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Review

Hospital Wastewater—Source of Specific Micropollutants, Antibiotic-Resistant Microorganisms, Viruses, and Their Elimination

by
Tomáš Mackuľak
1,
Klára Cverenkárová
2,
Andrea Vojs Staňová
3,4,
Miroslav Fehér
1,
Michal Tamáš
1,
Andrea Bútor Škulcová
1,
Miroslav Gál
5,
Monika Naumowicz
6,
Viera Špalková
5,7 and
Lucia Bírošová
2,*
1
Department of Environmental Engineering, Faculty of Chemical and Food Technology STU, Slovak University of Technology in Bratislava, Radlinského 9, 812 37 Bratislava, Slovakia
2
Department of Nutrition and Food Quality Assessment, Faculty of Chemical and Food Technology STU, Slovak University of Technology in Bratislava, Radlinského 9, 812 37 Bratislava, Slovakia
3
Department of Analytical Chemistry, Faculty of Natural Sciences, Comenius University in Bratislava, Ilkovičova 6, 842 15 Bratislava, Slovakia
4
South Bohemian Research Center of Aquaculture and Biodiversity of Hydrocenoses, Faculty of Fisheries and Protection of Waters, University of South Bohemia in Ceske Budejovice, Zatisi 728/II, CZ-389 25 Vodnany, Czech Republic
5
Department of Inorganic Technology, Faculty of Chemical and Food Technology STU, Slovak University of Technology in Bratislava, Radlinského 9, 812 37 Bratislava, Slovakia
6
Department of Physical Chemistry, Faculty of Chemistry, University of Bialystok, K. Ciolkowskiego 1K, 15-245 Bialystok, Poland
7
Department of Zoology and Fisheries, Faculty of Agrobiology, Food and Natural Resources, Czech University of Life Sciences Prague, Kamýcka 129, 165 00 Praha, Czech Republic
*
Author to whom correspondence should be addressed.
Antibiotics 2021, 10(9), 1070; https://0-doi-org.brum.beds.ac.uk/10.3390/antibiotics10091070
Submission received: 15 July 2021 / Revised: 25 August 2021 / Accepted: 31 August 2021 / Published: 4 September 2021
(This article belongs to the Special Issue Antibiotic Resistance in Wastewater and Its Treatment)
Browse Figure
Review Reports Versions Notes

Abstract

:
Municipal wastewaters can generally provide real-time information on drug consumption, the incidence of specific diseases, or establish exposure to certain agents and determine some lifestyle consequences. From this point of view, wastewater-based epidemiology represents a modern diagnostic tool for describing the health status of a certain part of the population in a specific region. Hospital wastewater is a complex mixture of pharmaceuticals, illegal drugs, and their metabolites as well as different susceptible and antibiotic-resistant microorganisms, including viruses. Many studies pointed out that wastewater from healthcare facilities (including hospital wastewater), significantly contributes to higher loads of micropollutants, including bacteria and viruses, in municipal wastewater. In addition, such a mixture can increase the selective pressure on bacteria, thus contributing to the development and dissemination of antimicrobial resistance. Because many pharmaceuticals, drugs, and microorganisms can pass through wastewater treatment plants without any significant change in their structure and toxicity and enter surface waters, treatment technologies need to be improved. This short review summarizes the recent knowledge from studies on micropollutants, pathogens, antibiotic-resistant bacteria, and viruses (including SARS-CoV-2) in wastewater from healthcare facilities. It also proposes several possibilities for improving the wastewater treatment process in terms of efficiency as well as economy.

Graphical Abstract

1. Introduction

As a result of human activity, water pollution has become a global challenge. This raises significant concerns, in particular as regards the presence and risk of pharmaceuticals, other chemical compounds, and pathogenic microorganisms in wastewater. Water pollution is a consequence of industrial production, laboratory research, high consumption of medicines, and, most importantly, the existence of healthcare facilities. Healthcare facilities are continuous point sources of contamination by various types of pharmaceuticals or diagnostic agents, such as contrast media [1,2]. Concentrations of such compounds in surface waters are relatively low, but information on their potential long-term effect on living organisms is still unknown.
It is unrealistic to generally expect a decline in the production or use of some dominant drug groups (especially antidepressants, antibiotics, or medication for cardiovascular diseases) in the near future. However, it is necessary to find ways for health care providers and the public to minimize the overuse of pharmaceuticals. At present, the use of CRP (C-reactive protein) tests by general practitioners is insufficient in several parts of Europe, despite the fact that their more frequent use could to some extent reduce the consumption and subsequent presence of antibiotics in the environment [3]. The use of antibiotics has a growing trend in the long run and its stagnation or decline is not expected [4]. Research is already responding to this, pointing to the possible use of new types of pharmaceuticals in combination with nanotechnologies to combat the emergence of resistance. New technologies use various nanomaterials based on carbon, titanium, silver, or gold with antibacterial activity [5]. The possibility of modifying classic materials to obtain good antibacterial properties and their subsequent possible use in healthcare facilities, for example in the treatment of wall surfaces in waiting rooms, is also being investigated [6]. However, all these substances would be additional and problematic wastewater pollutants.
Contrast agents, especially iodine-based substances, can also be a significant environmental problem in the future. A limited overview of the use of such types of compounds also means that the professional public does not have a comprehensive summary of their contribution to surface water contamination and their impact on various components of the environment in Slovakia, the Central European region, or elsewhere in the world. Compared to pharmaceutical products, these are extremely biologically inert and have only been studied to a limited extent. Another problem is the fact that even some innovative technologies, such as ozonation, cannot completely remove them from wastewater [7].
The presence of pharmaceuticals in surface waters points to the need for applications of new types of technologies (they can also be various combinations such as membrane technologies and oxidation processes or sorption materials), which could remove resistant types of microorganisms from wastewater in addition to micropollutants.
Generally, wastewater treatment at municipal WWTPs is often economically demanding, due to the significant flow of wastewater during the day. Therefore, it would be necessary to focus more on the treatment of dominant point sources of this type of pollution, such as healthcare facilities in this case, where the wastewater flow can be in volumes of up to 5000 m3 per day. These waters are significantly more contaminated with contrast agents, pharmaceuticals, and their metabolites compared to municipal wastewaters [8].
It should be emphasized that the monitoring of contrast agents, pharmaceuticals, and their metabolites in surface or drinking waters is often limited in time and money and therefore unsystematic. It regularly takes place only in some regions of Europe, which is why the ability of scientists to compare individual regions in terms of the presence of these micropollutants is limited [9].

2. Wastewater from Healthcare Facilities

2.1. Presence of Specific Micropollutants

Pharmaceuticals, hormones, contrast media, legal and illegal drugs, and their metabolites can be found in wastewater from various healthcare facilities at significant concentration levels [10]. With the exception of Denmark, where discharge limits are specified, most countries do not have special regulations for the disposal of wastewater from healthcare facilities [1]. The fate of these compounds in the environment is still largely unknown and published studies often deal only with their monitoring in wastewater and surface water [11]. On the other hand, values of other parameters for wastewater from healthcare facilities such as COD, NH4, etc. are similar to municipal wastewater (Table 1) [9].
According to published data, healthcare facilities are also perceived as a possible source of analgesics, antidepressants, antibiotics, or antiepileptics, but also antibiotic-resistant bacteria [10]. Heberer and Feldmann published a study aimed at discovering the occurrence of selected pharmaceuticals in wastewater from healthcare facilities in Berlin [12]. They found that pharmaceuticals were removed only to a limited extent by the sewage system and the treatment plant, with most of them entering surface waters. The authors point out that the main sources of carbamazepine and diclofenac in Berlin’s wastewater are predominantly households and hospitals with more than 12,000 beds. Saussereau et al. analyzed the hospital effluent in Rouen, France, and the results were then compared with the influent and effluent from a treatment plant [13]. Twenty frequently used pharmaceuticals were monitored in wastewater from healthcare facilities. The compounds with the highest measured concentrations were tramadol, venlafaxine, citalopram, caffeine, and oxazepam. Concentrations of these drugs in wastewater ranged from 0.1–2.4 μg·L−1.
Wastewater analyses in selected healthcare facilities in Slovakia, specifically in Bratislava, pointed to high amounts (showed elevated concentrations compared to municipal wastewaters) of pharmaceuticals such as tramadol (opioid analgesic) and midazolam (sedative) (Table 2). We observed an increased incidence of methamphetamine in wastewater from the Ružinov polyclinic, which may be related to the treatment of drug-addicted patients abusing this addictive substance. On the other hand, levels of cocaine, LSD, and MDMA occurred only to a limited extent, in concentrations below LOQ in this type of wastewater. Among legal drugs, caffeine predominates (bellow LOQ) in wastewater from healthcare facilities. Increased nicotine use results in increased concentrations of its metabolite cotinine (bellow 6700 ng/L).
The authors Yuan et al. (Table 3) monitored 22 psychoactive drugs in the effluent from two psychiatric hospitals in Beijing [14]. The pharmaceuticals with the highest concentrations in wastewater were representatives of neuroleptics: clozapine, quetiapine (antipsychotic medication used for the treatment of schizophrenia); sulpiride (a benzamide neuroleptic used in the treatment of schizophrenia and other psychotic disorders); antidepressants: fluvoxamine, citalopram (selective serotonin reuptake inhibitors indicated for depression and symptoms of depressive disorders); but also the popular carboxamide derivatives in our country: carbamazepine (antiepileptic drug) and benzodiazepine: oxazepam (anxiolytic).

