potential risk of bpa and phthalates in commercial water bottles : a minireview rouse da silva costa, tatiana sainara maia, edmilson de sousa almeida, juliene tome oliveira and ronaldo ferreira do nascimento abstract the global water bottling market grows annually. today, to ensure consumer safety, it is important to verify the possible migration of compounds from bottles into the water contained in them. potential health risks due to the prevalence of bisphenol a ( bpa ) and phthalates ( paes ) exposure through water bottle consumption have become an important issue. bpa, benzyl butyl phthalate ( bbp ), di - n - butyl phthalate ( dbp ) and di ( 2 - ethylhexyl ) phthalate ( dehp ) can cause adverse effects on human health. papers of literature published in english, with bpa, bbp, dbp and dehp detections during 2017, by 2019 by liquid chromatography and gas chromatography analysis methods were searched. the highest concentrations of bpa, bbp, dbp and dehp in all the bottled waters studied were found to be 5. 7, 12. 11, 82. 8 and 64. 0 μg / l, respectively. dbp was the most compound detected and the main contributor by bottled water consumption with 23. 7 % of the tdi. based on the risk assessment, bpa, bbp, dbp and dehp in commercial water bottles do not pose a serious concern for humans. the average estrogen equivalente level revealed that bpa, bbp, dbp and dehp in bottled waters may induce adverse estrogenic effects on human health. key words | bisphenol a, estrogenic effects, phthalates, risk assessment, water bottles highlights • dbp was the most compound @topic:1


##ates, risk assessment, water bottles highlights • dbp was the most compound detected. • an estimated intake of bpa, bbp, dbp and dehp was far below their tdis. • the risk assessment of bpa, bbp, dbp and dehp does not raise serious concern for humans. • the average estrogen equivalente level for bpa, bbp, dbp and dehp may induce adverse estrogenic effects on human health. • bpa, bbp, dbp and dehp in bottled water need more accurate data to avoid their effects on human health. rouse da silva costa tatiana sainara maia ( corresponding author ) edmilson de sousa almeida juliene tome oliveira ronaldo ferreira do nascimento department of analytical chemistry and physical chemistry, federal university of ceara, r. humberto monte s / n, 60455700 fortaleza, ce, brazil e - mail : tatisainara @ yahoo. com. br this is an open access article distributed under the terms of the creative commons attribution licence ( cc by 4. 0 ), which permits copying, adaptation and redistribution, provided the original work is properly cited ( http : / / creativecommons. org / licenses / by / 4. 0 / ). 1 © 2021 the authors journal of water and health | in press | 2021 doi : 10. 2166 / wh. 2021. 202 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest graphical abstract introduction reports show that, in 2018, 64 % of produced bottles has made of polyethylene terephthalate ( pet ), 34 % of high - den - @topic:1


##ephthalate ( pet ), 34 % of high - den - sity polyethylene ( hdpe ), 1. 8 % of polypropylene and 1 % other ( polycarbonate ( pc ) included here ) ( acc ). according to the american chemistry council ( acc ), in 2018, 0. 31 million pounds of postconsumer pc bottles were collected for recycling. pet and hdpe continued to dominate as selected resins to produce plastic bottles ( 97. 1 % by weight of produced bottles has made of pet or hdpe ) ( acc ). the bottled water industry is a phenomenon in practi - cally every region of the world. first, the bottled water became a mainstream commercial beverage category in western europe and later grew into a truly global beverage ( ibwa ). the bottled industry produces mainly two types of packaged water : packaged natural mineral drinking water and packaged drinking water. the last is water derived from any source of a potable water ( ground, well, bore well water, etc. ), which must be subjected to different treatment processes such as ﬁltration, aeration, decantation, and reverse osmosis ( jain et al. ). in 2018, for the ﬁrst time, global bottled water consumption has surpassed that 100 billion gallons is estimated to, and the per capita con - sumption exceeded 42 gallons ( 158, 987 liters ). it should be stressing that per capita consumption by individual regions or countries can differ from the global average ( ibwa ). in 2018, the rank of the 10 leading countries ’ con - sumption was china, united states, mexico, indonesia, brazil, india, thailand, germany, italy and france, respect - ively ( ibwa ). in 2018, approximately 7. 7 % ( 27. 64 million tons out of the total plastic production of 359 @topic:1


( 27. 64 million tons out of the total plastic production of 359 million tons ) of the plastic demand was constituted by pet worldwide was used in bot - tles for water, soft drinks, juices, and cleaners ( plastics europe ). pet is the packaging most used in water bot - tles ( coniglio et al. ). pet and pc as the packing materials have been widely used for chinese bottled water ( wang et al. ). bisphenol a ( bpa ), benzyl butyl phthalate ( bbp ), di - n - butyl phthalate ( dbp ) and di ( 2 - ethylhexyl ) phthalate ( dehp ) have recently been detected in commercial water bottles raising concerns and discussions on possible risks for human health ( dada et al. ; pinsrithong & bunkoed ; karayaka et al. ; wu et al. ). many countries included bpa, bbp, dbp and dehp in the priority list of pollutants ( pignotti et al. ; goeury et al. ; li et al. ; fard et al. ). acceptable exposure levels for these compounds have been creating to protect human health ( celic´ et al. ; fard et al. ). the maximum contami - nant level ( mcl ) is the highest level of a contaminant that is allowed in drinking water ( us epa ). the mcl for drinking water for bpa, bbp, dbp and dehp is in the sec - tion ‘ extraction techniques for detection ’. according to hassan et al. ( ), bpa and paes exhibit similar toxicogenomics and health effects. how bpa and paes are not bound to the matrix, they can leach out into 2 r. da silva costa et al @topic:1


matrix, they can leach out into 2 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest the surroundings by delicate changes in the environment, like temperature, ph and pressure alterations ( hassan et al. ). the regulation ( eu ) no. 10 / 2011 ( ec ) deﬁnes the speciﬁc migration limit ( sml ) as the maximum permitted amount of a given substance released from a material or article into food or food simulants. the sml values by the eu for bbp, dbp and dehp are 30, 0. 3 and 1. 5 mg / kg, respectively ( efsa ). the detection of very low bpa, bbp, dbp and dehp in water can be carry out by high - performance liquid ( hplc ) and gas ( gc ) chromatography ( gorji et al. ; karayaka et al. ; li et al. ; yin et al. ). the detection power can be improved by preconcentrating analytes before instru - mental measurement and the type of detector ( kumar et al. ; chang et al. 2019 ; farajzadeh et al. ; karayaka et al. ; li et al. ). in this context, due to the increasing popularity of bottled water consumption, the potential health effects of possible migration of chemical compounds from the bottles into the water can pose a health risk to consumers. the pur - pose of this minireview is to verify if recent @topic:1


the pur - pose of this minireview is to verify if recent bpa, bbp, dbp and dehp detections in commercial water bottles around the world using hplc and gas gc may pose a risk to human health. papers of literature published in english, that detected bpa and paes ( bbp, dbp and dehp ) in commercial bot - tles during 2017, by 2019 were searched. papers with storage studies were also taken into account. for data sources for further analysis were identiﬁed a total of 41 pub - lications from 17 countries. pc bottles were not considered. thus, this work hopes to aid decision - making in future research focusing on bpa, bbp, dbp and dehp in com - mercial water bottles using hplc and gc. moreover, this review hopes to avoid consumer exposure to these chemi - cals and to guarantee consumer safety. bpa and paes in pet bottled water the production process of water bottles uses pc plastics containing bpa ( antioxidant or monomer ) ( alfarhani et al. ; fikarova et al. ; liu et al. ). although bpa is not used in the manufacture of pet, it should consider the use of recycled pet ( r - pet ) as a possible source of bpa coming from cross - contamination, not only during the recy - cling process but also during the manufacture of virgin pet ( dreolin et al. ). bpa leachable from polymer packaging due to its moderate water solubility ( 120 – 300 mg / l : ph 7. 0 at 25 c ) and low log kow ( 3. 32 ) in water ( borrirukwisitsak et al. ; fikarova et al. ). guart et al. ( ) not detected bpa in pet @topic:1


