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Factors influencing the spatial and temporal distribution of

microplastics at the sea surface – A year-long monitoring case
study from the urban Kiel Fjord, southwest Baltic Sea

Nicolas Christian Ory, Andreas Lehmann, Jamileh Javidpour,

Rüdiger Stöhr, Grace L. Walls, Catriona Clemmesen

PII: S0048-9697(20)33010-2
DOI: https://doi.org/10.1016/j.scitotenv.2020.139493
Reference: STOTEN 139493

To appear in: Science of the Total Environment

Received date: 16 April 2020

Revised date: 14 May 2020
Accepted date: 15 May 2020

Please cite this article as: N.C. Ory, A. Lehmann, J. Javidpour, et al., Factors influencing
the spatial and temporal distribution of microplastics at the sea surface – A year-long
monitoring case study from the urban Kiel Fjord, southwest Baltic Sea, Science of the Total
Environment (2020), https://doi.org/10.1016/j.scitotenv.2020.139493

This is a PDF file of an article that has undergone enhancements after acceptance, such
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© 2020 Published by Elsevier.

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Factors influencing the spatial and temporal distribution of microplastics at the

sea surface – a year-long monitoring case study from the urban Kiel Fjord,

southwest Baltic Sea.

Nicolas Christian Orya,1, Andreas Lehmanna, Jamileh Javidpoura,b, Rüdiger Stöhrc, Grace L.

Wallsa, and Catriona Clemmesena.

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a
GEOMAR Helmholtz Centre of Ocean Research Kiel, Düsternbrooker Weg 20, 24105, Kiel,

Germany. -p
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University of Southern Denmark. Department of Biology, Campusvej 55, 5230 Odense-M,
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Denmark.
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One Earth - One Ocean, Wischofstr. 1-3, Geb 1, 24148 Kiel
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To whom correspondence should be addressed. E-mail: nory@geomar.de, Phone: (49) 431 600
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4558.

Running title: microplastic spatiotemporal abundance within the Kiel Fjord

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ABSTRACT

Microplastics are ubiquitous to most marine environments worldwide, and their management has

become one of the major challenges facing stakeholders. Here we monitored monthly, between

March 2018 and March 2019, the abundance of microplastics (0.3-18.2 mm) at the sea surface

within the Kiel Fjord, southwest Baltic Sea. Microplastics were sampled at eight locations, inside

and outside the fjord, near potential source of microplastics, such as the outlets of storm drains or

the Kiel-Bülk wastewater treatment plant, the Schwentine River mouth and the entrance of the

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Kiel Canal. Weather (wind, precipitations) and seawater (salinity, temperature) parameters were

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compared to the spatiotemporal distribution of the microplastics. We found an overall stable, and

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low (0.04 particles/m3), microplastic load within the Kiel Fjord compared to other urban areas
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worldwide with comparable population densities. No relationship was found between the

microplastic abundance and the environmental factors, but the few samples that yielded
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unusually high amount of microplastics were all preceded by rainfall and snow/ice melt. During
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such events, vast amounts of water, potentially contaminated with microplastics, were released

into the fjord via the storm drainage system. The microplastic abundances at the wastewater
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plant outflow were amongst the lowest of our survey, likely thanks to an efficient filtering
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system. The results of this study highlight the importance to repeat microplastic samplings over

time and space to determine with confidence baseline microplastic abundance and to detect

unusual acute contamination, especially during snow and ice melting. Overall, the microplastic

abundance within the Kiel Fjord was low, probably thanks to efficient waste management on

land. However, improvements are still needed to filter millimetre-sized particles within the storm

drainage system, which is likely a major source of microplastics into the marine environment.

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Keywords: microplastic contamination, sea surface, southwest Baltic Sea, long-term monitoring,

environmental factors, wastewater treatment plant

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INTRODUCTION

Plastic debris are the major constituent of anthropogenic marine litter (Galgani et al., 2015; Law,

2017) due to the ubiquitous use of non-biodegradable polymers and their improper waste

management. Plastic production, which exceeded 350 million tonnes in 2019, should increase in

the future, thus leading to further contamination of the marine environment if no efficient

mitigation measures are undertaken locally and globally (Lebreton and Andrady, 2019). Marine

plastic litter is not only an environmental threat but may also induce adverse socio-economic

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repercussions, and its proper management is one of the major challenges that stakeholders are

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currently facing.

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Although the deleterious impacts of large plastic items on marine organisms have been
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described since the end of the last century (Laist, 1987), the threat of millimetre-sized particles

(microplastics) have been largely overlooked until only more recently (Browne et al., 2007, but
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see e.g. Carpenter et al., 1972; Hoss and Settle, 1990 for earlier studies). Microplastics are
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primarily manufactured for industrial or domestic uses, or result from the gradual fragmentation

of larger items, under biological, chemical and/or mechanical constraints (Cole et al., 2011).
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Microplastics have been documented in most marine environments, even in the most remote
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areas of the world, and in the digestive tract of a wide range of marine organisms (reviewed by

Lusher, 2015; Thiel et al., 2018), thereby raising growing concerns about the threat microplastics

pose to the integrity of marine ecosystems.

The majority of the plastic litter found in coastal waters is assumed to come from

improper management on land (Jambeck et al., 2015) and, to a lesser extent, from marine

activities, such as aquaculture, fishing and shipping (Andrady, 2011). Plastic waste is supposedly

transported from land to the sea via rivers, surface runoffs, sewage system, wind and shore

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littering (Auta et al., 2017; Cole et al., 2011). However, the contribution of each of these

environmental and anthropogenic components to the total input of microplastics into the marine

environment is still poorly understood. Such information would be valuable to implement the

measures to prevent plastic waste from entering the marine environment.

Microplastic contamination in coastal waters is generally related to human density (Nel et

al., 2017; Yonkos et al., 2014), indicating that coastal urban hubs are local points of entry of the

plastic waste. Within these urban areas, wastewater treatment plants (WWTP) are suspected to

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be an important source of emission of microplastics into the marine environment because they

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are processing vast amount of water potentially contaminated with plastic particles from industry

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and household use (reviewed by Rezania et al., 2018). Nevertheless, recent studies found that the
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input of small plastic particles may be limited depending on the filtration system of the plant

(Carr et al., 2016).

