Estimating the Mass of Pharmaceuticals Harbored in Municipal Solid Waste Landfills by Analyzing Refuse Samples at Various Ages and Depths.

Pharmaceuticals have been detected at high concentrations in municipal solid waste (MSW) landfill leachates, which are recognized as an underestimated source of pharmaceutical residues in the environment. However, limited efforts have been made to characterize pharmaceuticals in MSW landfill refuse, which is also of significant concern given the potential long-term environmental impact. Herein, we excavated landfill refuse from six cells with landfill ages of 7-27 years in the largest MSW landfill in Shanghai (in each cell, landfill refuse was collected from different depths of 2-8 m) and analyzed samples for the presence of 55 pharmaceuticals, including antibiotics and non-antibiotics. The results reveal the presence of 42 pharmaceuticals in landfill refuse, with median concentrations ranging from 0.30 to 116 µg/kg. Antibiotic and non-antibiotic pharmaceuticals exhibited diverse concentration trends with age, related to changes in policy intervention and consumption over time. Different concentration variations of individual pharmaceuticals were observed in refuse samples excavated at different depths and positively correlated to their sorption ability. The mass of pharmaceuticals in the investigated landfill was estimated from the obtained concentrations to be 80-220 tons with 95% probability, based on Monte Carlo analysis. To the best of our knowledge, this study provides the first estimate of pharmaceutical mass in an MSW landfill. The results will be helpful for understanding the potential long-term environmental impact of pharmaceuticals in landfills.

Municipal Solid Waste Landfills: An Underestimated Source of Pharmaceutical and Personal Care Products in the Water Environment.

Pharmaceutical and personal care products (PPCPs) have been the focus of increasing concern in recent decades due to their ubiquity in the environment and potential risks. Out-of-date PPCPs are usually discharged into municipal solid wastes (MSWs), enter the leachates in MSW landfills, and have serious adverse effects on the surrounding water environment. However, the occurrence and removal of PPCPs from landfill leachates have rarely been examined to date. This lack of knowledge makes the landfill an underestimated source of PPCPs in the environment. In this review, we collected the relevant publications of PPCPs in landfill leachates, systematically summarized the occurrence of PPCPs in landfill leachates globally, evaluated the removal performances for various PPCPs by different types of on-site full-scale leachate treatment processes, and assessed the impacts of landfill leachates on PPCPs in the adjacent groundwater. In particular, influencing factors for PPCPs in landfill leachates, including the physicochemical properties of PPCPs, climate conditions, and characteristics of landfill sites (i.e., landfill ages) as well as sociological factors (i.e., economic development), were extensively discussed to understand their occurrence patterns. Future perspectives were also proposed in light of the identified knowledge gaps. To the best of our knowledge, this is the first review regarding the occurrence and removal of PPCPs from landfill leachates worldwide.

NOM fractionation and fouling of low-pressure membranes in microgranular adsorptive filtration.

Membrane fouling by natural organic matter (NOM) was investigated in microgranular adsorptive filtration (µGAF) systems, in which a thin layer of adsorbent is predeposited on low-pressure membranes. The adsorbents tested included heated aluminum oxide particles (HAOPs), ion exchange (IX) resin, and powdered activated carbon (PAC). Size exclusion chromatography (SEC) separated the NOM into four apparent MW fractions with significant UV254. HAOPs and the IX resin performed almost identically with respect to removal of these fractions, and differently from PAC. However, while HAOPs and PAC reduced fouling substantially, IX resin did not, indicating that fouling could not be attributed to the NOM fractions detected by SEC. Rather, the key foulants appear to comprise a very small fraction of the NOM with almost no UV254 absorbance. Alginate, a strongly fouling surrogate for natural polysaccharides, is adsorbed effectively by HAOPs, but not by IX resin or PAC, suggesting that polysaccharides sometimes play a key role in membrane fouling by NOM.

Effects of a Novel Adsorbent on Membrane Fouling by Natural Organic Matter in Drinking Water Treatment.

Irreversible fouling of water filtration membranes reduces filter longevity and results in higher costs associated with membrane maintenance and premature replacement. The search for effective pretreatment methods to remove foulants that tend to irreversibly foul membranes is ongoing. In this study, a novel adsorbent (Heated Aluminum Oxide Particles (HAOPs)) was deployed in a fully automated pilot system to remove natural organic matter (NOM) from the surface water source used at the UniVann water treatment plant (WTP) in Ullensaker County, Norway. The pilot plant treatment process consists of passing the water through a thin layer of HAOPs that has been deposited on a mesh support. The HAOPs layer acts as an active packed bed which removes NOM from the water. Fluxes around 120 L/m2/h (LMH) at transmembrane pressure (TMP) below 10.7 psi (0.7 bar) were achieved over production cycles excessing 12 h. Treatment achieved always >85% colour removal and effluent colour <5 mg Pt/L (the target of treatment), and always <0.01 NTU turbidity and non-detectable suspended solids in the permeate. The HAOPs mixture after saturated with NOM is easy to remove by disruption of the HAOPs by rinsing the mesh surface, and the sludge is easily dewatered to higher of dry solids content.

