Polybrominated diphenyl ethers

(PBDEs): challenges for the

environment
Date: October 2021
Contents

Executive summary.............................................................................................................. 2
1. Introduction...................................................................................................................... 4
2. Use pattern....................................................................................................................... 5
3. Sources, emissions and pathways................................................................................... 6
4. Environmental monitoring data....................................................................................... 12
5. Control measures........................................................................................................... 25
6. Discussion...................................................................................................................... 26
7. References..................................................................................................................... 27
8. List of abbreviations and acronyms................................................................................ 35
9. Glossary......................................................................................................................... 37

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Summary
Polybrominated diphenyl ethers (PBDEs) are a group of man-made organobromine
compounds. They have been used as flame retardants in a wide range of products
including electrical and electronic equipment, textiles and foams.

The persistent and bioaccumulative properties of PBDEs, along with their potential
adverse effects on aquatic life and humans have led to commercially supplied penta-,
octa- and decaBDE being classified as persistent organic pollutants under the Stockholm
Convention.

In addition, the specific compounds tetra-, penta-, hexa-, and heptaBDE, also components
of commercial penta- and octaBDE, are designated priority hazardous substances and
ubiquitous persistent, bioaccumulative and toxic compounds under the Water Framework
Directive (WFD) in the related Environmental Quality Standards Directive (EQSD)
(2008/105/EC amended by 2013/39/EU).).

This report considers those PBDEs listed in Annex I of the amended EQSD and includes
the 6 structurally similar compounds (congeners) most commonly used in commercial
penta- and octaBDE products. The term PBDEs, as used in this narrative, refers
specifically to these compounds. Where relevant, decaBDE is identified separately.

There are currently national and international measures in place to prevent the use of
PBDEs in products. However, there are a wide range of old consumer products used in
homes and businesses which contain PBDEs.

Releases occur during use and disposal of these products and they continue to enter
waste water treatment works (WwTWs). Much of the PBDEs in WwTWs partition to the
sewage sludge, however there are continuing widespread low level emissions of PBDEs to
surface waters through WwTWs’ effluent.

Evidence shows that concentrations of PBDEs in effluent have reduced compared with
those measured earlier this decade, with over 30% reduction in average concentrations in
effluents observed within a few years for 2 of the key congeners.

PBDEs may be present in soil as a result of the spreading of sludge to land. Based on the
properties of PBDEs, they are unlikely to leach from soil, but may be present on soil
particles entering the water environment as a result of rainfall.

PBDEs may also be released into the water column by the re-suspension of contaminated
sediment or the transformation of decaBDE, which is still in use in industrial products, to

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smaller congeners such as octa- and pentaBDE. This may mean that it will take a long
time for the environment to respond to reductions in emissions.

The marketing and use of decaBDE has been restricted under the REACH regulation
since March 2019. The only remaining permitted uses are in aircraft, and spare parts for
vehicles and machinery manufactured prior to the restriction.

All surface water sites assessed are above the biota environmental quality standard (EQS)
set in 2013 (2013/39/EU) of 0.0085 micrograms per kilogram (µg/kg) wet weight for
PBDEs in fish. While our monitoring is limited, our sampling locations are geographically
spread across river basin districts. The presence of PBDEs is widespread and at levels
significantly above the biota EQS.

The biota EQS for PBDEs was set by the EU based on protecting humans as the most
sensitive receptor. There are currently no regulatory food limits, following discussion on an
opinion from the European Food Safety Authority (EFSA) published in 2011. The need for
regulatory limits will be reviewed on the basis of any new EFSA opinions. The levels
observed are not a risk to aquatic life or wildlife eating the fish based on corresponding
standards developed for these protection goals in water and biota, respectively.

It will be some time before we have enough data to be able to say anything definitive
about trends in environmental concentrations of PBDEs. Available evidence indicates that
at some sampled locations in marine waters, concentrations in fish are declining.

There is little scope to increase source control measures on these substances and if the
current trends in reducing emissions from waste water treatment works WwTWs continue,
they are estimated to be an order of magnitude lower in the next 10 years. Advanced
treatment could be considered at waste water treatment plants to reduce emissions of
PBDEs even more, but even should this prove technically feasible this would be very
costly and energy intensive.

1. Introduction
Polybrominated diphenyl ethers (PBDEs) are a group of man-made organobromine
compounds. They have been used as flame retardants in polyurethane foams in
upholstery and in polymer resins and plastics used as components in electrical equipment.

PBDEs are persistent in the environment, with degradation half-lives estimated in the
range of months to years. They also have the potential for long-range transport and have
been detected in remote regions including the Arctic.

They adsorb to sediment and suspended particles and are present in sewage sludge
following sewage treatment.

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PBDEs bioaccumulate and bio magnify in food chains. They have been detected in top
predatory birds and mammals, such as gulls and seals. They also have potential adverse
effects on aquatic life and humans, including possible effects on the thyroid system,
potential endocrine disrupting effects, reproductive toxicity, and neurodevelopment toxicity.

The above hazardous properties of PBDEs have led to commercially supplied penta-,
octa- and decaBDE, which contain a range of PBDEs as well as the title substances, being
classified as persistent organic pollutants (POPs) under the Stockholm Convention on
Persistent Organic Pollutants.

The specific compounds tetra-, penta-, hexa-, and heptaBDE, also components of
commercial penta- and octaBDE, are designated priority hazardous substances and
ubiquitous persistent, bioaccumulative and toxic (uPBT) compounds under the Water
Framework Directive (WFD) (2000/60/EC) in the related Environmental Quality Standards
Directive (EQSD) (2008/105/EC) amended by the Priority Substances Directive
(2013/39/EU).

 tetra-

 penta-

 hexa-

 heptaBDE

 also components of commercial penta-

 octaBDE

This narrative considers those PBDEs listed in Annex I of the Priority Substances Directive
(2013/39/EU) and includes the 6 structurally similar compounds (congeners) most
commonly used in commercial penta- and octaBDE products. The term PBDEs, as used in
this narrative, refers specifically to the penta- and octaBDE congeners and not to
decaBDE. Where relevant, decaBDE is identified separately.

The requirements of the 2013 Priority Substances Directive (2013/39/EU) took effect in
December 2015 through national legislation (UK Government, 2015). Previous statutory
requirements for PBDEs under the EQSD (2008/105/EC) covered the same six congeners
and classified pentaBDE as a priority hazardous substance.

Directive 2013/39/EU introduced a biota standard of 0.0085 micrograms per kilogram

(µg/kg) wet weight for PBDEs in fish and removed the annual average environmental
quality standard (EQS) for concentrations in water. The setting of a biota EQS reflects the
persistent, bioaccumulative and toxic (PBT) characteristics of this group of substances.
The biota EQS is driven by risks to human health based on the assessment of human
health toxicity data (see Section 4).

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The focus of this narrative is on contributing effects to and assessment of the condition of
surface waters in relation to PBDEs. However, the contribution that groundwater makes to
the surface water status failures is also considered as part of the WFD and the
Groundwater Directive (2006/118/EC as amended by 2014/80/EU). If groundwater
contributes more than 50% of the PBDE load in any surface water status failure then the
groundwater body will also go to poor chemical status. We will be assessing this further as
we develop water body classifications for the draft river basin plans.

2. Use pattern
The family of PBDEs consists of 209 structurally similar compounds with degrees of
bromination ranging between 2 to 10 bromine atoms on the phenyl rings. Three products,
comprising different mixtures of congeners have been available commercially: a
‘pentaBDE product’, an ‘octaBDE product’ and a 'decaBDE product’. The penta- and
octaBDE products are mainly discussed in this narrative and are collectively referred to as
PBDEs.

PBDEs were used as flame retardants in rigid and flexible polyurethane foams, mostly
used in upholstery and furnishing, and in a variety of polymer resins and plastics,
particularly for components in electrical and electronic equipment (Environment Agency,
2013a). Typically, the flame retardants were added at concentrations between 5 and 30%
by weight, that is 1kg of polymer would contain 50–300g of flame retardant (European
Chemicals Bureau, 2001).

Historically there have been significant differences between EU countries on fire safety
requirements for furniture and fittings, with the most stringent in the UK and Ireland
(Guillame et al., 2000). This resulted in a greater demand for flame retardants in the UK
from the late 1980s onwards. The UK also saw a drop in furniture and furnishing related
deaths of 64% in 2002–2007 compared with 1981–1985 (BIS, 2009).

Estimates of the historic annual usage of total PBDEs are around 10,000–11,000
tonnes/year in the EU and 40,000 tonnes/year globally (European Chemicals Bureau,
2001). Production of PBDEs ceased in the UK in 1996. Imports into the UK have also
reduced to zero. The UK use of PBDEs peaked in the early 1990s followed by a steady
decline until 2004 when restrictions on marketing and use were imposed under
Commission Regulation (EC) No 552/2009 (Oakdene Hollis, 2010).

DecaBDE was used in electrical and electronic equipment and as a flame retardant in
textiles and various types of polymers. Most uses of decaBDE have been restricted since
March 2019 (see Section 5). The only remaining permitted uses are in the production of
aircraft and spare parts for motor and agricultural vehicles or machinery manufactured
prior to the restriction (Commission Regulation (EU) 2017/227).