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Weather parameters, such as wind and precipitations, with associated runoffs, participate
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to the input of microplastic at sea. For example, the abundance of microplastic in coastal waters

near large cities increased markedly shortly after heavy rainfall and storm (Moore et al., 2002;
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Yonkos et al., 2014). During rainfall or snow melt, plastic particles may be washed off
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impervious surfaces (e.g. road, sidewalks, and car parks) and transported throughout the storm

sewage system directly into the sea. However, the mechanisms underlying the transport of

microplastics from the land to the sea, and at sea, are still poorly understood (Akdogan and

Guven, 2019). The transport of the microplastics in open ocean is mostly driven by

hydrodynamic forcing (e.g. Eriksen et al., 2014) that are likely different in semi-enclosed areas,

especially in areas where the tide range is negligible, such as in the Baltic Sea.

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The few studies that have examined the abundance of microplastics in the seawater and

fishes within the western Baltic Sea (Beer et al., 2017; Lenz et al., 2016; Ogonowski et al., 2019;

Rummel et al., 2016) mainly focussed on offshore areas; their results may not be generalizable to

coastal areas where most of the microplastics originate. Microplastic contamination has yet not

been described within the Kiel Fjord, in the western Baltic Sea, which may be an important

source of contamination due to the presence of the city of Kiel, cruise ship and ferry terminals,

naval harbours and military bases, and an intensive naval transit throughout the Kiel Canal,

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which is the most used artificial waterway in the world. The Kiel Fjord, and the whole southwest

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Baltic Sea in general, are important spawning ground for several commercially and ecologically

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important fish species (e.g. Hüssy, 2011; Polte et al., 2013), and their exposure to microplastic
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contamination warrants to be clarified.

The Baltic Sea and the North Sea meet in the transitional area between the Kattegat and
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the Belt Sea, in the southwest part of the Baltic Sea. The encounter of brackish water (<10 psu),
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from the eastern Baltic Sea, with higher saline water (>20 psu), from the Kattegat, forms a

salinity front, the Belt Sea front, moving eastward or westward within the Kiel Bight under the
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influence of prevailing wind conditions (Javidpour et al., 2009). The Kiel Fjord is a small
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extension of the Kiel Bight, and any salinity changes in the latter, due to the displacement of the

Belt Sea front, are mirrored in the Kiel Fjord (Lenz, 1977). Furthermore, the movement of water

masses in and out of the Kiel Fjord are principally driven by baroclinic exchange flows rather

than wind driven currents (Lehmann, personal communication), which thus are expected to not

play a major role on the horizontal distribution of the microplastics floating at the surface of the

Kiel fjord.

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The aim of this study was to assess the spatial and temporal distribution of millimetre-

sized plastic debris at the surface of the Kiel Fjord, and to examine which environmental and

anthropogenic factors affect their distribution. Surface water samples were collected monthly for

13 months at different locations within and outside the Kiel Fjord using an epineuston trawl to

assess the abundance of microplastics. During the study period, weather (wind, precipitations)

and water (temperature, salinity) parameters were monitored daily and during each water

sampling to examine how they relate to the microplastic abundance. Sea water parameters were

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also used to estimate the water exchange between the Kiel Fjord and the surrounding Kiel Bight

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in relation to the distribution of the microplastics.

MATERIALS AND METHODS

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Study sites
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Surface water samples were collected once a month, between March 2018 and March 2019, at
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eight fixed stations, four within and four at the entrance of the Kiel Fjord (Fig. 1a-d). All the

stations were surveyed between 8h00 and 14h00, following the same chronological order. The
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station 1 (Fig. 1c) was chosen because it is near the most frequented seafront promenade in Kiel
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and near the outflow of the rainwater collection system of three catchment areas in a urbanised

area of Kiel (Fig. S1). The station 6 was on the opposite side of the fjord and at the mouth of the

Schwentine river, the unique source of freshwater into the Kiel Fjord (Fig. 1c). The stations 2

and 5 were at the entrance of the Kiel Canal and on the opposite side of the fjord, near a less

populated area, respectively (Fig. 1c). The station 3 was at the entrance of the Kiel Fjord (Fig.

1d) above the outflow pipes of the Kiel-Bülk waste water treatment plant (WWTP) that collects

and treats the domestic sewage waters from all urban areas around the Kiel Fjord. At this

location, three transects (3a, 3b and 3c), located directly above, 1000 m and 2000 m offshore,

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respectively, of the outflow pipes of the plant, were repeated one after the other, <10 min apart.

These transects were conducted to test the hypothesis that microplastic abundance would

diminish according to the distance from the wastewater outflow. The station 4 was on the

opposite side of the fjord entrance, offshore of the small Wendtorf harbour (Fig. 1d).

The first water sample was collected only at station 1 on the 8th of March 2018 during a

sampling trial. Stations 3b, 3c and 4 and stations 3a and 3c were not sampled on the 16th of

January and on the 21st of March 2019, respectively, due to bad weather conditions.

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Microplastic sampling

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Sea surface samples were collected using a 260-cm long net (300 μm mesh size;
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www.hydrobios.de) closed at one end by a soft net-bag. The other end of the net was mounted to

a rectangular (70 × 40 cm) stainless steel frame kept afloat with two lifting bodies fixed in the
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middle of each side of the frame, so that only the first 30 cm of the sea surface were sampled.
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The trawl was connected to a 20-m long steel cable and towed from the stern of a small research

vessel (F.B. Polarfuchs) at a constant speed of 3 knots for 5 min. On one day, the survey was
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conducted from another research vessel (Sagitta Laboe) due to mechanical problems on the F.B.
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Polarfuchs.