Individual and competitive removal of heavy metals using capacitive deionization.

This study presents the viability and preference of capacitive deionization (CDI) for removing different heavy metal ions in various conditions. The removal performance and mechanisms of three ions, cadmium (Cd(2+)), lead (Pb(2+)) and chromium (Cr(3+)) were investigated individually and as a mixture under different applied voltages and ion concentrations. It was found that CDI could effectively remove these metals, and the performance was positively correlated with the applied voltage. When 1.2 V was applied into solution containing 0.5mM individual ions, the Cd(2+), Pb(2+), and Cr(3+) removal was 32%, 43%, and 52%, respectively, and the electrosorption played a bigger role in Cd(2+) removal than for the other two ions. Interestingly, while the removal of Pb(2+) and Cr(3+) remained at a similar level of 46% in the mixture of three ions, the Cd(2+) removal significantly decreased to 14%. Similar patterns were observed when 0.05 mM was used to simulate natural contaminated water condition, but the removal efficiencies were much higher, with the removal of Pb(2+), Cr(3+), and Cd(2+) increased to 81%, 78%, and 42%, respectively. The low valence charge and lack of physical sorption of Cd(2+) were believed to be the reason for the removal behavior, and advanced microscopic analysis showed clear deposits of metal ions on the cathode surface after operation.

Characterization of dissolved organic matter using high-performance liquid chromatography (HPLC)-size exclusion chromatography (SEC) with a multiple wavelength absorbance detector.

High-performance liquid chromatography-size exclusion chromatography (HPLC-SEC) coupled with a multiple wavelength absorbance detector (200-445 nm) was used in this study to investigate the apparent molecular weight (AMW) distributions of dissolved organic matter (DOM). Standard DOM, namely humic acid, fulvic acid and hydrophilic acid, from the Suwannee River were tested to ascertain the performance and sensitivity of the method. In addition to four compounds groups: humic substances (Peak 1, AMW 16 kD), fulvic acids (Peak 2, AMW 11 kD), low AMW acids (Peak 3, AMW 5 kD), and low AMW neutral and amphiphilic molecules, proteins and their amino acid building blocks (Peak 4, AMW 3 kD), an new group that appears to include low AMW, 6-10 kD, humic substances was found based on investigating the spectra at various elution times. The spectroscopic parameter S(>365) (slope at wavelengths >365 nm) was determined to be a good predictor of the AMW of the DOM. The detector wavelength played an important role in evaluating the AMW distribution. For some fractions, such as the humic and low AMW non-aromatic substances, the error in measurement was ± 30% as determined by two-dimensional chromatograms detected at an artificially selected wavelength. HPLC-SEC with multiple wavelength absorbance detection was found to be a useful technique for DOM characterization. It characterized the AMW distributions of DOM more accurately and provided additional, potentially important information concerning the properties of DOM with varying AMWs.

NOM removal by adsorption and membrane filtration using heated aluminum oxide particles.

Heated aluminum oxide particles (HAOPs) are a newly synthesized adsorbent with attractive properties for use in hybrid adsorption/membrane filtration systems. This study compared removal of natural organic matter (NOM) from water by adsorption onto HAOPs with that by adsorption onto powdered activated carbon (PAC) or coagulation with alum or ferric chloride (FeCl3); explored the overlap between the NOM molecules that preferentially adsorb to HAOPs and those that are removed by the more conventional approaches; and evaluated NOM removal and fouling in hybrid adsorbent/membrane systems. For equivalent molar doses of the trivalent metals, HAOPs remove more NOM, and NOM with higher SUVA254, than alum or FeCl3. Most of the HAOPs-nonadsorbable fraction of the NOM can be adsorbed by PAC; in fact, that fraction appears to be preferentially adsorbed compared to the average NOM in untreated water. Predeposition of the adsorbents on a microfiltration membrane improves system performance. For the water tested, at a flux of 100 L/m2-hr, predeposition of 11 mg/L PAC and 5 mg/L HAOPs (as Al3+) allowed the system to operate 5 times as long before the transmembrane pressure increased by 1 psi and to remove 10-20 times as much NOM as when no adsorbents were added.