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Frontiers of Environmental Science & Engineering

Front. Environ. Sci. Eng.    2015, Vol. 9 Issue (1) : 16-38     https://doi.org/10.1007/s11783-014-0697-2
REVIEW ARTICLE |
Occurrence of bisphenol A in surface and drinking waters and its physicochemical removal technologies
Liping LIANG1,2,Jing ZHANG2,Pian FENG3,Cong LI4,Yuying HUANG1,*(),Bingzhi DONG3,Lina LI1,Xiaohong GUAN3,*()
1. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
2. State Key Lab of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China
3. State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
4. College of Civil Engineering and Architecture, Zhejiang University, Hangzhou 310058, China
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Abstract

Bisphenol A (BPA), an endocrine disrupting compound, has caused wide public concerns due to its wide occurrence in environment and harmful effects. BPA has been detected in many surface waters and drinking water with the maximum concentrations up to tens of μg·L-1. The physicochemical technology options in eliminating BPA can be divided into four categories: oxidation, advanced oxidation, adsorption and membrane filtration. Each removal option has its own limitation and merits in removing BPA. Oxidation and advanced oxidation generally can remove BPA efficiently while they also have some drawbacks, such as high cost, the generation of a variety of transformation products that are even more toxic than the parent compound and difficult to be mineralized. Only few advanced oxidation methods have been reported to be able to mineralize BPA completely. Therefore, it is important not only to identify the major initial transformation products but also to assess their estrogenic activity relative to the parent compounds when oxidation methods are employed to remove BPA. Without formation of harmful by-products, physical separation methods such as activated carbon adsorption and membrane processes are able to remove BPA in water effluents and thus have potential as BPA removal technologies. However, the necessary regeneration of activated carbon and the low BPA removal efficiency when the membrane became saturated may limit the application of activated carbon adsorption and membrane processes for BPA removal. Hybrid processes, e.g. combining adsorption and biologic process or combining membrane and oxidation process, which can achieve simultaneous physical separation and degradation of BPA, will be highly preferred in future.

Keywords Bisphenol A (BPA)      occurrence      conventional oxidation      advanced oxidation      adsorption      membrane filtration     
Corresponding Authors: Yuying HUANG   
Online First Date: 23 April 2014    Issue Date: 31 December 2014
 Cite this article:   
Liping LIANG,Jing ZHANG,Pian FENG, et al. Occurrence of bisphenol A in surface and drinking waters and its physicochemical removal technologies[J]. Front. Environ. Sci. Eng., 2015, 9(1): 16-38.
