Supplementary Data For s1

Supplementary Data for:

The relative sensitivity of freshwater species to antimony(III): Implications for water quality guidelines and ecological risk assessments

Maximilian Obinna Obiakora, Matthew Tighea, Zhen Wangb,c, Chigozie Damian

Ezeonyejiakud, Lily Perege, Susan C. Wilsona*

aSchool of Environmental and Rural Science, University of New England, Armidale, NSW,

Australia; bThe Swire Institute of Marine Science and School of Biological Sciences, The University of

Hong Kong, Pokfulam, Hong Kong, China; cCenter for Reservoir and Aquatic Systems Research, Baylor University, Waco, Texas, USA; dDepartment of Zoology, Nnamdi Azikiwe University, PMB 5025, Awka, Anambra, Nigeria eSchool of Science and Technology, University of New England, Armidale, NSW, Australia

*Corresponding author: [email protected]; Tel: +61 2 6773 2789; Fax: +61 2 67733238 Table S1. Summary of acute toxicity data used for Sb(III) species sensitivity distributions

(SSDs). The species name, taxonomic group (taxa), geometric mean lethal or effective concentration (LC50 or EC50) for each dataset are provided. Species with specific toxicity data points and origins are listed in Table S1E.

(A). All species dataset

Species name Taxa EC50/LC50 (µg L- 1) Selenastrum capricornutum Algae 750 Chlorohydra viridissima Invertebrates 1770 Hydra oligactis Invertebrates 1950 Macrobrachium nipponense Crustaceans 2790 Ceriodaphnia dubia Crustaceans 3470 Chironomus tentans Insects 4100 Americamysis bahia Crustaceans 4150 Simocephalus mixtus Crustaceans 4920 Moina macrocopa Crustaceans 8850 Macquaria novemaculeata Fish 13550 Cyprinus carpio Fish 14050 Lumbriculus variegatus Worms 25700 Pimephales promelas Fish 16040 Physa heterostropha Molluscs 16470 Bidyanus bidyanus Fish 18030 Caenorhabditis elegans Worms 20000 Hyalella azteca Crustaceans 21600 Ictalurus punctatus Fish 24600 Gammarus pseudolimnaeus Crustaceans 25700 Oncorhynchus mykiss Fish 25700 Lepomis macrochirus Fish 25800 Tanichthys albonubes Fish 38000 Daphnia magna Crustaceans 45840 Oryzias latipes Fish 173000 Pseudokirchneriella subcapitata Algae 206000

(B). Temperate species dataset

Species name Group/taxa EC50/LC50 (µg L-1) Selenastrum capricornutum Algae 750 Chlorohydra viridissima Invertebrates 1770 Hydra oligactis Invertebrates 1950 Ceriodaphnia dubia Crustaceans 3470 Chironomus tentans Insects 4100 Americamysis bahia Crustaceans 4150 Simocephalus mixtus Crustaceans 4920 Moina macrocopa Crustaceans 8850 Macquaria novemaculeata Fish 13550 Lumbriculus variegatus Worms 14200 Daphnia magna Crustaceans 15080 Pimephales promelas Fish 16040 Physa heterostropha Molluscs 16470 Bidyanus bidyanus Fish 18030 Caenorhabditis elegans Worms 20000 Hyalella azteca Crustaceans 21600 Ictalurus punctatus Fish 24600 Gammarus pseudolimnaeus Crustaceans 25700 Oncorhynchus mykiss Fish 25700 Lepomis macrochirus Fish 25800 Tanichthys albonubes Fish 38000 Oryzias latipes Fish 173000 Pseudokirchneriella subcapitata Algae 206000

(C). Crustaceans-specific dataset

Species Taxa LC50 (µg L-1) Macrobrachium nipponense Crustaceans 2790 Ceriodaphnia dubia Crustaceans 3470 Americamysis bahia Crustaceans 4150 Simocephalus mixtus Crustaceans 4920 Moina macrocopa Crustaceans 8850 Hyalella azteca Crustaceans 21600 Gammarus pseudolimnaeus Crustaceans 25700 Daphnia magna Crustaceans 45840