). guart et al. ( ) not detected bpa in pet bottles cut in pieces, but on the other hand, detected bpa in hdpe caps at concentrations of 0. 145 μg / dm2. bach et al. ( ) also indicated that the containers ’ caps, in pet bottled water, could be a source of bpa. the manufacturing of beverage bottles widely uses paes ( li et al. ) and like they are not chemically bound to polymers, they may also enter drinking samples. this process can occur through the production, packaging and storage ( bottling lines and water reﬁnement centers ) ( manzo et al. ; pacyga et al. ). according to bach et al. ( ), background pollution, as a source of paes, cannot be excluded. paes ’ presence in pet bottled water can be associated with paes in the source of water ( groundwater or tap water ) used to ﬁll in the bottles ( jeddi et al. ). the type of closure ( ‘ cap ’ ) on the bottles could be a more important source of paes than the bottle material ( glass or pet ) ( efsa ). the caps of plastic bottles are made of high - and low - density polyethylene ( hdpe and ldpe ) and polystyrene ( ps ) ( guart et al. ). guart et al. ( ) identiﬁed bpa in hdpe, ldpe and ps plastics. the adhesive used for sticking the bottle labels could thus be considered one of the sources of paes in water samples ( cincotta et al. ). aznar et al. ( ) identiﬁed dbp and dehp in adhesive based on vinyl acetate - ethylene. paes are hydrophobic organic compounds under normal conditions ( 25 c ) @topic:1


. paes are hydrophobic organic compounds under normal conditions ( 25 c ), very insoluble in water ( bbp : 2. 69 mg / l, dbb : 11. 2 mg / l and dehp : 0. 27 mg / l ) and have a particular afﬁnity for fats and alcohols ( grinbaum et al. ; pubchem ). however, exposure to these low levels in water may also cause signiﬁcant risks to humans under long - term chronic exposure by resulting in a considerable total health risk ( abtahi et al. ; chen et al. a ; abdelghani et al. ). exposure to that low level can cause problems such as spasms in arms and legs, bronchial obstruction in children, irritation of the eyes and endocrine disruption ( abdelghani et al. ). 3 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest chromatographic and extraction techniques for detection chromatographic techniques for detection a wide range of methods analyzes bpa and paes. the liquid chromatography ( lc ) and gas chromatography ( gc ) analysis methods for detection and respective extraction techniques used for the determination in commercial water bottles are presented in table 1. the choice of the detector and extraction inﬂuences the detection limit ( lod ) and the quantiﬁcation limit ( loq ) values obtained. hplc coupled with diode - array detection ( hplc – dad ) @topic:1


hplc coupled with diode - array detection ( hplc – dad ) was the most used in bpa detections. hplc is ade - quate for the analysis of bpa since it is a relatively polar compound. the dad detector allows simultaneous collec - tion of chromatograms over a range of wavelengths during a single run, providing more information on sample compo - sition than is provided by the use of a single wavelength detector ( waksmundzka - hajnos & sherma ). dad is preferable since it is sufﬁciently selective for compound identiﬁcation ( mcgowin ). gc coupled with mass spectrometry ( gc – ms ) was the most used technique in paes detections. gc can separate volatile and semi - volatile compounds with high resolution, and its combination with ms can identify them, providing detailed structural information on most compounds such that they can go identiﬁed correctly ( hussain & maqbool ). only karayaka et al. ( ) analyzed bpa by gc – ms and derivatization is not used. bpa has volatility and thermal stability suitable for detection and quantiﬁcation by gc – ms. however, derivatization can improve the sensi - tivity, selectivity and performance of the chromatographic properties ( nollet ). bpa analysis underivatized by gc – ms can be found in the literature because sensitivity can be improved using pre - concentration and liquid – liquid extraction ( oca et al. ). karayaka et al. ( ) used the sslme to preconcentrate bpa and improving the detection power of gc – ms. micro - extraction methods are eco - friendly because they use too small quantities of chemicals, no compromising extraction e @topic:1


friendly because they use too small quantities of chemicals, no compromising extraction efﬁciency and agree with green chemistry ( armenta et al. ). extraction techniques for detection the sample preparation has been considered as the achilles ’ heel ( fumes et al. ). matrix - related compounds can be co - extracted and can interfere in the analysis ; so, the sample preparation has a multifarious role related to target analyte extraction, preconcentration and cleanup from co - existing species ( gao et al. ). a preconcentration step is usually necessary before the ﬁnal analysis of compounds ( gao et al. ; feizi et al. ). however, some methods often require high amounts of organic solvents that are harmful to the environment ( gao et al. ; feizi et al. ; płotka - wasylka et al. ). a concept that has been approached is the green analytical chemistry, which decreases or eliminates organic solvents during the extrac - tion procedure ( fumes et al. ; płotka - wasylka et al. ). karayaka et al. ( ) developed a method to extract bpa from drinking water bottles using a switchable polarity solvent ( n, n - dimethylbenzylamine ), which is a green sol - vent. also, it very important to use a proper sample preparation to reach the required lower lods ( gao et al. ). discoveries in materials science may supply new tools for the preparation of samples ( jalili et al. ). mohammadnezhad et al. ( ) developed ionic liquid - bonded fused silica as a new solid - phase microextraction ( spme ) ﬁber for the liquid chromatographic determination of bpa in mineral water bottled in pet. wei et al. ( ) syn - thesized @topic:1


bottled in pet. wei et al. ( ) syn - thesized a novel magnetic solid - phase extraction ( mspe ) for the determination of six phthalic acid esters in mineral water ( including bbp, dbp and dehp ). the development of natural sorbents has also been investigated, which are cheap and readily available and sometimes their perform - ance was comparable with synthetic sorbents ( sajid et al. ). some works in table 1 developed extraction methods. gonzalez - salamo et al. ( ) used the ﬁrst application of core – shell poly ( dopamine ) magnetic nanoparticles as a sorbent for the extraction of a group of 11 phthalic acid esters of interest. pinsrithong & bunkoed ( ) syn - thesized a hierarchically porous composite nanostructure of polypyrrole, reduced graphene oxide, magnetite nano - particles and alginate hydrogel microspheres ( ppy - rgox - fe3o4 ). they applied as a magnetic solid - phase extraction 4 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest table 1 | extraction methods for the determination of bpa, bbp, dbp and dehp in commercial water bottles without migration study detected analyte ( s ) extraction method chromatographic technique lods ( μg / l ) loqs ( μg / l ) reference bpa spe uflc – ms / ms 0. 00 @topic:1


reference bpa spe uflc – ms / ms 0. 004 – 0. 055a 1. 4 × 102 – 1. 2 × 102a zhou et al. ( ) bpa sbse hplc – uv / vis 0. 02 0. 06 gorji et al. ( ) bpa usae - mip - μ - spe hplc – dad 0. 07 0. 15 rozaini et al. ( ) bpa mdmip - spe hplc – dad 0. 083 0. 114 chang et al. ( ) bpa spme hplc – dad 0. 20 not stated mohammadnezhad et al. ( ) bpa sllme gc – ms 0. 54 1. 8 karayaka et al. ( ) bpa bbp ; dbp ; dehp lle lc – ms / ms gc – ms not stated not stated wu et al. ( ) bbp ; dbp mip - spe hplc – ms 0. 16 ; 0. 84 0. 55 ; 2. 81 barciela - alonso et al. ( ) bbp ; dbp it - uaa - llme gc – ms 1. 67 ; 0. 75 5. 50 ; 2. 46 farahani et al. ( ) bbp ; dbp m - μdspe uhplc – ms / ms not stated 6 × 103 ; 11 × 103 santana - mayor et al. ( ) bbp ; dbp ; dehp mspe hplc – uv / vis 0. 0103 ; 0. 003b ; 0. 0167 0. 0342 ; 0. 022b ; 0. 0556 yin et al. ( ) bbp ; dbp ; dehp spe gc – ms / ms 0. 18 ; 0. 021 ; @topic:1


