Management of Macrolide Antibiotics (Erythromycin, Clarithromycin and Azithromycin) in the Environment: A Case Study of Environmental Pollution in Lithuania
- The ESAC-Net, which provides European reference data on antimicrobial consumption both in the community and the hospital sector. For the expression of antibiotic consumption, the system uses the number of Defined Daily Doses (DDDs) per 1000 inhabitants per day. All antibiotics are grouped according to the Anatomical Therapeutic Chemical (ATC) classification system.
- The State Medicines Control Agency of Lithuania (VVKT), which provides all consumed drugs (classified in ATC system) registered in Lithuania. The medicine consumption is expressed as DDD per 1000 inhabitants per day .
2. Materials and Methods
2.1. Macrolide Antibiotics Substance Flow Analysis
- As data presented in the international anatomic therapeutic chemical classification (ATC) system and the daily defined dose (DDD) methodology ;
- As data in monthly reports on the quantity of drugs sold in packages.
- Q(drug sold,j)—amount of drug sold, kg;
- S—drug strength, showing the quantity of substance in the pharmaceutical, mg;
- N—quantity of doses in package, pieces;
- M—number of packages sold, pieces.
2.2. Environmental Risk Assessment
- A(location, j)—amount of substance sold (j = 1,2,3,4 (Klaipeda, Palanga, Kretinga, Nida)), kg.
- A(Lithuania, j)—pharmaceutical substances sold in total, kg.
2.2.1. Study Area
2.2.2. Predicted Environmental Concentration, Adapted to Local Conditions of Antibiotics in WWTP Effluent and Surface Waters
- Ej—excretion coefficient, %.
- R,j—wastewater treatment coefficient, %.
- Alocation—a total sale data for the drug per year (kg).
- D—factor of wastewater dilution by surface water flow. When calculating PECj,eff, it was assumed that D = 0. In estimating PECj,sw, the dilution factor was 0 .
2.2.3. Environmental Management System
3. Results and Discussion
3.1. Analysis of the Macrolide Antibiotics Substance Flows (ASF) in Lithuania
3.1.1. System Definition
- Health institution sector and hospitals. According to the VVKT data, 26.74 kg (i.e., 3.8% of totally consumed macrolides) of macrolide antibiotics was sold directly for the health institution sector. According to the latest available data within the country, only a small portion of medicines remain unused in hospitals . It was assumed that only 5% of medicines were exposed to hazardous waste management equipment due to expired date or improper storage of medicines, while the remaining 95% were consumed by patients. A total of 33% of the total target macrolide antibiotics that entered the health institution sector were released in an active form by excretion in faeces and urine and ended up in sewage collection networks (see Section 2.1. for the excretion rates) .
- Public institutions and households. All the establishments that are not directly related to therapeutic activities can be attributed to the source of public institutions and households. The effluence of the pharmaceutical substances analyzed may occur in places such as retirement homes for the elderly, boarding houses or prisons. For this research, it was assumed that unused medicines makes up approximately 8% . The remaining 92% was assumed to be consumed and excreted through urine and feaces. See Figure 5 for the matrix of the loads estimated in households. The matrix defines only the output data from public institutions and households. Based on the literature analysis [25,28], consumers dispose of expired medicines in a few typical ways: they incinerate them at home, bring them to the pharmacies, dispose of them as municipal waste, continue using them or discharge them into the sewer systems; 21.6% were unaware of how to treat them. All of the sections in Figure 5 make up 100% (defined by the orange square). The schema shows that in the group of the 21.6% who were unaware of how to dispose of the waste, it is assumed that 75% of the unused medicines were disposed of as municipal waste and 25% flushed away into the sewage system. Moreover, all discharges to the wastewaters based on most typical wastewater treatments in Lithuania  were separated into urban WWTPs, individual treatment in wastewater pits and septic tanks, or direct effluents to surface waters. These three different types of treatments were used as the main approach for the expired and consumed medicine load calculations.
- Production of pharmaceutical substances. During the research, it was identified that target substances are not manufactured in Lithuania but are used in laboratories only for the scientific purposes or verification of complying with quality requirements. Even though the generated part of wastewater only from laboratories may be insignificant or irrelevant for the assessment of the balance in this specific case for Lithuania, it is still a source of pollution with pharmaceutical substances that might be crucial in a country having macrolide antibiotics-manufacturing facilities. In this case, it was assumed that only 0.01% of all consumed antibiotics were used in the SFA-block manufacture of pharmaceuticals. Such sources account for about 10% of hazardous wastewater that will be treated as hazardous, and the rest will be disposed of in a shared sewerage system .
