1. Karin Helwig MA, MSc, MCWIM Glasgow Caledonian University
The PILLS and noPILLS projects: Strategies for the reduction of pharmaceutical inputs into the aquatic environment
Karin Helwig MA, MSc, MCWIM
Glasgow Caledonian University

2. Presentation Outline Introduction to the projects
Waste water characterisations: UK and transnational
Technology results and overall conclusions
noPILLS rationale and outline
I will briefly introduce both projects. Then talk in more detail about the PILLS project: tell you in more detail what we did in Scotland, what was done in the partner countries and the overall conclusions. Then I will move on to describe what the noPILLS project is about and where we are with that.

3. The Partnership Over the two projects: 2 Water boards 2 Universities
Glasgow
Over the two projects:
2 Water boards
2 Universities
3 research institutes
PILLS: 2008 – 2012, €8M
noPILLS: 2012 – 2015, €7M
Zwolle
Utrecht
Essen
Luxemboug
The partners in PILLS and noPILLS are mostly the same:
Two University partners: GCU and Limoges University,
2 Water associations in Germany and (pills only) The Netherlands
And research institutes in Luxembourg, Switzerland (PILLS only, now advisory board), and the Netherlands (new for noPILLS
Emschergenossenschaft, a German water board, is the lead partner in both projects
The projects are funded to 50% by the EU-INTERREG IV-B-Programme and 50% by the project partners.
PILLS started in 2008 and concluded with a conference in Gelsenkirchen, Germany, in Sept noPILLS builds on the PILLS results and will continue to run til We want to present our results, to discuss our findings with you and open up the discussion on your thoughts on how this topic might develop.
Zürich
Limoges

4. The consumption of pharmaceuticals is increasing across OECD countries, particularly for antidiabetics and antidepressants
Background:
Looking at statistics, one can notice that
The consumption of some pharmaceuticals has nearly doubled from 2000 to 2009 in the OECD Countries
But also worldwide, a large and increasing amount of pharmaceuticals are used, for both: human pharmaceuticals and veterinary drugs .
Pharmaceuticals allow us a better quality of life.
But on the other side … they may also escape into the natural environment and cause negative effects.
Source: HEALTH AT A GLANCE 2011: OECD INDICATORS ©; OECD Health Data 2011, OECD (

5. Scope of PILLS and noPILLS
Factory
Human drugs
Veterinary drugs
Landfill
Groundwater
Care Homes
Households
Hospitals
Surface water
In PILLS, we focused on healthcare institutions as point sources, and on the use of advanced wastewater treatment at these point sources as a way to reduce pharmaceutical pollution.
In the noPILLS project, we are considering human pharmaceutical consumption in a wider context, this time including household consumption and disposal and considering the natural water environment, and here it is also about instigating a societal debate, where strategies other than effluent treatment are investigated – but more on that later.
Wastewater treatment
Drinking water

6. Acknowledgement Thanks to our supporters NHSScotland SEPA
Scottish Water
Before I move on to tell you more about what we did and what we found, I would like to take the opportunity to thank the organisations that have supported us with logistics, data, and expertise: NHS Scotland, SEPA and Scottish Water.

