine) after 11 stages. Coagulant dosage showed no influence on OMP removal, whereas a major part of DOC removal can be attributed to coagulation. Multi-stage adsorption is particularly beneficial for small PAC doses and significant PAC savings are feasible. A new model approach for predicting multi-stage OMP adsorption on the basis of a single-stage adsorption experiment was developed. It proved to predict OMP removals and PAC loadings accurately and thus contributes towards understanding the PAC recirculation process.
Advanced wastewater treatment with granular activated carbon (GAC) is a promising option to reduce emissions of organic micropollutants (OMP) into the aquatic environment. Frequent back-washes of the GAC filters are required due to high particle concentration in the treated wastewater but lead to stratification. Differences in adsorption capacities of individual strata are not known. The present study aimed at investigating physical and chemical differences at different filter depths of a stratified GAC filter. Two different commercial products were stratified during repeated filter bed expansions and sectioned into vertical fractions. Bulk densities, grain size distributions and ash contents of the individual fractions differed significantly. Adsorption tests with pulverized GAC from different levels showed great vertical differences in adsorption properties. OMP removals determined in the upper part of a GAC filter therefore cannot be extrapolated downwards. Both physical and chemical vertical heterogeneities with regard to adsorption capacities and residence times at different filter depths should be considered in the filter design, in the monitoring of a GAC filter, and in the interpretation of the GAC filter performance. Good correlations between abatements of UV light absorption and OMP removals were found for the virgin GAC throughout the non-uniform filter.
The competitive impacts of different fractions of wastewater treatment plant effluent organic matter (EfOM) on organic micro-pollutant (OMP) adsorption were investigated. The fractionation was accomplished using separation by nanofiltration (NF). The waters resulting from NF were additionally treated to obtain the same dissolved organic carbon (DOC) concentrations as the initial water. Using size exclusion chromatography (LC-OCD) it could be shown that the NF treatment resulted in an EfOM separation by size. Adsorption tests showed different competitive effects of the EfOM fractions with the OMP. While large EfOM compounds that were retained in NF demonstrated a reduced competition as compared to the raw water, the NF-permeating EfOM compounds showed an increased competition with the majority of the measured OMP. The effects of small size EfOM are particularly negative for OMP which are weak/moderate adsorbates. Adsorption analysis was carried out for the differently fractionized waters. The small sized EfOM contain better adsorbable compounds than the raw water while the large EfOM are less adsorbable. This explains the observed differences in the EfOM competitiveness. The equivalent background compound (EBC) model was applied to model competitive adsorption between OMP and EfOM and showed that the negative impacts of EfOM on OMP adsorption increase with decreasing size of the EfOM fractions. The results suggest that direct competition for adsorption sites on the internal surface of the activated carbon is more substantial than indirect competition due to pore access restriction by blockage. Another explication for reduced competition by large EfOM compounds could be the inability to enter and block the pores due to size exclusion.
Eight commercially available powdered activated carbons (PAC) were examined regarding organic micro-pollutant (OMP) removal efficiencies in wastewater treatment plant (WWTP) effluent. PAC characteristic numbers such as B.E.T. surface, iodine number and nitrobenzene number were checked for their potential to predict the OMP removal of the PAC products. Furthermore, the PAC-induced removal of UV254 nm absorption (UVA254) in WWTP effluent was determined and also correlated with OMP removal. None of the PAC characteristic numbers can satisfactorily describe OMP removal and accordingly, these characteristics have little informative value on the reduction of OMP concentrations in WWTP effluent. In contrast, UVA254 removal and OMP removal correlate well for carbamazepine, diclofenac, and several iodinated x-ray contrast media. Also, UVA254 removal can roughly describe the average OMP removal of all measured OMP, and can accordingly predict PAC performance in OMP removal. We therefore suggest UVA254 as a handy indicator for the approximation of OMP removal in practical applications where direct OMP concentration quantification is not always available. In continuous operation of large-scale plants, this approach allows for the efficient adjustment of PAC dosing to UVA254, in order to ensure reliable OMP removal whilst minimizing PAC consumption.