Before each trawling, the inside and outside of the net, with no net-bag attached, were

first rinsed thoroughly with seawater collected by the pumping system of the boat throughout a

PVC hose. Then, the net was rinsed from the outside to remove any plastic particles, which could

have originated from the hose, stuck inside the mesh. The net-bag was then connected to the net,

and the trawl was lowered down to the sea surface to start the sampling. The volume of the water

filtered through the mesh during each trawling was estimated with a Hydrobios mechanical

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flowmeter attached across the wide opening of the frame of the trawl. The distance of each trawl

was measured with the onboard GPS to calculate the total area sampled. After each trawl, the

content of the net-bag was transferred with a wash bottle filled with ultrapure water, to a

transparent 500-ml polypropylene flask, previously rinsed thoroughly with ultrapure water, and

then placed into a large plastic cooling box.

During each trawling, the wind and wave conditions were estimated by two observers on

board following a standard Beaufort scale. Trawls were not conducted when the Beaufort score

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was >4 (moderate breeze) because floating microplastics can be mixed within the water column

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under stronger wind conditions (Eriksen et al., 2013).

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Microplastic description

Once in the laboratory, the content of each sample flask was filtered through a 100 µm sieve,
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transferred into a 50 mL polypropylene flask, previously rinsed three times with 99% ethanol,
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filled with 70% ethanol and stored until analysed. Then, the content of the 50 ml flask was

poured into a glass petri dish divided into three equal compartments and visually examined under
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a Leica M125 stereomicroscope with 8−100× magnification. All potential microplastics were
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cautiously removed and placed individually at the bottom of a well of a polystyrene 24-wells

culturing plate placed into an oven at 60°C and dried for >48h. All the particles that had lost their

three-dimensional structure after drying were considered as non-plastic and discarded from the

analysis. All the other particles were then photographed with a digital camera mounted to a

stereomicroscope Nikon SMZ18 with 7.5−135× magnification, and then send to be chemically

analysed. The maximum length and width (perpendicular to the length) of a representative subset

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of 274 randomly chosen particles (60% of the total) was measured to the nearest 0.1 mm from

the pictures using the program Image J (imagej.nih.gov/ij/).

In this study, fibres (filament with a diameter <50 µm) were not taken into account in the

total estimation of the microplastics because of the risk of contamination with airborne particles

during field sampling (Frère et al., 2017). Other, fragments heavier than fibres are not a potential

source of airborne contamination (Dris et al., 2016).

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Polymer analysis

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The chemical composition of a representative subset of 224 randomly chosen particles (49% of

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the total) visually identified as potential plastic was analysed with a PerkinElmer Inc. brand
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Fourier transform infrared spectrometer (FTIR). Interferograms were measured with a high-

speed spectrometer Spectrum Two™ and the absorbance spectrum obtained by Fourier
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transformation. Each sample was placed individually on a diamond/KBr crystal plate and its
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surface was scanned 8 times with a beam of infrared light (4000 to 650 cm-1) with a resolution of

4 cm-1 at room temperature. The crystal plate was wiped dry with a cellulose cloth between two
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measurements. Each spectrum was automatically compared to a reference database of thousands

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of specific substances; spectra with a correspondence ≥70% (Lusher et al., 2013) were kept for

the description of the different types of polymers.

Each particle was then visually examined from the pictures to verify that their physical

features are consistent with their chemical composition. The FTIR analysis confirmed that 98%

of the particles were correctly visually identified as plastic.

Environmental data collection

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Before each trawl, the salinity and the temperature of the seawater was measured with a Sea &

Sun Technology 48M CTD fixed to a steel cable lowered with an A-frame, at the steer of the

boat, down to 50 cm above the seafloor of which depth was previously determined with the on-

board sonar. Salinity and temperature measurements were used to estimate the water exchange

between the Kiel Fjord and the Kiel Bight. Water salinity and temperature at 4, 8 and 13 m depth

were continuously monitored during the duration of the study at the Kiel lighthouse, ~10 km

from the entrance of the Kiel Fjord, by an automated weather station from the German Weather

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Service and GEOMAR.

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The daily total rainfall (mm), average wind speed (m/s) and direction (°), and air

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temperature (°C) were measured every 3 min during the duration of the study by a weather
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station on the roof of the GEOMAR building in Kiel (30 m height). Additionally, solid

precipitation (snow) was measured hourly with an optical disdrometer (Lempio and Bumke,
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2007). The mean wind direction and speed, rainfall and snowfall were calculated for a short
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(24h) and long (10d) period before each sampling day to examine the relationship between these

parameters and the microplastic abundance.

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Statistical analysis

The microplastic abundance was compared among the 3 transects at the outflow of the Kiel-Bülk

WWTP (3a, 3b and 3c), among all sampling stations (transect 3a,b and c pooled together as the

station 3), sampling dates (13 dates), and between the stations inside (stations 1, 2, 5 and 6

pooled together) and outside (stations 3 and 4 pooled together) the Kiel Fjord (Fig. 1) using

Kruskal-Wallis (H) rank tests when the homoscedasticity of the data was verified (see statistical

values in Table S1) or Welsch T tests otherwise. Significant tests were followed by post-hoc

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pairwise comparisons using individual Mann-Whitney tests with a Bonferroni correction (level

of error α=0.05% divided by the number of comparisons).

The relationship between the microplastic abundance and the mean wind direction, mean

wind speed, total rainfall and total snowfall 24h before each sampling day was examined using a

multiple regression model using an MM-estimator with coefficients of determination robust to

the presence of outliers that do not require any assumption on the distribution of the explanatory

variables (Renaud and Victoria-Feser, 2010).

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Homoscedasticity between groups was assessed using Leven tests. All statistical analysis

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and graphs were performed in RStudio v.1.2.1335 using the packages ‗car‘ v.3.0.3, ‗ggplot2‘

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v.3.2.1, ‗onewaytests‘ v.2.4 and ‗robust‘ v.0.4.18.2.
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RESULTS
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Microplastic abundance

From March 2018 to March 2019, a total number of 458 millimetre-sized anthropogenic debris
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were collected from the sea surface within and outside the Kiel Fjord. All but one (cellulose-
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type) of the subset of 224 particles (49% of the total) analysed by FTIR were confirmed to be

plastic polymers. The abundance of the plastics collected during a single trawl ranged from 0.0

to 1.8 particles/m3, with an overall median abundance of 0.04 ± interquartile range (IQR) 0.06

particles/m3 (25.3 ± 117.3 particles/km2; n = 100 trawls; Fig. 2a). The amount of microplastics

did not vary among the 13 months the study lasted (F = 1.21, df = 12, p = 0.33; Fig. 2b and see

Table S1 for the effect size values). However, five transects yielded substantially greater amount

of microplastics (i.e. outliers 1.5 times above the upper quartile; Fig. 2a) on 08 March 2018 (1.77

particles/m3 at the station 1), 21 March 2018 (0.9 and 0.4 particles/m3 at the station 2 and 5,

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respectively), 19 April 2018 (0.2 particles/m3 at the station 2) and 16 January 2019 (0.3

particles/m3 at the station 6).