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http://journal.hep.com.cn/fese/EN/10.1007/s11783-014-0697-2
http://journal.hep.com.cn/fese/EN/Y2015/V9/I1/16
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Liping LIANG
Jing ZHANG
Pian FENG
Cong LI
Yuying HUANG
Bingzhi DONG
Lina LI
Xiaohong GUAN
country water type number ofsampling points median ofconcentrations /(ng·L-1) range/(ng·L-1) reference
Spain river water (NE Spain-Catalonia) 11 4.5 under detection ~2970 [8]
river water (Spain-Granada) --- --- 52.0–219 [9]
Portugal river water (Portugal-Mondego River Estuary) 8 41.5 under detection ~ 590 [10]
river water (Portugal-the Douro River Estuary) 9 2.5 under detection ~10700 [11]
Switzerland river water (Switzerland-Glatt River) 3 0.0 under detection ~4.4 [12]
Korea river water (Korea-Talanta) 5 23.8 under detection ~39.4 [13]
Mexico river water (Mexico-a coastal lagoon) 4 12.3 under detection ~145 [14]
USA river and lake water (USA-New Orleans, Louisiana) 5 60 1.5–113 [15]
bayou River (USA) --- --- 9–44 [15]
China Changjiang River (China-Wuhan) 8 60.45 9.2–198.7 [16]
Pearl River/Dong River (China-Guangzhou) 31 231.9 43.5–639.1 [17]
Jiaozhou Bay (China-Qingdao) 156 18 .4786 .9 6 .7–37.862 .9–3035 [18]
Pearl rivers (Southern China) 15 285.3 2.2–1030 [19]
Pearl River (China-Guangzhou) 14 192.8 97.8–540 [20]
Japan river water (Japan-Tokyo Bay) 5 --- <500–900 [21]
surface seawater(Japan-Tokyo Bay) --- --- 20.2–30.1 [22]
Germany Elbe River (Germany) 16 35.4 16–100 [23]
drinking water (southern Germany) 16 1.1 0.50–2.0 [24]
Belgium river water (Belgium and Italian) 1 48.5 42–55 [25]
Tab.1  Occurrence of BPA in surface and drinking waters
property value
structural formula for BPA
CAS. No 80-05-7
molecular formula C15H16O2
molar mass 228.29 g·mol-1
water solubility (20°C–25 °C) 120–300 mg·L-1
density 1.20 g·cm-3
logKow (25°C) 2.2–3.82
melting point 158–159 °C
boiling point (4 mmHg) 220 °C
vapor pressure (190°C) 87 Pa
henry′s law contant (25°C) 1×10-10
appearance white crystalline solid
LD50a, rat, oral 3300–4240 mg·kg-1
LD50, mouse, oral 2500–5200 mg·kg-1
LD50, fish (Pimephales promelas), 96 h 4.6 mg·L-1
Tab.2  Physico-chemical characteristics of BPA
oxidants reaction rate/(mol-1·L·s-1) degradation products reference
ozone 1.3×104 (pH=2), 1.6×109 (pH=12) [27]
1.68×104 (BPA), 1.06×109 (BPA-), 1.11×109 (BPA2-) [28]
catechol, orthoquinone, muconic acid derivatives of BPA, benzoquinone, 2-(4-hydroxyphenyl)-propan-2-ol [29]
0.48×105 (pH=2), 0.94×105 (pH=5), 1.71×105 (pH=7), 1.16×105 (pH=10) [30]
catechol, resorcinol, acetone, formaldehyde, acetic acid, formic acid, maleic acid, oxalic acid [31]
p-tert-butylphenol, hydroquinone, methyl-dihydrobenzofuran, n-butyl acetate [32]
permanganate 45 (BPA), 6.09×103 (BPA-), 2.25×105 (BPA2-) [34]
12.7 (pH=5), 14.2 (pH=6), 35.8 (pH=7), 240 (pH=8), 870 (pH=9) [35]