2.2. Presence of Antibiotic-Resistant Microorganisms

Antibiotic and biocide-resistant bacteria have become a global challenge, which is slowly shifting our society into the so-called post-antibiotic era. European Commissioner for Health Stella Kyriakides said that in current pandemic times, COVID-19 and antimicrobial resistance call for a united approach across policies, countries, and all levels of society [15,16]. Many countries and global organizations are working to address this through various monitoring programs and measures (the One Health Action Plan in the EU, for example). The development and spread of antibiotic resistance is a complex process that involves many variables [17]. This phenomenon is largely influenced by the selection pressure induced by the presence of antimicrobials at subinhibitory concentrations. Pharmaceutically active compounds induce the formation of mutations leading to antibiotic resistance in bacteria. Some pharmaceuticals have been shown to increase the rate and likelihood of resistance genes transmission from resistant bacterial strains to susceptible ones, thereby contributing to the spread of resistance [18,19].
Wastewater from healthcare facilities, the source of various sensitive or antibiotic-resistant bacteria, is often discharged into the sewage system without prior treatment, thus contributing to an increase in the concentration and spectrum of pharmaceuticals as well as the number of antibiotic-resistant bacteria and antibiotic-resistance genes in municipal wastewater [20,21]. According to the data from the European Center for Disease Control (ECDC), at least one in three hospitalized patients and one in two patients undergoing surgery in the EU receives antibiotic treatment on any given day. Some of these uses may be unnecessary and may contribute to the spread of antimicrobial resistance [22]. Many hospitalized patients are infected with resistant bacteria or can be asymptomatic carriers of such bacteria. For example, a Europe-wide sequencing survey of 2000 samples of Klebsiella pneumoniae from patients in 244 hospitals in 32 countries showed that the hospital environment provides suitable space for the transfer of genes encoding carbapenemases (enzymes that cleave the latest generation of cephalosporins) [23]. In addition, the microbiota and microbiome of healthy individuals contain antibiotic-resistant bacteria and resistance genes [24]. The degree of bacterial resistance in healthcare facility effluents can be significantly different compared to other aquatic environments due to the use of specific antimicrobial agents in healthcare facility conditions. These are, for example, cefotiam, piperacillin, and vancomycin, which are used exclusively in the environment of healthcare facilities. Wastewater from healthcare facilities is therefore an important source not only of pharmaceuticals but also of antibiotic-resistant bacteria and resistance genes. Thus, it represents a very suitable environment for the development and spread of the antimicrobial resistance phenomenon [21,25,26,27].
Effluents from healthcare facilities in Slovakia and the Czech Republic contain relatively high levels of coliform bacteria (including E. coli) and gram-positive enterococci with the majority showing a multidrug resistance phenotype [25,28,29]. Such strains present in untreated wastewater from healthcare facilities can enter municipal WWTPs and, despite the high degree of dilution in the sewerage system, pass through the WWTP to the recipient and the environment [30]. Although antibiotic-resistant bacteria do not always pass through WWTPs, many antibiotics do and reach surface waters thus contributing to the development of antibiotic resistance. The numbers of antibiotic-resistant coliform bacteria in the wastewater of Slovak and Czech healthcare facilities are about one logarithmic order higher compared to the numbers at the WWTP inflow. The numbers of antibiotic-resistant E. coli and enterococci are at a similar level or slightly reduced compared to inflow waters [28,31]. However, hospital wastewater contains a high number of multidrug-resistant coliform bacteria and E. coli, we must consider the risk of the occurrence of strains producing broad-spectrum beta-lactamases (ESBLs). These strains can transfer multiple resistance genes through the conjugative plasmid and spread them to susceptible bacterial species. A massive occurrence of ESBL-producing bacteria has been recorded in wastewater from healthcare facilities. In addition, isolates from healthcare facility outlets are often characterized by carrying several different resistance genes on plasmids or chromosomes at the same time, making them able to resist a wide range of different antimicrobials [25,32,33].
In addition to ESBL-producing coliform bacteria, outlets from healthcare facilities are also considered to be the primary reservoir of vancomycin-resistant enterococci, which also belong to clinically relevant groups of bacteria. However, the monitoring of wastewater in Slovakia showed that these resistant’s occurred in municipal wastewater rather than in the effluents from healthcare facilities [28,31]. Another important issue is that low concentrations of non-antimicrobial pharmaceuticals such carbamazepine, atenolol, valsartan but also cotinine in wastewater can also contribute to the development of antibiotic resistance. However, hospital effluents contain a mixture of different pharmaceuticals at low concentrations, they can also significantly contribute to the development and spread of antibiotic and biocide-resistant bacteria and resistance genes [26].

2.3. Presence of Viruses in Wastewater from Healthcare Facilities

Nowadays, the most discussed topic is the presence of viruses in the wastewater due to the SARS-CoV-2 pandemic and their proven presence in municipal wastewater. However, the investigation of viruses in medical facilities wastewater is a topic of broader importance. Collected sewage from health facilities is abundant in large amounts of toxic substances and pathogenic organisms such as bacteria and viruses. Therefore, insufficient degradation of the medical wastewater might lead to pathogen circulation in the environment and recurring infections [34]. The most common viruses that can be found in the treated wastewater are enteric viruses such as Hepatitis A, but also noroviruses, rotaviruses, adenoviruses, and astroviruses. These cause a variety of diseases such as gastroenteritis, meningitis, and hepatitis. Most of them replicate massively in the intestinal tract and are shed into the feces in high concentrations [35].
SARS-CoV and SARS-CoV-2 were likewise detected in the hospital wastewater [36,37]. It was proven that SARS-CoV-2 binds to angiotensin-converting enzyme 2 (ACE2) located on the surface of enteric cells, replicates, and is shed into the feces similarly to enteric viruses. The fact was subsequently employed by many researchers and public health authorities to detect SARS-CoV-2 by RT-qPCR in the wastewater and used as an epidemiological tool for controlling the local SARS-CoV-2 epidemic [38]. Although reinfection by SARS-CoV-2 from wastewater has not been observed yet, further research is necessary as we know that many other viruses are found infectious in wastewaters including SARS-COV-1, and the presence of the SARS-CoV-2 was already detected in surface waters [39,40,41,42]. Cycle thresholds (CT) vary and reflect the pandemic situation in the population. Lately, the investigation involves genetic sequencing as a potential method for detecting mutations in the wastewater. The method will be even more crucial to employ at healthcare facilities as vaccination and the convalescence plasma treatment will increase selective pressure on the virus to mutate [43]. Analysis of new mutations and variants will again help epidemiologists in setting the right public health measures to contain the pandemic. Similarly, new mutations lead to higher infectivity of the virus, with fewer virus particles required for infection, which can play an important role in wastewater reinfections [44].
After the precise detection of viruses in the hospital wastewater, effective elimination is needed. Chlorination, ultraviolet, and ozone treatment are all commonly used disinfection technologies in hospital wastewater treatment plants and are also proven to be effective in the case of virus elimination [45]. On the contrary, a study by Zhang et al., reported detection of RNA SARS-CoV-2 in septic tanks after disinfection with sodium hypochlorite according to WHO guidelines [46]. Therefore, a combination of chlorination and other disinfection technologies such as plasma treatment, advanced oxidation reaction (e.g., Fenton reaction), ultrafiltration, or adsorption on nanoparticles is vital to avoid reinfections [47].