The microplastic abundance did not vary among the three transects at the outflow of the

Kiel-Bülk wastewater plant (stations 3a, 3b and 3c, n = 12, 12 and 11, respectively; H = 1.54, df

= 2, p = 0.46; Fig. 2c and see Table S1 for effect size values), and were thus pooled for each

sampling day, and referred as station 3 for the rest of the analysis. Overall, the microplastic

abundance varied among the six different stations (H = 24.29, df = 5, p < 0.001; Fig. 2c and see

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Table S1 for effect size values), essentially due to the lower microplastic load at the station 4

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(median = 0.02 ± IQR 0.03) compared to the stations 1, 5 and 6. Microplastics were overall more

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abundant inside (median number of particles at the stations 1, 2, 5 and 6 pooled together = 0.07 ±

IQR 0.08 particles.m-3, n = 53; Fig. 2c) than outside (median number of particles at the stations
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3a, 3b, 3c and 4 pooled together = 0.02 ± IQR 0.04 particles.m-3, n = 47; see Table S1 for effect
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size values) the Kiel Fjord (H = 15.5, df = 1, p <0.0001).

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Microplastic types and characteristics

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The infrared spectroscopy analysis revealed that the particles were mostly made of high-density
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polyethylene (PE-HD; 40% of the total number of particles; Fig. 3), polypropylene (PP; 17%),

polystyrene (PS; 8%), polyethylene (PE; 5%), nylon (4%) and rubber (3%). Four particles were

made of polybutylene (PB), three of polyamide resins (PA), two of high-chlorinated

polyethylene (HCPE) and one of polyethylene-vinyl acetate (PEVA). Ten particles were made of

synthetic textile fibre composed of casein (Azlon; 5%). The chemical signature of 24 particles

(11.1%) referred to different additives (benzyl butyl phthalate (BBP), butylstearate,

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glyceraldehyde, tetradecene, aminopropyltrimethoxysilane and ethylene glycol) commonly

combined with plastic polymers; the specific type of plastic of these particles was not defined.

Most of the plastics found at the sea surface were broken fragments 0.3 to 18.2 mm long

(median size = 1.3 ± IQR 1.4 mm; Table 1), which probably came from the degradation of

unidentified larger items. The majority of the microplastics were hard fragments (66%), and soft

fragments (14%; Fig. 3 and Table 1). Sixty-six particles (14% of all the microplastics) were

green (70%), red (21%), blue (6%) and orange (2%) paint-like flakes composed of various

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polymers or additives, amongst which the most common were benzyl butyl phthalate (BBP;

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37%), high chlorinated polyethylene (HCPE; 24%), polyethylene chlorosulfonated (CSPE; 8%),

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acrylic (8%), benzopyrene (8%) and butylstearate (8%; Fig. 3). Twenty-one particles made of
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intertwined fibres (5%) and five monofilaments (1%) made the rest of the types of microplastics

collected in the water samples.

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Environmental variables

The regression model revealed no significant relationship between the microplastic abundance
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and the mean wind direction (t = -2.08, P = 0.067), mean wind speed (t = -1.20, P = 0.259), total
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rainfall (t = 0.48, P = 0.644) and total snowfall (t = 1.34, P = 0.214) 24h before each sampling

(Fig. 4 and Table S2).

The analysis of the weather parameters (air temperature, rainfall, snowfall, and wind

direction and speed) during a 10-days period before the samplings (08/03/2018, 21/03/2018,

19/04/2018 and 16/01/2019) that yielded the five largest amount of microplastics (see above and

Fig. 2b) revealed that all these samplings were preceded by rainfall and/or snowfall (Fig. 5a-h)

events. The three largest microplastic loads were found after a period of eight (Fig. 5i) and three

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(Fig. 5j) days of freezing temperature that were then followed by positive temperature 48h and

24h before the samplings, respectively. The air temperature was always positive during the

period preceding the two other samples with the greatest microplastic loads (Fig. 5k,l).

The wind speed (Fig. 5m-p) was greatly variable before the samplings with the most

abundant microplastics; it decreased (Fig. 5m,o) or increased (Fig. 5p) gradually over the 10

days before sampling, or rapidly changed from minimum (~0.5 m/s) to maximum (~14 m/s)

values within few days (Fig. 5n). The day that yielded the greatest microplastic abundance at the

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station 1, on the western side of the fjord, was preceded by dominant easterly winds (Fig. 5q).

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The two second largest amount of microplastics were collected at the stations 5 and 6, located on

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the eastern side on the fjord, on a day (21/03/2018) that was preceded by easterly dominant
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winds (Fig. 5r). The two other sampling days with high microplastic loads, at the stations 2 and 6

located on each side of the fjord, were preceded by dominant westerly winds (Fig. 5s,t).
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The salinity at depth (13 m) at the entrance of the Kiel Fjord rapidly increased from 13 to
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22 psu in about two weeks between the middle of June and the beginning of July 2018 (Fig. S2),

which indicates a massive exchange of saline water from the Kiel Bight into the Kiel Fjord under
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the effects of north-west winds. By the end of August 2018, the change of salinity was observed
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throughout the whole water column, meaning that the water of the Kiel Fjord had been replaced

entirely. No other major changes in salinity occurred for the rest of the study.