(D). Fish-specific dataset

Species name Group/taxa LC50 (µg L-1) Macquaria novemaculeata Fish 13550 Cyprinus carpio Fish 14050 Pimephales promelas Fish 16040 Bidyanus bidyanus Fish 18030 Ictalurus punctatus Fish 24600 Oncorhynchus mykiss Fish 25700 Lepomis macrochirus Fish 25800 Tanichthys albonubes Fish 38000 Oryzias latipes Fish 173000 Toxicity data were ranked in ascending order, and percentiles were assigned from the formula i/(N + 1), where i is the rank of the datum in ascending order and N is the total number of data points (Wheeler et al., 2002) Table S1E. Toxicity data of Sb(III) for freshwater species extracted and screened from the ECOTOX database, literature, and unpublished reports for the SSD modelling and categorised per climatic zones.

Species name Group/ taxa Compound CAS number Exposure time (h) E/LC50 (µg L-1) Climatic zone Reference Macquaria Fish Antimony potassium tartrate 28300-74-5 96 13550 Temperate Obiakor et al. novemaculeata (2017) Bidyanus bidyanus Fish Antimony potassium tartrate 28300-74-5 96 18030 Temperate Obiakor et al. (2017) Ictalurus punctatus Fish Antimony trichloride 10025-91-9 96 24600 Temperate TAI- Environmental- Sciences-Inc. (1990) Pimephales Fish Antimony trichloride 10025-91-9 96 21900 Temperate Kimball (1978) promelas Pimephales Fish Antimony trioxide 1309-64-4 96 14400 Temperate Brooke et al. (1986) promelas Pimephales Fish Antimony trioxide 1309-64-4 96 9000 Temperate Tarzwell and promelas Henderson (1960) Pimephales Fish Antimony trioxide 1309-64-4 96 17000 Temperate Brooke et al. (1986) promelas Lepomis Fish Antimony trichloride 10025-91-9 96 25800 Temperate Spehar (1987) macrochirus Cyprinus carpio Fish Antimony trichloride 10025-91-9 96 14050 Temperate Chen and Yang (2007) Oncorhynchus Fish Antimony trioxide 1309-64-4 96 25700 Temperate Brooke et al. (1986) mykiss Tanichthys Fish Antimony potassium tartrate 28300-74-5 48 38000 Temperate Kitamura (1990) albonubes Oryzias latipes Fish Antimony potassium tartrate 28300-74-5 96 173000 Temperate Nam et al. (2009) Chironomus tentans Insects Antimony trichloride 10025-91-9 96 4100 Temperate TAI- Environmental- Sciences-Inc. (1990) Chlorohydra Invertebrates Antimony trichloride 10025-91-9 96 1770 Temperate TAI- viridissima Environmental- Sciences-Inc. (1990) Hydra oligactis Invertebrates Antimony trichloride 10025-91-9 96 1950 Temperate TAI- Environmental- Sciences-Inc. (1990) Caenorhabditis Worms Antimony trichloride 10025-91-9 96 20000 Temperate Williams and elegans Dusenbery (1990) Lumbriculus Worms Antimony trioxide 1309-64-4 96 25700 Temperate Brooke et al. (1986) variegatus Physa Molluscs Antimony trichloride 10025-91-9 96 19100 Temperate TAI- heterostropha Environmental- Sciences-Inc. (1990) Physa Molluscs Antimony trichloride 10025-91-9 96 14200 Temperate TAI- heterostropha Environmental- Sciences-Inc. (1990) Macrobrachium Crustaceans Antimony trichloride 10025-91-9 96 1960 Tropical Yang (2014) nipponense Macrobrachium Crustaceans Antimony trichloride 10025-91-9 96 6750 Tropical Yang et al. (2010) nipponense Macrobrachium Crustaceans Antimony trichloride 10025-91-9 96 1640 Tropical Yang et al. (2010) nipponense Gammarus Crustaceans Antimony trioxide 1309-64-4 96 25700 Temperate Brooke et al. (1986) pseudolimnaeus Americamysis Crustaceans Antimony trioxide 1309-64-4 96 4150 Temperate Syracuse-Research- bahia Corp. (1978) Ceriodaphnia dubia Crustaceans Antimony trichloride 10025-91-9 96 3470 Temperate Spehar (1987) Moina macrocopa Crustaceans Antimony potassium tartrate 28300-74-5 48 8850 Temperate Nam et al. (2009) Simocephalus Crustaceans Antimony potassium tartrate 28300-74-5 24 4920 Temperate Nam et al. (2009) mixtus Daphnia magna Crustaceans Antimony trichloride 10025-91-9 96 12100 Temperate Kimball (1978) Daphnia magna Crustaceans Antimony trioxide 1309-64-4 48 423450 Tropical Khangarot and Ray (1989) Hyalella azteca Crustaceans Antimony trichloride 10025-91-9 96 21600 Temperate TAI- Environmental- Sciences-Inc. (1990) Pseudokirchneriell Algae Antimony potassium tartrate 28300-74-5 72 206000 Temperate Nam et al. (2009) a subcapitata Selenastrum Algae Antimony trioxide 1309-64-4 96 740 Temperate USEPA (1977) capricornutum Selenastrum Algae Antimony trioxide 1309-64-4 96 760 Temperate USEPA (1977) capricornutum