Activated carbon is investigated as adsorptive barrier for organic micropollutants (OMP) within the Berlin water cycle. In a pilot plant using granular activated carbon (GAC) as upper layer in dual-media filtration, OMP concentrations in treated wastewater could be reduced without any negative impact on filtration efficiency. OMP breakthroughs occurred after shorter runtimes than estimated according to isotherm experiments with powdered activated carbon (PAC). Batch adsorption tests comparing the used GAC to new GAC showed that the capacity of the used GAC was not exhausted, indicating that besides direct site competition, pore blocking is also responsible for the poor GAC performance. A pilot plant application of PAC of the same type as GAC showed significantly higher OMP removals at lower dosages, taking advantage of immobilization of PAC particles in the filters. Both PAC and GAC applications can be integrated into tertiary wastewater treatment without significant constructional changes.
Powdered activated carbon (PAC) is a promising agent for the adsorptive removal of organic micro-pollutants (OMP) from wastewater treatment plant (WWTP) effluents. Reliable and predictive test methods are required for the selection and for the quality control of PAC. In the present investigation, a pragmatic test method using indicative target OMP and photometric analyses was developed. Eight different PAC were compared according to the test method and according to removals of individual OMP in WWTP effluent. The test method allowed identification of the PAC with the highest and the lowest removals of benzotriazole and elucidated differences of the PAC with regard to removals of individual OMP. In WWTP effluent both positive and negative correlations between OMP removals with different PAC were observed: Some PAC removed diclofenac, carbamazepine and metoprolol to a comparatively greater extent while other PAC are comparably more efficient for benzotriazole, methylbenzotriazole and acesulfame adsorption.
This study investigates the applicability of the rapid small-scale column test (RSSCT) concept for testing of granular activated carbon (GAC) for organic micro-pollutants (OMPs) removal from wastewater treatment plant (WWTP) effluent. The chosen experimental setup was checked using pure water, WWTP effluent, different GAC products, and variable hydrodynamic conditions with different flow velocities and differently sized GAC, as well as different empty bed contact times (EBCTs). The setup results in satisfying reproducibility and robustness. RSSCTs in combination with WWTP effluent are effective when comparing the OMP removal potentials of different GAC products and are a useful tool for the estimation of larger filters. Due to the potentially high competition between OMPs and bulk organics, breakthrough curves are likely to have unfavorable shapes when treating WWTP effluent. This effect can be counteracted by extending the EBCT. With respect to the strong competition observed in GAC treatment of WWTP effluent, the small organic acid and neutral substances are retained longer in the RSSCT filters and are likely to cause the majority of the observed adsorption competition with OMPs.
Adsorption onto powdered activated carbon (PAC) is a promising option to remove organic micro-pollutants (OMP) from drinking water sources or wastewater. Since this treatment option requires continuous PAC dosing, sufficient contact time and subsequent separation of the PAC, the integration into existing process chains is challenging. In the present investigation, the pre-loading of a deep bed filter with PAC used as fixed bed adsorber was investigated. The retention and distribution of an exemplary PAC in a pumice rapid filter were determined. Gravimetry combined with combustion of the PAC at 550 °C was applied to differentiate between PAC and filter material residues and revealed comparably high PAC immobilization in the upper third of the pumice filter. Comparative adsorption experiments in batch with suspended PAC and continuous filtration tests with immobilized PAC showed advantageous results for immobilized PAC with regard to the removal of OMP and the sum parameters dissolved organic carbon and UV light absorption at 254 nm wavelength. The results indicate that a conventional rapid filter together with PAC can be effectively utilized as fixed bed adsorption filter.
In urban areas, water often flows along a partially closed water cycle in which treated municipal wastewater is discharged into surface waters which are one source of raw waters used for drinking water supply. A number of organic micro-pollutants (OMP) can be found in different water compartments. In the near future, climatic and demographic changes will probably contribute to an increase of OMP and antibiotic-resistant pathogens in aquatic ecosystems. The occurrence of OMP, possible adverse effects on aquatic organisms and human health and the public perception must be carefully assessed to properly manage and communicate potentially associated risks and to implement appropriate advanced treatment options at the optimum location within the water cycle. Therefore, the interdisciplinary research project ASKURIS focuses on identification and quantification, toxicological assessment and removal of organic micro-pollutants and antibiotic-resistant pathogens in the Berlin water cycle, life cycle-based economic and environmental assessment, public perception and management of potential risks.