gc – ms / ms 0. 18 ; 0. 021 ; 0. 036 0. 60 ; 0. 070 ; 0. 12 li et al. ( ) bbp ; dbp ; dehp lle gc – ms / ms 1. 0 ; 1. 0 ; 0. 5 3. 0 ; 3. 0 ; 0. 15 tran - lam et al. ( ) bbp ; dbp ; dehp mspe gc – ms 5. 0 ; 1. 0 ; 5. 0 not stated wei et al. ( ) dbp tsp - llme gc – ms 0. 007 0. 021 chen et al. ( b ) dbp sva - llme gc – ms 0. 15 0. 50 mohebbi et al. ( ) dbp dspe – dllme gc – fid 1. 24 4. 11 farajzadeh et al. ( ) dbp spe hplc – uv / vis 2. 4 7. 9 salazar - beltran et al. ( ) dbp mispme hplc – uv / vis 3 10 soheilifar et al. ( ) dbp m - μdspe gc – ms / ms not stated 0. 009 gonzalez - salamo et al. ( ) dbp lle hplc – uv / vis not stated not stated dada et al. ( ) dbp hf - lpme gc – ms / ms not stated not stated gonzalez - salamo et al. ( ) dbp ; dehp meps – dllme gc – fid 0. 001 ; 0. 005 0. 003 ; 0. 015 amiri & ghaemi ( ) dbp ; dehp mspe gc – ms / ms 0. 005 ; 0. 008 0. 02 @topic:1


ms / ms 0. 005 ; 0. 008 0. 02 ; 0. 03 pinsrithong & bunkoed ( ) dbp ; dehp rdse gc – ms 0. 01 ; 0. 03 0. 04 ; 0. 10 manzo et al. ( ) dbp ; dehp lle gc – ms 0. 01 – 0. 05c 0. 03 – 0. 15c tri et al. ( ) dbp ; dehp meps gc – fid 0. 05 ; 0. 10 0. 10 ; 0. 25 amiri et al. ( ) dbp ; dehp lle gc – fid not stated not stated szendi et al. ( ) dehp dmims – spe gc – ms 0. 00039 0. 0013 ozer et al. ( ) dehp mspe gc – fid 0. 02 not stated chahkandi & amiri ( ) dehp dllme gc – fid 2 4 notardonato et al. ( ) ( continued ) 5 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest adsorbent for paes, including bbp, dbp and dehp. far - ajzadeh et al. ( ) developed a natural and costless adsorbent for the accomplishment of a dispersive solid - phase extraction ( dspe ) procedure followed by dispersive liquid – liquid microextraction ( dllme ) for @topic:1


##spersive liquid – liquid microextraction ( dllme ) for the extraction and preconcentration of paes and alkylphenols. none of the methods of table 1 present lod and loq values lower than the mcl to bpa in drinking water by ec ( 0. 1 μg / l ), but are lower than in china ( 10 μg / l ) ( ec ; gb - - ). currently, mcl has not been established for bbp ( us epa a ), although, in 1990, us epa proposed an mcl of 100 μg / l ( parks et al. ). in 2004, new jersey state pri - mary and secondary drinking water standards derived the same value, multiplying the drinking water equivalent level of 7 mg / l by the relative source contribution factor of 20 % and dividing the result by the additional uncertainty factor of 10 for possible human carcinogens ( njdep ). all methods show lod and loq below this pro - posed mcl value for bbp. table 1 | continued without migration study detected analyte ( s ) extraction method chromatographic technique lods ( μg / l ) loqs ( μg / l ) reference detected analyte ( s ) extraction method chromatographic technique lods ( mg / kg ) loqs ( mg / kg ) reference bbp ; dbp ; dehp lle gc – ms 0. 00031 ; 0. 00025 ; 0. 00042 0. 00096 ; 0. 0008 ; 0. 00122 yang et al. ( ) with migration study detected analyte ( s ) extraction method chromatographic technique lods ( μg / l ) loqs ( μg / l ) reference bpa pt - μ - spe hplc – fld 0. 001 0. 00 @topic:1


μ - spe hplc – fld 0. 001 0. 0032 kaykhaii et al. ( ) bbp ; dbp ; dehp μspe gc – fid 0. 025 ; 0. 017 ; 0. 031 not stated abtahi et al. ( ) bbp ; dbp ; dehp not stated lc – ms / ms 0. 20 ; 0. 20 ; 0. 30 0. 64 ; 0. 60 ; 0. 94 surhio et al. ( ) dbp mip - spme gc – fid 0. 12 not stated moghaddam & maddah ( 2018 ) dbp hs - spme gc – ms 0. 17 0. 57 cincotta et al. ( ) dbp ; dehp spe gc – ms 0. 015d not stated sulentic et al. ( ) dbp ; dehp lle gc – ms / ms 0. 043 ; 0. 062 not stated zaki & shoeib ( ) dbp ; dehp aallme gc – ms 0. 3 ; 0. 2 not stated yousefi et al. ( ) dehp ua - dllme gc – ms 10 – 100e 50 – 500e annamalai & namasivayam ( ) bpa, bisphenol a ; bbp, benzylbutyl phthalate ; dbp, di - n - butyl phthalate ; dehp, di ( 2 - ethylhexyl ) phthalate ; spe, solid - phase extraction ; sbse, stir bar sorptive extraction ; usae, ultrasound - assisted emulsiﬁcation ; mip, molecularly imprinted polymer ; μ - spe, micro - solid - phase extraction ; mdmip, magnetic dummy molecular @topic:1


, micro - solid - phase extraction ; mdmip, magnetic dummy molecularly imprinted polymer ; spme, solid - phase microextrac - tion ; sllme, switchable liquid – liquid microextraction ; lle, liquid – liquid extraction ; it - uaa, in tube ultrasonic and air - assisted ; llme, liquid – liquid microextraction ; m - μdspe, magnetic micro - dispersive solid - phase extraction ; mspe, magnetic solid - phase extraction ; tsp, temperature - sensitive polymer ; sva, solvent vapor - assisted ; dspe, dispersive solid - phase extraction ; dllme, dispersive liquid – liquid microextraction ; mispme, molecularly imprinted solid - phase microextraction ; hf - lpme, hollow ﬁber liquid - phase microextraction ; meps, microextraction in packed syringe ; rdse, rotating disk sorptive extraction ; dmims, dual - template molecularly imprinted mesoporous silica ; pt - μ - spe, pipette - tip micro - solid - phase extraction ; μspe, micro - solid - phase extraction ; hs, headspace ; aallme, air - assisted liquid – liquid microextraction ; ua, ultrasound - assisted ; gc, gas chromatography ; ms, mass spectrometry ; hplc, high - performance liquid chromatography ; dad, diode - array detection ; fid, ﬂame ionization detector ; uv / vis, dual - wavelength ultraviolet / visible ; ms / ms, tandem mass spectrometry ; uhplc, ultra - high - perform - ance liquid chromatography ; uflc, ultra - fast liquid chromatography ; uplc – ms, ultra - performance @topic:1


fast liquid chromatography ; uplc – ms, ultra - performance liquid chromatography – mass spectrometry ; fld, ﬂuorescence detector. acorresponds to four bisphenols – bpa ; bpb : bisphenol b ; bpf : bisphenol f ; bps : bisphenol s. bcorresponds to two phthalates – dbp : bis ( 2 - butoxyethyl ) phthalate / dbp. ccorresponds to nine phthalates – dep : diethyl phthalate ; dpp : dipropyl phthalate ; dibp : di - isobutyl phthalate ; dbp ; dchp : dicyclohexyl phthalate ; dnhp : dihexyl phthalate ; bzbp : benzyl butyl phthalate ; dnop : di ( n - octyl ) phthalate ; dehp. dcorresponds to three phthalates – dibp ; dbp ; dehp. ecorresponds to 14 phthalates – bbp ; dbp ; dehp ; dpp ; dep ; dibp ; dchp ; dnop : di - n - octyl phthalate ; dmp : dimethyl phthalate ; dhp : dihexyl phthalate ; dinp : di - isononyl phthalate ; didp : di - isodecyl phthalate ; bbep : bis ( 2 - n - butoxyethyl ) phthalate ; bmep : bis ( 2 - methoxy ethyl ) phthalate. 6 r. da silva costa et al. | potential risk of bpa and paes in commercial water @topic:1


