Occurrence and control of selected antibiotics and antiretroviral drugs in urban hydrological cycles

95 Pages·2017·2.75 MB·English

by  Elijah Ngumba

JYVÄSKYLÄ STUDIES IN BIOLOGICAL AND ENVIRONMENTAL SCIENCE
341
Elijah Ngumba
Occurrence and Control of Selected
Antibiotics and Antiretroviral Drugs
in Urban Hydrological Cycles
JYVÄSKYLÄ STUDIES IN BIOLOGICAL AND ENVIRONMENTAL SCIENCE 341
Elijah Ngumba
Occurrence and Control of Selected
Antibiotics and Antiretroviral Drugs in
Urban Hydrological Cycles
Esitetään Jyväskylän yliopiston matemaattis-luonnontieteellisen tiedekunnan suostumuksella
julkisesti tarkastettavaksi yliopiston Ambiotica-rakennuksen salissa YAA303
helmikuun 16. päivänä 2018 kello 12.
Academic dissertation to be publicly discussed, by permission of
the Faculty of Mathematics and Science of the University of Jyväskylä,
in building Ambiotica, auditorium YAA303, on February 16, 2018 at 12 o’clock noon.
UNIVERSITY OF JYVÄSKYLÄ
JYVÄSKYLÄ 2018
Occurrence and Control of Selected
Antibiotics and Antiretroviral Drugs in
Urban Hydrological Cycles
JYVÄSKYLÄ STUDIES IN BIOLOGICAL AND ENVIRONMENTAL SCIENCE 341
Elijah Ngumba
Occurrence and Control of Selected
Antibiotics and Antiretroviral Drugs in
Urban Hydrological Cycles
UNIVERSITY OF JYVÄSKYLÄ
JYVÄSKYLÄ 2018
Editors
Anssi Lensu
Department of Biological and Environmental Science, University of Jyväskylä
Pekka Olsbo, Sini Tuikka
Publishing Unit, University Library of Jyväskylä
Jyväskylä Studies in Biological and Environmental Science
Editorial Board
Jari Haimi, Anssi Lensu, Timo Marjomäki, Varpu Marjomäki
Department of Biological and Environmental Science, University of Jyväskylä
Cover photos: Tuula Tuhkanen and Elijah Ngumba
Permanent link to this publication: http://urn.fi/URN:ISBN:978-951-39-7344-5
URN:ISBN:978-951-39-7344-5
ISBN 978-951-39-7344-5 (PDF)
ISBN 978-951-39-7343-8 (print)
ISSN 1456-9701
Copyright © 2018, by University of Jyväskylä
Jyväskylä University Printing House, Jyväskylä 2018
ABSTRACT
Ngumba, Elijah
Occurrence and control of selected antibiotics and antiretroviral drugs in urban
hydrological cycles
Jyväskylä: University of Jyväskylä, 2018, 71 p.
(Jyväskylä Studies in Biological and Environmental Science
ISSN 1456-9701; 341)
ISBN 978-951-39-7343-8 (print)
ISBN 978-951-39-7344-5 (PDF)
Yhteenveto: Antibioottien ja antiretroviraalisten lääkeaineiden esiintyminen ja
kontrolli urbaanissa hydrologisessa kierrossa
Diss.
The occurrence of active pharmaceutical ingredients (APIs) including
antibiotics and antiretroviral drugs in the environment has been identified as an
environmental challenge in the last two decades. The main objective of this
thesis was to determine the occurrence and control of selected antibiotics and
antiretroviral drugs in the aquatic environment of three urban hydrological
cycles of Nairobi-Kenya, Lusaka-Zambia and Jyväskylä-Finland. First, a
multiresidue analytical method for trace determination of the analytes based on
solid phase extraction and liquid chromatography tandem mass spectrometry
was developed. In treated municipal wastewater, the maximum mean
concentrations for individual pharmaceuticals were 537 ng l-1 in Jyväskylä,
55760 ng l-1 in Lusaka and 3940 ng l-1 in Nairobi. Similarly, high surface water
concentrations of up to 13800 ng l-1 in Nairobi and 49700 ng l-1 in Lusaka
compared with 54 ng l-1 in Jyväskylä were measured. The compounds were
only sporadically present in Lusaka groundwater samples with concentration in
ranging from below the limit of quantification to 880 ng l-1. High individual
pharmaceutical concentrations of up to 12.8 mg l-1 were measured in Lusaka
source separated urine implying that source separation can be a significant
barrier to environmental contamination. The high antibiotics and antiretroviral
drugs concentrations in Nairobi and Lusaka was attributed to high disease
prevalence especially HIV/AIDS, unregulated sale of antibiotics as well as
inadequate or absence of waste collection and treatment facilities. Evaluation of
post-treatment removal of three of the antibiotics and three of the antiretroviral
drugs by UV photolysis and advanced oxidation processes (UV/Cl(cid:909) and
UV/H(cid:909)O(cid:909)(cid:4667)(cid:3)(cid:149)(cid:138)(cid:145)(cid:153)(cid:135)(cid:134)(cid:3)(cid:150)(cid:138)(cid:131)(cid:150)(cid:3)(cid:150)(cid:138)(cid:135) UV/H(cid:909)O(cid:909)(cid:3)(cid:146)(cid:148)(cid:145)(cid:133)(cid:135)(cid:149)(cid:149) required the lowest electrical
energy to remove 90 % of the pharmaceuticals.

