Detection, Occurrence, and Fate of Fluorotelomer Alcohols in

Jul 21, 2017 - For all of the municipal WWTPs, no rain event had taken place in the previous week of the campaign or during sampling days. Flow-propor...
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Detection, Occurrence and Fate of Fluorotelomer Alcohols in Municipal Wastewater Treatment Plants Hongrui Chen, Hui Peng, Min Yang, Jianying Hu, and Yu Zhang Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.7b00315 • Publication Date (Web): 21 Jul 2017 Downloaded from http://pubs.acs.org on July 22, 2017

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Environmental Science & Technology is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.

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Environmental Science & Technology

Unknown precursors of FTOHs? Screen

Horizontal- flow Primary grit chamber clarifier

Influent

Aerobic Biotransformation

Anaerobic

Anoxic

Aerobic

Primary effluent

Secondary clarifier

Rotary fiber disc filter Final effluent

Secondary effluent

Direct Discharge

Internal recycle External recycle

Excess sludge

Sludge thickener

FTOHs Anaerobic/Anoxic Biotransformation Further Transformation

Sludge disposal

8.36 cm×3.36 cm

ACS Paragon Plus Environment

Environmental Science & Technology

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Detection, Occurrence and Fate of Fluorotelomer Alcohols in Municipal

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Wastewater Treatment Plants

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Hongrui Chen1,4, Hui Peng3, Min Yang2,4, Jianying Hu3, Yu Zhang1,4,*

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1. Key Laboratory of Drinking Water Science and Technology, Research Center for

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Eco-Environmental Sciences, Chinese Academy of Sciences,Beijing 100085, China;

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2. State Key Laboratory of Environmental Aquatic Chemistry, Research Center for

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Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; 3. Laboratory for Earth Surface Processes, College of Urban and Environmental Sciences, Peking University, Beijing 100871, China; 4. University of Chinese Academy of Sciences, Beijing 100049, China.

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ACS Paragon Plus Environment

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Environmental Science & Technology

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ABSTRACT

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Fluorotelomer alcohols (FTOHs) are the most well-known precursors of

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perfluoroalkyl carboxylic acids (PFCAs), but limited information is available on their

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occurrence and fate in municipal wastewater treatment plants (WWTPs). The

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occurrence of FTOHs was investigated in influent, secondary effluent and sludge of

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12 municipal WWTPs in nine cities of China. FTOHs were detected in all WWTPs,

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and 8:2 FTOH was the predominant congener, with concentrations of 2.10-11.0 ng/L,

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3.05-12.4 ng/L and 0.36-1.91 ng/g dry weight in the influent, secondary effluent and

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sludge, respectively. Relatively high proportions of long-chain FTOHs (C10-16) were

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mainly detected in sludge samples. The mass balance of FTOHs and PFCAs in one of

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WWTPs with an anaerobic-anoxic-oxic process was further explored. The decrease of

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mass loads were observed for 4:2 FTOH (Mass change percentage: 21±3.3%), 8:2

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FTOH (22±1.5%), and 10:2 FTOH (29±7.3%) through aerobic treatment, while the

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increase

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(perfluorononanoic acid) to 165±15% (perfluorobutyric acid)), suggesting the

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potential biotransformation of FTOHs to PFCAs in the aerobic unit. This work

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provides the first report on the occurrence of FTOHs in sludge samples of municipal

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WWTPs and their mass balance, and highlights a new emission route to environment

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via WWTPs.

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Keywords: Biotransformation; Perfluoroalkyl carboxylic acids; Mass balance;

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Precursor; Derivatization

of

mass

loads

were

observed

for

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PFCAs

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(from

18±16%

Environmental Science & Technology

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INTRODUCTION

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Fluorotelomer alcohols (FTOHs) are a class of important industrial

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intermediates used in the synthesis of fluorinated surfactants and polymeric materials,

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and have been applied in a wide range of products such as paints, adhesives, waxes,

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polishes, metals, electronics, and caulks.1 It has been reported the production volume

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of fluorotelomer increased substantially after the phase-out of PFOS and related

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products around 2000.2 There is increasing evidence that FTOHs can cause endocrine

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disruptive effects in fish and human cells,3-5 and reproduction impairment in fish and

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rat.3,

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perfluoroalkyl carboxylic acids (PFCAs), and transformation of FTOHs to PFCAs has

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been documented in different environments including activated sludge,7 rats,8

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humans,9, 10 and the atmosphere.11 Previous studies have suggested that FTOHs might

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contribute to the increasing temporal trends of long-chain PFCAs (C ≥ 8) in human

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serum10 and eggs of gulls.12

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In addition, FTOHs have been reported to be important precursors of

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Previous studies have confirmed the global distribution of FTOHs in the air of

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Europe (181-288 pg/m3),9, 13 North America (11-165 pg/m3),14 and Asia (51.4-1210

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pg/m3).15 The first comprehensive investigation on FTOHs in water environment was

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conducted in 2008 in Osaka and Kyoto, Japan, and FTOHs were detected in rain

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water (1.43-4.07 ng/L), river water (