The input of freshwater from the Schwentine River during this study varied from 0.7 m3/s

(30/10/2018) to 14.0 m3/s (13/03/2018), with an average of 3.5 ± SD 3.4 m3/s (Fig. S3). One

month before the first sampling of this study (08 March 2018), the river outflow steadily

decreased from 17.0 m3/s to 9.4 m3/s, stabilized around this value for about two months, and then

decreased again to its lowest values (0.7-2.7 m3/s) during the summer and the autumn 2018, as a

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consequence of low precipitations (Fig. S4). The river flow then slowly increased from

December 2018 onwards to a maximum of 12 m3/s four days before the last sampling in March

2019. The Schwentine River runoff was too low to significantly affect the water budget of the

Kiel Fjord, especially during the dry year 2018.

DISCUSSION

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Microplastic abundance within the Kiel Fjord and the western Baltic Sea

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During the 13 months that our study lasted, the abundance of microplastics at the sea surface

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within the Kiel Fjord was overall stable with a median of 0.04 particles/m3 (25.3 particles/km2).

Such abundance was similar to what has been observed in other areas near urban centres along
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the Portuguese coast (Frias et al., 2014), but lower than that near other areas with relatively
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similar population densities and economic development as Kiel within the western Baltic Sea (2
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particles/m3 near the city of Stockholm in Sweden; Gewert et al., 2017), the English Channel

(0.3 particles/m3, Cole et al., 2014) or the northeast Atlantic (2.5 particles/m3, Lusher et al.,
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2014; 0.2 particles/m3, Frère et al., 2017), for example. One of the reasons for such differences
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may be due to the fact that those studies sampled microplastics over a shorter period of time

compared to this study, and the actual microplastic contamination may have been overestimated

at some locations. The load of microplastic fragments found within the Kiel Fjord in this study

was more representative of areas with low human density, such as in the Bay of Calvi in Corsica,

France (0.01 particles/m3, Collignon et al., 2014), or along the west coast of Sweden (0,01–0,14

particles per m3, Norén, 2007).

In some of our samples, the abundance of microplastic was unusually high, severalfold,

up to about 50 times, the median abundance measured during this study. Such high abundances

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were nevertheless much lower than those reported in surface waters near other urban areas in the

world with similar population size as in Kiel. For example, the abundance of non-fibre particles

in water samples was ~120 particles/m3 within the Durban Harbour, South Africa (Nel et al.,

2017), ~300 particles/m3 within the Strait of Georgia near Vancouver, Canada (Desforges et al.,

2014) or ~700 particles/m3 near the city of Qinzhou, China (Zhu et al., 2019). The findings of

this study thus indicate that microplastic contamination within the Kiel Fjord was low, even on

the few occasions when the load of microplastics was at its highest levels.

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A long-term monitoring within the southwest Baltic Sea revealed that the amount of

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microplastics in the water did not increase during the last three decades (Beer et al., 2017),

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suggesting a constant, and relatively low, input of microplastic within the area despite an
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exponential increase of the global plastic production (PlasticsEurope, 2019). Only few

microplastic fragments were found in clupeid fishes in the western Baltic Sea (Beer et al., 2017;
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Lenz et al., 2016; Rummel et al., 2016), thereby indicating that microplastic contamination
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within the southwest Baltic Sea is not a major threat for the fish compared to their commercial

overexploitation (ICES, 2018).

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Input of microplastics at sea

Large increases of microplastic load in coastal waters near large urban centres have often been

documented after heavy rainfall (Axelsson and van Sebille, 2017; Moore et al., 2002; Yonkos et

al., 2014). In our study, the sampling days that yielded the greatest amount of microplastics were

preceded by rainfall events, but no relationship was found between the amount of microplastics

and precipitations on the long run. For example, we did not observe an increase of microplastic

abundance within the Kiel Fjord during the first heavy rainfalls in August 2018 (Fig. S4) as it

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would have been expected after several months with low precipitations (Moore et al., 2011),

during which microplastics might have accumulated on land. ,.

All of the unusually high amounts of microplastics were collected days after snowfall and

snow/ice melting, during the first months of the year 2018 and 2019. The mechanisms

underlying the influence of snowfall on the input of microplastic into the marine environment are

yet to be clarified. Plastic fragments littered on the ground may be mixed with the snow that was

shovelled to clear the roads and walking paths, and thus gradually accumulated inside snow

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piles. In our study, the snow probably accumulated for several days because of freezing

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temperature; it melted shortly before some of the sampling dates, thus releasing into the Kiel

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Fjord vast amount of water potentially contaminated with microplastics. Further studies are
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needed to better understand whether and how snow and ice melt are related to an increase of

microplastic input into the sea.

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In most cities, storm waters running off impervious surfaces are first filtered at the street
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level by sewer grates and collectors which prevent items larger than a couple of centimetres to

enter the storm drain. In Kiel, water runoffs are conducted throughout the storm drainage system,
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which is independent of the sewage water system treated by the Kiel-Bülk wastewater treatment
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plant (see below), and released at different locations along the shore of the fjord (Fig. S1)

without being further filtered (D. Fuhrmann, personal communication). The bulk of the

microplastics is thus likely to enter the storm drainage system, and then released at sea within the

first moments after the beginning of a rainfall or ice/snow melt event.

On the 14/06/2019, we opportunistically observed the outflow of a storm drainage pipe

(number 37 in Fig. S1) along the seafront promenade in Kiel 30 min after a moderate rainfall

(2.8 mm of water within 3 h) (Fig. S5a). The plume of the water released from the storm drain

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spread rapidly at the surface of the Kiel Fjord (Fig. S5b) and carried away organic matter and

plastic fragments that had been transported via the storm drain (Fig. S5c). On the next morning,

no visible accumulation of microplastics nor organic matter was observed at the sea surface

within that area, indicating that floating particles had been quickly spread at the sea surface or

sank. This observation provide further evidences that the storm drainage system is an important

mean of transport of microplastics from the land to the sea.