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PBDEs have also been detected in samples taken from stack emissions from UK iron ore
sinter plants. These were already present in the raw materials, such as iron ores and coke
breeze, and a significant proportion of these PBDEs were estimated to be destroyed
during the sinter process (Drage et al., 2014).

3. Sources, emissions and pathways

No known natural sources of PBDEs have been identified, although related substances
are known (European Chemicals Bureau, 2001). Figure 1 shows the main sources and
pathways of PBDEs into surface water. The figure shows that PBDEs from consumer
products enter air, /landfill and waste water treatment works (WwTWs) which and
subsequently enter water courses either directly or through deposition and run-off.
Atmospheric releases of PBDEs are proportionally greatest, with indoor concentrations of
particle-bound PBDEs being significantly larger than outdoor air concentrations. Emissions
to soil and water are lower (Earnshaw et al., 2013).

Figure 1: Sources and pathways of polybrominated diphenyl ethers into the

environment

The production and use of penta- and octaBDEs are banned in the EU. Releases,
assuming no illegal imports, will be from historic use in items such as car seats and foam
furniture for the pentaBDE product, or electrical equipment, such as televisions and
computers, and other plastics for the octaBDE product.

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Decreasing UK ambient air concentrations of PBDEs between 1999 and 2012 suggest that
these regulatory controls have been effective in controlling emissions to the environment
(Graf et al., 2016). A Swiss study on e-waste showed a significant decline in the
concentrations of penta- (-93%), octa- (-77%) and decaBDE (-24%) between 2003 and
2011, also proving the restrictions effective (BAFU, 2017).

PBDEs are not chemically bound to the plastic or foam in which they are incorporated.
This means that at the production stage they were physically combined with the material
being treated rather than chemically combined (as in reactive flame retardants). Therefore,
there is potential for them to leach out of products.

The most probable route for this is transfer from furniture or gradual breakdown of foam or
plastic containing the chemicals contributing to household dust particles. Transfer of
PBDEs, particularly decaBDE, to dust can also occur via direct contact between the
treated products and dust (Rauert and Harrad, 2015).

High levels of PBDEs have been found in the UK in dust sampled from homes, offices,
classrooms and, in particular, car cabins (Harrad et al., 2008; Harrad and Abdallah, 2011;
Muenhor, 2011; Muenhor and Harrad, 2012; Kuang et al., 2016). Dust particles then
adhere to clothes and are released during washing, reaching WwTWs via the sewerage
system (Prevedouros et al., 2004; Earnshaw et al. 2013; 2015; Environment Agency,
2013a; Saini et al., 2016).

Furniture typically has a long lifetime in use and even when disposed of may be recycled
by another user, meaning that there are likely to be releases of PBDEs for years to come
(Bjorklund, 2011).

Volatilisation from PBDE-containing products and partitioning to dust particles will result in
emissions to air and subsequent deposition onto land, reaching surface waters during
rainfall as urban run-off (European Chemicals Bureau, 2001).

Monitoring of waste water in an urban catchment identified domestic waste water as the
main source of PBDEs to WwTWs (Rule et al., 2006; Comber et al., 2015). Even though
PBDE concentrations in effluents from WwTWs are relatively low, the large volumes of
effluent treated leads to these being a significant source of PBDEs to receiving waters.

PBDEs have very low water solubility and a significant proportion of the load in a WwTW
will partition to sewage sludge. Application of sludge to agricultural land may be a
significant exposure route. Elevated concentrations of PBDEs are reported in soils (Eljerrat
et al., 2008; Matscheko et al., 2002).

PBDEs are very persistent, and evidence of a cumulative effect of sludge application has
been reported by Eljerrat et al. (2008). Based on the properties of PBDEs, they are likely
to be immobile in soil (ATSDR 2017; European Chemicals Bureau, 2001), but may be
present on soil particles entering the water environment as a result of rainfall.

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In a West Midlands study on both soil and air, concentrations of PBDEs decrease with
increasing distance from the city centre, suggesting that urban conurbations are sources
of PBDEs to the wider environment (Harrad and Hunter, 2006; Drage et al., 2016). In a
rural study of airborne particles in north-west England, highest PBDE concentrations,
including decaBDE, were found when air masses passed over urban and industrial areas,
although small local influences from towns may also have contributed (Wilford et al. 2008).

As older furniture and other items containing PBDEs are disposed of, PBDEs enter the
waste stream. The final mode of disposal for polyurethane foam containing PBDEs is likely
to be ultimately to landfill or incineration (European Chemicals Bureau, 2001). Landfills
that are designed and operated with engineering requirements in accordance with the EU
Landfill Directive (Council Directive 1999/31/EC) include measures to minimise the
breakout of leachate, and hence minimise the potential for release of PBDEs present in
the leachate to the environment. However, leachate may be discharged off-site via a
treatment system with the potential for PBDEs to be discharged to the environment, if the
treatment technology does not remove PBDEs.

A number of studies are underway concerning the amount of POPs, including PBDEs, in
waste streams, and additionally in landfill leachate itself. Information from these studies
will become available progressively over the next 5 years and form part of the UK
Government’s endeavours to better understand the pathways and impacts of POPs in the
wider environment.

Further details of this work are periodically made available through the website of the
Stockholm Convention as part of the UK POPs National Implementation Plan.

Based on the highly sorptive properties of PBDEs, the chemicals are unlikely to be very
mobile. A screening study of leachate from a range of landfill sites did not find any PBDEs
in either landfill leachate or groundwater samples (Environment Agency, 2013b). Particle-
bound emissions of PBDEs generated during the unloading of waste and from vehicular
disturbances are thought to be the dominant pathways from landfill to the atmosphere
(Earnshaw et al., 2013).

The magnitude of loss of PBDEs following disposal from landfill, incineration or accidental
burning is considered to be negligible compared with losses during product use
(Prevedouros et al., 2004). PBDEs can form brominated dibenzofurans and brominated
dibenzo-p-dioxins on combustion and the total bromine load in waste has an effect on their
formation during the waste incineration process (European Chemicals Bureau, 2001).

Remobilisation of PBDEs buried at depth in sediment may also lead to re-release in the
future, as will transformation in sediment of decaBDE by loss of bromine atoms
(debromination) to lower brominated congeners such as octaBDE and pentaBDE (ECHA,
2012). This could be a significant source of PBDEs to surface waters, given the large
volumes of decaBDE produced in the last few decades (Earnshaw et al., 2013).

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The inventory of emissions, discharges and losses of priority and priority hazardous
substances is a formal requirement of the WFD under the EQSD 2008 (2008/105/EC). The
inventory for England can be found under the Emissions Inventory and Chemical Trends
information for the cycle 2 River Basin Management Plans. It provides estimates of
emissions, discharges and losses of PBDEs from both point and diffuse sources, by river
basin district, for the baseline year of reporting (2010).

Estimates have been determined using SAGIS (Source Apportionment Geographic

Information System, v2010), a GIS-based source apportionment tool and surface water
model (Comber et al., 2012), combined with estimates of releases to sea from long sewer
outfalls from the Pollution Inventory (PI).

We estimate that, despite restrictions on the use of PBDEs, approximately 11kg of PBDEs
were released to surface waters in England in 2010. These were estimated to be
predominantly owing to point source releases. Total emissions, discharges and losses of
PBDEs to water per river basin district are shown in Figure 2 (results for Solway Tweed
are reported by the Scottish Environmental Protection Agency and the Dee by Natural
Resources Wales).

Estimates of emissions of PBDEs to water are broadly similar across all river basin
districts (Figure 2), with emissions ranging from 0.58kg/year in Anglian to 2.69kg/year in
South East. This figure shows that the highest emissions are found in the South East and
North West river basin districts (>2kgs of emissions, /discharges and losses each) (Figure
2). Thames, Severn and Northumbria lose emit between 1 and 2kgs, and South West,
Anglian and Humber <1kgs.

Emissions of PBDEs are considered to have peaked around 1997 and, based on our
knowledge of use, are now considered to be declining (Prevedouros et al., 2004;
Earnshaw et al., 2013; 2015).

Estimates of emissions of PBDEs to water are broadly similar across all river basin
districts, with emissions ranging from 0.58kg/year in Anglian to 2.69kg/year in South East.

With only one year of data in the inventory we cannot yet describe any temporal trends in
emissions. The next update of the inventory will be published as part of the 3rd cycle river
basin management plans in 2021.

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Figure 2. Baseline year (2010) total emissions, discharges and losses to water for
polybrominated diphenyl ethers (PBDEs) (as listed in Annex I of the Priority
Substances Directive 2013/39/EU) for each river basin district

We have reviewed PI data up until the most recent year reported (2017). Highest levels of
emissions in 2017 were reported for the Thames river basin district, followed by the
Humber and North West.

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Reported emissions of PBDEs to water dropped from 51kg in 2012 to 3kg in 2013.
Emissions have remained at similar level since suggesting controls have influenced inputs
into the water environment from large regulated industrial sites to some extent.

Given the data are generated in a different manner to the baseline inventory and focus
solely on point sources, it is not possible to draw any further conclusions.