3.1.3. Discharge and Disposal
- Wastewater treatment plants. In assessing the effluents of pharmaceutical residues to surface waters via wastewater treatment plants (WWTPs), a wastewater treatment efficiency of 78.6% for AZI, 53.3% for ERY and 54% for CLA was accepted. The average rates were estimated on the scientific research base of target antibiotics already performed at WWTPs [22,29,30,31,32]. The target macrolide antibiotics part that was removed from the effluents is considered in sludge. In 2014–2019, the Department of Environmental Protection carried out 3028 inspections in household units handling municipal sewage centrally, and 8% of municipal wastewater treatment offenses were determined. A total of 70% of them were released into surface waters incompletely treated, 16% were untreated and 14% revealed other handling breaches, such as clogged sewage collection systems, improper equipment installation or exploitation and others. According to the produced report, this accounted for 1% of the total number of respondents . Thus, it is assumed that due to wastewater collection systems, which are not fully repaired or exploitable, effluents from wastewater collection networks to surface waters will account for 1%. It defines only the effluent leakage into the soil.
- Untreated wastewater. According to the annual national reports of wastewater management and treatment, 24.2% of centrally untreated or insufficiently treated municipal wastewater is discharged into the environment every year. For SFA, it was assumed that 24.2% of water effluents from the WWTPs are not treated. This block involves only the input from WWTPs. It was assumed that improper exploitation of wastewater collection networks causes losses of 15% of discharge leakage into the soil, while the remaining 85% reach surface waters.
- Individual wastewater treatment. A total of 21% of the Lithuanian population individually treats wastewater generated by the residents themselves . The residents treat wastewater in several ways: by draining wastewater into tanks and collecting it there, collecting wastewater in septic tanks or using individual treatment plants, which, in most cases, are low-capacity biological wastewater treatment plants . The analysis of the water supply and wastewater treatment in Lithuania showed that, in most cases, tanks and septic tanks are unsuitable for use because they are old, leaking and improperly exploited. In most cases, constructions are not sealed, with an open bottom, which creates excellent conditions for pollutants to sink into soil and groundwater. It was assumed that discharge from individual wastewater treatment split into 60% of pollutants leakage into soil from septic tanks and wastewater pits, 30% to WWTPs from septic tanks and 10% to surface waters from small-capacity individual treatment plants.
- Incineration. All unused drugs collected from residents in pharmacies, as well as from health facilities or laboratories, are transferred to the hazardous waste managers and dispatched for combustion. The analyzed literature revealed that there is no evidence of concentrations of antibiotic residues in the air ; thus, it is assumed that active antibiotics fully decompose by incineration.
- Landfills. Landfills still pose a risk because leachates may pollute groundwater and surface water, even though they are commonly redirected to a municipal WWTP [33,34,35]. The Review of Regional Waste Management Centres (RWMC) provided information that revealed that 11 of the currently exploited landfills are fully equipped with leachate collection systems. Nine of them collect wastewater in tanks and return them for treatment in urban wastewater treatment plants, two of them treat wastewater in biological wastewater treatment plant and by the reverse osmosis method on site, and one treats wastewater in a tank, partly using a reverse osmosis system, and partly returns the water to central wastewater treatment networks (approximately 60%). Based on the proportion of municipal waste generated regionally, the part that is discharged back to urban WWTPs comprises 77%, and 23% is treated on site to surface waters. The determined antibiotics removal rates in biological and reverse-osmosis wastewater treatments used on landfill sites were 37% and 79%, respectively . Moreover, in these two flows, leakage to groundwaters must be considered. Scientists all around the world detect antibiotic residues in the soil and groundwaters of landfills [37,38,39]. Even though such research has not been carried out in Lithuania yet, according to the RWMC’s annual reports about groundwater monitoring on landfill sites, it is systematically detected that chloride, ammonium and other controlled parameters (which differ between regions) exceed the limit values of specified concentrations according to the Surface Wastewater Management Regulation. Reports declare that higher values do not pose a potential risk to the environment and must be monitored; however, this shows a potential pollution pathway to the environment. It was cautiously assumed that 5% of antibiotic residues are discharged to soil.
- Sludge. Sewage sludge is a by-product of wastewater treatment. According to the Environmental Protection Agency of Lithuania’s summary of treated waste quantities in 2020, 38% of urban sewage treatment sludge was recycled (14.6% was used for biogas extraction), 31.6% was incinerated, 26.8% was processed in land and 3.6% was disposed of in other ways. Overall, it is assumed that 68.4% of the target substances are discharged into soil, and the remaining 31.6% are disposed of by incineration.