In our study, the abundance of microplastics at the sampling locations near the mouth of

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the Schwentine River (stations 1 and 6; Fig. 1) was the greatest during winter months, when the

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volume of the river outflow was the highest. Although large rivers are important vector of

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transport of microplastics from land into the marine environment (Lebreton and Andrady, 2019),
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it is unlikely that a small river such as the Schwentine River, with an average outflow of 3.5

m3/s, was a major source of microplastics contamination in our study. Also, most of the river‘s
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path runs across rural areas with no major source of contamination (e.g. industry, large urban
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hub, WWTP). Other than large research vessels sometimes docking for a couple of days at the

GEOMAR pier, at the mouth of the river, only small recreational boats or canoe navigate on the
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river. We assume that the occasionally high amounts of microplastics found at the mouth of the
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river were probably mostly transported with the rainwater from the sewage pipes nearby (see

Fig. S1).

Input of microplastics via wastewater treatment plants

The amounts of microplastics collected near the outflow of the Kiel-Bülk wastewater treatment

plant (WWTP) were amongst the lowest of our studied. The low microplastic load found near the

outflow of the Kiel-Bülk WWTP is most unlikely due to low levels of contamination in the

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influent of the treatment plant. Indeed, many of the estimated three-figure tonnes of

microplastics still in use in 2015 in cosmetics, commercial cleansing and blasting abrasives in

Germany should enter the municipal sewage systems (Essel et al., 2015). It is therefore likely

that the 52,000 m3 of sewage waters entering the Kiel-Bülk plant daily contained vast amounts of

microplastics, as it has also been found in WWTP in other European countries (Magnusson and

Norén, 2014; Murphy et al., 2016; Talvitie et al., 2015).

At the time of this study, the Kiel-Bülk plant treated the sewage water using a three-stage

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purification system (M. Wuttke, personal communication). The latest stage consisted in filtering

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the water through a filter cloth made of different layers of microfibers with a nominal pore size

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of 40-60 µm that can retain up to 93% of solid fragments <500 µm long (Mintenig et al., 2017).
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Therefore, most of the microplastics >300 µm (i.e. the lower size limit of the particles examined

in this study) still present in the sewage water after the first two filtering stages were likely
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retained by the filter cloth. However, particles <40 µm are susceptible to be released in the
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marine environment. The evaluation of the abundance of such small particles in the water

samples was beyond the scope of this study, and should be examined in future studies, especially
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because nanoparticles are potentially detrimental to many marine organisms (Koelmans et al.,
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2015).

Some of the microplastics may have previously accumulated into the organic sludge

produced during the skimming and the sedimentation of the sewage water during the first two

purification stages (see Mintenig et al., 2017). Many studies have confirmed the presence of

microplastics in the sewage sludge from WWTP in Germany (Mintenig et al., 2017; Weithmann

et al., 2018) and worldwide (Carr et al., 2016; Murphy et al., 2016). The sludge may be

ultimately used as fertilizer in agriculture, and thus represents a potential source of plastic

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contamination on land (Akdogan and Guven, 2019) that still needs to be fully acknowledge by

environmental laws. Indeed, the German law, although one of the strictest in the world, does not

enforce the control of plastic particles <1 mm in sludge used as fertilizers (Kehres, 2019).

Microplastic transport at sea

Here we did not find a clear relationship between the overall microplastic abundance and the

wind speed or direction. Wind speed was highly variable during the days preceding the

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samplings when the greatest amount of microplastics were collected, and could therefore not be

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directly related to the high levels of contamination found on these specific days. The transport

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and accumulation of microplastics at the surface of the open ocean are mainly driven by Ekman
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and geostrophic currents (Onink et al., 2019). In enclosed areas, the drift of small particles

floating at the sea surface is mainly due to direct wind and Stokes drift (Lehmann, personal
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communication). However, the small width of the inner part of the Kiel fjord and the presence of
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tall buildings and trees limit the surface drift created by westerly and easterly winds. Only

northerly and southerly winds, i.e. longitudinal to the fjord, could blow without being disrupted
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over a distance enough to create a surface drift capable of transporting small floating particles
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(A. Lehmann, personal communication). During the weeks following the greatest inputs of

microplastics into the Kiel fjord (March and April 2018, and January 2019), southerly winds

were dominant (Fig. S4), which should have maintained the microplastics inside the fjord.

However, the amount of microplastics constantly decreased overtime, indicating that wind had

only a limited effect on their distribution.

Large water mass movements, and potentially of floating millimetre-sized particles,

within the Kiel Fjord are mostly due to water movements between the fjord and the Kiel Bight

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through baroclinic exchanges (Lehmann, personal communication). During this study, the water

within the Kiel Fjord has been exchanged entirely once, during the month of June 2018, with a

massive import of saline water from the Kiel Bight that replaced the less saline waters of the Kiel

Fjord within about two weeks. Such import of external waters was not accompanied by an

increase of microplastics within the fjord, which suggests that the water entering the fjord from

the Kiel Bight was not a source of microplastics. Also, the unusually high abundances of

microplastics found in March and April 2018 constantly diminished and were already at their

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lowest one month before the water exchange, which hence cannot satisfactorily explain the

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diminution of the microplastic abundance at the sea surface of the Kiel Fjord observed during the

first months of our study.

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Part of the microplastics floating at the sea surface may have sunk to the bottom because

they aggregated with organic matter or were rapidly overgrown by a biofilm (Andrady, 2017).
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Another part of the microplastics may also have been deposited on the shoreline and beaches
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present along the Kiel Fjord. Beaches are important sinks for the plastic litter that can explain

part of the removal of the plastic from the sea surface (Critchell and Lambrechts, 2016; Zhang,
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2017). It is however challenging to disentangle the proportion of the microplastics found in the
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beach sediments that were littered locally and that have been transported at sea. Microplastics

littered onshore can accumulate over time into the sediment, up to several meters deep (Turra et

al., 2014), and can then resuspend at sea during storms (Critchell and Lambrechts, 2016). The

microplastics in the beach sand thus represent a potential source of contamination that should be

controlled by regular beach cleaning campaigns.

