the efficiency of constructed wetlands for the removal of the antimicrobial agent triclosan from ...

189 Pages·2012·4.63 MB·English

THE EFFICIENCY OF CONSTRUCTED WETLANDS
FOR THE REMOVAL OF THE ANTIMICROBIAL AGENT TRICLOSAN
FROM WASTEWATER

A DISSERTATION
SUBMITTED TO THE GRADUATE SCHOOL
IN PARTIAL FULFILLMENT OF THE REQUIREMENTS
FOR THE DEGREE
DOCTOR OF EDUCATION IN SCIENCE
BY
ELIZABETH R. ZINN
DISSERTATION ADVISOR: DR. JARMILA POPOVICOVA

BALL STATE UNIVERSITY
MUNCIE, INDIANA
DECEMBER, 2012
To Raymond and Gail Zinn who always believed in me

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ACKNOWLEDGEMENTS

Over the past seven years I have received support and encouragement from a
great number of individuals. Dr. Jarmila Popovicova has graciously given time, energy
and expertise to this project. I appreciate all of her support and guidance in this process.
I would like to thank my dissertation committee of Dr. Amy Gregg, Dr. Melody Bernot,
Dr. Thalia Mulvihill, and Dr. Lee Florea for their support as I moved from an idea to a
completed study. In addition, Dr. Holmes Finch provided valuable statistical advice and
Dr. James Elflin and Connie Tyner helped me navigate a complicated graduate degree
program. During data collection and writing, Alfredo Garcia at the LaGrange County
Health Department provided help with my study sites and encouraged me to see the value
of this research. My colleagues at Merry Lea Environmental Learning Center graciously
supported me as I juggled work, school and research. I would also like to thank the
undergraduate student researchers from Goshen College who helped in the pilot study
research. Finally, I would like to thank Hannah Miller who spent countless hours
proofreading, listening to me talk about my research, and providing support and
encouragement.

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TABLE OF CONTENTS

ABSTRACT ……………………………………………………………………. ...... iii
DEDICATION ……………………………………………………………………. .. iv
ACKNOWLEDGEMENTS ……………………………………………………… .... v
LIST OF TABLES ……………………………………………………………….. .... x
LIST OF FIGURES ……………………………………………………………… xiv
Chapter

1. REVIEW OF RELEVANT LITERATURE ………………………………. ... 1
a. Introduction ………………………………………………………… . 1
b. PPCPs in the Environment …………………………………………. . 3
i. The Antibacterial Agent Triclosan ………………………… .. 4
c. The Fate of Triclosan in the Environment and its Potential
Effects ………………………………………..……………………. 5
i. The Fate of Triclosan in the Environment …………..……… 6
ii. The Effects of Triclosan on the Environment ………...……. . 7
iii. Triclosan and Human Health ……………………...………. 10
iv. Implication for Triclosan Derivatives ……………...……… 11
d. Centralized Wastewater Treatment for PPCPs and Triclosan …..…. 12
i. PPCPs and Wastewater Treatment …………………….…… 13
ii. Concentrations of Triclosan in Wastewater ……………....... 14
iii. Triclosan Removal in Centralized Wastewater Treatment .... 15
iv. Triclosan Removal Through Primary Treatment ………….. 17
v. Triclosan Removal Through Secondary Treatment ……...... 17
vi. Triclosan Removal Through Finishing Treatments ……...... 21
vii. Triclosan Concentrations in Sludge …………………...….. 22
e. Onsite Wastewater Treatment and Triclosan Removal ……….….... 23
i. Use of Onsite Systems in the United States ……….........… . 23
ii. Triclosan in Septic Tanks ………………………………..…. 24
f. Constructed Wetlands for Wastewater Treatment and
Potential for Triclosan Removal …………………………….....… 26
i. BOD, TSS and Nutrient Removal in Constructed
Wetlands ………………………………...………..…….. . 29
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ii. The Effects of Conditions and Design on Removal
Efficiencies ………………………...………………..…. .. 32
iii. Comparison of Horizontal Flow (HF) and Vertical
Flow (VF) Wetlands ……………………………...…....... 33
iv. Research on Non-Nutrient Chemicals
in Constructed Wetlands ………………………..……….. 35
v. Mechanisms for Removal of Triclosan in Constructed
Wetlands …………………………………………………. 37
vi. Triclosan Removal in Pilot Scale Studies and Constructed
Wetlands …………………………………..…………….. 38
g. Conclusion …………………………………………………………. 40
h. Citations ………………………………………………………….. .. 44