3.1.4. Distribution in Environment
- Soil and surface waters. Pharmaceutical residues that have penetrated into aquaculture with sediment will enter the soil by filtration, and due to water circulation, will eventually enter the food chain through drinking water [40,41,42]. However, pharmaceutical substances that flow between water bodies have not been analyzed in SFA. Discharges end up in soil and surface waters. It was assumed that pharmaceuticals migrate, as after being affected and absorbed by aquacultures, they precipitate and enter the groundwater.
3.1.5. Results of ASF Analysis
- Treated in individual wastewater treatment—17.3%.
- Collected via central sewage networks and treated in WWTPs—66.0%.
- Treated by incineration—6.4%.
- Disposed of in landfills—8.2%.
- Directly entered surface waters from households—2.0%.
- The main macrolide antibiotic streams to the environment are via water bodies. Discharges that affect the natural environment are distributed as presented below:
- Surface waters—41.4%.
- Totally incinerated and assumed that no active compound will leave after this combustion—16.7%.
- Accumulate in sludge of leachate treated in landfills—1.1%, and it might be assumed that it will end up in soil.
3.2. Environmental Risk Assessment
3.2.1. Predicted Concentrations of Selected Antibiotics in Surface Waters
3.2.2. Discussion of Selected Measured Environmental Concentrations Values in Target Area
3.2.3. Results of Risk Quotients (RQs)
3.3. Application of the Environmental Management System Theory to Manage the Concentrations of Pharmaceutical Substances and Antibiotics in Wastewater
- up to 2025 Xin→1/4Xout
- up to 2030 Xin→1/2Xout
- up to 2035 Xin→0Xout
- Integration of efficient, more-modern management processes in the water and wastewater treatment plants of Lithuanian cities.
- Legal changes in connection with the removal of pharmaceutical substances from wastewater.
- More active monitoring of the flows of pharmaceutical substances.
- Households as the main source of pollution by the pharmaceutical residues (96.3% of total discharge);
- Treatment plants as the main source of pollution release into the environment (83.3% of total discharge).
- Pharmaceutical usage and consumption in general;
- Prescribing minimized doses of medications to patients only when necessary;
- Advanced and high-quality pharmaceutical residues treatment from healthcare facilities and WWTPs.
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
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|Macrolide Antibiotic||Excreted in Active Form, %|
|Treatment Section in WWTP||Klaipeda||Palanga||Kretinga||Nida|
|Mechanical processing (lattice, sand traps, settlers, etc.)||applicable|
|Biological processing||Four aerotanks with nitrogen and phosphorus removal.||Two aerotanks with nitrogen and phosphorus removal; denitrification basin; anaerobic, anoxic and oxy phases; the effluent stream entering the biological processing is divided into denitrification and dephosphation.||Two aeration tanks are used for nitrogen removal by activated sludge technology.||For the nitrogen removal, activated sludge technology is used.|
|Sedimentation after biological treatment||Part of the sludge is returned back to the biological step.Excess sludge removal.||applicable|
|Chemical processing||Organic carbon is sometimes used to support denitrification.||Chemical treatment is sometimes performedusing flocculantsAl2O3 and BrentapilusVP1.||NA||NA|
|Sedimentation||Sedimentation and sludge removal.|
|Target Substance||Year||Quantity of Drug Sold, kg/a||Share, %|
|Target Pharmaceutical Substance||Pharmaceutical Sales in Klaipeda, Palanga, Kretinga and Nida, kg/a||PECj,eff,|
|1 Ej, |
|2 Rj, |
|3 PNEC, ng/L|
|2017 Summer Season||2018 Winter Season|
|Klaipeda City||Palanga City||Kretinga City||Nida City||Klaipėda City||Palanga City||Kretinga City||Nida City|
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Baranauskaite-Fedorova, I.; Dvarioniene, J. Management of Macrolide Antibiotics (Erythromycin, Clarithromycin and Azithromycin) in the Environment: A Case Study of Environmental Pollution in Lithuania. Water 2023, 15, 10. https://doi.org/10.3390/w15010010
Baranauskaite-Fedorova I, Dvarioniene J. Management of Macrolide Antibiotics (Erythromycin, Clarithromycin and Azithromycin) in the Environment: A Case Study of Environmental Pollution in Lithuania. Water. 2023; 15(1):10. https://doi.org/10.3390/w15010010Chicago/Turabian Style
Baranauskaite-Fedorova, Inga, and Jolanta Dvarioniene. 2023. "Management of Macrolide Antibiotics (Erythromycin, Clarithromycin and Azithromycin) in the Environment: A Case Study of Environmental Pollution in Lithuania" Water 15, no. 1: 10. https://doi.org/10.3390/w15010010