Many types of contaminants of emerging concern (CECs), including per- and poly-fluoroalkyl substances (PFAS), have been found in leachate of operating municipal landfills. However, there is only limited information on CECs presence in leachate of historic landfills (≥3 decades since closure, often lacking engineered liners or leachate collection systems) at concentrations that may pose a risk to nearby wells and surface water ecosystems. In this study, 48 samples of leachate-impacted groundwater were collected from 20 historic landfills in Ontario, Canada. The CECs measured included artificial sweeteners (ASs), PFAS, organophosphate esters (OPE), pharmaceuticals, bisphenols, sulfamic acid, perchlorate, and substituted phenols. The common presence of the AS saccharin, a known indicator of old landfill leachate, combined with mostly negligible levels of the AS acesulfame, an indicator of modern wastewater, revealed that most samples were strongly influenced by leachate and not cross-contaminated by wastewater (which can contain these same CECs). Several landfills, including ones closed in the 1960s, had total PFAS concentrations similar to those previously measured at modern landfills, with a maximum observed here of 12.7 μg/L. Notably elevated concentrations of several OPE, sulfamic acid, cotinine, and bisphenols A and S were found at many 30-60 year-old landfills. There was little indication of declining concentrations with landfill age, suggesting historic landfills can be long-term sources of CECs to groundwater and that certain CECs may be useful tracers for historic landfill leachate. These findings provide guidance on which CECs may require monitoring at historic landfill sites and wastewater treatment plants receiving their effluent.

Pollution by chemical substances is of concern for the maintenance of healthy and sustainable aquatic environments. While the occurrence and fate of numerous emerging contaminants, especially pharmaceuticals, is well documented in freshwater, their occurrence and behavior in coastal and marine waters is much less studied and understood. This study investigates the occurrence of 58 chemicals in the open surface water of the Western Mediterranean Sea for the first time. 70 samples in total were collected in 10 different sampling areas. 3 pesticides, 11 pharmaceuticals and personal care products and 2 artificial sweeteners were detected at sub-ng to ng/L levels. Among them, the herbicide terbuthylazine, the pharmaceuticals caffeine, carbamazepine, naproxen and paracetamol, the antibiotic sulfamethoxazole, the antibacterial triclocarban and the two artificial sweeteners acesulfame and saccharin were detected in all samples. The compound detected at the highest concentration was saccharin (up to 5.23 ng/L). Generally small spatial differences among individual sampling areas point to a diffuse character of sources which are likely dominated by WWTP effluents and runoffs from agricultural areas or even, at least for pharmaceuticals and artificial food additives, from offshore sources such as ferries and cruising ships. The implications of the ubiquitous presence in the open sea of chemicals that are bio-active or toxic at low doses on photosynthetic organisms and/or bacteria (i.e., terbuthylazine, sulfamethoxazole or triclocarban) deserve scientific attention, especially concerning possible subtle impacts from chronic exposure of pelagic microorganisms.

Artificial sweeteners are gaining acceptance as tracers of human wastewater in the environment. The 3 artificial sweeteners analyzed in this study were detected in leachate or leachate-impacted groundwater at levels comparable to those of untreated wastewater at 14 of 15 municipal landfill sites tested, including several closed for >50 years. Saccharin was the dominant sweetener in old (pre-1990) landfills, while newer landfills were dominated by saccharin and acesulfame (introduced 2 decades ago; dominant in wastewater). Cyclamate was also detected, but less frequently. A case study at one site illustrates the use of artificial sweeteners to identify a landfill-impacted groundwater plume discharging to a stream. The study results suggest that artificial sweeteners can be useful tracers for current and legacy landfill contamination, with relative abundances of the sweeteners potentially providing diagnostic ability to distinguish different landfills or landfill cells, including crude age-dating, and to distinguish landfill and wastewater sources.

The artificial sweeteners sucralose (SCL), acesulfame (ACS), saccharin (SAC), and cyclamate (CYC) have been detected in environmental waters in Europe and North America. Higher environmental levels are expected in view of the increasing consumption of these food additives. In this study, an isotope-dilution mass spectrometry (IDMS) LC–MS/MS method was developed and validated for quantifying the four artificial sweeteners in boreal lakes (n = 3) and rivers (n = 12). The highest concentrations of ACS, SAC, CYC and SCL were 9,600, 490, 210 and 1000 ng/L, respectively. ACS and SAC were detected in all studied samples, and CYC and SCL in 98% and 56% of the samples. Seasonal trends of ACS and SAC were observed in some rivers. ACS and SCL concentrations in rivers correlated linearly with population equivalents of the wastewater treatment plants in the catchment areas, whereas SAC and CYC concentrations depend more on the source.

Artificial sweeteners are food additives widely used, mainly in reduced sugar or sugar-free foods and beverages. Acesulfame potassium (ACE-K) and sodium saccharin (SAC) are among the most widely consumed sweeteners worldwide. These compounds when ingested are not metabolized by the body, being excreted unchanged. They arrive at treatment plants, where they are partially degraded and consequently released directly into water bodies. For this reason, artificial sweeteners have been detected in the most diverse aquatic environments, being recognized as emerging contaminants. In this work, aqueous solutions of ACE-K and SAC, submitted to heterogeneous photocatalysis (TiO₂/UV-A) for 60 min, showed degradations of more than 99% and maximum mineralization of 57% for ACE-K and 49% for SAC. The effects of certain variables were evaluated, with pH having a greater influence on the degradation of acesulfame and the mass of semiconductor on that of saccharin. The degradation of ACE-K and SAC followed a pseudo-first-order kinetic model according to the Langmuir–Hinshelwood model. Assays using Artemia salina as the test organism demonstrated the low toxicity of the photocatalyzed solutions of ACE-K and SAC. The contribution of different reactive species to the photocatalysis was investigated using specific radical inhibitors; the results indicate that singlet oxygen (¹O₂) has a fundamental role in the photocatalytic degradation of ACE-K and SAC. Graphical Abstract ᅟ

The removal of artificial sweetener saccharin (SAC) in aqueous solution by electrochemical advanced oxidation using electro-Fenton process was performed. Experiments were carried out in an undivided cylindrical glass cell with a carbon-felt cathode and a Pt or boron-doped diamond (BDD) anode. The removal of SAC by electrochemically generated hydroxyl radicals followed pseudo-first-order kinetics with both Pt and BDD anode. The absolute rate constant of the SAC hydroxylation reaction was determined for the first time using the competition kinetic method and found to be (1.85 ± 0.01) × 10⁹ M⁻¹ s⁻¹. The comparative study of TOC removal efficiency during electro-Fenton treatment indicated a higher mineralization rate with BDD than Pt anode. The identification and evolution of short-chain carboxylic acids and inorganic ions formed during oxidation process were monitored by ion-exchange chromatography and ion chromatography, respectively. The assessment of toxicity of SAC and/or its reaction by-products during treatment was performed using Microtox® method based on the Vibrio fischeri bacteria luminescence inhibition. Results showed that the process was able to efficiently detoxify the treated solution.