2. CHAPTER 2 – EFFICIENCY OF CONSTRUCTED WETLANDS TO
REMOVE AN ANTIMICROBIAL AGENT TRICLOSAN FROM
WASTEWATER ………………………………………………………. ... 53
a. Abstract …………………………………………………………... .. 53
b. Introduction ………………………………………………………. .. 54
c. Materials and Methods ………..…………………………………... . 60
i. Studies ……………………………………………………. .. 60
ii. Study Sites …………………………………………………. 60
iii. Triclosan Injection Study ……………………………….… . 63
iv. Sampling Collection ……………………………………… .. 64
v. Analysis of triclosan …………………………………….… 65
vi. Recording Environmental Variables ……………………..... 66
vii. Analysis of Plant Composition ……………………………. 67
viii. Data Analysis ……………………………………………... . 68
d. Results and Discussion ………………………………………….… 69
i. Triclosan Injection Study ………………………………….. 69
ii. Triclosan Removal in Three HF Wetlands ……...………… 70
iii. Plant Composition in Constructed Wetlands ……………... . 74
iv. Horizontal Flow and Vertical Flow Wetland Design
Comparison ……………………………………….…..… . 75
1. Historical Wetland Performance ………………..… . 75
2. Triclosan Removal ………………….…………….. . 79
3. Wetland Design Comparison ………..…………..… 82
v. The Role of HRT in Triclosan Removal ………………. ....... 84
vi. Sorption as a Removal Mechanism in Constructed
Wetlands ………………………………………………. ..... 85
vii. Research Implications ……………………………………. ... 87
e. Conclusion ………………………………………….……………… 88
f. Citations …………………………………………….……………. .. 90

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3. CHAPTER 3 – THE REMOVAL OF TRICLOSAN FROM LABORATORY
SCALE CONSTRUCTED WETLANDS WITH FOUR SPECIES OF
WETLAND PLANTS …………………………………………………. .. 96
a. Abstract ……………………………………………………………. 96
b. Introduction ………………………………………………………. .. 97
c. Materials and Methods ……………………………………………. 101
d. Results and Discussion …………………………………………….105
e. Research Implications …………………………………………. ..... 111
f. Conclusion ……………………………………………………….. 112
g. Citations ………………………………………………………….. 113

4. CHAPTER 4 – ADDITIONAL RESEARCH: DETERMINATION OF THE
HYDRAULIC RETENTION TIME IN AN OPERATIONAL SUBSURFACE
CONSTRUCTED WETLAND …………………..………..…………... . 117
a. Abstract ……………………………………………………….….. 117
b. Introduction …………………………………………………….… 117
i. Research Goals ………………………………………….... 117
ii. Hydraulic Retention Time Background ………………….. 118
c. Materials and Methods ………………………………….……….. . 120
d. Results and Discussion ………………………………….………... 122
e. Conclusion ……………………………………………….……….. 125
f. Citations. ………………………………………………………….. 126

5. CHAPTER 5: ADDITIONAL RESEARCH METHODS: THE EVALUATION
OF A SUBSURFACE CONSTRUCTED WETLAND FOR THE
TREATMENT OF IRON, PHOSPHORUS,AMMONIA, NITRITE, NITRATE,
DISSOLVED OXYGEN, PH, AND E. COLI ……….……….……….. . 128
a. Purpose and Background …………………………………….. ....... 128
b. Constructed Wetland Background ……………………………….. 128
c. Materials and Methods .......................................................... .......... 130
d. Citations………………………………………………………… .... 134

Appendix

A. PERFORMANCE DATA FOR THE RIETH VILLAGE CONSTRUCTED
WETLAND (SITE C) ……………………………………….………… . 135

B. VEGETATION DATA COLLECTED FOR CONSTRUCTED WETLANDS
SITES A-F …………………………………….………………………. . 137

C. RESULTS FOR DYE TRACING STUDY IN THE RIETH VILLAGE
CONSTRUCTED WETLAND (SITE C) …………………...………… . 139

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D. RESULTS FROM TRICLOSAN INJECTION INTOSITE C (RIETH VILLAGE)
CONSTRUCTED WETLAND ……………………………………….. ... 141

E. APPENDIX E – RESULTS FROM TRICLOSAN AND PHYSICO-CHEMICAL
TESTING ON CONSTRUCTED WETLAND SITES (A-F)…………….. 143

F. APPENDIX F – QUALITY CONTROL AND CALIBRATION ……….. . 157

G. APPENDIX G – RESULTS FROM LABORATORY SCALE TESTS OF
TRICLOSAN REMOVAL ………………………………………….... ...... 174

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LIST OF TABLES

Table 1.1 – Research summary of data collection times and chapter
locations ………………………………………………………………………. . 43

Table 2.1 – Summary of wetland sites investigated by this study. ……………… .. 62

Table 2.2 – Mean results for three of the five selected wetland sites for
a range of parameters ………………………………………………………… ... 71

Table 2.3 – Removal of triclosan at Sites C, G, and H constructed wetlands …. ... 71

Table 2.4 – Species in Sites A-H …………………………………………………. 75

Table 2.5 - Mean values for water quality parameters in studied horizontal
flow (HF) and vertical flow (VF) constructed wetlands (2004-2008) ………….77

