Evaluating sewer exfiltration in groundwater by pharmaceutical tracers after the 2016 Kumamoto earthquakes, Japan
Graphical Abstract
Introduction
Groundwater is an important drinking water resource globally; thus, its conservation is vital. Sewer systems are a crucial part of water quality conservation and hygiene, and maintenance and replacement of old sewer pipes are required to prevent contamination of groundwater through sewage leakage from sewer pipes, a process called sewer exfiltration (Reynolds and Barrett, 2003, Roehrdanz et al., 2017).
Major earthquakes, which measure more than magnitude (M) 7, occur frequently in East Asia, including Japan, China, and Indonesia. In April 2016, a series of earthquakes (M 7.3 on the Japan Meteorological Agency scale) occurred in Kumamoto Prefecture in southwestern Japan, killing at least 50 people and causing serious damage to buildings, fields, and social infrastructure, including water supply and sewerage systems. Changes in the groundwater level and flow rate of spring water in the area were observed after the earthquakes (Hosono et al., 2018, Ide et al., 2020, Kagabu et al., 2020). Furthermore, 2.1% of sewer pipes (52 km of a total of 2544 km) in Kumamoto City were damaged, and breakages, cracks, and slack were found (Civil Engineering Department, Kumamoto Prefecture, 2017). Although most of the damaged sewer pipes were repaired within about a month (Kumamoto City Waterworks and Sewage Bureau, 2016), potential contamination of groundwater by sewer exfiltration has been a great concern because almost 100% of the drinking water originates from groundwater in the Kumamoto area. Evaluating the change in sewer exfiltration after a major earthquake would provide important insights into the extent of sewage contamination in groundwater.
To evaluate sewer exfiltration in groundwater, contaminants of emerging concern (CEC) have been proposed as tracers (McCance et al., 2018), including pharmaceuticals such as carbamazepine and crotamiton (Kuroda et al., 2012, Nakada et al., 2008, Ruzicka et al., 2011), perfluoroalkyl acids (Kuroda et al., 2014), artificial sweeteners (Buerge et al., 2009, Tran et al., 2014), and anthropogenic gadolinium (hereafter, Gd-anth), which is used as a contrast media for magnetic resonance imaging (Brünjes et al., 2016, Kuroda et al., 2016). Tryptophan-like fluorescent dissolved organic matter has also been suggested as a tracer (Roehrdanz et al., 2017). Regional-scale sewer exfiltration rates have been reported in Tokyo, Japan (Kuroda et al., 2012), Leipzig, Germany (Musolff et al., 2010), and Nottingham, UK (Yang et al., 1999) based on these tracers. Suitable tracers may differ by region (Kahle et al., 2009), and thus multiple tracers are more useful than a single tracer for assessing groundwater pollution. In addition, these previous studies were performed in urban areas, and sewer exfiltration in areas with paddies has not been studied. In the Kumamoto area, irrigation water for paddies is important in recharging groundwater, and thus the input of tracers from irrigation, which originate from river water, must be considered to estimate the exfiltration rate precisely. Furthermore, long-term monitoring of tracers in groundwater is important for tracking groundwater pollution, especially after an earthquake. However, there are few long-term studies of CECs in groundwater (Drewes et al., 2003, Ternes et al., 2007).
In this study, we evaluated sewer exfiltration in groundwater in the Kumamoto area based on long-term monitoring of multiple tracers after the 2016 Kumamoto earthquakes. We used 14 pharmaceuticals, Gd-anth, and tryptophan-like fluorescence as tracers, and seasonally investigated concentrations of these tracers as well as general water quality parameters from September 2016 to November 2017. To our knowledge, this is the first study of multiple pharmaceuticals in groundwater affected by major earthquakes.