Table S2. Hazardous concentrations 5% and 10% (HC5 and HC10; µg L-1) with 95% confidence intervals (95% CIs) in parenthesis for whole data species sensitivity distribution (SSD) of Sb(III). Model parameters for each parametric fitting approach are also provided. * indicates the best fit model determined by both Shapiro-Francia (SF) test (statistic W’, critical value Z = 1.645 under significant level of 0.05) and the Anderson-Darling (AD) test (statistic AD, critical value AD = 0.752 for log-normal, log-logistic and log-triangular; and critical value AD = 0.757 for Gompertz, Weibull, Fisher-Tippett and Burr type

III, under significance level of 0.05) passed; and corresponding minimum corrected Akaike information criterion (Min-AICc).

Model parameters Goodness of fit Best fit Hazardous concentration (95% CI, µg L-1) Min-AICc SF AD HC5 HC10

Burr type III* b (scale) 10.68 0.26 0.41 -153 781 (580, 1203) 1685 (1323, 2375) c (shape) 43.53 k (shape) 0.15

Fisher-Tippett L (location) 3.87 0.64 0.78 -127 1629 (1165, 2092) 2265 (1684, 2830) s (scale) 0.57

Gompertz µ (location) 4.31 0.18 0.91 -139 603 (411, 864) 1476 (1108, 1952) σ (scale) 0.46

Log-logistic α (location) 4.12 -0.83 0.49 -141 961 (748, 1195) 1843 (1509, 2201) β (scatter) 0.36

Log-normal μ (location) 4.11 -0.76 0.50 -140 1039 (797, 1311) 1801 (1442, 2192) σ (scatter ) 0.60

Log-triangular a (intercept) 2.88 0.20 0.50 -136 1822 (1437, 5507) 2632 (1881, 7299) b (slope) 5.31

Weibull κ (shape) 8.60 -0.94 0.61 -139 603 (410, 863) 1476 (1110, 1945) λ (scale) 4.31

Table S3. Hazardous concentrations 5% and 10% (HC5 and HC10; µg L-1) with 95% confidence intervals (95% CIs) in parenthesis for temperate specific species sensitivity distribution (SSD) of Sb(III). Model parameters for each parametric fitting approach are also provided. * indicates the best fit model determined by both Shapiro-Francia (SF) test (statistic W’, critical value Z = 1.645 under significant level of 0.05) and the Anderson-Darling (AD) test

(statistic AD, critical value AD = 0.752 for log-normal, log-logistic and log-triangular; and critical value AD = 0.757 for Gompertz, Weibull, Fisher-Tippett and Burr type III, under significance level of 0.05) passed; and corresponding minimum corrected Akaike information criterion (Min-AICc).