Type of microplastics

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All the microplastics found in this study were broken fragments, likely coming from larger items

of which the origin was mostly not possible to assess. A majority of these fragments were made

of polyethylene, mainly high-density polyethylene (HDPE), and polypropylene (PP), which were

also the types of polymers most commonly found at the sea surface elsewhere (Schwarz et al.,

2019). Such prevalence of polyethylene fragments is not surprising because these polymers are

used to manufacture many common objects, such as bottles (food products, detergents,

cosmetics), food containers and packaging, household goods, toys, automotive equipment, crates

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and boxes and pipes (PlasticsEurope, 2019). The density of both PP (0.9 g/cm3) and HDPE (0.96

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to 0.97 g/cm3) is lower than that of the brackish waters of the Kiel Fjord (~1 g/cm3), meaning

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that the fragments should float at the sea surface, at least for some time before sinking under the
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effects of mechanical and biological processes (Andrady, 2017).

No polyethylene terephthalate (PET) fragments were found in our samples, despite the
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widespread use of such polymers for the production of many common plastic objects, such as
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bottles for soft drinks, packaging (PlasticsEurope, 2019). Such absence might be explained by

the fact that the PET particles are negatively-buoyant (1.29 to 1.40 g/cm3) and should sink to the
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seafloor shortly after being introduced at sea. Polyethylene is also commonly used to synthesize
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fibres, which are the most common microplastics found in some studies (e.g. Beer et al., 2017;

Gewert et al., 2017), but was not accounted for in this study because of the lack of efficient

method to control for airborne contamination during sampling. Also, rubber fragments from the

abrasion of car tires are considered to be an important source of microplastics into the marine

environment near urban centres (Leads and Weinstein, 2019; Sommer et al., 2018). No such

partices were found here, perhaps because most of the fragments, which are usually covered with

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road dust (Kreider et al., 2010), sink to the sea bottom near where they have been introduced

(Leads and Weinstein, 2019).

Paint-like flakes, mostly green, red and blue, were also regularly found in our samples.

Although we cannot exclude that some of these particles came from the boat we used during the

survey, the different colours and polymer types of the fragments we found suggest that the

particles did not come from the same boat. In addition, green flakes were also found in the

samples from January 2019 when the trawls were conducted with another boat than the one we

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used during all the other trawls. The large majority of the flakes we collected during our survey

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probably came from the paint of the hull of the many commercial, recreational and military ships

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that navigate every day within the Kiel Fjord and throughout the Kiel Canal, one of the most
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used in the world.
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CONCLUSION AND OUTLOOK

The year-long monthly survey we conducted at different locations within the Kiel Fjord allowed
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us to determine the overall microplastic contamination within the Kiel Fjord as well as to detect
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unusual events of acute microplastic contamination following rainfall, and ice and snow melt.

The findings of this study indicate that microplastics were probably introduced into the marine

environment mostly via the storm drainage system; such assumption warrants to be tested by

measuring the amount of microplastics directly at the storm drainage outlets before and shortly

after rainfall and snow melt, and after periods of drought or ice during which the microplastics

may accumulate on land. Also, the quantification of microplastics in the sediments at varying

distances from the storm drain outlets should be studied to clarify the settling and transport

processes of the particles once at sea. The results of such studies would help to disentangle the

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sources and fate of microplastics into the marine environment near urban centres in general.

Rainfall sewage systems are usually not designed to filter millimetre-sized particles. Innovative

measures, such as retention tanks, where the stormwater could be store temporarily and filtered

efficiently, should be included within the storm drain to control the release of microplastics into

the environment.

The proportion of microplastics found at the sea surface that fragmented first on land or

once at sea is still unknown. This information should be estimated to better understand the

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pathways of microplastics into the marine environment and, in turn, implement efficient

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mitigation measures. No large plastic items were found in our samples nor visually observed

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floating at the sea surface during the samplings, probably thanks to landfill bans and efficient
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waste management in Germany (PlasticsEurope, 2019). However, we observed that many plastic

protective caps from consumer firework rockets littered during the 2020 New Year‘s evening
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were already broken into small fragments, some of few millimetres, few days after the event
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(Fig. S6). Many of the fragments were small enough to enter the sewage system, and could have

thus been flushed into the Kiel Fjord during the abundant rainfalls in January 2020. Consumer
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fireworks, in addition to impacting the air quality and the wildlife, are thus also a potential
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source of plastic contamination in the environment, and their use by the general public should be

controlled.

ACKNOWLEDGEMENTS

We are grateful to Katrin Knickmeier and the plastic pirates of the Kieler Forschungswerkstatt in

Kiel to have lent us the epineuston trawl for the duration of the study. We kindly thank Mr.

Michael Wuttke, process engineer of the Kiel-Bülk wastewater treatment plant, for his very

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interesting introduction to the functioning of the plant, and Mr. Dirk Fuhrmann, from the civil

engineering office in Kiel, for the maps and his thorough description of the Kiel storm drainage

system. We also thank Paulina Engel, Rebecca Piontek, Aurelia Laubscher for the analysis of the

water samples, Ivy Harms for the FTIR analysis of the microplastics, and Paulina Engel, Thea

Hamm, Anett Jannasch and Katharina Fietz for their help during the sampling. We are thankful

to Evelyn Lostarnau for the design and creation of the illustration used in the graphical abstract

of this publication. NCO was supported by a postdoctoral grant (No. D21/18) from ―The Future

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Ocean‖ Cluster of Excellence funded within the framework of the Excellence Initiative by the

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Deutsche Forschungsgemeinschaft on behalf of the German federal and state governments. This

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work was also partly supported by GoJelly project funded by the European Union‘s Horizon
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2020 research and innovation programme (Grant agreement no. 774499) and by the UFOTriNet

project funded by the Federal Ministry of Food and Agriculture (BMEL) based on a decision of
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the Parliament of the Federal Republic of Germany via the Federal Office for Agriculture and
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Food (BLE) under the innovation support programme (funding number 2819111918).
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vehicle for the entry of microplastic into the environment. Science Advances 2018; 4:
eaap8060.
Yonkos LT, Friedel EA, Perez-Reyes AC, Ghosal S, Arthur CD. Microplastics in four estuarine
rivers in the Chesapeake Bay, U.S.A. Environmental Science & Technology 2014; 48:
14195-14202.
Zhang H. Transport of microplastics in coastal seas. Estuarine, Coastal and Shelf Science 2017;
199: 74-86.
Zhu J, Zhang Q, Li Y, Tan S, Kang Z, Yu X, et al. Microplastic pollution in the Maowei Sea, a
typical mariculture bay of China. Science of The Total Environment 2019; 658: 62-68.