SAGIS (v2010) estimates of emissions of PBDEs by industry sector show that WwTWs are
the main source of PBDEs to surface waters. There are also minor emissions of PBDEs
from urban run-off and other water company discharges such as those from combined
sewer overflows and storm tanks.

Monitoring data collected from 2010 to 2013 through the Chemicals Investigation
Programme (CIP) undertaken by water companies (UKWIR, 2014a; 2014b) has been used
as input data in the SAGIS tool for estimating chemical loads per river basin district. The
CIP data suggest that sewage treatment can remove over 85% of PBDEs entering the
works.

Monitoring data collected as part of the second phase of the Chemicals Investigation
Programme (CIP2) (UKWIR, 2019) suggest that restrictions on use are having an impact
on emissions, with declines observed in concentrations of PBDEs in effluents. At 29 sites
common to both CIP, which finished in 2013, and CIP2 monitoring conducted from 2015 to
2017, the average concentrations of two of the main congeners of PBDEs – BDE-47 and
BDE-99 – have decreased in effluent by over 30%. More-recent CIP2 monitoring at
common sites to CIP suggests further significant declines, although the sites studied differ
from those above.

Analysis of measured concentrations of BDE-47 in WwTWs’ effluent (UKWIR, 2019)

suggests that levels in effluent will have declined by roughly an order of magnitude by
2027, posing lower environmental risk. This assumes a continued decline owing to control
measures in place.

4. Environmental monitoring data

We have recent monitoring data for PBDEs in surface waters and biota – fish and blue
mussels – from both English freshwaters and estuarine and coastal waters. In addition,
CIP2 measures concentrations of PBDEs in effluent and in water around WwTWs across
England (UKWIR, 2019); data collection and analysis are ongoing and the current results
are summarised in Section 4.2. Marine monitoring programmes under the Oslo Paris
Convention (OSPAR) have also included the analysis of levels of PBDEs in biota and
sediment in UK coastal waters over time (Section 4.4). We use saline waters in this report
to cover estuaries and coastal waters out to 12 nautical miles (territorial waters).

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We can compare our data against EQSs to get an understanding of risk. The 2013 Priority
Substances Directive (2013/39/EU) lists the PBDEs given in Section 1 of this report as
WFD priority hazardous substances. It specifies a biota-based EQS of 0.0085µg/kg for the
sum of the concentrations of 6 PBDE congeners – BDE-28, BDE-47, BDE-99, BDE-100,
BDE-153, and BDE-154. This EQS refers to the presence of this group of substances in
fish and is derived from human health toxicity data. It represents a level that is considered
to be protective against risks to the environment and human health from the consumption
of contaminated fish.

The data used to derive this value are summarised in the EQS dossier (European
Commission, 2012).

The Directive removed previous annual average EQSs in surface waters for PBDEs.

4.1. Biota monitoring data

As part of the programme of work to assess risks from PBT substances in England, we
have gathered data on PBDE residues in freshwater and saline biota from a limited
number of locations around England.

Our sampling began in 2015. Between 2015 and 2019, we have sampled at 44 freshwater
sites for fish (brown trout, chubb or roach), 21 saline sites for fish (dab and flounder) and
at 26 saline sites for blue mussels ‘Mytilus edulis’. The number of sites and their locations
have varied year on year, although a subset of sites have been consistently sampled and
can be used to observe trends in concentrations over time (see Section 4.4).

In 2018, we extended our freshwater sampling programme to generate biota data from
more widespread locations and by the end of this year should have data from about 40%
of WFD management catchments.

Similarly our saline monitoring was extended to include fish (flounder and dab) from 15
sites in 2018. Originally sampling focused on blue mussels for trend analysis and water
body risk assessment. However, questions regarding the trophic level correction factors
necessary to compare mussel tissue (trophic level 2) with EQSs set for fish (trophic level
4) has resulted in the inclusion of whole fish sampling in recent years to make sure they
are equivalent. We are currently considering our future approach to biological sampling
based on our experiences to date.

A summary of the concentrations of PBDEs we have measured in freshwater and saline

fish, as well as in blue mussels is presented below. We have looked at mean measured
concentrations based on the most recent 3 years of data where available. The results for
fish relative to the biota EQS are shown in Figure 3.

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Because PBDEs are hydrophobic and tend to partition to lipids, fish with different lipid
content may have different concentrations of the substances. Normalisation to a default
lipid content reduces the variability in the data and allows comparison between different
fish. Therefore, when we consider fish results for PBDEs, the concentrations we use are
lipid normalised using a default of 5% lipid content (European Commission, 2014).

In freshwater fish, mean concentrations of PBDEs range from 1.4 to 36.2μg/kg wet weight
(lipid normalised). All sites (100%) exceed the EQS (Figure 3) and 34% of sites are over
1000 times greater than this value. The highest mean concentrations of PBDEs are
recorded for the River Seven and River Trent in the Midlands at values over 4000 times
the EQS.

Fish from all saline waters sampled have mean lipid-normalised concentrations above the
EQS threshold (Figure 3). Mean concentrations of PBDEs in saline fish range from 0.25 to
15.3μg/kg wet weight (lipid normalised).

Some of the site results for saline waters are based on only one replicate. Highest mean
concentrations in saline waters were recorded in the Thames and Mersey Humber
estuaries (Figure 3).

The results in both types of water suggest the EQS is exceeded in widespread locations
across the country (Figure 3). While the measured values are relatively high, they do not
appear to be confined to extremely populated areas. However, there are relatively few
data in heavily populated areas for comparison.

Mean measured concentrations in blue mussels in saline waters range from 0.018– to 1.2
μg/kg wet weight (lipid normalised). Similar to freshwaters, 100% of sites exceeded the
EQS.

While levels in blue mussels are lower than those in saline fish, it should be noted these
represent a lower trophic level, and the recorded measured concentrations are still high.
The highest measured concentration is at a site near Southampton.

There is no obvious association between the estimated levels of current emissions,

discharges and losses to water for each river basin district (see Figure 2) and the location
of high levels of PBDEs from our biota monitoring data (Figure 3). This suggests
atmospheric contributions also play a significant role in environmental concentrations in
the water column.

The EQS dossier for PBDEs (European Commission, 2012) calculated a biota standard of
44μg/kg wet weight for the protection of predators from secondary poisoning. This was not
proposed as a statutory value as the protection goal of human health was the driver for the
final EQS. However, based on a comparison against the secondary poisoning standard,
our monitoring data in biota suggest there is no risk to wildlife eating fish.

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Figure 3. Site results showing three-year mean concentrations of PBDEs in
freshwater and saline fish from 2015 to 2019 compared against the biota EQS

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Data for figure 3
Sample Type Easting Northing Mean EQS Bands
Fresh 506372 249294 1.95518939 150
Fresh 575800 272800 7.89176904 500
Saline 529700 411400 15.3268495 500
Saline 555500 380000 2.03653709 150
Fresh 559700 180390 6.03657998 500
Saline 590500 349000 1.10558555 100
Saline 625730 234440 2.31682777 150
Saline 622372 233103 1.5140272 150
Fresh 534183 402331 7.12563573 500
Fresh 619900 309800 1.43749704 150
Fresh 620600 309500 1.44245461 150
Fresh 385160 240750 36.2624404 2500
Fresh 375988 208885 7.87161807 500
Fresh 384880 226160 4.95109449 500
Fresh 389370 233220 20.8734528 500
Fresh 408310 251410 6.69010714 500
Fresh 480792 361022 34.5452872 2500
Fresh 449200 330200 14.1224956 500
Fresh 438103 355506 15.7824894 500
Saline 430000 606000 0.25140232 20
Fresh 436300 510700 15.6457989 500
Fresh 446013 518975 17.3394048 500
Saline 454446 526476 1.39691589 150
Saline 459300 527000 1.25858978 100
Fresh 459334 444561 21.5779588 2500
Fresh 453008 457548 5.43995454 500
Fresh 435575 466848 3.17046463 150
Fresh 456820 403898 21.2968925 2500
Fresh 456604 403688 12.0236288 500
Fresh 471329 455658 2.67766773 150
Fresh 365895 373768 5.84822214 500
Saline 323101 404274 1.37752955 150
Saline 334945 426284 1.57281509 150
Fresh 360051 418978 4.62299837 500
Saline 334595 444819 1.89612982 150
Saline 342942 455981 1.9407924 150
Saline 292540 531626 1.52290835 150
Saline 328100 460400 3.82254101 150
Fresh 573457 153535 8.30304898 500
Fresh 601815 143653 4.76297718 500
Fresh 578303 117680 5.22979209 500
Fresh 476920 123200 13.9321959 500

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 Sample Type Easting Northing Mean EQS Bands
Fresh 503750 121650 9.68362806 500
Saline 583000 108200 0.87574165 100
Saline 523100 103500 1.79269117 150
Fresh 435327 120875 7.20684599 500
Fresh 460179 109263 16.5896746 500
Fresh 521648 129149 1.57379206 150
Fresh 382396 112026 4.21909978 150
Fresh 343763 142684 4.0555908 150
Saline 285119 56182 0.34171807 20
Saline 246000 46100 0.71029061 50
Fresh 200704 49470 13.2591084 500
Fresh 391885 173211 7.54090111 500
Fresh 361700 175500 7.59765925 500
Fresh 460100 167100 3.95685699 150
Fresh 518049 214231 15.3759677 500
Fresh 536302 193775 5.85713737 500
Fresh 514790 169070 7.40667745 500
Fresh 485210 186172 3.33074469 150
Fresh 453043 201190 5.85160171 500
Fresh 459700 192100 4.02588387 150
Saline 596150 180700 0.78216265 50
Saline 544980 180450 7.75784482 500
Saline 572133 179803 4.49891193 500

Recent data and literature from other organisations support the widespread presence of
PBDEs in freshwater and marine biota.