Model parameters Goodness of fit Best fit Hazardous concentration (95% CI, µg L-1) Min-AICc SF AD HC5 HC10 Burr type III* b (scale) 10.60 -0.26 0.76 -137 976 (706, 1654) 2012 (1548, 3053) c (shape) 66.75 k (shape) 0.10

Fisher-Tippett L (location) 3.89 -0.40 0.91 -113 1609 (1071, 2176) 2247 (1560, 2929) s (scale) 0.54

Gompertz µ (location) 4.30 -0.60 1.36 -119 591 (377, 870) 1459 (1049, 1973) σ (scale) 0.42

Log-logistic α (location) 4.13 -1.57 0.56 -124 944 (670, 1232) 1824 (1390, 2257) β (scatter) 0.33

Log-normal μ (location) 4.12 -1.67 0.62 -121 1023 (714, 1345) 1783 (1326, 2240) σ (scatter) 0.56

Log-triangular a (intercept) 2.88 -0.18 0.45 -121 1822 (1312, 6618) 2632 (1654, 8648) b (slope) 5.31

Weibull κ (shape) 9.47 -1.56 0.90 -119 591 (380, 874) 1459 (1049, 1984) λ (scale) 4.30

Table S4. Hazardous concentrations 5% and 10% (HC5 and HC10; µg L-1) with 95% confidence intervals (95% CIs) in parenthesis for crustaceans-specific species sensitivity distribution (SSD) of Sb(III). Model parameters for each parametric fitting approach are also provided. * indicates the best fit model determined by both Shapiro-Francia (SF) test (statistic W’, critical value Z = 1.645 under significant level of 0.05) and the Anderson-Darling (AD) test

(statistic AD, critical value AD = 0.752 for log-normal, log-logistic and log-triangular; and critical value AD = 0.757 for Gompertz, Weibull, Fisher-Tippett and Burr type III, under significance level of 0.05) passed; and corresponding minimum corrected Akaike information criterion (Min-AICc).

Model parameters Goodness of fit Best fit Hazardous concentration (95% CI, µg L-1) Min-AICc SF AD HC5 HC10 Burr type III b (scale) 3.86 -3.91 0.17 -45.0 1632 (73, 2043) 2103 (210, 2548) c (shape) 7.84 k (shape) 494

Fisher-Tippett* L (location) -15.83 -3.54 0.19 -45.5 1547 (1006, 2131) 2075 (1432, 2752) s (scale) 0.48

Gompertz µ (location) 16.37 -3.29 0.24 -40.3 497 (135, 1085) 1012 (380, 1885) σ (scale) 0.51

Log-logistic α (location) 32.11 -3.05 0.24 -42.4 837 (409, 1387) 1530 (881, 2302) β (scatter) 0.35

Log-normal μ (location) 2.96 -3.38 0.21 -43.0 978 (517, 1527) 1598 (951, 2317) σ (scatter ) 0.59

Log-triangular a (intercept) 3.45 -2.53 0.40 -23.2 4342 (3855, 6067) 5216 (4408, 7101) b (slope) 4.66

Weibull κ (shape) 0.86 -3.29 0.24 -40.3 497 (135, 1084) 1151 (451, 2095) λ (scale) 15900

Table S5. Hazardous concentrations 5% and 10% (HC5 and HC10; µg L-1) with 95% confidence intervals (95% CIs) in parenthesis for fish-specific species sensitivity distribution (SSD) of Sb(III). Model parameters for each parametric fitting approach are also provided. * indicates the best fit model determined by both Shapiro-Francia (SF) test (statistic W’, critical value Z = 1.645 under significant level of 0.05) and the Anderson-Darling (AD) test (statistic AD, critical value AD = 0.752 for log-normal, log-logistic and log-triangular; and critical value AD = 0.757 for Gompertz, Weibull, Fisher-Tippett and Burr type

III, under significance level of 0.05) passed; and corresponding minimum corrected Akaike information criterion (Min-AICc).