et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest almost all methods exhibit lod and loq lower than dbp by china for drinking water ( 3 μg / l ) ( gb - - ). all methods show lod and loq lower than dehp by us fda for bottled water ( 6 μg / l ) and by who, codex ali - mentarius, china for drinking water ( 8 μg / l ) ( codex alimentarius ; gb - - ; who ; ecfr ). yang et al. ( ) analyzed bbp, dbp and dehp by gc – ms / lle. the values of lod and loq are given in mg / kg. the lod and loq are lower than the sml values by the eu for bbp ( 30 mg / kg ), dbp ( 0. 3 mg / kg ) and dehp ( 1. 5 mg / kg ) ( efsa ). detections of bpa and paes the detected levels of bpa, bbp, dbp and dehp in com - mercial water bottles without the storage study are present in table 2 and figure 1. wei et al. ( ) and yang et al. ( ) are not included in figure 1 because the units are in mg / kg. the detected levels of bpa, bbp, dbp and dehp in commercial water bottles with the storage study are pre - sent in table 3 and figure 2. for articles with concentration ranges, averages were used to @topic:1


3 and figure 2. for articles with concentration ranges, averages were used to generate figures 1 and 2. a better understanding of the methods used in storage studies can be veriﬁed in their respective articles. some papers presented values above the mcl to bpa ( 0. 1 μg / l ) by ec ( ec ). all the papers exhibited levels lower than mcl to bpa by china ( gb - - ). even though there is no speciﬁc legislation for bbp so far, all the papers showed levels lower than mcl of 100 μg / l pro - posed by us epa. it should be noted that this is a proposed value and has not been deﬁned as a standard, but the pro - posed value serves to analyze the results for the moment. almost all papers exhibited dbp levels low than 3 μg / l ( gb - - ) and displayed dehp levels low than 6 or 8 μg / l ( codex alimentarius ; gb - - ; who ; ecfr ). the values of bbp, dbp and dehp obtained by wei et al. ( 2017 ) and yang et al. ( ) are lower than the sml values by the eu for bbp ( 30 mg / kg ), dbp ( 0. 3 mg / kg ) and dehp ( 1. 5 mg / kg ) ( efsa ). the countries with the reported highest levels of bpa, bbp, dbp and dehp were turkey ( 5. 7 μg / l – figure 1 ), pakistan ( 12. 11 μg / l – figure 2 ), mexico ( 82. 8 μg / l – figure 1 ) and thailand ( 64. 0 μg / l – figure 1 ), respectively. the pae values detected were highest than those estab - lished by legislation. thailand also was @topic:1


were highest than those estab - lished by legislation. thailand also was the country with the ﬁrst rank with dehp ( 94. 1 μg / l ) in bottled waters in the review by luo et al. ( ). the value was obtained by uansiri et al. ( ) in bottled water contained in plastic con - tainers. dehp is known as a dominant pae in bottled water ( keresztes et al. ; guart et al. ; zaki & shoeib ; abtahi et al. ). dbp was the most compound detected. luo et al. ( ) also veriﬁed that dbp was the pae with more detection fre - quency in bottled water. all the samples ( 10 brands ) analyzed by soheilifar et al. ( ) present dbp. among 16 paes studied by zhang et al. ( ), dbp was the most ubiqui - tous and dominant contaminant in the study population. soheilifar et al. ( ) optimized a molecularly imprinted polymer as a highly selective sorbent toward dbp. dada et al. ( ) also analyzed packaged sachet water, and dbp concentrations were almost four - time higher ( 160 μg / l ) rela - tive to bottled water. sachet water is packaging in plastic bags ( semey et al. ) made of ldpe ( jnr et al. ), and it is relatively cheaper than a water bottle ( dada et al. ). kaykhaii et al. ( 2019 ) veriﬁed that the water sample pre - sented more bpa migration ( figure 2 ) when brought to boiling in a steel jar, quickly poured into the bottle and after cooled at ambient temperature ( figure 2 ). surhio et al. @topic:1


cooled at ambient temperature ( figure 2 ). surhio et al. ( ) detected the highest value of bbp migration studied with the inﬂuence of sunlight in pakistan ( figure 2 ). the intensity of sunlight may affect the degradation degree of paes ( lertsirisopon et al. ), and the occurrence of paes in water stored in pet bottles depended mainly on the country of origin of the bottle ( schmid et al. ; keresztes et al. ). all the papers that no speciﬁed the type of bottle demonstrated dbp levels above the mcl ( 3 μg / l ). yousefi et al. ( ) also studied pet bottled water exposed to sunlight and as well as surhio et al. ( ) veriﬁed an increase in dbp concentration. dbp values at room temperature were lower than at freezing for hashemi - moghaddam & maddah ( ), while the reverse occurred for sulentic et al. ( ). the presence of dbp may be due to different production facilities used by the different brands tested ( al - saleh et al. ; guart et al. ). annamalai & namasivayam ( ) obtained bigger values to dehp at 4 c and smaller values at 37 c. to 7 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest table 2 | levels of bpa, bbp, dbp and dehp in commercial water bottles without the storage study detected @topic:1


, dbp and dehp in commercial water bottles without the storage study detected analyte sample country type of bottle number of brands or samples concentration ( μg / l ) reference bpa drinking water bottle turkey not stated 3 5. 7 karayaka et al. ( ) bpa mineral water bottle iran peta 1 5. 5 mohammadnezhad et al. ( ) bpa mineral water malaysia not stated 6 1. 25 rozaini et al. ( ) bpa plastic bottled mineral water china not stated 1 0. 127 chang et al. ( ) bpa bottled mineral water iran not stated 3 0. 07 gorji et al. ( ) bpa bottled water china not stated not stated 0. 05 – 0. 08 zhou et al. ( ) bpa bottled water china not stated 17 0. 01 wu et al. ( ) bbp mineral water iran pet 3 2. 9 – 5. 5 farahani et al. ( ) bbp bottled water china not stated 17 1. 86 wu et al. ( ) bbp bottled water in plastic spain not stated 4 0. 75 – 1. 9 barciela - alonso et al. ( ) bbp mineral water china not stated 5 0. 515 – 0. 690 yin et al. ( ) bbp mineral water vietnam not stated 14 0. 30 – 0. 95 tran - lam et al. ( ) bbp bottled drinking water china not stated 60 0. 019 – 0. 032 li et al. ( ) bbp mineral water bottled in plastic spain not stated 1 < loq santana - mayor et al. ( ) dbp plastic bottled water nigeria not stated 15 42 dada et al. ( ) dbp drinking water mexico pet 10 20. 5 – 82. 8 salazar - beltran et al. ( ) dbp mineral water china not stated 5 8. 98 – 11. @topic:1