Studies on the levels of PBDEs in freshwater fish, including roach and trout, sampled from
locations across the UK have shown widespread occurrence of PBDEs, frequently at
levels above the biota EQS (Jurgens et al., 2013; Rose and Fernandes, 2010). This was
also the finding from a number of studies of marine fish, such as grey mullet and mackerel,
sampled from waters around the UK (The Food and Environment Research Agency, 2015;
Aznar-Alemany et al., 2017).

Studying 3 rivers in South Wales, Windsor et al. (2019) found that contaminants such as
PBDEs were significantly higher in invertebrates in areas with greater urban land cover
and wastewater discharge. The sites with high contamination also showed
macroinvertebrate communities with reduced taxonomic and functional diversity, simplified
food webs and less abundant prey for apex predators. The data support the idea that
contaminant mixtures containing substances such as PBDEs, may inhibit the complete
recovery of macroinvertebrate food webs from the past effects of gross pollution.

17 of 39
4.2. Water column monitoring

The water company CIP2 is ongoing and includes contaminants in rivers upstream and
downstream of over 600 WwTWs, as well as in sewage effluent from those works. The
sites were selected because the receiving waters for their effluent offer low dilution and,
therefore, they represent sites at greatest risk of contamination.

The findings from the CIP2 to date covers results for sites monitored for the 6 PBDE
congeners of interest between 2015 and 2019 (UKWIR, 2019). Mean results for samples
of individual congeners taken at up to 448 sites upstream and downstream of WwTWs’
discharge locations were 0.22 to 0.27ng/l and 0.23 to 0.27ng/l, respectively. The similarity
in these values is in part a reflection of the fact that many samples were below the chosen
limit of detection for the investigations.

We took samples at our routine water monitoring sites between 2016 and 2018; 272
freshwater and 51 saline sites were assessed. The majority of sites were monitored for
two years with 41 sites having only 1 year’s data and 55 sites having 3 years’ worth.
Between 3 and 37 samples were taken at the sites. The mean concentrations of PBDEs in
freshwaters ranged from 0.0006 to 1.6ng/l. For saline waters, the concentrations of PBDEs
ranged from 0.0006 to 0.77ng/l.

Assessment of risk using water column monitoring data is difficult because there is no
statutory value to compare against. The EQS dossier for PBDEs (European Commission,
2012) calculated water concentrations equivalent to the biota EQS of 4.9 x 10-8 and 2.4 x
10-9μg/l for fresh and saline waters, respectively, but recommended caution over their
use. These values, therefore, were not included in the Priority Substances Directive
(2013/39/EU).

The dossier (European Commission, 2012) also calculated standards to reflect long-term
risks to aquatic life owing to direct toxic effects. These values are far less stringent than
the values that were considered equivalent to the biota EQS at 0.049 and 0.0049μg/l for
fresh and saline waters, respectively. These are not statutory values as the protection goal
of human health was the driver for the final EQS.

None of our monitoring data or that undertaken by water companies upstream and
downstream of their WwTWs exceeds these values suggesting that the levels in water are
below those likely to result in direct toxic effects to aquatic organisms.

The Priority Substances Directive (2013/39/EU) also sets out maximum allowable
concentration EQSs (MAC EQSs) for PBDEs of 0.14 and 0.014µg/l for inland surface
waters and other surface waters, respectively. The MAC EQS is a threshold intended to
protect the aquatic environment from short-term toxic effects. The MAC EQSs should be
applied where the biota EQS is applied or where emissions or environmental
concentrations indicate potential short-term risk.

18 of 39
All our measured concentrations in fresh and saline waters are below the MAC EQSs.

Cristale et al. (2013) analysed water samples from sites along the River Aire for PBDEs.
Whilst the main congener of decaBDE, BDE-209, was detected in the majority of water
samples, none of the congeners from either penta- or octaBDE was detected. This is
broadly consistent with other studies, which also report a dominance of decaBDE and
lower concentrations of both penta- and octaBDE in water, sediment and biota samples at
most locations (Law et al., 2014, OSPAR, 2010; Law, 2014).

4.3. Trends in freshwaters

As described in Section 4.1, we have been measuring PBDE residues in biota since 2015.
Sampling locations have changed over time and we only have one freshwater site where
residues of PBDEs in fish have been sampled for consecutive years from 2015 to 2019.
We have visually examined the data for trends rather than applying any statistical analysis
to the data because we do not yet have sufficient data. Overall, there is no consistent
temporal trend observed at the site. We will continue to collect data on trends to enable
future analysis.

There are only limited environmental monitoring data reported for PBDEs in the wider
scientific literature. There is a general consensus that although elevated levels of penta-
and octaBDE in biota and sediments are still present and there is substantial spatial
variation, concentrations have probably peaked and, at some UK sites are now declining
(Law et al., 2014, OSPAR, 2010; Law, 2014; Yang et al., 2016). A downward trend is not
however observed at all sites, and in some locations sediment concentrations of PBDEs,
including BDE-209, are still increasing (Yang et al., 2016).

A study by Walker et al. (2012) measuring levels of PBDEs in the livers of the Eurasian
otter ‘Lutra lutra’ reported PBDE concentrations of 3 to 718ng/g wet weight. These levels
were within the range previously reported between 1995 to 2005; implying little decline in
concentrations since restrictions were introduced.

Birds have been widely used as monitors or sentinels of environmental contaminants

including PBDEs. Trends in residues of PBDEs in archive sparrowhawk ‘Accipiter nisus’
eggs collected between 1985 and 2007 in the UK as part of the Predatory Bird Monitoring
Scheme show little decline in concentrations following a peak in the 1990s. Crosse et al.
(2012a) suggest that these data may indicate some formation of pentaBDE congeners as
a result of debromination of decaBDE.

Another study of PBDE concentrations in sparrowhawk livers has revealed sparrowhawks

in Britain accumulate some of the highest PBDE residues reported for terrestrial feeding
birds (Crosse et al., 2013).

19 of 39
In a study on decaBDE in wild birds from the UK, Sweden and the Netherlands, there was
no significant change in sparrowhawk concentrations between 1973 and 2001, although in
later years concentrations were found more frequently above the limit of detection. In
peregrine falcons, peak concentrations were measured in 1995, followed by a decline until
2001 (Leslie et al., 2011)).

4.4. Trends in transitional and coastal waters

Under OSPAR, the Clean Seas Environment Monitoring Programme (CSEMP) has
collected data on concentrations of PBDEs in UK marine waters over several years. Data
generated under this programme is collated for the International Council for the
Exploration of the Sea (ICES) and can be viewed using the Database on Oceanography
and Marine Ecosystems (DOME) web portal. Data are available for the 6 congeners of
interest.

An overview of the trend monitoring data collected through the CSEMP for BDE-47 within
English territorial waters (12 nautical miles), the saline area to which the Priority
Substance Directive (2013/39/EU) applies, is given in Figure 4.

Trend information has been reported for residues of BDE-47 in the livers of common dab
‘Limanda limanda’ sampled at 8 sites around England between 2003 and 2017 (South
coast, North West and North East). At 7 of these sites, downward trends were observed.
Only one site in Northumberland showed no trend.

For the other congeners, the majority of sites that can be assessed for trends also show
declines in PBDE residues over time.

Law et al. (2014) compiled and reviewed recent reports of PBDEs in the marine
environment between 2010 and 2012. They concluded that despite some evidence of
declining trends in some fish species and locations, significant concentrations of PBDEs
were still being reported.

In contrast to the high residues of PBDEs reported in terrestrial feeding birds (Crosse et
al., 2012a; 2013), PBDE concentrations in the eggs of the Northern gannet (Morus
bassanus) from two UK colonies showed a rise in the late 1980s, peaking in 1994, and a
steady decline until 2002, where levels fell back to pre-1980 levels (Crosse et al, 2012b).

A study of PBDEs in ringed seals from the Baltic Sea between 1974 and 2015 also
reported an increasing trend until the end of the 1990s, followed by a decreasing trend
until the end of the period (Bjurlid et al., 2018).

Since 2009, CEFAS (2012) have monitored PBDEs in coastal sediments around the UK.
Whilst there are insufficient data to report a temporal trend yet, results show that tetraBDE

20 of 39
and pentaBDE were present. Samples were dominated by decaBDE. Similar results have
been reported by Vane et al. (2010).

A study by Sühring et al. (2015) investigated brominated flame retardants, including

PBDEs, in sediments around the UK east coast. High concentrations of BDE-209 were
detected in North Sea sediments, which were expected owing to high use in Europe.
Samples with the highest overall PBDE concentrations were found near the UK coast with
BDE-100 being the main congener followed by BDE-154, BDE-47 and BDE-99,
components of technical penta-BDE.