Section snippets
Site description
Kumamoto Prefecture is located in the center of Kyushu, the southernmost of Japan’s four main islands. The Kumamoto groundwater area consists of 11 municipalities, including Kumamoto City (Fig. 1), which has a population of about 970,000. The area (945 km2) has rich groundwater resources, which are the main source of water for domestic, industrial, and agricultural uses. Almost 100% of the area’s drinking water comes from groundwater; the daily abstraction for the domestic water supply is
Concentrations of tracers in groundwater
Twelve of the 14 pharmaceuticals were detected in the groundwater samples (n = 97). The concentrations of the 14 pharmaceuticals and Gd-anth are listed in Table S3. Here, we discuss the labile markers (caffeine and ibuprofen) and reliable markers (carbamazepine, crotamiton, and Gd-anth). The detection frequency of caffeine (38/97), carbamazepine (34/97), crotamiton (44/97), and ibuprofen (28/97) in the groundwater samples ranged from 29% to 45% (Table S3). Gd (86/97 samples) was detected in
Conclusions
We investigated sewer exfiltration by using persistent pharmaceuticals and Gd-anth as tracers after the 2016 Kumamoto earthquakes. At an attenuation rate of 80% for recharge from paddy fields, the sewer exfiltration rates in September 2016 estimated using carbamazepine, crotamiton, and Gd-anth were 0.59 ± 0.27%, 0.66 ± 0.47%, and 0.11 ± 0.18% of sewage dry weather flow, respectively. These results show that the sewer exfiltration was small after the Kumamoto earthquakes owing to the quick
CRediT authorship contribution statement
Jun Kobayashi: Investigation, Data curation, Formal analysis, Writing - original draft. Keisuke Kuroda: Conceptualization, Investigation, Writing - review & editing, Supervision. Chinatsu Miyamoto: Investigation. Yukiko Uchiyama: Investigation. Kenshi Sankoda: Investigation, Writing - review & editing. Daisuke Nakajima: Supervision.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
Part of this study was supported by the Kurita Water and Environment Foundation, Japan (16B051, 17K002, and 19B078). The authors thank Yuko Kitazaki, Ichiro Fuchigami, Maki Miyagawa, Mana Furukawa, Kento Ikeda, and Ryousuke Nakamura of the Prefectural University of Kumamoto for their support with sampling. The authors are grateful to Professors Haruhiko Nakata and Takahiro Hosono of Kumamoto University for their guidance on the sampling in Kumamoto City. The authors thank the staff at the
References (65)
- et al.
Anthropogenic origin of positive gadolinium anomalies in river waters
Earth Planet. Sci. Lett.
(1996) - et al.
Sorption and biodegradation of organic micropollutants during river bank filtration: a laboratory column study
Water Res.
(2014) - et al.
Anthropogenic gadolinium in freshwater and drinking water systems
Water Res.
(2020) - et al.
Anthropogenic gadolinium as a transient tracer for investigating riverbank filtration
Sci. Total Environ.
(2016) - et al.
Carbamazepine as a possible anthropogenic marker in the aquatic environment: investigations on the behavior of carbamazepine in wastewater treatment and during groundwater infiltration
Water Res.
(2004) - et al.
The use of δ15N and δ18O tracers with an understanding of groundwater flow dynamics for evaluating the origins and attenuation mechanisms of nitrate pollution
Water Res.
(2013) - et al.
Elimination of COD, microorganisms and pharmaceuticals from sewage by trickling through sandy soil below leaking sewers
Water Res.
(2003) - et al.
Changes of groundwater flow systems after the 2016 Mw 7.0 Kumamoto earthquake deduced by stable isotopic and CFC-12 compositions of natural springs
J. Hydrol.
(2020) - et al.
Acesulfame as a suitable sewer tracer on groundwater pollution: a case study before and after the 2016 Mw 7.0 Kumamoto earthquakes
Sci. Total Environ.
(2021) - et al.
Groundwater age determination using 85Kr and multiple age tracers (SF6, CFCs, and 3H) to elucidate regional groundwater flow systems
J. Hydrol. Reg. Stud.
(2017)
Describing coseismic groundwater level rise using tank model in volcanic aquifers, Kumamoto, southern Japan
J. Hydrol.
Investigating sources and pathways of perfluoroalkyl acids (PFAAs) in aquifers in Tokyo using multiple tracers
Sci. Total Environ.
Pepper mild mottle virus as an indicator and a tracer of fecal pollution in water environments: comparative evaluation with wastewater-tracer pharmaceuticals in Hanoi, Vietnam
Sci. Total Environ.
Occurrence and distribution of pharmaceutical and personal care products, artificial sweeteners, and pesticides in groundwater from an agricultural area in Korea
Sci. Total Environ.
Pan-European survey on the occurrence of selected polar organic persistent pollutants in ground water
Water Res.
The impact of variable temperatures on the redox conditions and the behaviour of pharmaceutical residues during artificial recharge
J. Hydrol.
Contaminants of emerging concern as novel groundwater tracers for delineating wastewater impacts in urban and peri-urban areas
Water Res.
Removal of selected pharmaceuticals and personal care products (PPCPs) and endocrine-disrupting chemicals (EDCs) during sand filtration and ozonation at a municipal sewage treatment plant
Water Res.