Keywords: Antibiotics; antiretroviral drugs; groundwater; post-treatment;
source separated urine; surface water; wastewater.

Elijah Ngumba, University of Jyväskylä, Department of Biological and Environmental
Science, P.O. Box 35, FI-40014 University of Jyväskylä, Finland
Author’s address Elijah Ngumba
Department of Biological and Environmental Science
P.O. Box 35
FI-40014 University of Jyväskylä
Finland
[email protected]

Supervisors Professor Tuula Tuhkanen
Department of Biological and Environmental Science
P.O. Box 35
FI-40014 University of Jyväskylä
Finland

Professor Anthony Gachanja
Department of Chemistry
Jomo Kenyatta University of Agriculture and Technology
P.O. Box 62000
00200 Nairobi
Kenya

Reviewers Dr Anna-Lea Rantalainen
Department of Environmental Sciences
University of Helsinki
Niemenkatu 73
FI-15140 Lahti
Finland

Professor Marina Trapido
Tallinn University of Technology
Ehitajate Tee 5
19086 Tallinn
Estonia

Opponent Dr Jerker Fick
Department of Chemistry
Umeå University
SE-90187 Umeå
Sweden
CONTENTS
ABSTRACT
CONTENTS
LIST OF ORIGINAL PUBLICATIONS