ferrate 8.2×102 (BPA), 0.8×105 (BPA-), 2.6×105 (BPA2-) [39]
phenol, p-isopropylphenol, 4-isopropanolphenol, (1-phenyl-1-butenyl)benzene, styrene, p-hydroxyacetophenone, 4-isopropyl-cyclohexa-2,5-dienone, propanedioic acid, oxalic acid [40]
1094 (initial pH=5.5) [41]
chlorine 4-chloro-BPA, 2,6-dichloro-BPA, 2,6-dichloro-BPA, 2,2',6'-trichloro-BPA, 2,2',6,6'-tetrachloro-BPA, trichlorophenol, 4-isopropyl-2'-hydroxylphenol, six kinds of polychlorinated phenoxyphenols [43]
3.10×104 (BPA-), 6.62×104 (BPA2-) [44]
2-chloro BPA (MCBPA), 2,6-dichloro BPA (2,6-D2CBPA), 2,2’-dichloro BPA (2,2’-D2CBPA), 2,2’,6-trichloro BPA (T3CBPA) and 2,2’,6,6’-tetrachloro BPA (T4CBPA), 2,4,6-trichlorophenol (T3CP), 2,6-dichloro-1,4-benzoquinone (D2CBQ), 2,6-dichloro-1,4-hydroquinone (D2CHQ), C9H10Cl2O2, C9H8Cl2O and C10H12Cl2O2 [45]
Tab.3  Reaction rates and degradation products of BPA with traditional oxidants
type of AOPs reaction conditions degradation efficiency/% mineralization efficiency /% reference
sonochemical degradation [BPA]=500 μmol·L-1, ultrasonic system (404 kHz, 3.5 kW·m-2) ~100 (10 h) [76]
[BPA]=500 μmol·L-1, ultrasonic system (404 kHz, 9 kW·m-2) ~100 (3 h) 15.4 (10 h)
[BPA]=500 μmol·L-1, ultrasonic system (404 kHz, 12.9 kW·m-2) ~100 (2 h)
[BPA]=500 μmol·L-1, ultrasonic system (404 kHz, 9 kW·m-2), Fe(II)=4.0 mmol·L-1 ~100 (3 h) 50.2 (10 h)
sonochemical degradation [BPA]=118 μmol·L-1, ultrasonic system (300 kHz, 80 W), 22°C, saturating gas: oxygen, pH=7.0. ~100 (105 min) 9 (105 min) [77]
photo-Fenton [BPA]=118 μmol·L-1, [Fe2+]=100 μmol·L-1, [H2O2]=96 μmol·h-1, 22°C, saturating gas: oxygen, pH=7.0, UV irradiation: solar simulator. ~100 (180 min) 14 (180 min)
sequential helio-photo-Fenton process [BPA]=118 μmol·L-1, ultrasonic system (300 kHz, 80 W), [Fe2+]=100 μmol·L-1, [H2O2]=96 μmol·h-1, 22°C, saturating gas: oxygen, pH=7.0. 92 (60 min) 70 (240 min)
sonochemical degradation [BPA]=118 μmol·L-1, pH=3.0, ultrasonic system (300 kHz, 80 W), 20±2°C 100 (90 min) 5 (180 min) [47]
Fenton process [BPA]=118 μmol·L-1, pH=3.0, [Fe2+]=100 μmol·L-1, [H2O2]=110 μmol·h-1, 20±2°C 100 (90 min) 20 (180 min)
sonochemical degradation [BPA]=0.44 μmol·L-1, pH=6.5, 25±0.5°C, ultrasonic system (20 kHz, 40 W·cm-2) 44.9 (120 min) [50]
[BPA]=0.44 μmol·L-1, pH=6.5, 25±0.5°C, ultrasonic system (20 kHz, 60 W·cm-2) 34.6 (60 min), 51.1 (120 min)
[BPA]=0.44 μmol·L-1, pH=6.5, 25±0.5°C, ultrasonic system (20 kHz, 80 W·cm-2) 55 (120 min)
O3 [BPA]=0.44 μmol·L-1, pH=6.5, 25±0.5°C, O3=10 mL·min-1 63 (60 min)
US+O3 [BPA]=0.44 μmol·L-1, pH=6.5, 25±0.5°C, 20 kHz, 60 W·cm-2, O3=10 mL·min-1 ~100 (60 min)
ultrasonication [BPA]=10 μmol·L-1, ultrasonic system (300 kHz, 0.19 W mL-1), 0.15l min-1 air injection, pH=3.0 ~100 (60 min) [49]
[BPA]=10 μmol·L-1, ultrasonic system (300 kHz, 0.19 W·mL-1), 0.15l min-1 air injection, pH=6.0 ~100 (60 min)
[BPA]=10 μmol·L-1, ultrasonic system (300 kHz, 0.19 W·mL-1), 0.15l min-1 air injection, pH=10.5 90.9 (60 min)