3. Innovative Processes Efficient in the Treatment of Wastewater from Healthcare Facilities

Current research is focused not only on monitoring the known pharmaceuticals and their metabolites in wastewater but also on studying the potential of new degradation processes. The study by Yuan et al. dealt with the ability of treatment plants to remove these types of micropollutants from the wastewater and to decrease the load on the environment [14]. The results showed only a limited ability to treat wastewater using biological processes (activated sludge) implemented in treatment plants. The complex structures of some compounds (especially pharmaceuticals with two aromatic rings) are highly resistant to biological purification, leading to a limited ability to degrade them. The lowest removal efficiency was obtained for oxazepam. In the case of sulpiride and carbamazepine, we even observed an increase in their concentration in the treatment plant from psychiatric hospital B. The collection time, the retention time, the sorption/desorption in the treatment plant, and the physicochemical properties of the studied compounds influence the concentration of the compounds [14]. An experimental technique based on the sub- and super-critical water oxidation of wastewater was used for amoxicillin and ciprofloxacin elimination. The feasibility of the method was tested in the temperature range from 473 K to 773 K and at flow rates of 3 and 5 mL/min. The highest COD and TOC reductions were achieved at the highest temperature of 773 K, where they were reduced by 76% and 63%, respectively [48]. However, conventional treatment (based mainly on mechanical and biological processes) is not efficient enough [49,50,51]. New treatment processes (see examples in Table 4) include various membrane bioreactors, nanomaterials, ferrates, Fenton reaction, ozonation, heterogeneous catalysis, ultrasound, aquatic plants, and adsorption e.g., on biochar or activated carbon [51,52,53,54].
Hospital wastewaters often contain significant amounts of fecal coliforms, which exhibit resistant or multi-resistant properties to various types of antibiotics [52,53,58,59,60]. Therefore, the degradation processes are investigated in terms of removal efficiency not only for a wide range of micropollutants but also for pathogenic microorganisms, so the disinfection ability is evaluated [61,62].
Currently, many different methods for the treatment of wastewater from healthcare facilities are being researched, which often combine chemical and biological degradation procedures in different ways [63,64,65]. A combination of ozonation with active sorbent (e.g., activated carbon), UV-C and H2O2, MBR (membrane bioreactor), and AOPs (advanced oxidation processes) dominates [52,66,67,68,69]. The historically used methods for disinfection of these types of waters are chlorination and UV-C radiation [69,70]. However, the main drawback of chlorination is the risk of the formation of various chlorine-rich organic by-products, which can negatively affect water organisms [52]. As in municipal wastewater, wastewater treatment from healthcare facilities can be performed by conventional chemical (e.g., coagulation) [71], and biological processes—where nitrification [52] predominates. In addition, research can be observed in various innovative processes such as the applicability of the enzymes themselves [72] or their combination with a root treatment plant [63], the combination of activated sludge using vermifiltration [65], the applicability of wood-destroying fungi [20], or various modifications of nanomaterials, sorbents and related e.g., photocatalysis (Table 5) [61,73].
Advanced oxidation processes (AOPs) and their various combinations with biological processes [67,74] achieve the best efficiencies in the treatment of wastewater in terms of chemical and biological pollution. An essential step in the effectiveness of AOPs is the production of free radicals, where the hydroxyl radical and various forms of reactive oxygen species (ROS) predominate [52,53,59,71,75,76,77,78]. AOPs that are frequently investigated include electrochemical AOPs [75,78,79,80].
In general, the most effective AOPs that are currently being intensively investigated in terms of wastewater treatment include the Fenton reaction (FR), photo-Fenton reaction(pFR), ozonation, and their modifications [29,52,53,75,76,77,81,82]. The combination of FR with biological processes also appears to be interesting [58,59]. The combination of a Fenton or photo-Fenton reaction, followed by purification of the effluent from a healthcare facility using activated sludge has been described in a study by Kajitvichyanukul et al. [58]. In a study by Miralles-Cuevas et al., nanofiltration was placed before the photo-Fenton reaction [83]. In addition to already described procedures, and the abilities of ferrates-iron (VI)—use in water purification and disinfection [53] are becoming a topical issue. Ferrates are very strong oxidizing agents that are able to degrade a wide range of drugs present in wastewater [84,85,86]. Currently, there is limited information from published literature about their disinfection power and purification of concentrated point sources of micropollutants such as healthcare facilities.
Current advances in the development of new technologies and materials in the degradation of micropollutants (pharmaceuticals, drugs, pesticides) in wastewater offer the use of boron-doped diamond electrodes [53]. The advantage of these electrodes is the significant increase in wastewater disinfection efficiency, as their application generates radical forms of oxygen (singlet oxygen, hydroxyl radical).

4. Conclusions and Suggestions

Various analytical procedures are used to monitor the presence and concentration of micropollutants, which may ultimately be reflected in an inaccurate description of the current situation. As part of a systematic collection, it would be interesting to obtain results directly from the WWTP (inflow and outflow). However, placing analytical equipment (mostly LC-MS/MS) in treatment plants seems unrealistic for application for several reasons. The price of the instrument, its operation and the need of a specially trained analytical chemist dominate. Therefore, it would be necessary to have central laboratories in different regions of Europe to regularly collect and evaluate water samples to monitor micropollutants.
After precise monitoring, efficient degradation should take place. Currently, hospital wastewaters are treated with a combination of physical and chemical processes. Membrane technologies, sorbents, UV irradiation, and chlorination are the most commonly used but oftentimes insufficient in degrading complex micropollutants and organisms. These should be further combined with AOPs for the successful treatment of such wastewater for alleviating the burden on the environment.
Another possibility is the development and utilization of novel (bio)sensors that can continuously monitor the selected micropollutants in wastewater and transfer the recorded data wirelessly to the monitoring station. There, the situation will be assessed and, if necessary, steps can be taken to eliminate the current environmental burden.
It would also be necessary to improve the life cycle of the released pharmaceuticals. Targeted consumer motivation can be an example of how to solve this problem so that it does not end in improper disposal, for example in sewers (after the expiration date or the patient’s death).
The last, but not the least, possibility is the improvement of treatment technologies based on AOPs. In combination with automatic monitoring systems present directly in the sewer or at the wastewater treatment plant, the wastewater treatment processes with AOPs can be started automatically and instantly, and thus react immediately to the unfavorable environmental situation.

Author Contributions

All authors have contributed to this review equally. All authors have read and agreed to the published version of the manuscript.

Funding

This work was supported by the Slovak Research and Development Agency under contracts no APVV-19-0250, APVV-17-0183, PP-COVID-20–0019. This article was also realized because of the support for infrastructure equipment by the Operation Program Research and Development for the projects “Centre for the investigation of synthesis and transformation of nutritional substances in the food chain in interaction with potentially harmful substances of anthropogenic origin: comprehensive assessment of soil contamination risks for the quality of agricultural products” (No. CZ.02.1.01/0.0/0.0/16_019/0000845) and “University science park STU Bratislava” (ITMS 26240220084), which were co-financed by the European Regional Development Fund. This work was also supported by the Scientific Grant Agency of the Ministry of Education of the Slovak Republic (MESR) and of the Slovak Academy of Sciences (SAS) VEGA 1/0464/21 and VEGA 1/0343/19. This study was financially supported by project VIR-SCAN—Wastewater monitoring data as an early warning tool to alert COVID-19 in the population (“EOSCsecretariat.eu has received funding from the European Union’s Horizon Program call H2020-INFRAEOSC-05-2018-2019. This article was also written thanks to the generous support under the Operational Program Integrated Infrastructure for the project: “Strategic research in the field of SMART monitoring, treatment and preventive protection against coronavirus (SARS-CoV-2)”, Project no. 313011ASS8, co-financed by the European Regional Development Fund.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare no conflict of interest. The funders had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or in the decision to publish the results.