21 of 39
Figure 4. Trends in concentrations of BDE-47, as proxy for PBDEs, in fish liver (dab)
in English coastal waters over the period from 2003 to 2017.

Data accessed from the ICES DOME portal, extraction 15 February, 2019; downloaded
May 2019. Chemical data for the OSPAR Coordinated Environmental Monitoring
Programme, reporting laboratories through the British Oceanographic Data Centre (UK).
ICES, Copenhagen.

22 of 39
23 of 39
Data for figure 4
Easting Northing species Trend
597705 111230 Limanda limanda downward trend
541156 97492 Limanda limanda downward trend
249937 25144 Limanda limanda downward trend
455458 540866 Limanda limanda downward trend
562244 485746 Limanda limanda downward trend
697515 242381 Limanda limanda downward trend
710874 611838 Limanda limanda downward trend
661212 582479 Limanda limanda downward trend
609142 553573 Limanda limanda downward trend
703641 523447 Limanda limanda downward trend
648099 469684 Limanda limanda downward trend
670441 414428 Limanda limanda downward trend
220828 186297 Limanda limanda downward trend
310046 398076 Limanda limanda downward trend
287887 401700 Limanda limanda downward trend
283967 514423 Limanda limanda downward trend
307465 446347 Limanda limanda downward trend
257800 386923 Limanda limanda downward trend
279931 457551 Limanda limanda downward trend
447402 600537 Limanda limanda no trend
455296 622722 Limanda limanda no trend
720536 334335 Limanda limanda no trend
561855 382725 Limanda limanda no trend
570989 363557 Limanda limanda no trend
291994 390029 Limanda limanda no trend
291994 390029 Merlangius merlangus no trend
670441 414428 Pleuronectes platessa no trend
283967 514423 Pleuronectes platessa no trend
307465 446347 Pleuronectes platessa no trend
291994 390029 Pleuronectes platessa no trend
310046 398076 Scomber scombrus no trend
307465 446347 Scomber scombrus no trend
257800 386923 Scomber scombrus no trend

24 of 39
5. Control measures

5.1. Restrictions

Commercial penta- and octaBDE were originally restricted in 2003 in Europe under the
Marketing and Use Directive (2003/11/EC) and then in 2006 by the REACH Regulation
(EC 1907/2006). These restrict the placing on the market and use of penta- and octaBDE
above 0.1% by weight.

In 2009, penta- and octaBDE were designated as Annex A POPs at the 4th Conference of
the Parties to the Stockholm Convention. Parties to the Stockholm Convention must take
measures to eliminate production and use of these substances.

This international agreement was implemented into EU legislation through a Council

Decision in 2006 (2006/507/EC) as an amendment to Regulation (EC) No 850/2004 on
POPs which prohibits the production and placing on the market of the substances listed in
Annex I of the legislation and regulates the management of waste containing these
substances.

DecaBDE was designated as an Annex A POP at the 8th meeting of the parties to the
Stockholm Convention in spring 2017.

DecaBDE, along with other PBDEs, has been banned for use in electrical and electronic
equipment since 2008 under the Directive on the Restriction of the Use of Certain
Hazardous Substances in Electrical and Electronic Equipment (2011/65/EU). Most other
uses of decaBDE (at or above 0.1%) have now been restricted under the REACH
regulation since March 2019 (Commission Regulation (EU) 2017/227). The only remaining
permitted uses are in aircraft, and spare parts for vehicles and machinery manufactured
prior to the restriction.

The EU Regulation on POPs was recast in June 2019 (Regulation (EU) 2019/1021) to
include decaBDE and specifies a concentration limit for PBDEs, including decaBDE, in
waste of 1000mg/kg. This limit is to be reviewed by the European Commission by July
2021 with a view to lowering it to 500mg/kg.

Land spreading of sewage sludge is regulated by the Sludge (Use in Agriculture)

(Amendment) Regulations 1990 (SI 1990/880) which set limits for the amounts of certain
trace metals. There are currently no limits set on the levels of PBDEs in sewage sludge
spread to agricultural land.

25 of 39
We have continued to develop and improve the way we assess the risks from waste
applications to agricultural land under the Environmental Permitting Regulations (SI
2016/1154).

The biota EQS for PBDEs was set by the EC based on protecting humans as the most
sensitive receptor. There are currently no regulatory food limits, following discussion on an
opinion from the European Food Safety Authority (EFSA) published in 2011 (EFSA, 2011).
The need for regulatory limits will be reviewed on the basis of any new EFSA opinions.

6. Discussion
PBDEs are stable and very persistent compounds which have potential adverse effects on
aquatic life and humans.

Data, such as that generated through the CIP and CIP2 and in the Pollution Inventory,
show declines in emissions to water suggesting that restrictions on use have influenced
inputs to some extent.

The evidence we have from monitoring data in biota suggests that the presence of PBDEs
is widespread across England. The biota monitoring reports concentrations of PBDEs
several orders of magnitude greater than the biota EQS. As such, widespread failure of
this EQS in the future seems likely.

It will be some time before we have enough data to be able to say anything definitive
about trends in environmental concentrations of PBDEs. The available evidence indicates
that at some sampled locations, particularly in marine waters, concentrations are declining.
However, this is not true for all sites. The continued release of PBDEs from historic
sources and potentially from the breakdown of decaBDE, as well as their persistence and
potential to bioaccumulate means that in some instances, little or no decline in
environmental concentrations is observed.

PBDEs are already heavily restricted, and there is little scope to increase source control
measures on these substances. We continue to monitor compliance with these
restrictions. Even if complete compliance with these restrictions is achieved, it is unclear
how long it will be before environmental concentrations of PBDEs are no longer
problematic because of the persistence of these substances in the environment and the
amounts still in use by society.

The limited evidence available suggests that environmental concentrations will take
decades to decline significantly (Earnshaw et al., 2015). DecaBDE may remain a source of
lower level congeners in the environment for some time. DecaBDE has been used in high
volumes until recently, but rigorous enforcement of recent restrictions could help bring
down emissions and reduce the potential for them to form PBDEs as they de-brominate.

26 of 39
The stability of these substances also means that they are not amenable to destruction by
traditional waste water treatment technology, making ‘end of pipe’ control difficult. Most of
the PBDE load will be removed to sludge. If the current trends in reducing emissions from
WwTWs continue, PBDE concentrations in effluents are estimated to be an order of
magnitude lower in the next 10 years. Advanced treatment could be considered at
WwTWs to reduce emissions of PBDEs even more, but even should this prove technically
feasible this would be very costly and energy intensive and it is uncertain what this would
deliver in terms of improved compliance with biota standards.

Further work is needed to understand what environmental improvements could be

achieved. We will continue to develop our understanding of this and will engage with
stakeholders on the implications as our knowledge improves.

7. References
ATSDR (2017) Toxicological profile for polybrominated diphenyl ethers (PBDEs). U.S.
Department of Health and Human Services, Public Health Service, Agency of Toxic
Substances and Disease Registry. March 2017. Atlanta, Georgia: ATSDR. Available at:
https://www.atsdr.cdc.gov/toxprofiles/tp207.pdf [Accessed 9 September 2019].

Aznar-Alemany, Ò., Trabalón, L., Jacobs, S., Barbosa, V. L., Fernández Tejedor, M.,
Granby, K., Kwadijk, C., Cunha, S. C., Ferrari, F., Vandermeersch, G., Sioen, I., Verbeke,
W., Vilavert, L., Domingo, J. L., Eljarrat, E., Barceló, D. (2017). Occurrence of halogenated
flame retardants in commercial seafood species available in European markets. Food and
Chemical Toxicology 104: pp.35-47. Available at:
https://www.sciencedirect.com/science/article/pii/S0278691516304951#bib74 [Accessed
15 September 2019].

Bjorklund, J. (2011) Brominated flame retardants and perfluoroalkyl acids in Swedish

indoor microenvironments. Implications for human exposure. PhD thesis [online].
Stockholm University. Available at:
http://www.diva-portal.org/smash/get/diva2:451881/FULLTEXT02.pdf [Accessed 9
February 2015].

Bjulid, F., Roos, A., Ericson Jogsten, I. and Hagberg, J. (2018). Temporal trends of
PBDD/Fs, PCDD/Fs, PBDEs and PCBs in ringed seals from the Baltic Sea (Pusa hispida
botnica) between 1974 and 2015. Science of The Total Environment 616-617: pp. 1374-
1383 [online]. Available at:
https://www.sciencedirect.com/science/article/pii/S0048969717328899 [Accessed 13
September 2018].

Bundesamt für Umwelt, BAFU (2017) Substance flows in Swiss e-waste (Summary).
Federal Office for the Environment (FOEN), Bern, 2017 [online]. Available at:
https://www.bafu.admin.ch/bafu/en/home/topics/chemicals/publications-studies/

27 of 39
publications/stofffluesse-im-schweizer-elektronikschrott.html [Accessed 11 September
2018].

CEFAS (2012). Monitoring of the quality of the marine environment, 2008–2010. Sci. Ser.
Aquat. Environ. Monit. Rep., CEFAS Lowestoft, 63: 111pp.