) dbp mineral water china not stated 5 8. 98 – 11. 5 yin et al. ( ) dbp bottled water in plastic spain not stated 4 4. 6 – 8. 2 barciela - alonso et al. ( ) dbp plastic bottled water thailand not stated 1 17. 0 pinsrithong & bunkoed ( ) dbp plastic bottled water iran not stated 1 5. 2 mohebbi et al. ( ) dbp mineral water cyprus not stated not stated 4. 35 farajzadeh et al. ( ) dbp bottled mineral water iran not stated 1 4. 5 amiri & ghaemi ( ) dbp mineral water china not stated 1 2. 68 chen et al. ( b ) dbp bottled water china not stated 17 1. 34 wu et al. ( ) dbp mineral water iran not stated 3 1. 1 – 2. 5 amiri et al. ( ) dbp mineral water iran pet 3 1. 1 – 1. 7 farahani et al. ( ) dbp mineral water spain not stated 1 < 1 gonzalez - salamo et al. ( ) dbp mineral bottled water spain pet 1 0. 36 gonzalez - salamo et al. ( ) dbp water packed in plastic bottle ( still, sparkling and light sparkling ) chile not stated 5 ( 2 – still, 2 – sparkling, 1 – light sparkling ) 0. 353 – 2. 756 manzo et al. ( ) dbp plastic bottled water iran not stated 10 0. 26 – 1. 13 soheilifar et al. ( ) dbp plastic bottled beverages ( water ) vietnam not stated 8 0. 24 – 1. 86 tri et al. ( ) ( continued ) 8 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 un @topic:1


in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest table 2 | continued detected analyte sample country type of bottle number of brands or samples concentration ( μg / l ) reference dbp mineral water bottled in plastic spain not stated 1 0. 184 santana - mayor et al. ( ) dbp mineral water vietnam not stated 14 0. 09 – 0. 95 tran - lam et al. ( ) dbp bottled drinking water china not stated 60 0. 021 – 0. 51 li et al. ( ) dbp bottled mineral water hungary pet 4 < 0. 005 – 0. 2 szendi et al. ( ) dehp plastic bottled water thailand not stated 1 64. 0 pinsrithong & bunkoed ( ) dehp bottled water italy not stated 2 22. 9 – 24. 4 notardonato et al. ( ) dehp plastic bottled beverages ( water ) vietnam not stated 8 10. 3 – 42. 3 tri et al. ( ) dehp plastic bottled water turkey not stated not stated 10. 06 – 11. 90 ozer et al. ( ) dehp bottled mineral water iran not stated 1 3. 0 amiri & ghaemi ( ) dehp bottled mineral water iran not stated 2 2. 6 chahkandi & amiri ( ) dehp bottled water china not stated 17 2. 50 wu et al. ( ) dehp water packed in plastic bottle ( still, sparkling and light sparkling ) chile not stated 5 ( 2 – still, 2 – sparkling, 1 – light sparkling ) 1. 258 – 4. 321 manzo et al. @topic:1


light sparkling ) 1. 258 – 4. 321 manzo et al. ( ) dehp mineral water iran not stated 3 0. 5 – 3. 5 amiri et al. ( ) dehp mineral water vietnam not stated 14 0. 46 – 1. 8 tran - lam et al. ( ) dehp mineral water china not stated 5 < loq – 0. 733 yin et al. ( ) dehp bottled mineral water hungary pet 4 < 0. 29 – 11. 289 szendi et al. ( ) dehp bottled drinking water china not stated 60 0. 013 – 0. 021 li et al. ( ) detected analyte sample country type of bottle number of brands or samples concentration ( mg / kg ) reference bbp mineral water china not stated 1 0. 001 wei et al. ( ) dbp 0. 014 dehp 0. 018 bbp mineral water soda water china not stated not stated 0. 32 × 104 – 1. 1 × 104 < lod – 1. 3 × 104 yang et al. ( ) dbp mineral water soda water 1. 3 × 104 – 10. 2 × 104 1. 6 × 104 – 63. 4 × 104 dehp mineral water soda water 2. 2 × 104 – 43. 9 × 104 5. 7 × 104 – 72. 9 × 104 bpa, bisphenol a ; bbp, benzylbutyl phthalate ; dbp, di - n - butyl phthalate ; dehp, di ( 2 - ethylhexyl ) phthalate. apolyethylene terephthalate. 9 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. @topic:1


##corrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest zaki & shoeib ( ) occurred the reverse. these authors analyzed dehp in pet bottled water. the migration of paes in bottled water results from the combined effects of multiple factors, as reported by luo et al. ( ). the possible reason for the migration of paes is the usage of low - quality plastic as well as solubility in water ( saeed et al. ). the plastic type is that inﬂuences the pres - ence of speciﬁc contaminants, where the migration of plasticizers from the cap material plays an important role ( guart et al. ). jeddi et al. ( ) noted that the effect of temperatures and sunlight exposure on the release of the bbp, dbp and dehp into the water is more than the effect due to storage duration. keresztes et al. ( ) analyzed identical brands of water samples in pet containers having different volumes. the authors veriﬁed that how much higher is the contact surface between water and pet material, higher concentrations of bbp, dbp and dehp were observed. risk assessment daily intake - associated risk assessment to compare the health risk via commercial water bottle con - sumption was used the risk assessment. the highest levels of bpa, bbp, dbp and dehp in commercial water bottles are figure 1 | bpa, bbp, dbp and dehp concentrations detected in commercial water bottles without the storage study. the number in ‘ sample - type of bottle ’ represents different samples. ns is ‘ not stated ’. 10 r. da silva costa et al @topic:1


ns is ‘ not stated ’. 10 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest table 3 | levels of bpa, bbp, dbp and dehp in commercial water bottles with the storage study detected analyte sample country type of bottle number of brands or samples storage study concentration ( μg / l ) reference bpa bottled drinking water iran not stated 4 freezing temperature ( 24 h ) a 0. 0023 sunlight ( for a week ) 0. 007 kaykhaii et al. ( ) boiled in a steel jar and quickly poured into the bottle ( cooled to ambient temperature ) a 0. 016 bbp mineral water bottle pakistan not stated 5 sunlight ( 7 days with 10 h / day – 46 – 48 c ) ndb – 12. 11 ( median : 7. 43 ) surhio et al. ( ) bbp bottled water iran petc 10 sunlight ( roof on sunny days for 1 week ) 0. 03 – 0. 13 abtahi et al. ( ) dbp mineral water bottle pakistan not stated 5 sunlight ( 7 days with 10 h / day – 46 – 48 c ) ndb – 26. 16 ( median : 21. 7 ) surhio et al. ( ) dbp bottled water iran pet 10 sunlight ( roof on sunny days for 1 week ) ndb – 0. 12 ( median : 0. 10 ) abtahi et al. ( ) dbp bottled water romania not stated not stated room temperature 1 – 4 ca 6. 11 5. 12 @topic:1


stated not stated room temperature 1 – 4 ca 6. 11 5. 12 sulentic et al. ( ) dbp water in plastic bottle iran not stated 3 room temperaturea freezing temperaturea 5. 32 10. 12 hashemi - moghaddam & maddah ( ) dbp bottled mineral water italy pet 15 6 months at 25 c 12 months at 60 c 18 months at 60 c 1. 23 3. 14 6. 01 cincotta et al. ( ) dbp bottled water egypt pet 5 1 months ( 4 ± 1 c ) 2 months ( 4 ± 1 c ) 4 months ( 4 ± 1 c ) 1 months ( 40 ± 5 c ) 2 months ( 40 ± 5 c ) 4 months ( 40 ± 5 c ) 2 months ( 25 ± 5 c ) 6 months ( 25 ± 5 c ) 0. 107 0. 128 0. 173 0. 124 0. 167 0. 229 0. 136 0. 227 zaki & shoeib ( ) dbp drinking water bottled iran pet 5 first week of the production sunlight ( 23 ± 2 c at 5 days ) incubator ( 25 c for 75 days ) incubator ( 42 c for 15 days ) 0. 80 5. 86 not stated not stated yousefi et al. ( ) dehp mineral water bottle pakistan not stated 5 sunlight ( 7 days with 10 h / day – 46 – 48 c ) 20. 23 surhio et al. ( ) ( continued ) 11 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf @topic:1