photodegradation [BPA]=520 μmol·L-1, pH=6.7, low-pressure mercury lamp, 15 W, λ=254 nm, 25°C 7.3 (15 min) [78]
[BPA]=520 μmol·L-1, pH=6.7, low-pressure mercury lamp, 15 W, λ=254 nm, 25°C, [H2O2]= 500 μmol·L-1 35 (15 min)
photooxidation [BPA]=8.8 μmol·L-1, pH=3.5, Fe(III)=10.0 μmol·L-1, [Ox]=120.0 μmol·L-1, 28°C, 491 kHz, high-pressure mercury lamp, 125 W, λ≥365 nm 90.2 (40 min) [65]
[BPA]=21.9 μmol·L-1, pH=3.5, Fe(III)=10.0 μmol·L-1, [Ox]=120.0 μmol·L-1, 28 oC, 491 kHz, high-pressure mercury lamp, 125 W, λ≥365 nm 75.4 (80 min)
[BPA]=43.8 μmol·L-1, pH=3.5, Fe(III)=10.0 μmol·L-1, [Ox]=120.0 μmol·L-1, 28°C, 491 kHz, high-pressure mercury lamp, 125 W, λ≥365 nm 38.6 (80 min)
solar photocatalysis [BPA]=438 μmol·L-1, pH=6.0, sunlight, 1.3 mW·cm-2, [TiO2]=5 g·L-1, 30°C ~60 (60 min) 100 (11 h) [61]
H2O2 –assisted photoelectrocatalytic oxidation [BPA]=49.1 μmol·L-1, 8 W, 0.68 mW·cm-2, λ=365 nm, Ti/TiO2 electrode, current intensity 0 mA 13 (180 min) [55]
[BPA]=49.1 μmol·L-1, 8 W, 0.68 mW·cm-2, λ=365 nm, Ti/TiO2 electrode, current intensity 0.2 mA 68 (180 min)
[BPA]=49.1 μmol·L-1, 8 W, 0.68 mW·cm-2, λ=365 nm, Ti/TiO2 electrode, current intensity 1.5 mA 99 (180 min)
photocatalysis (TiO2 powder) [BPA]=21.9 μmol·L-1, TiO2 0.5 g·L-1, blue light, pH=6.0±0.2 with 1.25 mmol·L-1 NaCl as the background electrolyte 35 (2 h) 38 (6 h) [62]
photocatalysis (TiO2 hollow sphere) [BPA]=21.9 μmol·L-1, TiO2 hollow sphere 0.5 g·L-1, blue light, pH 6.0±0.2 with 1.25 mmol·L-1 NaCl as the background electrolyte 40 (2 h) 49 (6 h)
photocatalysis (nitrogen-doped TiO2 hollow sphere) [BPA]=21.9 μmol·L-1, nitrogen-doped TiO2 hollow sphere 0.5 g·L-1, blue light, pH 6.0±0.2 with 1.25 mmol·L-1 NaCl as the background electrolyte 90 (2 h) 66 (6 h)
Co2+/PMS [BPA]=500 μmol·L-1, pH=7.0, [PMS]=0.1 mmol·L-1, [Co2+]=8.5×10-7 mol, T=25°C ~100 38 [79]
UV/Co2+/PMS [BPA]=500 μmol·L-1, pH=7.0, [PMS]=0.1 mmol·L-1, [Co2+]=8.5×10-7 mol, T=25°C, λ=254 nm ~100 45
[BPA]=500 μmol·L-1, pH=7.0, [PMS]=0.1 mmol·L-1, [Co2+]=8.5×10-7 mol, T=25°C, λ=365 nm ~100 49
photolysis (UV) One 1 kW medium-pressure (MP) UV lamp, λ=200-300 nm, 1000 mJ·cm-2 14.5 [69]
four 15 W low-pressure (LP) UV lamp, λ=254 nm, 1000 mJ·cm-2 <5
UV/H2O2 One 1 kW medium-pressure (MP) UV lamp, λ=200-300 nm, 1000 mJ·cm-2, [H2O2]=15 mg·L-1 ~90
four 15 W low-pressure UV lamp, λ=254 nm, 1000 mJ·cm-2, [H2O2]=15 mg·L-1 ~90
UV/H2O2 [BPA]=60 μmol·L-1, low pressure Hg lamp (15 W, 253.7 nm), 3000 mJ·cm-2, room temperature, [H2O2]=10 mg·L-1 80 [72]
[BPA]=60 μmol·L-1, low pressure Hg lamp (15 W, 253.7 nm), 3000 mJ·cm-2, room temperature, [H2O2]=25 mg·L-1 97
[BPA]=60 μmol·L-1, low pressure Hg lamp (15 W, 253.7 nm), 3000 mJ·cm-2, room temperature, [H2O2]=50 mg·L-1 >99
Fenton [BPA]=43.8 μmol·L-1, [H2O2]=4×10-4 mol, [Fe2+]=4×10-5 mol, pH=4.0 90 (9 min) [75]
photo-Fenton [BPA]=43.8 μmol·L-1, [H2O2]=4×10-4 mol, [Fe2+]=4×10-5 mol, pH=4.0, a Xe lamp, λ=320-410 nm, 0.5 mW·cm-2. 100 (9 min) 90 (36 h)