Comber, S., Daldorph P., Gardner M., Murrell K., Smith R., Constantino C., Buchanan, L.,
Hasthorpe, J. and Mills D. (2012) Chemical source apportionment under the WFD. UKWIR
WW02.

Comber, S., Gardner, M., Jones V. and Ellor B. (2015) Source apportionment of trace
contaminants in urban sewer catchments. Environmental Technology 36(5): pp.573–587.

Commission Directive 2009/90/EC of 31 July 2009 laying down, pursuant to Directive

2000/60/EC of the European Parliament and of the Council, technical specifications for
chemical analysis and monitoring of water status. Official Journal of the European Union:
pp.L201/36–L201/38. Available at: http://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?
uri=CELEX:32009L0090&qid=1441097444505&from=EN [Accessed 1 September 2015].

Commission Directive 2014/80/EU of 20 June 2014 amending Annex II to Directive

2006/118/EC of the European Parliament and of the Council on the protection of
groundwater against pollution and deterioration. Official Journal of the European Union:
pp.L182/52–L182/55. Available at: https://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?
uri=CELEX:32014L0080&from=EN [Accessed 24 September 2019].

Commission Regulation (EC) No 552/2009 of 22 June 2009 amending Regulation (EC) No

1907/2006 of the European Parliament and of the Council on the Registration, Evaluation,
Authorisation and Restriction of Chemicals (REACH) as regards Annex XVII. Official
Journal of the European Union: pp.L164/7–L164/31. Available at: https://eur-
lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:32009R0552&from=GA. [Accessed
25 September 2019].

Commission Regulation (EU) 2017/227 of 9 February 2017 amending Annex XVII to

Regulation (EC) No 1907/2006 of the European Parliament and of the Council concerning
the Registration, Evaluation, Authorisation and Restriction of Chemicals (REACH) as
regards bis(pentabromophenyl)ether. Official Journal of the European Union: pp.L35/6-
L35/9. Available at: https://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?
uri=CELEX:32017R0227&from=EN [Accessed 8 September 2019]. Corrigendum
published in Official Journal of the European Union: pp.L249/18 on 4 October 2018.
Available at: https://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?
uri=CELEX:32017R0227R%2801%29&from=EN [Accessed 8 September 2019].

Committee on the Toxicity of Chemicals in Food, Consumer Products and the

Environment (2015) Statement on the potential risks from polybrominated diphenyl ethers
(PBDEs) in the infant diet. Available at: http://cot.food.gov.uk/committee/committee-on-

28 of 39
toxicity/cotstatements/cotstatementsyrs/cot-statement-2015/cot-statement-on-
polybrominated-diphenyl-ethers-pbdes [accessed 10th June 2015].

Council Decision of 14 October 2004 concerning the conclusion, on behalf of the

European Community, of the Stockholm Convention on Persistent Organic Pollutants
(2006/507/EC). 31 July 2006. Official Journal of the European Union: p.L209/1ff. Available
at: https://eur-lex.europa.eu/legal-content/EN/TXT/?uri=celex:32006D0507 [Accessed 14
September 2019].

Cristale, J., Katsoyiannis, A., Sweetman, A. J., Jones, K. C. and Lacorte, S. (2013)
Occurrence and risk assessment of organophosphorus and brominated flame retardants in
the River Aire (UK). Environmental Pollution 179: pp.194–200. Available at:
https://www.sciencedirect.com/science/article/pii/S0269749113002029 [Accessed 13
September 2019].

Crosse, J. D., Shore, R. F., Jones, K. C. and Pereira, M. G. (2012a) Long-term trends in
PBDEs in sparrow hawk (Accipiter nisus) eggs indicate sustained contamination of UK
terrestrial ecosystems. Environmental Science and Technology 46(24): pp.13504–13511
[online]. Available at: http://pubs.acs.org/doi/ipdf/10.1021/es303550f [Accessed 1
September 2015].

Crosse, J. D., Shore, R. F., Jones, K. C. and Pereira, M. G. (2012b) Long term trends in
PBDE concentrations in gannet (Morus bassanus) eggs from two UK colonies.
Environmental Pollution 161: pp.93–100 [online]. Available at:
http://www.sciencedirect.com/science/article/pii/S0269749111005628 [Accessed 1
September 2015].

Crosse, J. D., Shore, R. F., Jones, K. C. and Pereira M. G. (2013) Key factors affecting
liver PBDE concentrations in sparrowhawks (Accipiter nisus). Environmental Pollution 177:
pp.171–176.

Department for Business, Innovation, and Skills, BIS (2009) A statistical report to
investigate the effectiveness of the Furniture and Furnishings (Fire) (Safety) Regulations
1988. December 2009. London.

Directive 2000/60/EC of the European Parliament and of the Council of 23 October 2000
establishing a framework for Community action in the field of water policy. Official Journal
of the European Union: pp.L327/1–L327/72 [online]. Available at:
http://eur-lex.europa.eu/legal-content/EN/TXT/?
qid=1441097627937&uri=CELEX:32000L0060 [Accessed 1 September 2015].

Directive 2003/11/EC of the European Parliament and of the Council of 6 February 2003
amending for the 24th time Council Directive 76/769/EEC relating to restrictions on the
marketing and use of certain dangerous substances and preparations
(pentabromodiphenyl ether, octabromodiphenyl ether) [2003] pp.L42/45 [online]. Available

29 of 39
at: http://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?
uri=CELEX:32003L0011&from=EN.

Directive 2006/118/EC of the European Parliament and of the Council of 12 December

2006 on the protection of groundwater against pollution and deterioration. Official Journal
of the European Union: pp.L372/19. Available at:
https://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:02006L0118-
20140711&from=EN [Accessed 20 August 2019].

Directive 2008/105/EC of the European Parliament and of the Council of 16 December

2008 on environmental quality standards in the field of water policy, amending and
subsequently repealing Council Directives 82/176/EEC, 83/513/EEC, 84/156/EEC,
84/491/EEC, 86/280/EEC and amending Directive 2000/60/EC of the European
Parliament and of the Council. Official Journal of the European Union: pp.L348/84–
L348/97 [online]. Available at: http://eur-lex.europa.eu/LexUriServ/LexUriServ.do?
uri=OJ:L:2008:348:0084:0097:en:PDF [Accessed 30 June 2015].

Directive 2011/65/EU of the European Parliament and of the Council of 8 June 2011 on
the restriction of the use of certain hazardous substances in electrical and electronic
equipment. Official Journal of the European Union: pp.L174/88–L174/110 [online].
Available at: http://eur-lex.europa.eu/legal-content/EN/TXT/?uri=celex:32011L0065
[Accessed 1 September 2015].

Directive 2013/39/EU of the European Parliament and of the Council of 12 August 2013
amending Directives 2000/60/EC and 2008/105/EC as regards priority substances in the
field of water policy. Official Journal of the European Union: L226/14 [online]. Available at:
http://eur-lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:32013L0039&from=EN.

Drage, D. S., Aries, E. and Harrad, S. (2014) Studies into the formation of PBDEs and
PBDD/Fs in the iron ore sintering process. Science of The Total Environment 485-486:
pp.497-507 [online]. Available at: https://doi.org/10.1016/j.scitotenv.2014.03.093
[Accessed 31 May 2018].

Drage, D. S, Newton, S., de Wit, C. A. and Harrad, S. (2016) Concentrations of legacy and
emerging flame retardants in air and soil on a transect in the UK West Midlands.
Chemosphere 148: pp.195-203 [online]. Available at:
https://doi.org/10.1016/j.chemosphere.2016.01.034 [Accessed 31 May 218].

Earnshaw, M. R., Jones K. C. and Sweetman A. (2013) Estimating European historical

production, consumption and atmospheric emissions of decabromodiphenylether. Science
of the Total Environment 447: pp.133–142.

Earnshaw, M. R., Jones K. C. and Sweetman A. (2015) A first European scale multimedia
fate modelling of BDE-209 from 1970 to 2020. Environment International 74: pp.71–81.

30 of 39
Available at: https://www.sciencedirect.com/science/article/pii/S0160412014002852
[Accessed 14 September 2019].

Eljerrat, E., Marsh, G., Labandeira, A. and Barcelo D. (2008) Effect of sewage sludges
contaminated with polybrominated diphenylethers on agricultural soils. Chemosphere 71:
pp.1079–1086

European Chemicals Bureau (2001) Diphenyl ether, pentabromo derivative

(pentabromodiphenyl ether), CAS-No: 32534-81-9, EINECS-No: 251-084-2. Summary
Risk Assessment Report. European Commission, Joint Research Centre [online].
Available from: http://echa.europa.eu/documents/10162/05a9c558-9472-4163-9496-
1a8ab1ee6918. [Accessed 5 February 2015].

European Food Safety Authority, EFSA (2011). Scientific opinion on polybrominated

diphenyl ethers (PBDEs) in food. EFSA Panel on Contaminants in the Food Chain
(CONTAM). EFSA Journal 9(5): pp.2156. Parma, Italy: European Food Safety Authority.