/ 869656 / jwh2021202. pdf by guest presented in table 4 and figure 3. the bpa in pet bottled water suggests other sources of contamination beside the packaging itself. the presence of bpa in pc packaging is known. in the case of pet bottled water, bpa can result from leaching by bottle caps or contamination of the water before bottling ( guart et al. ; bach et al. ; rowell et al. ). the water quality intended for bottling can be affected by the leaching of pollutants from unprotected agri - cultural and industrial areas ( bono - blay et al. ). bono - blay et al. ( ) studied spanish water sources intended for bottling, where bpa was one of the most frequently detected compounds at concentrations between 0. 031 and 0. 203 μg / l. although the estimation daily intake ( edi ) of bpa, bbp, dbp and dehp detected in pet bottled waters ana - lyzed was below the legislative values ( table 4 ), considering all types of food, it may contribute to the total daily intake of these compounds. the highest contributions via commercial water bottles of bpa, bbp, dbp and dehp in all the bottled waters studied were 4. 1, 0. 069, 23. 7 and 3. 66 % of tdi, respectively ( figure 3 ). the results demon - strate that contribution via commercial water bottles ( table 4 ) could represent a substantial source of exposure to these compounds ( considering the highest contributions ), when the daily consumption rate, of 2. 0 l / day of bottled water and body weight of 70 kg, is used according to the table 3 | continued detected analyte sample country type of bottle number of brands or samples storage study concentration ( μg / l ) reference de @topic:1


of brands or samples storage study concentration ( μg / l ) reference dehp bottled water iran pet 10 sunlight ( roof on sunny days for 1 week ) 0. 7 – 0. 12 abtahi et al. ( ) dehp drinking water bottled iran pet 5 first week of the production sunlight ( 23 ± 2 c at 5 days ) incubator ( 25 c for 75 days ) incubator ( 42 c for 15 days ) 0. 77 not stated 9. 62d and 12. 67e 10. 33f yousefi et al. ( ) dehp bottled water romania not stated not stated room temperature 1 to 4 ca 0. 52 2. 00 sulentic et al. ( ) dehp bottled water india pet not stated 2 months at 4 c 2 months at 37 c 4 months at 4 c 4 months at 37 c 6 months at 4 c 6 months at 37 c 0. 303 0. 081 0. 40 0. 2010 1. 09 0. 59 annamalai & namasivayam ( ) dehp bottled water egypt pet 5 1 months ( 4 ± 1 c ) 2 months ( 4 ± 1 c ) 4 months ( 4 ± 1 c ) 1 months ( 40 ± 5 c ) 2 months ( 40 ± 5 c ) 4 months ( 40 ± 5 c ) 2 months ( 25 ± 5 c ) 6 months ( 25 ± 5 c ) 0. 135 0. 235 0. 307 0. 190 0. 306 0. 432 0. 274 0. 396 zaki & shoeib ( ) bpa, bisphenol a ; bbp, benzylbutyl phthalate ; dbp, di - n - butyl phthalate ; dehp, di ( 2 - ethylhexyl ) phthalate. aunspeciﬁed temperature. bnot detected. cpolyethylene ter @topic:1


##ciﬁed temperature. bnot detected. cpolyethylene terephthalate. dmean concentration. ehighest mean concentration. fmaximum amount. 12 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest figure 2 | levels of bpa, bbp, dbp and dehp variation in commercial water bottles with the storage study. the number in ‘ sample - type of bottle ’ represents different samples. ns is ‘ not stated ’. table 4 | estimation of exposure to bpa, bbp, dbp and dehp in commercial water bottles without the storage study detected analyte country concentration ( μg / l ) a edi ( μg / kg - bw / day ) b contribution via bottled water ( % ) c elcrd reference bpa turkey 5. 7 ≈0. 163 ≈4. 1 – karayaka et al. ( ) bpa iran 5. 5 ≈0. 157 ≈3. 9 – mohammadnezhad et al. ( ) bpa malaysia 1. 25 ≈3. 6 × 102 ≈0. 9 – rozaini et al. ( ) bpa china 0. 127 ≈3. 6 × 103 ≈0. 09 – chang et al. ( ) bpa china 0. 08 ≈2. 3 × 103 ≈0. 058 – zhou et al. ( ) bpa iran 0. 07 2. 0 × 103 ≈0. 05 – gorji et al. ( ) bpa china 0. 01 @topic:1


– gorji et al. ( ) bpa china 0. 01 ≈2. 9 × 104 ≈7. 3 × 103 – wu et al. ( ) bbp iran 5. 5 ≈0. 157 ≈0. 03 – farahani et al. ( ) bbp spain 1. 9 ≈5. 4 × 102 ≈1. 1 × 102 – barciela - alonso et al. ( ) bbp china 1. 86 5. 3 × 102 ≈1. 1 × 102 – wu et al. ( ) bbp vietnam 0. 95 ≈2. 7 × 102 ≈5. 4 × 103 – tran - lam et al. ( ) bbp china 0. 690 ≈2. 0 × 102 ≈4. 0 × 103 – yin et al. ( ) bbp china 0. 032 ≈9. 1 × 104 ≈1. 8 × 104 – li et al. ( ) bbp spain < loq ( 0. 006 ) < 1. 7 × 104 < 3. 4 × 105 – santana - mayor et al. ( ) dbp mexico 82. 8 2. 37 23. 7 – salazar - beltran et al. ( ) ( continued ) 13 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest table 4 | continued without the storage study detected analyte country concentration ( μg / l ) a edi ( μg / kg - bw / day ) b contribution via bottled water ( % ) c elcrd reference dbp nigeria 42 @topic:1


via bottled water ( % ) c elcrd reference dbp nigeria 42 1. 2 12 – dada et al. ( ) dbp thailand 17. 0 ≈0. 486 ≈4. 86 – pinsrithong & bunkoed ( ) dbp china 11. 5 ≈0. 329 ≈3. 29 – yin et al. ( ) dbp spain 8. 2 ≈0. 234 ≈2. 34 – barciela - alonso et al. ( ) dbp iran 5. 2 ≈0. 149 ≈1. 49 – mohebbi et al. ( ) dbp iran 4. 5 0. 129 1. 29 – amiri & ghaemi ( ) dbp iran 4. 35 ≈0. 124 1. 24 – farajzadeh et al. ( ) dbp china 2. 68 ≈7. 7 × 102 ≈0. 77 – chen et al. ( b ) dbp iran 2. 5 ≈7. 1 × 102 ≈0. 71 – amiri et al. ( ) dbp vietnam 1. 86 5. 3 × 102 0. 53 – tri et al. ( ) dbp iran 1. 7 ≈4. 9 × 102 ≈0. 49 – farahani et al. ( ) dbp china 1. 34 ≈3. 8 × 102 ≈0. 38 – wu et al. ( ) dbp iran 1. 13 ≈3. 2 × 102 ≈0. 32 – soheilifar et al. ( ) dbp spain < 1 < 2. 9 × 102 < 0. 29 – gonzalez - salamo et al. ( ) dbp vietnam 0. 95 ≈2. 7 × 102 ≈0. 27 – tran - lam et al. ( ) dbp china 0. 51 ≈1. 5 × 102 0. 15 – li et al. ( ) dbp spain 0 @topic:1


102 0. 15 – li et al. ( ) dbp spain 0. 36 1. 0 × 102 0. 1 – gonzalez - salamo et al. ( ) dbp hungary < 0. 2 < 5. 7 × 103 < 0. 057 – szendi et al. ( ) dbp spain 0. 184 ≈5. 3 × 103 ≈0. 053 – santana - mayor et al. ( ) dehp thailand 64. 0 ≈1. 83 ≈3. 66 ≈3. 0 × 105 pinsrithong & bunkoed ( ) dehp vietnam 42. 3 ≈1. 21 2. 42 ≈2. 0 × 105 tri et al. ( ) dehp china 2. 50 ≈7. 1 × 102 ≈1. 42 ≈1. 2 × 106 wu et al. ( ) dehp italy 24. 4 ≈0. 697 ≈1. 39 ≈1. 1 × 105 notardonato et al. ( ) dehp turkey 11. 90 0. 34 0. 68 ≈5. 6 × 106 ozer et al. ( ) dehp hungary < 11. 289 < 0. 323 < 0. 646 ≈ < 5. 3 × 106 szendi et al. ( ) dehp chile 4. 321 ≈0. 123 ≈0. 246 ≈2. 0 × 106 manzo et al. ( ) dehp iran 3. 5 0. 1 ≈0. 2 ≈1. 6 × 106 amiri et al. ( ) dehp iran 3. 0 0. 086 0. 172 ≈1. 4 × 106 amiri & ghaemi ( ) dehp vietnam 1. 8 5. 1 × 102 ≈0. 1 ≈8. 53 × 107 tran - lam et al. ( ) dehp china 0. 733 ≈2. 1 × 102 ≈0. 042 ≈3 @topic:1