7. Main PILLS objectives WP 1
Analysis
Characterisation of waste water from point sources:
Chemical, ecotox, antibiotic resistant bacteria
Design, construction and operation of advanced waste water treatment technologies at point sources
WP 2
Technology
Assessment of different advanced treatment technologies (Removal of pharmaceuticals, of ecotoxicological effects and antibiotic resistant bacteria; costs and environmental balance)
WP 3
Assessment
WP 4
Communication
The work content of the project has been divided in 4 work packages.
Work package 1 deals with the Characterisation of waste water from point sources regarding their chemical quality as well as their ecotoxicological potential and their relevance of antibiotic resistance bacteria.
In Work package 2, Design, construction and operation of waste water treatment plants at hospital locations are in the focus. Technologies for removal of pharmaceuticals from hospital waste water were further developed and tested in practice.
In Work package 3, the efficiency of the advanced treatment technologies were evaluated regarding the elimination of pharmaceuticals, the reduction of ecotoxicological effects and antibiotic resistant bacteria. Also costs, energy consumption and the overall environmental impact (using a life-cycle assessment methodology) of the advanced treatment technologies were evaluated.
Las but not least, Work package 4 deals with communication issues of the project.
I should mention here that the project was accompanied by a Scientific Advisory Board. with Experts from the Pharmaceutical Industry, from Research Institutions and from Administration.
Dr Andreas Hartman (Novartis Pharma AG, CH); Dr Steger-Hartmann (Bayer Schering Pharma AG, DE); Mark Heggie (Scottish Environment Protection Agency SEPA, UK); Dr Florian Keil (keep it balanced kib); Luc Zwank (Administration de la Gestion de l’Eau, LU); Dr. Thomas Schwartz (Forchungszentrum Karlsruhe, DE); Prof. Dr Pim de Voogt (Institute for Biodiversity and Ecosystem Dynamics, University of Amsterdam, NL)
Communication of the issues and of the results of the project.

8. Drugs selected for monitoring
Out of the 3000 licensed pharmaceuticals, we had to make a selection for monitoring. Criteria central to that were toxicity (PNEC), consumption, hospital contribution, persistency, therapeutic group, and very importantly Commonality of interest.

9. Karin Helwig, Glasgow Caledonian University
UK Rural Situation
Geriatric + Psychiatric Facility
42 Beds
3123 m3/a
Sampler 1
Main Hospital (wards, A&E, theatres, restaurant)
300 Beds
35292 m3/a
60579 m3/a
Sampler 2
Laundry , Nurses housing, Creche
22164 m3/a
WASTE
WATER
TREATMENT
WORKS
Residential population
14200
In Scotland, our main aim was to characterise various effluents in a rural and an urban situation.
Rural – a large regional hospital, connected to a medium sized treatment works. So the hospital is very large for the size of the town, resulting in 22 beds per 1000 population.
We sampled combined effluent from a geriatric and psychiatric lodge, as well as the total hospital effluent just before it leaves the hospital compound. We also had the opportunity to sample an effluent at the treatment works that was nearly all residential, so before the hospital wastewater is mixed in.
Sampler 3
m3/a
Minor Industry
Karin Helwig, Glasgow Caledonian University

10. Karin Helwig, Glasgow Caledonian University
Urban situation
Wastewater Treatment Works 2
Wastewater Treatment Works 1
Sampler 1
Sampler 2
Sampler 3
General Hospital
318 beds
Water Use: 190m3a-1bed-1
Geriatric hospital
120 beds
Water use: 113m3a-1bed-1
1320 beds in 4 hospitals
Residential population
585,000
Other trade
The urban situation is more complicated.
There were two relevant treatment works. They are similar in size and the number of hospital beds, with over half a million residents each and some 1100, 1300 hospital beds. That is a bed provision of just 2.5 per We could not sample at the WWTW that our partner hospitals were connected to, but we assume that in terms of pharmaceutical load they are similar.
It is important to note that there were no less than 10 hospitals connected to the treatment plant, which of course, is important if you consider the option of point source treatment – you would need to build 10 advanced installations to get the hospital contribution out.
We sampled again at a geriatric hospital and at a general hospital.
1145 beds in 8 other hospitals
Residential population of
600,000
Other trade
*other trade effluent not included
Karin Helwig, Glasgow Caledonian University

11. Scottish Sampling Programme
Flow proportionate regime at hospital sites
Time proportionate regime at WWTWs
7 day composite samples at all locations
Sept 2010 to Jan2012:
Hospital sites every week
WWTWs every 4 to 6 weeks
Sampling affected by debris, weather and equipment problems
The sampling regime at the hospitals was flow proportionate but discontinuous, so drugs that are used infrequently might be missed or underrepresented. The pumping station was a very good sampling point in this respect as it allowed us to sample all the flow. At the treatment works, we expected a more even consumption so we used time proportionate sampling. We collected weekly composite samples over a period of about a year, and for one week we also collected 24hour composites.
3 analyses were made for the characterisations: chemical, ecotoxicological and multi-drug resistant bacteria.
Firstly, the pharmaceutical content.