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FIGURES

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Figure 1. (a) Location map of the Kiel Fjord (red square), within the Kiel Bight (KB). (b) Insert
of the sampling areas, within and at the entrance of the Kiel Fjord (red shaded areas), and
representation of the eight sampling transects (yellow lines). Close-up of the location of the
transects (c) within the Kiel Fjord in front of the seafront promenade (1), at the mouth of the
Schwentine river (6), at the entrance (2) and on the opposite shore (5) of the Kiel Canal, and (d)
at the entrance of the Kiel Fjord, above the outflow pipes of treated sewage water from the Kiel-
Bülk wastewater plant (WWTP), and 500 m and 1000 m offshore (3a, 3b and 3c, respectively),
and offshore the recreational Wendtorf harbour (4).

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Figure 2. Median microplastic abundance (particles per m3) of (a) all the different sampling (n = 100), and at the different (b) dates and (c)
stations inside (green square) and outside (blue square) the Kiel Fjord. Horizontal lines indicate median values; circles indicate each individual
sample; the 25th and 75th range is represented by the lower and upper limit of the boxes, respectively. Whiskers extend to the maximum values.
Filled circles represent outliers (1.5 times above the upper quartile).

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Figure 3. Proportion (% of the total number) of the most common types of polymers and of
the proportion of the different types of additives (insert) determined by infrared spectrometer
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analysis (spectra correspondence >70%; see text) of the microplastics collected at the sea
surface within the Kiel Fjord between March 2018 and March 2019; (1-17) examples of
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microplastics (1-5: Polyethylene high-density (PE-HD); 6-8: Polypropylene (PP); 9,10:

Benzyl butyl phthalate (BBP); 11: Polystyrene (PS); 12: Polyethylene isotactic (PE); 13,14:
Azlon (caffeine protein); 15: Nylon, 16: Polyamide (PA); 17: Ethylene-vinyl acetate (EVA)).
The scale bars represent 0.5 mm (pictures 1-6, 8, 10-14 and 16-17), 1 mm (pictures 9 and 15)
and 2 mm (picture 7).

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Figure 4. Microplastic abundance (particles/m3) in relation to the (a) mean wind direction
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(°), (b) rainfall (mm), (c) mean wind speed (m/s) and (d) snowfall (mm) 24h before each
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sampling day (dots; n = 13). Blue lines represent the fit of the linear models by robust

regression using an M estimator. Grey shades represent the standard error of the fit. The

equation of the model and the adjusted coefficient of determination R2 are shown above each

fitted lines.

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Figure 5. (a-d) Rainfall (mm), (e-h) snowfall (mm), (i-l) air temperature (°C), (m-p) wind
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speed (mm) and (q-t) wind direction (°) during a 10-days period before the four sampling
days (08/03/2018, 21/03/2018, 19/04/2018 and 16/01/2019) that yielded the five largest
microplastic abundances (numbers above the upper plots, in particles per m3; the numbers
within brackets indicate the station number where each sample was collected). Two of these
samples were collected on the same day (21/03/2019). Vertical red line indicates the
sampling day.

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TABLES

Table 1. Type, number (percentage of the total), the five most common colours of each particle type (% of the total), length and width

surface within and outside the Kiel Fjord.

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(maximum, minimum, median and inter-quartile range of the median) of the subset of 271 (59% of the total) microplastics collected at the sea

Type n (%) Colours (%)

Length (n = 271)

p
Min. Max. Median IQR ro Width (n = 271)
Min. Max. Median IQR

ALL 458 (100)

White (24), translucent (18),
0.27 18.2
e -
1.28 1.36 0.13 6.99 0.69 0.72

Hard fragments 303 (66)

blue (11), green (11), black (5)
White (24), translucent (23),
P
0.27 r 11.5 1.23 1.15 0.13 6.99 0.7 0.61
blue (12), yellow (7),black (7)
White (52), blue (14),
a l
Soft fragments 63 (14)

r n
translucent (10), brown (8), 0.50 9.37 1.98 2.09 0.17 4.58 1.32 1.47

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green (6)

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Green (70), red (21), blue (7),
Paint flake 66 (14) 0.38 3.7 0.77 0.71 0.14 2.77 0.52 0.40

Intertwined fibre
matrix
21 (5)
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orange (2)
White (29), translucent (24),
grey (14), blue (14), black 0.50 18.2 2.3 5.16 0.46 4.56 0.69 2.03
(10)
Green (40), blue (20), brown
Monofilament 5 (1) 1.57 2.94 2.10 0.74 0.14 1.11 0.17 0.27
(20), translucent (20)

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Declaration of interests

☒ The authors declare that they have no known competing financial interests or

personal relationships that could have appeared to influence the work reported in this paper.

☐The authors declare the following financial interests/personal relationships which may be
considered as potential competing interests:

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Credit Author Statement

Nicolas Christian Ory lead the conceptualization, the supervision, the methodology,

the investigation, the formal analysis of the results, the funding acquisition and the writing of

this publication.

Andreas Lehmann participated in the analysis of the results and the writing of this

publication.

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Jamileh Javidpour participated in the conceptualization of the study and the funding
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acquisition to support the project that lead to this publication.
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Rüdiger Stöhr participated in the analysis of the samples, the resources and the
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writing of this publication.

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Grace L. Walls participated in the collection and the analysis of the samples.
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Catriona Clemmesen participated in the conceptualization, the supervision, the

resources, the methodology and the writing of this publication.

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Graphical abstract

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Highlights

- Microplastic abundance was overall low and not related to environmental

parameters.

- High microplastic loads were found on few occasions after rainfall and snowmelt.

- Microplastics were mainly hard fragments of PE and PP in various colours.

- Microplastic contamination from the wastewater treatment plant was the lowest.

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- Stormwater drains are important source of microplastics into the marine

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