References

  1. Yilmaz, G.; Kaya, Y.; Vergili, I.; Beril Gönder, Z.; Özhan, G.; Ozbek Celik, B.; Altinkum, S.M.; Bagdatli, Y.; Boergers, A.; Tuerk, J. Characterization and toxicity of hospital wastewaters in Turkey. Environ. Monit. Assess. 2017, 189, 55:1–55:19. [Google Scholar] [CrossRef] [PubMed]
  2. Castillo Meza, L.; Piotrowski, P.; Farnan, J.; Tasker, T.L.; Xiong, B.; Weggler, B.; Murrell, K.; Dorman, F.L.; Vanden Heuvel, J.P.; Burgos, W.D. Detection and removal of biologically active organic micropollutants from hospital wastewater. Sci. Total Environ. 2020, 700, 134469:1–134469:8. [Google Scholar] [CrossRef]
  3. van Buul, L.W.; van der Steen, J.T.; Doncker, S.M.M.M.; Achterberg, W.P.; Schellevis, F.G.; Veenhuizen, R.B.; Hertogh, C.M.P.M. Factors influencing antibiotic prescribing in long-term care facilities: A qualitative in-depth study. BMC Geriatr. 2014, 14, 136:1–136:11. [Google Scholar] [CrossRef] [Green Version]
  4. Klein, E.Y.; Milkowska-Shibata, M.; Tseng, K.K.; Sharland, M.; Gandra, S.; Pulcini, C.; Laxminarayan, R. Assessment of WHO antibiotic consumption and access targets in 76 countries, 2000–2015: An analysis of pharmaceutical sales data. Lancet Infect. Dis. 2021, 21, 107–115. [Google Scholar] [CrossRef]
  5. Sánchez-López, E.; Gomes, D.; Esteruelas, G.; Bonilla, L.; Lopez-Machado, A.L.; Galindo, R.; Cano, A.; Espina, M.; Ettcheto, M.; Camins, A.; et al. Metal-based nanoparticles as antimicrobial agents: An overview. Nanomaterials 2020, 10, 292. [Google Scholar] [CrossRef] [Green Version]
  6. Palza, H.; Nuñez, M.; Bastías, R.; Delgado, K. In situ antimicrobial behavior of materials with copper-based additives in a hospital environment. Int. J. Antimicrob. Agents 2018, 51, 912–917. [Google Scholar] [CrossRef]
  7. Sengar, A.; Vijayanandan, A. Comprehensive review on iodinated X-ray contrast media: Complete fate, occurrence, and formation of disinfection byproducts. Sci. Total Environ. 2021, 769, 144846:1–144846:23. [Google Scholar] [CrossRef] [PubMed]
  8. Khan, M.T.; Shah, I.A.; Ihsanullah, I.; Naushad, M.; Ali, S.; Shah, S.H.A.; Mohammad, A.W. Hospital wastewater as a source of environmental contamination: An overview of management practices, environmental risks, and treatment processes. J. Water Process Eng. 2021, 41, 101990:1–101990:17. [Google Scholar] [CrossRef]
  9. Mackuľak, T.; Bodík, I.; Bírošová, L. Drogy a liečivá ako mikropolutanty, 1st ed.; FCHPT STU v Bratislave: Bratislava, Slovakia, 2016; ISBN 978-80-89597-34-5. [Google Scholar]
  10. Aydin, S.; Aydin, M.E.; Ulvi, A.; Kilic, H. Antibiotics in hospital effluents: Occurrence, contribution to urban wastewater, removal in a wastewater treatment plant, and environmental risk assessment. Environ. Sci. Pollut. Res. 2019, 26, 544–558. [Google Scholar] [CrossRef]
  11. Ngigi, A.N.; Magu, M.M.; Muendo, B.M. Occurrence of antibiotics residues in hospital wastewater, wastewater treatment plant, and in surface water in Nairobi County, Kenya. Environ. Monit. Assess. 2019, 192, 18:1–18:16. [Google Scholar] [CrossRef]
  12. Heberer, T.; Feldmann, D. Contribution of effluents from hospitals and private households to the total loads of diclofenac and carbamazepine in municipal sewage effluents—Modeling versus measurements. J. Hazard. Mater. 2005, 122, 211–218. [Google Scholar] [CrossRef] [PubMed]
  13. Saussereau, E.; Lacroix, C.; Guerbet, M.; Cellier, D.; Spiroux, J.; Goullé, J.P. Determination of levels of current drugs in hospital and urban wastewater. Bull. Environ. Contam. Toxicol. 2013, 91, 171–176. [Google Scholar] [CrossRef] [PubMed]
  14. Yuan, S.; Jiang, X.; Xia, X.; Zhang, H.; Zheng, S. Detection, occurrence and fate of 22 psychiatric pharmaceuticals in psychiatric hospital and municipal wastewater treatment plants in Beijing, China. Chemosphere 2013, 90, 2520–2525. [Google Scholar] [CrossRef] [PubMed]
  15. ECDC. Antimicrobial Resistance and Consumption Remains High in the EU/EEA and the UK, according to New ECDC Data. Available online: https://www.ecdc.europa.eu/en/news-events/antimicrobial-resistance-and-consumption-remains-high-press-release (accessed on 13 July 2021).
  16. Zhou, C.; Wu, J.; Dong, L.; Liu, B.; Xing, D.; Yang, S.; Wu, X.; Wang, Q.; Fan, J.; Feng, L.; et al. Removal of antibiotic resistant bacteria and antibiotic resistance genes in wastewater effluent by UV-activated persulfate. J. Hazard. Mater. 2020, 388, 122070:1–122070:8. [Google Scholar] [CrossRef]
  17. Pärnänen, K.M.M.; Narciso-da-Rocha, C.; Kneis, D.; Berendonk, T.U.; Cacace, D.; Do, T.T.; Elpers, C.; Fatta-Kassinos, D.; Henriques, I.; Jaeger, T.; et al. Antibiotic resistance in European wastewater treatment plants mirrors the pattern of clinical antibiotic resistance prevalence. Sci. Adv. 2019, 5, eaau9124:1–eaau9124:10. [Google Scholar] [CrossRef] [Green Version]
  18. Jiao, Y.-N.; Chen, H.; Gao, R.-X.; Zhu, Y.-G.; Rensing, C. Organic compounds stimulate horizontal transfer of antibiotic resistance genes in mixed wastewater treatment systems. Chemosphere 2017, 184, 53–61. [Google Scholar] [CrossRef]
  19. Liu, Y.; Tong, Z.; Shi, J.; Jia, Y.; Yang, K.; Wang, Z. Correlation between Exogenous Compounds and the Horizontal Transfer of Plasmid-Borne Antibiotic Resistance Genes. Microorganisms 2020, 8, 1211. [Google Scholar] [CrossRef]
  20. Mir-Tutusaus, J.A.; Parladé, E.; Villagrasa, M.; Barceló, D.; Rodríguez-Mozaz, S.; Martínez-Alonso, M.; Gaju, N.; Sarrà, M.; Caminal, G. Long-term continuous treatment of non-sterile real hospital wastewater by Trametes versicolor. J. Biol. Eng. 2019, 13, 47:1–47:13. [Google Scholar] [CrossRef]
  21. Wang, Q.; Wang, P.; Yang, Q. Occurrence and diversity of antibiotic resistance in untreated hospital wastewater. Sci. Total Environ. 2018, 621, 990–999. [Google Scholar] [CrossRef]
  22. Vandael, E.; Latour, K.; Goossens, H.; Magerman, K.; Drapier, N.; Catry, B.; Versporten, A.; Andre, M.; Aouachria, S.; Aoun, M.; et al. Point prevalence survey of antimicrobial use and healthcare-associated infections in Belgian acute care hospitals: Results of the Global-PPS and ECDC-PPS 2017. Antimicrob. Resist. Infect. Control 2020, 9, 13:1–13:13. [Google Scholar] [CrossRef] [Green Version]
  23. David, S.; Reuter, S.; Harris, S.R.; Glasner, C.; Feltwell, T.; Argimon, S.; Abudahab, K.; Goater, R.; Giani, T.; Errico, G.; et al. Epidemic of carbapenem-resistant Klebsiella pneumoniae in Europe is driven by nosocomial spread. Nat. Microbiol. 2019, 4, 1919–1929. [Google Scholar] [CrossRef]
  24. Bírošová, L.; Kislíková, K.; Lépesová, K. Antibiotic resistant coliforms: From human gut to wastewater. In Nutrients, Wastewater and Leachate: Testing, Risks and Hazards; Amimul, A., Ed.; Nova Publishers: New York, NY, USA, 2018; ISBN 978-1-53613-949-5. [Google Scholar]