Positive gadolinium anomalies in wastewater treatment plant effluents and aquatic environment in the Hérault watershed (South France)
Chemosphere
Mobility of pharmaceuticals carbamazepine, diclofenac, ibuprofen, and propyphenazone in miscible-displacement experiments
J. Contam. Hydrol.
Irrigation of treated wastewater in Braunschweig, Germany: an option to remove pharmaceuticals and musk fragrances
Chemosphere
Suitability of artificial sweeteners as indicators of raw wastewater contamination in surface water and groundwater
Water Res.
Impacts of land use on surface waters at the watershed scale in southeastern China: insight from fluorescence excitation-mission matrix and PARAFAC
Sci. Total Environ.
The nonparametric Behrens‐Fisher problem: asymptotic theory and a small‐sample approximation
Biom. J.
Ubiquitous occurrence of the artificial sweetener acesulfame in the aquatic environment: an ideal chemical marker of domestic wastewater in groundwater
Environ. Sci. Technol.
Fate of trace organic compounds during vadose zone soil treatment in an onsite wastewater system
Environ. Toxicol. Chem.
Fate of pharmaceuticals during ground water recharge
Ground Water Monit. Remediat.
Quantification of sewer exfiltration using the anti-epileptic drug carbamazepine as marker species for wastewater
Water Sci. Technol.
Sorption and biodegradation characteristics of the selected pharmaceuticals and personal care products onto tropical soil
Water Sci. Technol.
Cited by (9)
The telltale fluorescence fingerprints of sewer flows for interpreting the low influent concentration in wastewater treatment plant
2024, Journal of Environmental ManagementAquifer heterogeneity controls to quality monitoring network performance for the protection of groundwater production wells
2022, Water ResearchCitation Excerpt :However, despite these measures, waterborne outbreaks are regularly reported in North America, Europe and elsewhere (Moreira and Bondelind 2016; Onyango et al. 2015), indicating that testing the production well alone does not provide sufficient warning for mitigation actions to be successful. Furthermore, in areas of significant seismic activity and following large earthquake events, groundwater is prone to pollution from damaged wastewater infrastructure (Ishii et al. 2021; Kang et al. 2013; Kobayashi et al. 2021; Sarikaya and Koyuncu 1999) and changes to the permeability of aquifer and aquitards (Elkhoury et al. 2006; Zhang et al. 2019; Liu et al. 2010), that may affect groundwater quality and safety (Nakagawa et al. 2021; Wang et al. 2016; Wang et al. 2004). A common protective measure is to restrict the land use surrounding supply wells (USEPA 1987), however complete restriction is often impractical or impossible (particularly in urban areas), and the full extent of the well capture zone is almost always uncertain (Frind and Molson 2018).
Occurrence and point-of-use treatment of contaminants of emerging concern in groundwater of the Nzoia River basin, Kenya
2022, Environmental PollutionCitation Excerpt :Recently, the use of PhACs as tracers for wastewater contamination has attracted increased attention (Lim et al., 2017). In this regard, carbamazepine has been considered as a viable candidate (Cary et al., 2013; Gasser et al., 2011; Kobayashi et al., 2021). Given that carbamazepine was detected at concentrations being one order of magnitude lower than in wastewater (K'oreje et al., 2018), this suggests that it could be an applicable tracer of groundwater contamination through wastewater in the area.
Occurrence, source apportionment and potential risks of selected PPCPs in groundwater used as a source of drinking water from key urban-rural settings of Pakistan
2022, Science of the Total EnvironmentCitation Excerpt :Thus, PC2 can highly suggest domestic sewage sources. As carbamazepine is a well-known pharmaceutical tracer compound for sewage exfiltration in groundwater (Ishii et al., 2021; Kobayashi et al., 2021). PC3 was associated with high loading of diclofenac signifying the potential source could be animal husbandry/livestock in rural areas.
Fate and transport of pharmaceuticals and personal care products in soils and groundwater
2022, Emerging Contaminants in Soil and Groundwater Systems: Occurrence, Impact, Fate and TransportThe rapid survey method of chemical contamination in floods caused by Typhoon Hagibis by combining in vitro bioassay and comprehensive analysis
2022, Environment InternationalCitation Excerpt :Therefore, determining the levels of chemical pollution after a disaster is important to protect the health of disaster victims and to support the restoration activities carried out by volunteers. In fact, the importance of risk assessments based on chemical approaches, such as chemical analysis and bioassays, in disaster-hit areas has been recently suggested by a number of studies (Frogner-Kockum et al., 2020; Kobayashi et al., 2021; Ponting et al., 2021; Crawford et al., 2022). However, a rapid evaluation system for environmental pollution and the human health risk posed by chemicals after a disaster has not yet been established.