12. Sample analysis Analysis by LC-MS/MS Sample matrix very variable.
Required clean-up using SPE and SLE (supported liquid extraction).
Dilution 1:8 to minimise matrix effects.

13. Analytical Results
So what did we find? I present the analytical results in 3 groups. These are drugs for chronic conditions as well as a pain killer. As expected, we see these drugs in comparable concentrations in residential and hospital effluents.

14. Mean concentrations (ug/l) Contrast agents, cytostatics, anaesthetics
Also as per expectation, x-ray contrast agents, cytostatics and the anaesthetic lidocaine, are found almost exclusively in general hospital effluent.

15. Mean concentrations Antibiotics
For anti biotics, we were not quite so sure what to expect because they are also used a lot in the community, but found significantly higher concentrations in the general hospital and still quite high in the geriatric hospitals.

16. Hospital contribution to load - transnational
Hospital contribution to pharmaceutical loads in investigated catchment areas (%)
We have reported that about 20% of pharmaceuticals are administrated at hospitals whereas 80% are distributed in the community.
But still, considering regional and local catchments hospitals can be seen as hot spots for pharmaceuticals emission to wastewater; especially for substances such as cytostatics, antibiotics and x-ray contrast media, and there is a lot of variation from region to region.
6.1 to 14.1 beds per 1,000 inhabitants

17. Eco-tox principles
Test species are surrogates for all fauna in the aquatic ecosystem
Primary Producers
Primary Consumers
Secondary Consumers
The second characterisation that was made was the ecotox analysis.

18. Bioassay objectives within PILLS
1. Characterisation of the hospital wastewater
Comparison between hospital wastewater and community wastewater looking at the whole effluent sample.
- Complex mixtures
- Interactive effects
- Bioavailability
- Unknown chemicals
Partners involved: UK; DE; NL; CH
2. Assessment of advanced wastewater treatment on toxicity

19. UK Ecotox results
On the left, t.he results from the algal test (growth inhibition). On the right, the bacterial test (bioluminescence). The way to read these is that if the value here is 1, then the undiluted effluent would result in an effect in 50% of the organisms. You see that the general hospital effluent was the most toxic.

20. Combined results from all PILLS partners
Transnational Characterisation of the hospital wastewater
Combined results from all PILLS partners
End point
Bio assay
Community
Hospital
Specific
Cytotoxicity
MTT test
no negative effects
weak or moderate effect
Mutagenicity
Ames test
Non-specific
luminescence inhibition
Vibrio fischeri
strong effect
photosynthesis inhibition
Selenastrum capricornutum
growth rate inhibition
Desmodesmus subspicatus
Mortality
Gammarus fossarum
Raw hospital WW toxic to a range of test organisms
Across the PILLS partners, hospital WW was more toxic than community WW
Not all hospitals are the same: general hospitals were more toxic than geriatric hospitals

21. Antibiotic resistance
I won’t go into the antibiotic resistance testing in detail but will just say that the relative abundance of multi-drug resistant bacteria was higher in hospital effluent than in other waters.

22. Technology - Investigated advanced treatment processes
Membrane filtration
Oxidation processes
Adsorption on activated carbon
Microfiltration
Ozonation
Powdered activated carbon
Ultrafiltration
Advanced oxidation processes (UV/Ozone, UV/H2O2, Ozone/H2O2, Fenton reactions, UV/TiO2. )
Granulated activated carbon
Reverse osmosis
WP Technology
This slide shows the treatment processes which were investigated in the PILLS project.
Micro-filtration and Ultra-filtration were not intended to eliminate pharmaceutical residues. These processes are integrated in the biological treatment as a Membrane Bioreactor. In this way, the suspended solids are separated from the water effluent that can then be efficiently treated with the advanced treatment processes which can focus directly on micropollutants.
As you can see, we have investigated a broad range of currently discussed techniques for the elimination of micropollutants in waste water.