  25. Lépesová, K.; Olejníková, P.; Mackuľak, T.; Cverenkárová, K.; Krahulcová, M.; Bírošová, L. Hospital Wastewater—Important Source of Multidrug Resistant Coliform Bacteria with ESBL-Production. Int. J. Environ. Res. Public Health 2020, 17, 7827. [Google Scholar] [CrossRef]
  26. Bírošová, L.; Lépesová, K.; Grabic, R.; Mackuľak, T. Non-antimicrobial pharmaceuticals can affect the development of antibiotic resistance in hospital wastewater. Environ. Sci. Pollut. Res. 2020, 27, 13501–13511. [Google Scholar] [CrossRef] [PubMed]
  27. Thai-Hoang, L.; Charmaine, N.; Hongjie, C.; Zhu, Y.X.; Hsien, K.T.; Sebastian, B.T.M.; Zhi, Z.; Yew-Hoong, G.K. Occurrences and Characterization of Antibiotic-Resistant Bacteria and Genetic Determinants of Hospital Wastewater in a Tropical Country. Antimicrob. Agents Chemother. 2021, 60, 7449–7456. [Google Scholar] [CrossRef] [Green Version]
  28. Lépesová, K. Výskyt, Štúdium a Možnosti Redukcie Vybraných Baktérií Rezistentných Voči Antibiotikám v Kaloch a Vodách z Čistiarní Odpadových Vôd. Ph.D. Thesis, Slovak University of Technology, Bratislava, Slovakia, 2018. [Google Scholar]
  29. Domínguez, J.R.; González, T.; Palo, P.; Cuerda-Correa, E.M. Fenton + Fenton-like Integrated Process for Carbamazepine Degradation: Optimizing the System. Ind. Eng. Chem. Res. 2012, 51, 2531–2538. [Google Scholar] [CrossRef]
  30. Katouli, M.; Thompson, J.M.; Gündoğdu, A.; Stratton, H.M. Antibiotic Resistant Bacteria in Hospital Wastewaters and Sewage Treatment Plants. In Proceedings of the Science Forum and Stakeholder Engagement: Building Linkages, Collaboration and Science Quality, Brisbane, Australia, 19–20 June 2012; Begbie, D.K., Kenway, S.J., Biermann, S.M., Wakem, S.L., Eds.; Urban Water Security Research Alliance: Brisbane, Australia, 2012. [Google Scholar]
  31. Lépesová, K.; Olejníková, P.; Mackuľak, T.; Tichý, J.; Birošová, L. Annual changes in the occurrence of antibiotic-resistant coliform bacteria and enterococci in municipal wastewater. Environ. Sci. Pollut. Res. 2019, 26, 18470–18483. [Google Scholar] [CrossRef]
  32. Maheshwari, M.; Yaser, N.H.; Naz, S.; Fatima, M.; Ahmad, I. Emergence of ciprofloxacin-resistant extended-spectrum β-lactamase-producing enteric bacteria in hospital wastewater and clinical sources. J. Glob. Antimicrob. Resist. 2016, 5, 22–25. [Google Scholar] [CrossRef] [PubMed]
  33. Lépesová, K.; Mackuľak, T.; Birošová, L. Vplyv odpadovej vody na vznik a šírenie bakteriálnej rezistencie voči antibiotikám. Chem. List. 2017, 111, 374–380. [Google Scholar]
  34. Prado, T.; Silva, D.M.; Guilayn, W.C.; Rose, T.L.; Gaspar, A.M.C.; Miagostovich, M.P. Quantification and molecular characterization of enteric viruses detected in effluents from two hospital wastewater treatment plants. Water Res. 2011, 45, 1287–1297. [Google Scholar] [CrossRef]
  35. Chahal, C.; van den Akker, B.; Young, F.; Franco, C.; Blackbeard, J.; Monis, P. Pathogen and Particle Associations in Wastewater. In Advances in Applied Microbiology; Sariaslani, S., Geoffrey, M.G., Eds.; Academic Press: Cambridge, MA, USA, 2016; Volume 97, pp. 63–119. ISBN 0065-2164. [Google Scholar]
  36. Mandal, P.; Gupta, A.K.; Dubey, B.K. A review on presence, survival, disinfection/removal methods of coronavirus in wastewater and progress of wastewater-based epidemiology. J. Environ. Chem. Eng. 2020, 8, 104317:1–104317:10. [Google Scholar] [CrossRef] [PubMed]
  37. Gonçalves, J.; Koritnik, T.; Mioč, V.; Trkov, M.; Bolješič, M.; Berginc, N.; Prosenc, K.; Kotar, T.; Paragi, M. Detection of SARS-CoV-2 RNA in hospital wastewater from a low COVID-19 disease prevalence area. Sci. Total Environ. 2021, 755, 143226:1–143226:7. [Google Scholar] [CrossRef]
  38. Medema, G.; Heijnen, L.; Elsinga, G.; Italiaander, R.; Brouwer, A. Presence of SARS-Coronavirus-2 RNA in Sewage and Correlation with Reported COVID-19 Prevalence in the Early Stage of the Epidemic in The Netherlands. Environ. Sci. Technol. Lett. 2020, 7, 511–516. [Google Scholar] [CrossRef]
  39. Wang, X.-W.; Li, J.-S.; Guo, T.-K.; Zhen, B.; Kong, Q.-X.; Yi, B.; Li, Z.; Song, N.; Jin, M.; Xiao, W.-J.; et al. Concentration and detection of SARS coronavirus in sewage from Xiao Tang Shan Hospital and the 309th Hospital. J. Virol. Methods 2005, 128, 156–161. [Google Scholar] [CrossRef]
  40. Corpuz, M.V.A.; Buonerba, A.; Vigliotta, G.; Zarra, T.; Ballesteros, F.J.; Campiglia, P.; Belgiorno, V.; Korshin, G.; Naddeo, V. Viruses in wastewater: Occurrence, abundance and detection methods. Sci. Total Environ. 2020, 745, 140910. [Google Scholar] [CrossRef]
  41. Rimoldi, S.G.; Stefani, F.; Gigantiello, A.; Polesello, S.; Comandatore, F.; Mileto, D.; Maresca, M.; Longobardi, C.; Mancon, A.; Romeri, F.; et al. Presence and infectivity of SARS-CoV-2 virus in wastewaters and rivers. Sci. Total Environ. 2020, 744, 140911. [Google Scholar] [CrossRef]
  42. Carraturo, F.; Del Giudice, C.; Morelli, M.; Cerullo, V.; Libralato, G.; Galdiero, E.; Guida, M. Persistence of SARS-CoV-2 in the environment and COVID-19 transmission risk from environmental matrices and surfaces. Environ. Pollut. 2020, 265, 115010:1–115010:6. [Google Scholar] [CrossRef]
  43. Kemp, S.A.; Collier, D.A.; Datir, R.P.; Ferreira, I.A.T.M.; Gayed, S.; Jahun, A.; Hosmillo, M.; Rees-Spear, C.; Mlcochova, P.; Lumb, I.U.; et al. SARS-CoV-2 evolution during treatment of chronic infection. Nature 2021, 592, 277–282. [Google Scholar] [CrossRef]
  44. Ong, S.W.X.; Chiew, C.J.; Ang, L.W.; Mak, T.-M.; Cui, L.; Toh, M.P.H.; Lim, Y.D.; Lee, P.H.; Lee, T.H.; Chia, P.Y.; et al. Clinical and Virological Features of SARS-CoV-2 Variants of Concern: A Retrospective Cohort Study Comparing B.1.1.7 (Alpha), B.1.315 (Beta), and B.1.617.2 (Delta). SSRN Electron. J. 2021. [Google Scholar] [CrossRef]
  45. Wang, J.; Shen, J.; Ye, D.; Yan, X.; Zhang, Y.; Yang, W.; Li, X.; Wang, J.; Zhang, L.; Pan, L. Disinfection technology of hospital wastes and wastewater: Suggestions for disinfection strategy during coronavirus Disease 2019 (COVID-19) pandemic in China. Environ. Pollut. 2020, 262, 114665:1–114665:10. [Google Scholar] [CrossRef] [PubMed]
  46. Zhang, D.; Ling, H.; Huang, X.; Li, J.; Li, W.; Yi, C.; Zhang, T.; Jiang, Y.; He, Y.; Deng, S.; et al. Potential spreading risks and disinfection challenges of medical wastewater by the presence of Severe Acute Respiratory Syndrome Coronavirus 2 (SARS-CoV-2) viral RNA in septic tanks of Fangcang Hospital. Sci. Total Environ. 2020, 741, 140445:1–140445:5. [Google Scholar] [CrossRef] [PubMed]