European Chemicals Agency, ECHA (2012) Agreement of the member state committee on
the identification of bis(pentabromophenyl) ether [decabromodiphenyl ether] as a
substance of very high concern according to Articles 57 and 59 of Regulation (EC)
1907/2006 [online]. Available at: http://echa.europa.eu/documents/10162/1f83d2de-8eaf-
405a-90a1-a9e2d0651459.

European Commission (2012) Polybrominated diphenyl ethers. PolyBDEs EQS dossier

2011 [online]. Available at: https://circabc.europa.eu/sd/a/d07ed9f5-0760-4561-b642-
04bc1e4a580e/PBDE%20EQS%20dossier%202011.pdf [Accessed 25 June 2019].

European Commission (2014) Common implementation strategy for the Water Framework
Directive (2000/60/EC): guidance document no. 32 on biota monitoring (the
implementation of EQSbiota) under the Water Framework Directive. Technical report – 2014
– 083. Luxembourg: European Union. Available at:
https://circabc.europa.eu/sd/a/62343f10-5759-4e7c-ae2b-12677aa57605/Guidance%20No
%2032%20-%20Biota%20Monitoring.pdf [Accessed 12 September 2019].

Council Directive 1999/31/EC of 26 April 1999 on the landfill of waste. Official Journal of
the European Communities: pp.L182/1–L182/19 [online]. Available at: https://eur-
lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:31999L0031&from=EN [Accessed
24 September 2019].

Environment Agency (2013a) Water Framework Directive Progress Review. Brominated

diphenyl ether. Draft. Unpublished.

Environment Agency (2013b) Landfill Leachate Composition Project Version 1 (December

2013). Internal report. Unpublished.

31 of 39
European Food Safety Authority, EFSA (2011) Scientific opinion on polybrominated
diphenyl ethers (PBDEs) in food. EFSA Panel on Contaminants in the Food Chain
(CONTAM). EFSA, Parma, Italy. 4 August 2011. EFSA Journal, 9(5), pp. 2156ff. Available
at: https://efsa.onlinelibrary.wiley.com/doi/epdf/10.2903/j.efsa.2011.2156 [Accessed 26
September 2019].

Fernandes, A., Mortimer, D., Gem, M., Dicks, P., Smith, F., White, S. and Rose, M. (2009)
Brominated dioxins (PBDD/Fs) and PBDEs in marine shellfish in the UK. Food additives &
Contaminants: Part A 26(6): pp.918-927 [online]. Available at:
https://www.tandfonline.com/doi/full/10.1080/02652030902803026?
scroll=top&needAccess=true [Accessed 4 June 2018].

The Food and Environment Research Agency (2015) Geographical Investigation for
chemical contaminants in fish collected from UK and proximate marine waters. Report to
the Food Standards Agency. March 2015 [online]. Available at:
https://www.food.gov.uk/sites/default/files/media/document/fs102005reportfinal.pdf
[Accessed 26 September 2019].

Graf, C., Katsoyiannis, A., Jones, K. C. and Sweetman, A. J. (2016) The TOMPs ambient
air monitoring network – Continuous data on UK air quality for over 20 years.
Environmental Pollution 217: pp.42-51 [online]. Available at:
https://doi.org/10.1016/j.envpol.2016.01.033 [Accessed 31 May 2018].

Guillaume, E., Chivas, C. and Sainrat A. (2000) Regulatory issues and flame retardant
usage in upholstered furniture In Europe LNE – CEMATE – Fire Behaviour Division
Research, Studies Fire Safety Engineering Activities [online]. Available at:
https://www.fireseat.eng.ed.ac.uk/sites/fireseat.eng.ed.ac.uk/files/images/04-Guillaume.pdf
[Accessed 9 September 2019].

Harrad, S. and Hunter, S. (2006) Concentrations of Polybrominated Diphenyl Ethers in Air

and Soil on a Rural−Urban Transect Across a Major UK Conurbation. Environmental
Science & Technology 40(15): pp.4548-4553 [online]. Available at:
https://doi.org/10.1021/es0606879 [Accessed 31 May 2018].

Harrad, S., Ibarra, C., Abdallah, M. A-E., Boon, R., Neels, H. and Covaci, A. (2008)
Concentrations of brominated flame retardants in dust from United Kingdom cars, homes,
and offices: Causes of variability and implications for human exposure. Environment
International 34(8): pp.1170-1175 [online]. Available at:
https://doi.org/10.1016/j.envint.2008.05.001 [Accessed 30 May 2018].

Harrad, S. and Abdallah, M. A-E. (2011) Brominated flame retardants in dust from UK cars
– Within-vehicle spatial variability, evidence for degradation and exposure implications.
Chemosphere 82(9): pp.1240-1245 [online]. Available at:
https://doi.org/10.1016/j.chemosphere.2010.12.038 [Accessed 30 May 2018].

32 of 39
Jürgens, M. D., Johnson, A. C., Jones, K. C., Hughes, D. and Lawlor, A. J. (2013). The
presence of EU priority substances mercury, hexachlorobenzene, hexachlorobutadiene
and PBDEs in wild fish from four English rivers. Science of The Total Environment 461-
462: pp.441-452 [online]. Available at: https://doi.org/10.1016/j.scitotenv.2013.05.007
[Accessed 1 June 2018].

Kuang, J., Ma, Y. and Harrad, S. (2016) Concentrations of “legacy” and novel brominated
flame retardants in matched samples of UK kitchen and living room/bedroom dust.
Chemosphere 149: pp.224-230 [online]. Available at:
https://doi.org/10.1016/j.chemosphere.2016.01.092 [Accessed 30 May 2018].

Law, R. J. (2014). An overview of time trends in organic contaminant concentrations in

marine mammals: going up or down? Marine Pollution Bulletin 82(1–2): pp.7–10.

Law, R. J., Covaci, A., Harrad, S., Herzke, D., Abdallah, M. A., Fernie, K., Toms, L. M. L.
and Takigami, H. (2014) Levels and trends of PBDEs and HBCDs in the global
environment: status at the end of 2012. Environment International 65: pp.147–158.

Leslie, H. A., Leonards, P. E. G., Shore, R. F., Walker, L. A., Bersuder, P. R. C., Morris,
S., Allchin, C. R. and de Boer, J. (2011) Decabromodiphenylether and
hexabromocyclododecane in wild birds from the United Kingdom, Sweden and The
Netherlands: Screening and time trends. Chemosphere 82(1): pp.88-95 [online]. Available
at: https://doi.org/10.1016/j.chemosphere.2010.09.073 [Accessed 1 June 2018].

Matscheko, N., Tysklind, M., de Wit, C., Bergek, S., Andersson, R. and Sellström, U.
(2002) Application of sewage sludge to arable land-soil concentrations of polybrominated
diphenyl ethers and polychlorinated dibenzo-p-dioxins, dibenzofurans, and biphenyls, and
their accumulation in earthworms. Environmental Toxicology and Chemistry 21: pp.2515–
5225.

Muenhor, D. (2011) Polybrominated diphenyl ethers (PBDEs) in indoor and outdoor

environments. Doctor of Philosophy (Ph.D.), University of Birmingham, Birmingham
[online]. Available at: http://etheses.bham.ac.uk/2854/1/Meunhor11PhD.pdf [Accessed 4
June 2018].

Muenhor, D. and Harrad, S. (2012) Within-room and within-building temporal and spatial
variations in concentrations of polybrominated diphenyl ethers (PBDEs) in indoor dust.
Environment International 47: pp.23-27 [online]. Available at:
https://doi.org/10.1016/j.envint.2012.06.001 [Accessed 30 May 2018].

OSPAR (2010) Quality Status report 2010. Status and trend in marine chemical pollution.
OSPAR Commission [online]. Available at:
http://qsr2010.ospar.org/media/assessments/p00395_Chemical_status_and_trend_HA-
6.pdf?zoom_highlight=brominated%2Bflame%2Bretardants#search="brominated flame
retardants" [Accessed 21 April 2015].

33 of 39
Oakdene Hollins (2010). A study to facilitate the implementation of the waste related
provisions of Regulation (EC) No 850/2004 on persistent organic pollutants [online].
Available at: http://randd.defra.gov.uk/Document.aspx?Document=CB0438(updated).pdf
[Accessed 30 January 2015].

Prevedouros, K., Jones, K. C. and Sweetman A. J. (2004) Estimation of the production,

consumption and atmospheric emissions of pentabrominated diphenyl ether in Europe
between 1970 and 2000. Environmental Science and Technology 38(12): pp.3224–3231.

Rauert, C. and Harrad, S. (2015) Mass transfer of PBDEs from plastic TV casing to indoor
dust via three migration pathways — A test chamber investigation. Science of The Total
Environment, 536: pp.568-574 [online]. Available at:
https://doi.org/10.1016/j.scitotenv.2015.07.050 [Accessed 31 May 2018].

Regulation (EC) No 850/2004 of the European Parliament and of the Council of 29 April
2004 on persistent organic pollutants and amending Directive 79/117/EEC. 29 June 2004.
Official Journal of the European Union: pp.L229/5-L229/22. Available at: https://eur-
lex.europa.eu/LexUriServ/LexUriServ.do?uri=OJ:L:2004:229:0005:0022:EN:PDF
[Accessed 14 September 2019].