23. Good effluent quality of MBR (COD, N, P)
Efficient removal of some compounds
Half of the analyzed compounds removed to < 50%
When decentralized treatment should be built, we found out that a MBR is an important first step for pharmaceuticals elimination. MBR guarantee a good effluent quality regarding classical parameters such as COD, Nitrogen and Phosphorus. MBR also removes some of the investigated pharmaceuticals efficiently, but not all of them.

24. Removal efficiencies of ozone and activated carbon are mostly similar
After the MBR, the removal rates of pharmaceuticals by ozone or activated carbon are comparable.
Ozone or PAC leads to 80% removal for most compounds, but not for all. A fresh GAC filter with RO led to high elimination rates for all compounds.

25. Efficient removal of multi resistant bacteria Integrons by MBR
GAC
Furthermore, MBR was also very efficient to remove antibiotic resistant bacteria from wastewater, when ultrafiltration membranes were used.
The removal rates of these bacteria by ozone and activated carbon were negligible compared to those of the ultrafiltration membranes.

26. Costs are dominated by components which are necessary for the biological treatment
The main part of the costs for investment and operation are spent for the biological treatment. The costs increased only marginally by implementation of the advanced treatment processes.
* Including all components except the advanced treatment processes

27. Key Conclusions from PILLS
Hospitals can be seen as a ‘hot spot’ for pharmaceuticals but strong variation by compound
A single hospital in a rural situation has a much greater contribution to load than a single hospital in an urban situation
Hospital effluent considerably more toxic than community effluent
Higher proportion of multi-resistant bacteria in hospital effluent, which can reach the environment via e.g. CSOs
Point source treatment can reduce both ecotox risk and risk from multi-resistant bacteria

28. Key Conclusions from PILLS
MBR treatment leads to good quality wastewater in terms of COD, nutrients and bacteria but insufficient removal for (some) pharmaceuticals
GAC with RO leads to high removal for all compounds
Oxidation processes can lead to increased toxicity
GAC can result in increased multidrug resistance

29. Key Conclusions from PILLS
Although advanced treatment at point sources can be effective, either centralised or decentralised treatment will be expensive and has a high energy cost.
Removal of all pharmaceuticals from wastewater is hardly reasonable and a reduction of inputs should be explored

30. NoPILLS Key fields of interest
1) Awareness raising
Campaigns on sub catchment levels
Advising campaigns for target groups
Data dissemination via blogs, apps or social networks
2) Demonstration tools
Advanced treatment facilities in Germany and Luxembourg
3) Impact assessment and evaluation:
load before and after advising campaigns
recommendations for strategic / technical approaches
4) Project related communication and exchange
feed into societal debate

31. The GCU Interdisciplinary Team:
Social Sciences:
Attitudes, behaviours and preparedness to consumption and disposal behaviour
Supply chain analysis and stakeholder mapping
Environmental Management:
Catchment analysis of sources, pathways and receiving waters
Water management and treatment evaluation
Biological and Biomedical Sciences:
Ecotoxicological effects of pharmaceuticals and effluents
Chemical Analytical Sciences:
Quantifying pollutants in effluents and environmental waters

32. Monitoring Proposal 3-pronged environmental research programme:
Removal efficiencies of existing treatment facilities
Effects of diverting surface drainage away from the foul sewer via SUDS
Distributions in a river catchment

33. Gauging Station Adapted from [1] and [2] 6.22m3/s 0.56m3/s 4.36m3/s
Whitburn Gauging Station
Almondell Gauging Station
Craigiehall Gauging Station 1 3 2 5 6 7 8 9
0 – 200 PE
200 – 10,000 PE
10,000 – 50,000 PE
50,000 PE
WWWTW by Treatment Capacity in Population Equivalents
0.80m3/s
= mean annual flow
0.8m3 4
0.95m3/s
0.89m3/s
0.16m3/s
4.36m3/s
6.22m3/s
0.56m3/s
Adapted from [1] and [2]

34. Thank you Further information: www.pills-project.eu www.no-pills.eu
Summary report available
for download

35. References
[1] SEPA (2011) River Almond Catchment Profile, available from: accessed 20/8/2013
[2] CEH (no date) National River Flow Archive, available from: accessed 24/8/2013