  47. Achak, M.; Alaoui Bakri, S.; Chhiti, Y.; M’hamdi Alaoui, F.E.; Barka, N.; Boumya, W. SARS-CoV-2 in hospital wastewater during outbreak of COVID-19: A review on detection, survival and disinfection technologies. Sci. Total Environ. 2021, 761, 143192:1–143192:15. [Google Scholar] [CrossRef]
  48. Stavbar, S.; Hrnčič, M.K.; Premzl, K.; Kolar, M.; Turk, S.Š. Sub- and super-critical water oxidation of wastewater containing amoxicillin and ciprofloxacin. J. Supercrit. Fluids 2017, 128, 73–78. [Google Scholar] [CrossRef]
  49. Lado Ribeiro, A.R.; Moreira, N.F.F.; Li Puma, G.; Silva, A.M.T. Impact of water matrix on the removal of micropollutants by advanced oxidation technologies. Chem. Eng. J. 2019, 363, 155–173. [Google Scholar] [CrossRef] [Green Version]
  50. Jaén-Gil, A.; Castellet-Rovira, F.; Llorca, M.; Villagrasa, M.; Sarrà, M.; Rodríguez-Mozaz, S.; Barceló, D. Fungal treatment of metoprolol and its recalcitrant metabolite metoprolol acid in hospital wastewater: Biotransformation, sorption and ecotoxicological impact. Water Res. 2019, 152, 171–180. [Google Scholar] [CrossRef] [PubMed]
  51. Czölderová, M.; Behúl, M.; Filip, J.; Zajíček, P.; Grabic, R.; Vojs-Staňová, A.; Gál, M.; Kerekeš, K.; Híveš, J.; Ryba, J.; et al. 3D printed polyvinyl alcohol ferrate(VI) capsules: Effective means for the removal of pharmaceuticals and illicit drugs from wastewater. Chem. Eng. J. 2018, 349, 269–275. [Google Scholar] [CrossRef]
  52. Verlicchi, P.; Al Aukidy, M.; Zambello, E. What have we learned from worldwide experiences on the management and treatment of hospital effluent?–An overview and a discussion on perspectives. Sci. Total Environ. 2015, 514, 467–491. [Google Scholar] [CrossRef] [PubMed]
  53. Mackuľak, T.; Grabic, R.; Špalková, V.; Belišová, N.; Škulcová, A.; Slavík, O.; Horký, P.; Gál, M.; Filip, J.; Híveš, J.; et al. Hospital wastewaters treatment: Fenton reaction vs. BDDE vs. ferrate(VI). Environ. Sci. Pollut. Res. 2019, 26, 31812–31821. [Google Scholar] [CrossRef]
  54. Bimová, P.; Roupcová, P.; Klouda, K.; Matějová, L.; Staňová, A.V.; Grabicová, K.; Grabic, R.; Majová, V.; Híveš, J.; Špalková, V.; et al. Biochar–An efficient sorption material for the removal of pharmaceutically active compounds, DNA and RNA fragments from wastewater. J. Environ. Chem. Eng. 2021, 9, 105746:1–105746:9. [Google Scholar] [CrossRef]
  55. Tasca, A.L.; Clematis, D.; Stefanelli, E.; Panizza, M.; Puccini, M. Ciprofloxacin removal: BDD anode coupled with solid polymer electrolyte and ultrasound irradiation. J. Water Process Eng. 2020, 33, 101074. [Google Scholar] [CrossRef]
  56. Tasca, A.L.; Clematis, D.; Panizza, M.; Vitolo, S.; Puccini, M. Chlorpyrifos removal: Nb/boron-doped diamond anode coupled with solid polymer electrolyte and ultrasound irradiation. J. Environ. Heal. Sci. Eng. 2020, 18, 1391–1399. [Google Scholar] [CrossRef]
  57. Butor Škulcová, A.; Tamášová, K.; Vojs Staňová, A.; Bírošová, L.; Krahulcová, M.; Gál, M.; Konečná, B.; Janíková, M.; Celec, P.; Grabicová, K.; et al. Effervescent ferrate(VI)-based tablets as an effective means for removal SARS-CoV-2 RNA, pharmaceuticals and resistant bacteria from wastewater. J. Water Process Eng. 2021, 43, 102223. [Google Scholar] [CrossRef]
  58. Kajitvichyanukul, P.; Suntronvipart, N. Evaluation of biodegradability and oxidation degree of hospital wastewater using photo-Fenton process as the pretreatment method. J. Hazard. Mater. 2006, 138, 384–391. [Google Scholar] [CrossRef] [PubMed]
  59. Nielsen, U.; Hastrup, C.; Klausen, M.M.; Pedersen, B.M.; Kristensen, G.H.; Jansen, J.L.C.; Bak, S.N.; Tuerk, J. Removal of APIs and bacteria from hospital wastewater by MBR plus O3, O3 + H2O2, PAC or ClO2. Water Sci. Technol. 2013, 67, 854–862. [Google Scholar] [CrossRef]
  60. Paulus, G.K.; Hornstra, L.M.; Alygizakis, N.; Slobodnik, J.; Thomaidis, N.; Medema, G. The impact of on-site hospital wastewater treatment on the downstream communal wastewater system in terms of antibiotics and antibiotic resistance genes. Int. J. Hyg. Environ. Health 2019, 222, 635–644. [Google Scholar] [CrossRef]
  61. Bagheri, H.; Afkhami, A.; Noroozi, A. Removal of pharmaceutical compounds from hospital wastewaters using nanomaterials: A review. Anal. Bioanal. Chem. Res. 2016, 3, 1–18. [Google Scholar] [CrossRef]
  62. Luo, Y.; Feng, L.; Liu, Y.; Zhang, L. Disinfection by-products formation and acute toxicity variation of hospital wastewater under different disinfection processes. Sep. Purif. Technol. 2020, 238, 116405:1–116405:10. [Google Scholar] [CrossRef]
  63. Vo, H.N.P.; Koottatep, T.; Chapagain, S.K.; Panuvatvanich, A.; Polprasert, C.; Nguyen, T.M.H.; Chaiwong, C.; Nguyen, N.L. Removal and monitoring acetaminophen-contaminated hospital wastewater by vertical flow constructed wetland and peroxidase enzymes. J. Environ. Manag. 2019, 250, 109526:1–109526:9. [Google Scholar] [CrossRef]
  64. Vo, T.-K.-Q.; Bui, X.-T.; Chen, S.-S.; Nguyen, P.-D.; Cao, N.-D.-T.; Vo, T.-D.-H.; Nguyen, T.-T.; Nguyen, T.-B. Hospital wastewater treatment by sponge membrane bioreactor coupled with ozonation process. Chemosphere 2019, 230, 377–383. [Google Scholar] [CrossRef]
  65. Shokoohi, R.; Ghobadi, N.; Godini, K.; Hadi, M.; Atashzaban, Z. Antibiotic detection in a hospital wastewater and comparison of their removal rate by activated sludge and earthworm-based vermifilteration: Environmental risk assessment. Process Saf. Environ. Prot. 2020, 134, 169–177. [Google Scholar] [CrossRef]
  66. Tang, K.; Spiliotopoulou, A.; Chhetri, R.K.; Ooi, G.T.H.; Kaarsholm, K.M.S.; Sundmark, K.; Florian, B.; Kragelund, C.; Bester, K.; Andersen, H.R. Removal of pharmaceuticals, toxicity and natural fluorescence through the ozonation of biologically-treated hospital wastewater, with further polishing via a suspended biofilm. Chem. Eng. J. 2019, 359, 321–330. [Google Scholar] [CrossRef]
  67. Kovalova, L.; Siegrist, H.; von Gunten, U.; Eugster, J.; Hagenbuch, M.; Wittmer, A.; Moser, R.; McArdell, C.S. Elimination of Micropollutants during Post-Treatment of Hospital Wastewater with Powdered Activated Carbon, Ozone, and UV. Environ. Sci. Technol. 2013, 47, 7899–7908. [Google Scholar] [CrossRef] [Green Version]
  68. Echevarría, C.; Valderrama, C.; Cortina, J.L.; Martín, I.; Arnaldos, M.; Bernat, X.; De la Cal, A.; Boleda, M.R.; Vega, A.; Teuler, A.; et al. Techno-economic evaluation and comparison of PAC-MBR and ozonation-UV revamping for organic micro-pollutants removal from urban reclaimed wastewater. Sci. Total Environ. 2019, 671, 288–298. [Google Scholar] [CrossRef]
  69. Moussavi, G.; Fathi, E.; Moradi, M. Advanced disinfecting and post-treating the biologically treated hospital wastewater in the UVC/H2O2 and VUV/H2O2 processes: Performance comparison and detoxification efficiency. Process Saf. Environ. Prot. 2019, 126, 259–268. [Google Scholar] [CrossRef]