733 ≈2. 1 × 102 ≈0. 042 ≈3. 4 × 107 yin et al. ( ) dehp china 0. 021 6. 0 × 104 1. 2 × 103 ≈9. 9 × 109 li et al. ( ) detected analyte country concentration ( μg / kg ) a edi ( μg / kg - bw / day ) b contribution via bottled water ( % ) c crd reference bbp china mineral water ( mw ) : 0. 11 soda water ( sw ) : 0. 13 ≈3. 1 × 103 ≈3. 7 × 103 ≈6. 2 × 104 ≈7. 4 × 104 – yang et al. ( ) ( continued ) 14 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest standard who ( ). if reference dose ( rfd ) were con - sidered ( table 5 ), which is more restrictive for dehp, the contribution would be much higher ( 9. 15 % ). the carcinogenic risk ( excess lifetime cancer risks – elcr ) posed by the highest concentration of dehp in bottled water was negligible for all papers, with extremely below or between the accepted risk level of 106 – 104 cancer risk ( who ). as mentioned by who ( ), daily water intake can vary signiﬁcantly in different parts of the world and location - speciﬁc data on drinking water table 4 | continued without the storage study detected analyte country concentration ( μg / l ) a ed @topic:1


storage study detected analyte country concentration ( μg / l ) a edi ( μg / kg - bw / day ) b contribution via bottled water ( % ) c crd reference dbp mineral water : 1. 02 soda water : 6. 34 ≈2. 9 × 102 ≈0. 181 ≈0. 29 ≈1. 8 – dehp mineral water : 4. 3 soda water : 7. 29 ≈0. 123 ≈0. 208 ≈0. 246 ≈0. 416 ≈5. 2 × 108 ≈3. 4 × 106 with storage study detected analyte country concentration ( μg / l ) a edi ( μg / kg - bw / day ) b contribution via bottled water ( % ) c crd reference bpa iran 0. 016 ≈4. 6 × 104 ≈1. 2 × 102 – kaykhaii et al. ( ) bbp pakistan 12. 11 0. 346 ≈0. 069 – surhio et al. ( ) bbp iran 0. 13 ≈3. 7 × 103 ≈7. 4 × 104 – abtahi et al. ( ) dbp pakistan 26. 16 ≈0. 747 7. 47 – surhio et al. ( ) dbp iran 10. 12 ≈0. 289 ≈2. 89 – moghaddam & maddah ( 2018 ) dbp iran 8. 45 ≈0. 241 ≈2. 41 – yousefi et al. ( ) dbp romania 6. 11 ≈0. 175 ≈1. 75 – sulentic et al. ( ) dbp italy 6. 01 ≈0. 172 ≈1. 72 – cincotta et al. ( ) dbp egypt 0. 229 ≈6. 5 × 103 ≈0. 065 – zaki & shoeib ( ) dbp iran 0. 12 ≈3. @topic:1


##ki & shoeib ( ) dbp iran 0. 12 ≈3. 4 × 103 ≈0. 034 – abtahi et al. ( ) dehp pakistan 20. 23 0. 578 ≈1. 16 ≈9. 5 × 106 surhio et al. ( ) dehp iran 12. 67 0. 362 ≈0. 724 ≈6. 0 × 106 yousefi et al. ( ) dehp romania 2. 00 ≈5. 7 × 102 ≈0. 114 9. 4 × 107 sulentic et al. ( ) dehp egypt 0. 432 ≈1. 2 × 102 ≈0. 024 ≈2. 0 × 107 zaki & shoeib ( ) dehp iran 0. 12 ≈3. 4 × 103 ≈6. 8 × 103 ≈5. 6 × 108 abtahi et al. ( ) dehp india 1. 09 ≈3. 1 × 102 ≈0. 062 ≈5. 1 × 107 annamalai & namasivayam ( ) bpa, bisphenol a ; bbp, benzylbutyl phthalate ; dbp, di - n - butyl phthalate ; dehp, di ( 2 - ethylhexyl ) phthalate. athe worst - case scenario ( the maximum level of each compound ) was employed. bedi ¼ ( c × ir ) / bw, where c is the concentration of target compounds ( μg / l or mg / kg ), ingestion rate ( ir ) is the daily consumption rate of bottled water ( l / day or g / day ), and bw is body weight ( luo et al. 2018 ), and the ir was assumed to be 2. 0 l / day or and 2. 0 kg / day for a 70 kg for adult ( bw ) @topic:1


. 0 kg / day for a 70 kg for adult ( bw ) ( who 2005 ). the value of 2. 0 l / day refers to all water sources that includes water from all supply sources such as community water supply ( i. e., tap water ), bottled water, etc. μg / kg - bw / day : microgram per kilogram of the body weight of the person taking per day. ccontribution via drinking water ¼ ( edi / tdi ) × 100 ( zaki & shoeib 2018 ), where the tdi for bpa, bbp, dbp, and dehp are available for reference as established by efsa ( 4, 500, 10 and 50 μg / kg - bw / day ). delcr is the excess lifetime cancer risks due to exposure to chemicals through the use of bottled water. elcr ¼ dwur × mc, where drinking water unit risk is equal to 4. 7 × 107 μg / l of dehp in water, and mc is the maximum concentration ( μg / l or μg / kg ) of dehp in bottled water ( jeddi et al. 2015 ). here was considered the value of 4. 7 × 107 μg / kg for papers with con - centrations give in mg / kg. ethis value appears only in table 1 of this article, without specifying the conditions under which this value was found. 15 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest consumption @topic:1


##656 / jwh2021202. pdf by guest consumption are preferred. as reported by leung et al. ( ), infants and children have been subject to increased risks that are approximately six times greater than those in adolescents and adults due to their high drinking water con - sumption based on body weight. as speciﬁed by us epa ( ), older adults ( 65 years of age ) and pregnant are other susceptible groups due to their physiological proper - ties change. as reported by gerba et al. ( ), the elderly may be less able to create an effective defense against con - taminants because of a pre - existing disease or weakened immune system. the risk is inherent to the pregnant and also to the fetus ( wee & aris ). table 5 shows more detailed the risk assessment to other population groups based on only the ingestion of bottled water. the values of bottled water ingestion are based on us epa ( ) and us epa ( b ). us epa figure 3 | bpa, bbp, dbp and dehp contribution via commercial water bottles. the number in parentheses represents articles from the same country with different concentrations. mw is mineral water and sw is soda water. 16 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest table 5 | estimated human exposure and estrogenic effects of bpa, bbp, dbp and dehp via commercial bottled water ingested for other population groups bpa bbp dbp dehp reference karayaka et al @topic:1


groups bpa bbp dbp dehp reference karayaka et al. ( ) surhio et al. ( ) salazar - beltran et al. ( ) pinsrithong & bunkoed ( ) maximum concentration ( μg / l ) 5. 7 12. 11 82. 8 64. 0 edi ( μg / kg - bw / day ) infants ( birth to < 12 months ) * a ≈0. 042 ≈0. 089 ≈0. 61 ≈0. 471 children ( 1 to < 3 years ) * b ≈0. 106 ≈0. 225 ≈1. 539 ≈1. 19 children ( 3 to < 11 years ) * c ≈0. 072 ≈0. 154 ≈1. 051 ≈0. 813 teenage ( 11 to < 16 years ) * d ≈0. 053 ≈0. 112 ≈0. 767 ≈0. 593 young adult ( 16 < 21 years ) * e ≈0. 061 ≈0. 129 ≈0. 882 ≈0. 682 adult ( 21 years ) * f ≈0. 060 ≈0. 128 ≈0. 876 ≈0. 677 pregnant ( 15 – 44 ) * g ≈0. 046 ≈0. 097 ≈0. 662 0. 512 elderly ( 65 years ) * h ≈0. 057 ≈0. 120 ≈0. 821 ≈0. 635 tolerable daily intake ( μg / kg - bw / day ) 4 500 10 50 contribution via bottled water ( % ) # infants ( birth to < 12 months ) * a ≈1. 05 ≈1. 78 × 102 ≈6. 10 ≈0. 942 children ( 1 to < 3 years ) * b ≈2. 65 ≈4. 50 × 102 ≈15. 40 ≈2. 38 children ( @topic:1