Regulation (EC) No 1907/2006 of the European Parliament and of the Council of 18

December 2006 concerning the Registration, Evaluation, Authorisation and Restriction of
Chemicals (REACH), establishing a European Chemicals Agency, amending Directive
1999/45/EC and repealing Council Regulation (EEC) No 793/93 and Commission
Regulation (EC) No 1488/94 as well as Council Directive 76/769/EEC and Commission
Directives 91/155/EEC, 93/67/EEC, 93/105/EC and 2000/21/EC. 30 December 2006.
Official Journal of the European Union: pp. L396/1-L396/849. Available at: https://eur-
lex.europa.eu/legal-content/EN/TXT/PDF/?uri=CELEX:32006R1907 [Accessed 14
September 2019]. Corrigendum published in Official Journal of the European Union: pp.
L136/3–L136/280 on 29 May 2007. Available at:
https://eur-lex.europa.eu/LexUriServ/LexUriServ.do?
uri=OJ:L:2007:136:0003:0280:en:PDF [Accessed 29 September 2019].

Regulation (EU) 2019/1021 of the European Parliament and of the Council of 20 June
2019 on persistent organic pollutants (recast). 25 June 2019. Official Journal of the
European Union: pp.L169/45-L160/77. Available at: https://eur-lex.europa.eu/legal-
content/EN/TXT/PDF/?uri=CELEX:32019R1021&from=EN [Accessed 14 September
2019].

Rose, M. and Fernandes, A. (2010) FD 09/07 Environmental contaminants in fish from

unmanaged inland UK waterways, Food and Environment Research Agency [online].
Available at:
http://webarchive.nationalarchives.gov.uk/20141103172011/http:/www.foodbase.org.uk/
admintools/reportdocuments/571-1-

34 of 39
1002_C01041_Contaminants_in_fish_and_shellfish_from_unmanaged_inland_UK_water
ways_final_reportx.pdf [Accessed 14 September 2018].

Rule, K. L., Comber, S. D. W., Ross, D., Thornton, A., Makropoulos, C. K. and Rautiu R.
(2006) Sources of priority substances entering an urban wastewater catchment—trace
organic chemicals. Chemosphere 71: pp.1079–1086.

Saini, A., Rauert, C., Simpson, M. J., Harrad, S. and Diamond, M. L. (2016) Characterizing
the sorption of polybrominated diphenyl ethers (PBDEs) to cotton and polyester fabrics
under controlled conditions. Science of The Total Environment, 563-564: pp.99-107
[online]. Available at: https://doi.org/10.1016/j.scitotenv.2016.04.099 [Accessed 31 May
2018].

Statutory Instrument 1990 No. 880. The Sludge (use in Agriculture) (Amendment)
Regulations 1990. [Online]. Available at:
http://www.legislation.gov.uk/uksi/1990/880/contents/made [Accessed 13 October 2015].

Statutory Instrument 2016 No. 1154. The Environmental Permitting (England and Wales)
Regulations 2016. [Online]. Available at:
https://www.legislation.gov.uk/uksi/2016/1154/made [Accessed 27 September 2016].

Sühring, R., Barber, J. L., Wolschke, H., Danijela, K. and Ebinghaus, R. (2015) Fingerprint
analysis of brominated flame retardants and Dechloranes in North Sea sediments.
Environmental Research, 140 pp. 569-578 [online]. Available at:
https://www.sciencedirect.com/science/article/pii/S0013935115001644?via%3Dihub
[Accessed 19 September 2018].

UK Government (2015). The Water Framework Directive (Standards and Classification)

Directions (England and Wales) 2015. Available at:
https://www.legislation.gov.uk/uksi/2015/1623/pdfs/uksiod_20151623_en_auto.pdf
[Accessed 24 September 2019].

UKWIR (2014a) Chemical Investigation Programme: Volume 1 – Main report

(13/EQ/01/6). ISBN: 1 84057 667 7.

UKWIR (2014b) Chemical Investigation Programme: Volume 4 – Overview of technical

investigations (13/EQ/01/9). ISBN 1 84057 714 2.

UKWIR (2019) The national Chemical Investigations Programme 2015-2020. Volume 1

Part 3 (2017-2019): monitoring of sewage effluents and surface waters - tranche 3. 14
March 2019. Final report, internal. London: UK Water Industry Research Ltd.

35 of 39
Vane, C. H., Ma, Y.-J., Chen, S.-J. And Mai, B.-X. (2010) Increasing polybrominated
diphenyl ether (PBDE) contamination in sediment cores from the inner Clyde Estuary, UK.
Environmental Geochemistry and Health 32(1): pp.13–21.

Walker, L. A., Moeckel, C., Pereira, M. G., Beith, S. J., Potter, E. D., Chadwick, E. A. and
Shore R.F. (2012) Polybrominated diphenyl ethers (PBDEs) in Eurasian otters (Lutra lutra)
collected from Britain in 2010: a Predatory Bird Monitoring Scheme (PBMS) report.
Lancaster: Centre for Ecology and Hydrology. 14pp.

Wilford, B. H., Thomas, G. O., Jones, K. C., Davison, B. and Hurst, D. K. (2008)
Decabromodiphenyl ether (deca-BDE) commercial mixture components, and other
PBDEs, in airborne particles at a UK site. Environment International 34(3): pp.412-419
[online]. Available at: https://doi.org/10.1016/j.envint.2007.09.007 [Accessed 31 May
2018].

Windsor, F. M., Pereira M. G., Tyler, C. R. and Ormerod S. J. (2019) Persistent

contaminants as potential constraints on the recovery of urban river food webs from gross
pollution. Water Research 163(2019), 114858: pp1-12. Available at:
https://www.sciencedirect.com/science/article/pii/S0043135419306244 [Accessed 15
September 2019].

Yang, C., Rose, N. L., Turner, S. D., Yang, H., Goldsmith, B., Losada, S., Barber, J. L. and
Harrad, S. (2016) Hexabromocyclododecanes, polybrominated diphenyl ethers, and
polychlorinated biphenyls in radiometrically dated sediment cores from English lakes, ~
1950–present. Science of The Total Environment 541: pp.721-728 [online]. Available at:
https://www.sciencedirect.com/science/article/pii/S0048969715307622 [Accessed 13
September 2019].

8. List of abbreviations and acronyms

BDE-47 pentaBDE: 2,2′,4,4′-tetrabromodiphenyl ethBDEer; a congener present in
commercial

BDE-99 pentaBDE: 2,2′,4,4′,5-pentabromodiphenyl ether; a congener present in

commercial

BDE-209: decabromodiphenyl ether (decaBDE)

BDE: bromodiphenyl ether

BIS: Department for Business, Innovation and Skills

CEFAS: Centre for Environment, Fisheries and Aquaculture Science

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CIP: Chemicals Investigation Programme

CSEMP: Clean Seas Environment Monitoring Programme

DOME: Database on Oceanography and Marine Ecosystems

ECHA : European Chemicals Agency

EFSA: European Food Safety Authority

EQS: Environmental quality standard

EQSD: Environmental Quality Standards Directive

ICES: International Council for the Exploration of the Sea

LOQ: Limit of quantification

MAC: Maximum allowable concentration

OSPAR: Oslo Paris Convention

PBDEs: Polybrominated diphenyl ethers

POPs : Persistent organic pollutants

QA/QC: Quality assurance/quality control

REACH: Registration, Evaluation, Authorisation and Restriction of Chemicals

SAGIS: Source Apportionment Geographic Information System

TraC: Transitional and coastal

UKWIR: UK Water Industry Research

WFD: Water Framework Directive

WwTWs: Waste water treatment works

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9. Glossary
Adsorb: A sorption process in which one substance becomes attached to another through
adhesion to the surface

Bioaccumulate: The accumulation of a substance, such as a toxic chemical, in various

tissues of a living organism

Biomagnify: When the concentration of a substance in an organism exceeds the

background concentration of the substance in its diet

Congeners: Chemical substances related to each other by origin, structure or function

Debromination: Loss of bromine atoms from compound

Limit of qualification: The lowest concentration of a substance in a sample that can be

reliably quantified with an acceptable level of precision and accuracy

Lipid normalisation: Normalisation of measured concentrations of PBDEs by taking into

account actual lipid content in a fish and adjusting the concentrations relative to a default
lipid content of 5%. PBDEs are hydrophobic and tend to partition into the lipids of
organisms. This approach allows for comparability across results for different fish.

Organobromine: Organic molecule containing one or more bromine atoms

OSPAR: The mechanism by which 15 governments and the EU cooperate to protect the
marine environment of the North-East Atlantic

Passive samplers: Sampling device left in situ in the water column

Pollution inventory: The inventory collates data from large regulated industrial sites on
emissions of specified substances to air and controlled waters and sewers, as well as
quantities of waste transferred off site.

Stockholm Convention: The Stockholm Convention is a global treaty to protect human

health and the environment from persistent organic pollutants (POPs) and came into force
in May 2004.

Sorption: A physical or chemical process in which one substance takes up or holds

another

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Wet weight: Whole weight, fresh weight and wet weight refer to the sample as it is
received whole or wet, regardless of whether it is a whole organism or parts of the
organism.

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