  70. Nardi, G.; Feretti, D.; Bracchi, U.; Tanzi, M.L.; Dore, F.; Francesconi, A.; Grottolo, M.; Bragonzi, G.; Perna, M.C.; Monarca, S. Acque reflue ospedaliere. Valutazione di un trattamento di disinfezione con biossido di cloro. Inquinamento 1995, 7, 77–83. [Google Scholar]
  71. Suarez, S.; Lema, J.; Omil, F. Pre-treatment of hospital wastewater by coagulation–flocculation and flotation. Bioresour. Technol. 2009, 100, 2138–2146. [Google Scholar] [CrossRef] [PubMed]
  72. Pereira, C.S.; Kelbert, M.; Daronch, N.A.; Michels, C.; de Oliveira, D.; Soares, H.M. Potential of enzymatic process as an innovative technology to remove anticancer drugs in wastewater. Appl. Microbiol. Biotechnol. 2020, 104, 23–31. [Google Scholar] [CrossRef] [PubMed]
  73. Le Minh Tri, N.; Kim, J.; Giang, B.L.; Al Tahtamouni, T.M.; Huong, P.T.; Lee, C.; Viet, N.M.; Quang Trung, D. Ag-doped graphitic carbon nitride photocatalyst with remarkably enhanced photocatalytic activity towards antibiotic in hospital wastewater under solar light. J. Ind. Eng. Chem. 2019, 80, 597–605. [Google Scholar] [CrossRef]
  74. Serna-Galvis, E.A.; Silva-Agredo, J.; Botero-Coy, A.M.; Moncayo-Lasso, A.; Hernández, F.; Torres-Palma, R.A. Effective elimination of fifteen relevant pharmaceuticals in hospital wastewater from Colombia by combination of a biological system with a sonochemical process. Sci. Total Environ. 2019, 670, 623–632. [Google Scholar] [CrossRef] [PubMed]
  75. Ahmadzadeh, S.; Dolatabadi, M. Removal of acetaminophen from hospital wastewater using electro-Fenton process. Environ. Earth Sci. 2018, 77, 53:1–53:11. [Google Scholar] [CrossRef]
  76. Arslan, A.; Veli, S.; Bingöl, D. Use of response surface methodology for pretreatment of hospital wastewater by O3/UV and O3/UV/H2O2 processes. Sep. Purif. Technol. 2014, 132, 561–567. [Google Scholar] [CrossRef]
  77. Karaolia, P.; Michael, I.; García-Fernández, I.; Agüera, A.; Malato, S.; Fernández-Ibáñez, P.; Fatta-Kassinos, D. Reduction of clarithromycin and sulfamethoxazole-resistant Enterococcus by pilot-scale solar-driven Fenton oxidation. Sci. Total Environ. 2014, 468–469, 19–27. [Google Scholar] [CrossRef] [PubMed]
  78. Mackuľak, T.; Vojs, M.; Grabic, R.; Golovko, O.; Staňová, A.V.; Birošová, L.; Medveďová, A.; Híveš, J.; Gál, M.; Kromka, A.; et al. Occurrence of pharmaceuticals, illicit drugs, and resistant types of bacteria in hospital effluent and their effective degradation by boron-doped diamond electrodes. Mon. Chem. 2016, 147, 97–103. [Google Scholar] [CrossRef]
  79. Ouarda, Y.; Tiwari, B.; Azaïs, A.; Vaudreuil, M.-A.; Ndiaye, S.D.; Drogui, P.; Tyagi, R.D.; Sauvé, S.; Desrosiers, M.; Buelna, G.; et al. Synthetic hospital wastewater treatment by coupling submerged membrane bioreactor and electrochemical advanced oxidation process: Kinetic study and toxicity assessment. Chemosphere 2018, 193, 160–169. [Google Scholar] [CrossRef] [PubMed]
  80. Rajab, M.; Heim, C.; Letzel, T.; Drewes, J.E.; Helmreich, B. Electrochemical disinfection using boron-doped diamond electrode–The synergetic effects of in situ ozone and free chlorine generation. Chemosphere 2015, 121, 47–53. [Google Scholar] [CrossRef] [PubMed]
  81. Vasconcelos, T.G.; Kümmerer, K.; Henriques, D.M.; Martins, A.F. Ciprofloxacin in hospital effluent: Degradation by ozone and photoprocesses. J. Hazard. Mater. 2009, 169, 1154–1158. [Google Scholar] [CrossRef]
  82. Munoz, M.; Garcia-Muñoz, P.; Pliego, G.; Pedro, Z.M.D.; Zazo, J.A.; Casas, J.A.; Rodriguez, J.J. Application of intensified Fenton oxidation to the treatment of hospital wastewater: Kinetics, ecotoxicity and disinfection. J. Environ. Chem. Eng. 2016, 4, 4107–4112. [Google Scholar] [CrossRef] [Green Version]
  83. Miralles-Cuevas, S.; Oller, I.; Pérez, J.A.S.; Malato, S. Removal of pharmaceuticals from MWTP effluent by nanofiltration and solar photo-Fenton using two different iron complexes at neutral pH. Water Res. 2014, 64, 23–31. [Google Scholar] [CrossRef]
  84. Lee, Y.; von Gunten, U. Oxidative transformation of micropollutants during municipal wastewater treatment: Comparison of kinetic aspects of selective (chlorine, chlorine dioxide, ferrateVI, and ozone) and non-selective oxidants (hydroxyl radical). Water Res. 2010, 44, 555–566. [Google Scholar] [CrossRef]
  85. Zhou, Z.; Jiang, J.-Q. Reaction kinetics and oxidation products formation in the degradation of ciprofloxacin and ibuprofen by ferrate(VI). Chemosphere 2015, 119, 95–100. [Google Scholar] [CrossRef] [Green Version]
  86. Mackuľak, T.; Birošová, L.; Bodík, I.; Grabic, R.; Takáčová, A.; Smolinská, M.; Hanusová, A.; Híveš, J.; Gál, M. Zerovalent iron and iron(VI): Effective means for the removal of psychoactive pharmaceuticals and illicit drugs from wastewaters. Sci. Total Environ. 2016, 539, 420–426. [Google Scholar] [CrossRef] [PubMed]
  87. Kosma, C.I.; Lambropoulou, D.A.; Albanis, T.A. Occurrence and removal of PPCPs in municipal and hospital wastewaters in Greece. J. Hazard. Mater. 2010, 179, 804–817. [Google Scholar] [CrossRef]
  88. Lin, A.Y.-C.; Yu, T.-H.; Lin, C.-F. Pharmaceutical contamination in residential, industrial, and agricultural waste streams: Risk to aqueous environments in Taiwan. Chemosphere 2008, 74, 131–141. [Google Scholar] [CrossRef] [PubMed]
  89. Sim, W.-J.; Lee, J.-W.; Lee, E.-S.; Shin, S.-K.; Hwang, S.-R.; Oh, J.-E. Occurrence and distribution of pharmaceuticals in wastewater from households, livestock farms, hospitals and pharmaceutical manufactures. Chemosphere 2011, 82, 179–186. [Google Scholar] [CrossRef]
  90. Gómez, M.J.; Petrović, M.; Fernández-Alba, A.R.; Barceló, D. Determination of pharmaceuticals of various therapeutic classes by solid-phase extraction and liquid chromatography–tandem mass spectrometry analysis in hospital effluent wastewaters. J. Chromatogr. A 2006, 1114, 224–233. [Google Scholar] [CrossRef] [PubMed]
  91. Langford, K.H.; Thomas, K.V. Determination of pharmaceutical compounds in hospital effluents and their contribution to wastewater treatment works. Environ. Int. 2009, 35, 766–770. [Google Scholar] [CrossRef]
  92. Verlicchi, P.; Al Aukidy, M.; Galletti, A.; Petrovic, M.; Barceló, D. Hospital effluent: Investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Sci. Total Environ. 2012, 430, 109–118. [Google Scholar] [CrossRef]
  93. Kovalova, L.; Siegrist, H.; Singer, H.; Wittmer, A.; McArdell, C.S. Hospital Wastewater Treatment by Membrane Bioreactor: Performance and Efficiency for Organic Micropollutant Elimination. Environ. Sci. Technol. 2012, 46, 1536–1545. [Google Scholar] [CrossRef] [PubMed] [Green Version]