Model parameters Goodness of fit Best fit Hazardous concentration (95% CI, µg L-1) Min-AICc SF AD HC HC10 5 Burr type III* 0.30 -49.1 107 12157 (9030, 13210) 65 (65 b (scale) -2.94 63, 119 7.24 06) c (shape) 20.28 k (shape) 470.9

Fisher-Tippett 0.19 660 9 (27 L (location) -29.75 -3.67 -40.7 8307 (4003, 13119) 47, 109 59) s (scale) 0.38

Gompertz 0.19 224 9 µ (location) 25.02 -3.71 -34.3 (13, 4589 (123, 10934) 671 4) σ (scale) 0.43

Log-logistic 0.13 384 1 (58 α (location) 55.01 -4.49 -37.9 6255 (1522, 11858) 5, 832 9) β (scatter) 0.28

Log-normal μ (location) 8.76 -4.16 0.15 -37.4 425 6363 (1257, 12140) 9 (51 4, 903 5) σ (scatter) 0.48

Log-triangular 0.27 202 69 (15 a (intercept) -2.85 -17.0 002 23948 (15649, 27299) , 233 4.13 61) b (slope) 5.24

Weibull 0.19 224 9 κ (shape) 1.01 -3.71 -34.3 (14, 4589 (126, 10905) 679 2) λ (scale) 42645 Table S6. Summary of current water quality guidelines (WQGs) of antimony(Sb) for drinking water and freshwater ecosystems. NA indicates that data is not available.

Water quality guideline (WQG, µg L-1) Country/ region Drinking Freshwater Type/ valency Remark Reference Australia and New 3 9 Sb(III) Low ANZECC-and-ARMCANZ (2000) Zealand reliability freshwate r Sb value for indicative interim working level. Value derived for Sb(III)

Canada 6 NA Sb CCME (2014)

China 5 NA Sb China-Drinking-Water-Standard (2007)

Europe 5 NA Sb (EC-Surface-Water-Regulations 2009; EU-Drinking-Water-Regulations 2014)

Ireland 5 NA Sb Parametri EPAI (2001) c value (PQ). Antimon y levels limited under Drinking Water Directive (98/83/E C)

Japan 15 NA Sb Interim Ministry-of-Health-Labour-and-Welfare value for (2004) Sb; complim entary item value to set the targets for water quality managem ent

Jordan 5 NA Sb JISM (2001)

Lebanon 10 300 Sb Maximu Lebanese-Ministry-of-Environment m limit (2001); WHO (2006) for wastewat er discharge into inland surface water

Palestine 5 NA Sb Adopted WHO (2006) from WHO and Jordanian standards

South Africa <10& NA Sb Guideline DWAF (2005) derived for health associate d with drinking water 10-50^

Sudan 4 NA Sb WHO (2006)

Syrian Arab 5 NA Sb WHO (2006) Republic

USA 30# Sb(III) Guideline USEPA (1988) values for protectio n of freshwate r derived for Sb(III) 88* Manitoba, Canada 6 Sb Maximu Manitoba-Water-Stewardship (2011) m Acceptab le Concentr ation for surface or ground water for drinking

Ontario, Canada 20 Sb Interim Ontario-Ministry-of-the-Environment Provincia (1994) l Water Quality Objective s (PWQO’ s) to protect aquatic life and recreatio n uses but still under developm ent

Colorado, USA 6 NA Sb Chronic Colorado-Water-Quality-Control (2013) value for domestic water supply

Connecticut, USA 5.6 NA Sb Guideline Connecticut-Department-of- for Sb in Environmental-Protection (2011) drinking water Indiana, USA 6 NA Sb Guideline Indiana-Government (1996) for Sb in drinking water

Minnesota, USA 5.5* Guideline Minnesota-Pollution-Control-Agency s derived (2008) for total Sb in Class 2A waters; aquatic life and recreatio n 90$ 180# New York, USA 3 NA Sb Drinking New-York-State-Department-of- water Environmental-Conservation (1998) guideline for total Sb

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