TiO2 photocatalysis [BPA]=118 μmol·L-1, [TiO2]=10 mg·L-1, pH=3.0, temperature: 22±2 °C, solar simulator irradiation 66 (75 min) 5 (4 h) [80]
ultrasound [BPA]=118 μmol·L-1, pH=3.0, temperature: 22±2 oC, ultrasound: 300 kHz, 80 W 100 (120 min) 6 (4 h)
ultrasound, Fe2+ and TiO2 photoassisted- process [BPA]=118 μmol·L-1, [TiO2]=10 mg·L-1, [Fe2+]=5.6 mg·L-1, pH=3.0, temperature: 22±2 °C, ultrasound: 300 kHz, 80 W, solar simulator irradiation 100 (75 min) 93 (4 h)
UV-Na2S2O8 /H2O2-Fe(II) [BPA]=50 μmol·L-1, [Na2S2O8]=0.05 mmol·L-1, 15 W UV lamp, λ=254 nm, [Fe(II)]=0.045 mmol·L-1, [H2O2]=0.1579 mmol·L-1, 25°C 100 (90 min) 91 (300 min) [81]
[BPA]=50 μmol·L-1, [Na2S2O8]=0.05 mmol·L-1, 15 W UV lamp, λ=254 nm, [Fe(III)]=0.045 mmol·L-1, [H2O2]=0.1579 mmol·L-1, 25°C 100 (90 min) 87 (300 min)
Tab.4  Summary of BPA removal by advanced oxidation processes
type adsorbent pH T/°C BET area/(m2·g-1) qmax/(mg·g-1) reference
carbon nanomaterials fullerene NAa RTb 7.21 2.4 [82]
single-walled carbon nanotubes NAa RTb 541 591
multiwalled carbon nanotubes (outer diameters of 8–15 nm) NAa RTb 174 121
multiwalled carbon nanotubes (outer diameters of 20–30 nm) NAa RTb 107 77
multiwalled carbon nanotubes (outer diameters of 30–50 nm) NAa RTb 94.7 103
carbon carbonaceous material prepared at 600°C from by-products of wood processing NAa 25 NA 4.2–18.2 [83]
carbonaceous material prepared at 800°C from by-products of wood processing NAa 25 NA 24.1–31.4
activated carbon purchased from Takeda (coconut shell based) NAa 25 1119 23.5
activated carbon purchased from Sorbonorit (charcoal based) 6.5–7.0 25 1225 129.6 [84]
activated carbon purchased from Merck (charcoal based) 6.5–7.0 25 1084 263.1
activated carbon from almond shells 6.5–7.0 25 1216 188.9
activated carbon purchased from Sorbonorit (charcoal based)-treatment with HCl 6.5–7.0 25 1277 285.7
activated carbon purchased from Merck (charcoal based) -treatment with HCl 6.5–7.0 25 1158 303
activated carbon purchased from Calgon (coconut shell based) 7.0 25 916 328.3 [85]
activated carbon purchased from Calgon (bituminous coal based) 7.0 25 1060 263.2
carbon WV A1100 purchased from Westvaco 7.0 25 1777 378.3 [86]
thermally treated carbon WV A1100 7.0 25 1760 430.3
HNO3-treated carbon WV A1100 7.0 25 1.27 57.1
carbon F400 purchased from Calgon 7.0 25 996 317.7
thermally treated carbon F400 7.0 25 1000 223.5
HNO3-treated carbon F400 7.0 25 900 115.4
porous carbon prepared at 400°C from Moso bamboo NAa 23 2.5 2.1 [87]
porous carbon prepared at 700°C from Moso bamboo NAa 23 251 11.4
porous carbon prepared at 1000°C from Moso bamboo NAa 23 300 41.8
activated carbon purchased from Wako NAa 23 1350 56.5
mesoporous carbon CMK-3 NAa 10 920 276 [88]
NAa 25 920 296
NAa 45 920 263
Tab.5  The adsorption capacity of BPA by various carbon type adsorbents
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