1(cid:3) INTRODUCTION ..................................................................................................... 7(cid:3)
1.1(cid:3) General introduction ...................................................................................... 7(cid:3)
1.2(cid:3) Selected pharmaceuticals .............................................................................. 9(cid:3)
1.3(cid:3) Pharmaceuticals in WWTPs, surface water and groundwater .............. 11(cid:3)
1.4(cid:3) Ecological sanitation and control environmental contamination ......... 16(cid:3)
1.5(cid:3) Analytical techniques .................................................................................. 16(cid:3)
1.5.1(cid:3) Solid Phase Extraction ......................................................................... 16(cid:3)
1.5.2(cid:3) Liquid chromatography-mass spectrometry and calibration ....... 17(cid:3)
1.6(cid:3) Removal of pharmaceuticals in WWTPs .................................................. 19(cid:3)
1.6.1(cid:3) Removal by conventional activated sludge process ....................... 19(cid:3)
1.6.2(cid:3) Removal by wastewater stabilization ponds ................................... 20(cid:3)
1.7(cid:3) Post-treatment removal of pharmaceuticals in wastewater ................... 21(cid:3)
1.7.1(cid:3) Direct UV photolysis ........................................................................... 21(cid:3)
1.7.2(cid:3) UV/Hydrogen peroxide advanced oxidation process ................... 21(cid:3)
1.7.3(cid:3) UV/Chlorine advanced oxidation process ...................................... 22(cid:3)
2(cid:3) OBJECTIVES OF THE STUDY .............................................................................. 24(cid:3)
3(cid:3) MATERIALS AND METHODS ............................................................................ 25(cid:3)
3.1(cid:3) Chemicals ...................................................................................................... 25(cid:3)
3.2(cid:3) Sampling ........................................................................................................ 25(cid:3)
3.3(cid:3) Post-treatment removal of pharmaceuticals (IV) ..................................... 27(cid:3)
3.4(cid:3) Analytical methods ...................................................................................... 28(cid:3)
3.4.1(cid:3) SPE-LC-MS/MS optimization (I, II) .................................................. 28(cid:3)
3.4.2(cid:3) Matrix-matched and internal standard quantification (II) ............ 29(cid:3)
4(cid:3) RESULTS AND DISCUSSION .............................................................................. 30(cid:3)
4.1(cid:3) Analytical methods ...................................................................................... 30(cid:3)
4.1.1(cid:3) LC-MS/MS optimization (I, II) .......................................................... 30(cid:3)
4.1.2(cid:3) Solid phase extraction (I, II) ............................................................... 33(cid:3)
4.1.3(cid:3) Analytical method performance (I, II) .............................................. 34(cid:3)
4.1.4(cid:3) Matrix-matched and internal standard quantification (II) ............ 35(cid:3)
4.2(cid:3) Pharmaceuticals in the WWTPs (I, II, III) ................................................. 36(cid:3)
4.3(cid:3) Pharmaceuticals in surface waters (I, II, III) ............................................. 38(cid:3)
4.4(cid:3) Pharmaceuticals in groundwater (III) ....................................................... 41(cid:3)
4.5(cid:3) Pharmaceuticals in source separated urine (III) ...................................... 44(cid:3)
4.6(cid:3) Post-treatment removal of pharmaceuticals (IV) ..................................... 46
4.6.1(cid:3) Removal of pharmaceuticals by direct UV photolysis (IV) ........... 46(cid:3)
4.6.2(cid:3) Effect of H(cid:909)O(cid:909) and Cl(cid:909) in UV post-treatment of wastewater (IV) 46(cid:3)
4.6.3(cid:3) Energy consumption by UV post-treatment processes (IV) .......... 48(cid:3)
5(cid:3) CONCLUSIONS ...................................................................................................... 49(cid:3)
5.1(cid:3) Occurrence and control of pharmaceuticals ............................................. 49(cid:3)
5.2(cid:3) Suggestions for future work ....................................................................... 50(cid:3)
Acknowledgements ............................................................................................................ 51(cid:3)
YHTEENVETO (RÉSUMÉ IN FINNISH) .................................................................... 53(cid:3)
REFERENCES .................................................................................................................. 55(cid:3)
LIST OF ORIGINAL PUBLICATIONS
This thesis is based on the following four original publications, referred to in
the text by roman numerals I–IV.
In papers I and IV, Ngumba Elijah (NE) planned and performed the
experiments, interpreted the results and wrote the paper with inputs from
Tuhkanen Tuula (TT) and Gachanja Anthony (GA). In paper II, NE planned the
experiments, Kosunen Päivi (KP) did the preliminary experiments, NE
interpreted the results and wrote the paper with inputs from TT, GA and KP. In
paper III, NE planned the experiments, Maldonado Johanna (MJ) did the
sampling and sample preparation, NE did the final sample analysis, interpreted
the results and wrote the paper with inputs from TT, GA, MJ and James
Nyirenda.
I.(cid:3) Ngumba E., Gachanja A. & Tuhkanen T. 2016. Occurrence of selected
antibiotics and antiretroviral drugs in Nairobi River Basin, Kenya. Science
of the Total Environment 539: 206–213.
II.(cid:3) Ngumba E., Kosunen P., Gachanja A. & Tuhkanen T. 2016. A
multiresidue analytical method for trace level determination of
antibiotics and antiretroviral drugs in wastewater and surface water
using SPE-LC-MS/MS and matrix-matched standards. Analytical Methods
8: 6720–6729.
III.(cid:3) Ngumba E., Maldonado J., Nyirenda J., Gachanja A. & Tuhkanen T.
Occurrence of antibiotics and antiretroviral drugs in source separated
urine, groundwater surface water and wastewater in the peri–urban
area of Chunga in Lusaka, Zambia. (Submitted manuscript)
IV.(cid:3) Ngumba E., Gachanja A. & Tuhkanen T. Removal of selected antibiotics
and antiretroviral drugs during post-treatment of municipal wastewater
with UV, UV/chlorine and UV/hydrogen peroxide. (Manuscript)