* f ≈1. 20 × 103 ≈2. 56 × 104 ≈8. 76 × 103 ≈3. 39 × 102 pregnant ( 15 – 44 ) * g ≈9. 20 × 104 ≈1. 94 × 104 ≈6. 62 × 103 2. 56 × 102 elderly ( 65 years ) * h ≈1. 14 × 103 ≈2. 4 × 104 ≈8. 21 × 103 ≈3. 18 × 103 sf ( based on maximum concentration ) infants ( birth to < 12 months ) * a 1, 190 5, 620 164 42. 5 children ( 1 to < 3 years ) * b 472 2, 220 65 16. 8 children ( 3 to < 11 years ) * c 694 3, 250 95. 1 24. 6 teenage ( 11 to < 16 years ) * d 943 4, 460 130 33. 7 young adult ( 16 < 21 years ) * e 820 3, 880 113 29. 3 adult ( 21 years ) * f 833 3, 910 114 29. 5 ( continued ) 17 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest ( b ) includes only bottled water consumed directly as a beverage, not including bottled water used in the prep - aration of foods. as stated by hossain et al. ( ), the regional variability in water intake can due to differences in weather conditions and food intake habits of the popu - lation. as can be seen in table 5, the results demonstrate that bottled water can represent a substantial source of exposure @topic:1


5, the results demonstrate that bottled water can represent a substantial source of exposure to these compounds. children ( 1 to < 3 years ) had a higher edi, and as a result, a high contribution via bottled water consumption ( 15. 4 % ) and high hazard quoti - ent ( hq ). as previously reported, if rfd for dehp were considered, the contribution would be much higher ( 5. 95 % ). the highest hq for the compounds via bottled water consumption was much lower than 1 for all com - pounds, indicating an absence of risk ( us epa ). the safety factor ( sf ) calculated for the selected compounds with the maximum concentrations was all far above 1 for all groups, denoting that the bpa, bbp, dbp and dehp concentrations disclosed in bottled water should not rep - resent grave safety concerns, corroborating with the review by luo et al. ( ). potential estrogenic effect of paes despite the safety factor indicates that the levels of the com - pounds in bottled waters are acceptable in terms of water safety, the potential estrogenic effects of the compounds by an average estrogen equivalente ( eeq ) level in bottled waters are based on the highest concentrations that were evaluated ( table 5 ). the eeq provides valuable information on human exposure to estrogen - like compounds, aiding in the estimation of the total dietary intake of estrogenicity ( schiliro et al. ). the potential estrogenic effects of bbp and dbp in bottled water should not be ignored due to their relatively high concentrations. as can be seen in table 5, the average eeq level in the bottled waters is sig - niﬁcantly at 6. 1652 ng e2 / l, which was 22. 8 times higher than those that cause adverse estrogenic effects on zebraﬁsh ( 0. 27 @topic:1


that cause adverse estrogenic effects on zebraﬁsh ( 0. 27 ng e2 / l ) as reported by soares et al. ( ). thus, the average eeq level indicated that bpa, bbp, dbp and dehp in bottled waters may induce adverse estrogenic effects on human health. conclusions although the governments have published the guideline tolerance values of bisphenol a and paes in drinking water, they are still detected in water bottles. hplc – dad was the most used in bpa detections, while gc – ms was the most used in pae detections. new methods to improve the extraction of bpa, bbp, dbp and dehp from commercial water bottles have been developed. dbp and dehp have still been detected in concentrations table 5 | continued bpa bbp dbp dehp pregnant ( 15 – 44 ) * g 1, 090 5, 150 151 39. 1 elderly ( 65 years ) * h 877 4, 170 122 31. 5 estrogenic potency ( ep ) 5. 9e05l 2e4m 4. 1e5m 3e7n eeq ( ng e2 / l ) & 0. 336 2. 42 3. 39 0. 0192 total compounds 6. 1652 * the values of weights and bottled water ingested are based on us epa ( 2011 ) and us epa ( 2019b ) : a0. 0685 l / day for 9. 3 kg, b0. 2305 l / day for 12. 45 kg, c0. 3365 l / day for 26. 5 kg, d0. 517 l / day for 55. 8 kg, e0. 753 l / day for 70. 7 kg ; f0. 84 l / day for 79. 4 kg ; g0. 6 l / @topic:1


l / day for 79. 4 kg ; g0. 6 l / day for 75 kg ; h0. 749 l / day for 75. 5 kg ( table 8 – 24, 8 – 25, 8 – 29, 3 – 34, 3 – 71, and table a - 2 ). # contribution via drinking water ¼ ( edi / tdi ) × 100 ( zaki & shoeib 2018 ), where the tdi for bpa, bbp, dbp, and dehp are available for reference as established by efsa. ius epa ( 2019a ) ; us epa ( 1987b ) ; us epa ( 1988 ) ; us epa ( 1987a ). jhazard quotient ( hq ) ¼ edi / rfd, where hq is associated with the exposure via the speciﬁed exposure route ( unitless ) ( jeddi et al. 2015 ). ksafety factor ( sf ) ¼ rfd / edi ( luo et al. 2018 ). & eeq ¼ epi × ci, where ep and c denote the estrogenic potency of an individual estrogenic compound ( in vitro bioassays ) and its corresponding concentration ( liu et al. 2009 ). llegler et al. ( 1999 ). mkim & ryu ( 2006 ). ncavanagh et al. ( 2018 ). 18 r. da silva costa et al. | potential risk of bpa and paes in commercial water bottles journal of water and health | in press | 2021 uncorrected proof downloaded from http : / / iwaponline. com / jwh / article - pdf / doi / 10. 2166 / wh. 2021. 202 / 869656 / jwh2021202. pdf by guest greater good than those established by legislation. contra - dictory @topic:1


by guest greater good than those established by legislation. contra - dictory observations, with decreasing and increasing concentrations on pae concentration in bottled water, are reported. no consistent or clear trends regarding the effects of storage conditions, on pae concentration in bottled water, are demonstrated. based on the risk assess - ment, bpa, bbp, dbp and dehp in commercial water bottles do not raise serious concern for humans. the aver - age eeq level revealed that bpa, bbp, dbp and dehp in bottled waters may induce adverse estrogenic effects on human health. besides that, the use of bottled water kept in unsuitable conditions is not appropriate and especially for sensitive groups. thus, the occurrence of individual bpa, bbp, dbp and dehp and their association in bottled water need to be veriﬁed to avoid their synergistic effects on human health. data availability statement all relevant data are included in the paper or its supplemen - tary information. references abdelghani, j. i., freihat, r. s. & el - sheikh, a. h. magnetic solid phase extraction of phthalate products from bottled, injectable and tap waters using graphene oxide : effect of oxidation method of graphene. journal of environmental chemical engineering 8 ( 2 ), 103527. https : / / doi. org / 10. 1016 / j. jece. 2019. 103527. abtahi, m., dobaradaran, s., torabbeigi, m., jorﬁ, s., gholamnia, r., koolivand, a., darabi, h., kavousi, a. & saeedi, r. health risk of phthalates in water environment : occurrence in water resources @topic:1


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