Table 2.6 - Mean and standard deviations for pH and dissolved oxygen
concentrations at studied wetlands ……………………………………………. 78

Table 2.7 - Mean with standard deviation, median, maximum and minimum
concentrations for air and water temperature during the time of sampling ….. . 79

Table 2.8 - Concentrations of triclosan found in the influent and effluent of six
constructed wetlands …………………………………………………………. 77

Table 2.9 - Mean percent removal of triclosan in the six constructed wetlands in the
wetlands design comparison study ……………………………………………. 82

Table 2.10 - Percent removal from three different studies conducted on Site C .. ... 84

Table 3.1 – Mean values for plant biomass, daily water replacement and pH in
the test containers …………………………………………………………… . 105

Table 4.1 – Mean temperature and precipitation and the maximum daily
precipitation during the test periods for Run 1 and Run 2 ………………… ... 123

Table A.1 - Measured concentrations of various chemicals in the
Reith Village …………………………………………………………… ......... 129

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Table A.2 – Mean concentrations of iron, phosphorus, ammonia, nitrite, and nitrate
in the influent and effluent of the Rieth Village constructed wetland ……… .. 130

Table A.3 – E. coli density (cfu per 100 ml of sample) at the influent and effluent
at Rieth Village constructed wetland ……………………………………. ...... 130

Table A.4 – Measured concentrations and means for DO, pH, water temp.
and depth in the influent and effluent water of the Rieth Village
constructed wetland ……………………………………………………… ...... 130

Table B.1 - Relative frequencies for vegetation found in the six constructed
wetlands (Sites A-F) ………………………………………………………… . 131

Table B.2 - Relative frequencies for vegetation found in constructed wetland
Sites G and H …………………………………………………………… 132
Table C.1- Concentration of dye in the wetland effluent each day after dye
injection for Run #1 ………………………………………………………… .. 133

Table C.2- Concentration of dye in the wetland effluent each day after dye
injection for Run #2 ………………………………………………………… .. 134

Table C.3 – Mean precipitation for the periods of June 2-25, 2009 (Run 1) and
July 1-24, 2009 (Run 2) …………………………………………………… .... 134

Table D.1- Triclosan concentrations in influent and effluent after injection in
Rieth Village constructed wetland (Site C) ……………………………… ...... 135

Table E.1 - Triclosan concentrations in the influent and effluent of the six
constructed wetlands for each sample day ………………………………… ... 137

Table E.2 – Table E.2 – Triclosan concentrations in the influent and effluent
water for constructed wetland Sites C, G and H …………………………… .. 137

Table E.3—Air temperature at the time of water sample collection at the six
constructed wetlands ………………………………………………………… 141

Table E.4 - Water temperature of influent water in constructed wetlands at the
time of water sample collection …………………………………………… .... 142

Table E.5—Water temperature in effluent water at constructed wetlands at the
time of water sample collection ……………………………………………….143

Table E.6 - Dissolved oxygen concentrations in the constructed wetland influent
at the time of water sample collection ……………………………………… .. 144
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Table E.7 - Dissolved oxygen concentrations in the constructed wetland effluent
at the time of water sample collection ………………………………………. . 145

Table E.8 - The distance from the constructed wetland surface to the top of the
water table at the time of water sample collection ………………………… ... 146

Table E.9 - Total rainfall amounts for the week preceding the time water sample
collection ........................................................................................................... 147

Table E.10 - The mean air temperature for the week proceeding each water sample
collection time. ................................................................................................... 148

Table E.11 - pH concentrations in the constructed wetland influent water at
the time of sample collection. ............................................................................. 149

Table E.12 - pH levels in the constructed wetland effluent water at the time
of sample collection ………………………………………………………… .. 150

Table E.13 – Dissolved oxygen, temperature, pH, and depth for
Sites C, G, and H. .............................................................................................. 150

Table F.1 – Quality control samples for triclosan test run on 8/22/08 ………… . 151
Table F.2 – Quality control samples for triclosan test run on 9/05/08 ………… . 152
Table F.3 – Quality control samples for triclosan test run on 9/16/08 ………… . 153
Table F.4 – Quality control samples for triclosan test run on 9/27/08 ……… ..... 154
Table F.5 – Quality control samples for triclosan test run on 10/10/08 ………… 155
Table F.6 – Quality control samples for triclosan test run on 10/21/08 ……… ... 156
Table F.7- Quality Control Standards and Blanks for Iron, Phosphorus,
Ammonia, Nitrite and Nitrate on Reith Village Constructed Wetland …… ..... 157

Table F.8 – Duplicate sample runs for testing of influent and effluent water in
the Rieth Village constructed wetland ……………………………………… .. 157

Table F.9 – Triplicate plate counts for E. coli on influent and effluent water
samples taken from Rieth Village constructed wetland in June, 2007 …… ..... 158

Table F.10 – Quality control samples for triclosan tests run between 6/16/07
and 7/27/07 on constructed wetlands C, G, and H ……………………………158
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