  94. Perrodin, Y.; Christine, B.; Sylvie, B.; Alain, D.; Jean-Luc, B.-K.; Cécile, C.-O.; Audrey, R.; Elodie, B. A priori assessment of ecotoxicological risks linked to building a hospital. Chemosphere 2013, 90, 1037–1046. [Google Scholar] [CrossRef]
  95. Lin, A.Y.-C.; Wang, X.-H.; Lin, C.-F. Impact of wastewaters and hospital effluents on the occurrence of controlled substances in surface waters. Chemosphere 2010, 81, 562–570. [Google Scholar] [CrossRef]
Table
Table 1. Basic parameters of wastewater from hospitals and healthcare facilities [9].
Table 1. Basic parameters of wastewater from hospitals and healthcare facilities [9].
Parameters Range of Values
Water qualitypH6–9
Redox potential (mV)850–950
Conductivity (μS·cm−1)300–1000
Chlorides (mg·L−1)80–400
Nitrogen (mg N2·L−1)60–98
NH4 (mg NH4·L−1)10–68
Nitrites (mg NO2·L−1)0.1–0.58
Nitrates (mg NO3·L−1)1–2
PO4 (mg P-PO4·L−1)6–19
Soluble compounds (mg·L−1)120–400
Oils (mg·L−1)50–210
COD (mg·L−1)1350–2480
TOC (mg·L−1)31–180
BOC5/CHSK0.3–0.4
AOX (mg·L−1)0.55–100
MicroorganismsE. coli103–106
Enterococci103–106
Fecal coliforms103–104
Total coliforms105–107
EC50 (Daphnia), TU9.8–117
OrganicsTotal disinfective substances (mg·L−1)2–200
Total antibiotics (mg·L−1)0.03–0.2
Cytostatics (mg·L−1)0.005–0.05
Lipides regulators (mg·L−1)0.001–0.01
Beta-blocators (mg·L−1)0.0004–0.025
Table
Table 2. Composition of wastewater in selected Bratislava healthcare facilities with emphasis on the presence of specific micropollutants (pharmaceuticals and drugs) [9].
Table 2. Composition of wastewater in selected Bratislava healthcare facilities with emphasis on the presence of specific micropollutants (pharmaceuticals and drugs) [9].
Substance DFNsPUNB PetržalkaPolyclinic Ružinov
(ng·L−1)
Caffeine<LOQ<LOQ<LOQ
Cotinine11002806700
Codeine21<LOQ10
Amphetamine<LOQ<LOQ190
Oxycodone<LOQ<LOQ<LOQ
Methamphetamine28251100
MDMA<LOQ<LOQ<LOQ
Norketamine<LOQ<LOQ<LOQ
Mephedrone<LOQ<LOQ<LOQ
Ketamine1829<LOQ
Benzoylecgonine<LOQ<LOQ<LOQ
Tramadol2605102400
Cocaine<LOQ<LOQ<LOQ
LSD<LOQ<LOQ<LOQ
Venlafaxine75<LOQ600
Oxazepam38<LOQ52
Citalopram17347250
Midazolam68018<LOQ
Buprenorphine<LOQ<LOQ<LOQ
EDDP<LOQ<LOQ<LOQ
Methadone<LOQ<LOQ<LOQ
THC-COOH52<LOQ<LOQ
Terbutaline1524020
Atenolol<LOQ160<LOQ
Bisoprolol423205200
Ampicillin<LOQ<LOQ<LOQ
Penicillin V<LOQ<LOQ<LOQ
Clonazepam<LOQ<LOQ<LOQ
Atorvastatin1240294
Flumequine<LOQ<LOQ<LOQ
Metoprolol963102600
Ranitidine31140032
Furosemide450340560
Table
Table 3. Average drug concentrations determined in the effluent from psychiatric hospitals (A, B) and at the effluent of the relevant WWTP [14].
Table 3. Average drug concentrations determined in the effluent from psychiatric hospitals (A, B) and at the effluent of the relevant WWTP [14].
Substance (ng·L−1)Effluent Psych. Hospital ASecondary Effluent from WWTPEffluent Psych. Hospital BSecondary Effluent from WWTP
Clozapine560030050001200
Oxazepam940750290190
Sulpiride2800430980011,000
Quetiapine2000<LOQ50001200
Citalopram6719260160
Carbamazepine88<LOQ160180
Table
Table 4. Technological processes and their combinations in the treatment of wastewater from healthcare facilities [9,51,52,53,55,56,57].
Table 4. Technological processes and their combinations in the treatment of wastewater from healthcare facilities [9,51,52,53,55,56,57].
Treatment ProcessAim
OzonationDisinfection/degradation
ChlorinationDisinfection
Photo-Fenton reactionDisinfection/degradation
Fenton reaction and modificationsDisinfection/degradation
Coagulation—filtration—disinfection Disinfection/degradation
Ozonation/UV radiationDisinfection/degradation
Ozonation/UV radiation/H2O2Disinfection/degradation
Ozonation/UV radiation/H2O2/biological degreeDisinfection/degradation
Septic/anaerobic filterDegradation
Septic/Fenton reactionDisinfection/degradation
Flocculation/activated sludgeDegradation
Anaerobic and aerobic reactor with stabilized biofilmDegradation
Aerobic reactor with stabilized biofilm/ozonationDisinfection/degradation
Activated sludgeDegradation
Activated sludge/chlorinationDisinfection/degradation
Bioreactor—filamentous fungiDegradation
Membrane bioreactor (MBR)Degradation
MBR in combination with sorbents, AOPs, chlorination, catalysisDisinfection/degradation
BDD—boron-doped diamond electrodeDisinfection/degradation
Ferrates (Fe6+)
Anodic Oxidation with solid polymer electrolyte
Ultrasound irradiation		Disinfection/degradation
Disinfection/Degradation
Disinfection/Degradation
Table
Table 5. Monitoring of the occurrence of specific micropollutants in effluents from healthcare facilities after the treatment process.
Table 5. Monitoring of the occurrence of specific micropollutants in effluents from healthcare facilities after the treatment process.
CompoundEffluent Concentration (µg·L−1)Study
Caffeine12.3–42[87]
15.6[88]
12.1–182[89]
<7.2[53]
Carbamazepine0.03–0.07[90]
<0.017–1.7[87]
LOD–0.24[14]
0.7–2.7[91]
0.64–1.2[92]
0.222[93]
0.018–6.08[89]
0.003–0.036[94]
0.163[88]
Citalopram0.019–0.322[14]
47–490[53]
Cocaine0.05[95]
<19[53]
Benzoylecognine (metabolite cocaine)0.029[95]
<7[53]
Codeine0.378[95]
0.01–5.7[90]
0.26–3.2[92]
<2.3–58[53]
6-acetylcodeine<0.002[95]
Diazepam<0.001–0.038[92]
0.069[93]
Ketamine0.206[95]
<4.2–29[53]
Lorazepam0.17–0.79[92]
LOD–0.353[14]
Lidocaine9.133[93]
Methamphetamine0.26[95]
<4.2–1100[53]
Morphine1.24[95]
3.679[93]
6-acetylmorphine<0.0005–0.039[95]
Oxazepam0.186–0.942[14]
1.123[93]
<24–52[53]
Tramadol0.958[14]
260–2400[53]
Venlafaxine0.811[14]
<24–600[53]
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Mackuľak, T.; Cverenkárová, K.; Vojs Staňová, A.; Fehér, M.; Tamáš, M.; Škulcová, A.B.; Gál, M.; Naumowicz, M.; Špalková, V.; Bírošová, L. Hospital Wastewater—Source of Specific Micropollutants, Antibiotic-Resistant Microorganisms, Viruses, and Their Elimination. Antibiotics 2021, 10, 1070. https://0-doi-org.brum.beds.ac.uk/10.3390/antibiotics10091070

AMA Style

Mackuľak T, Cverenkárová K, Vojs Staňová A, Fehér M, Tamáš M, Škulcová AB, Gál M, Naumowicz M, Špalková V, Bírošová L. Hospital Wastewater—Source of Specific Micropollutants, Antibiotic-Resistant Microorganisms, Viruses, and Their Elimination. Antibiotics. 2021; 10(9):1070. https://0-doi-org.brum.beds.ac.uk/10.3390/antibiotics10091070

Chicago/Turabian Style

Mackuľak, Tomáš, Klára Cverenkárová, Andrea Vojs Staňová, Miroslav Fehér, Michal Tamáš, Andrea Bútor Škulcová, Miroslav Gál, Monika Naumowicz, Viera Špalková, and Lucia Bírošová. 2021. "Hospital Wastewater—Source of Specific Micropollutants, Antibiotic-Resistant Microorganisms, Viruses, and Their Elimination" Antibiotics 10, no. 9: 1070. https://0-doi-org.brum.beds.ac.uk/10.3390/antibiotics10091070

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