Long-term monitoring of pesticides in air and atmospheric deposition in

Sweden

Jenny Kreuger & Bodil LindströmSwedish University of Agricultural Sciences (SLU), Uppsala, Sweden

IUPACGhent, Belgium 20 May 2019

Background• Long-term monitoring of

environmental fate of pesticides in Sweden since 2002• Main focus on surface

water*• To a lesser extent, also

monitoring of pesticides in atmospheric deposition and in air

* Boye et al (2019) Journal of Environmental Quality – in press DOI:10.2134/jeq2019.02.0056

Sampling sites

Vavihill – 2002-2016

Hallahus – from 2017

Aspvreten - 2009-2016

• Sampling sites located jointly with other international/national atmospheric monitoring programs (e.g. EMEP & ICOS)

• Located in rural background areas, surrounded by forests, >1 km from treated fields

Norunda - from 2017

• Event related sampling using a bulk sampler (a stainless steel funnel, area 0.5 m2, above a fridge)

• Ca 12-15 samples/season• Ca 140 pesticides analysed today• Sampling during main growing

season • From 2009 April-October • Previously May-June + October

• Started in 2002 at Vavihill & in 2009 at Aspvreten (further north)

Methods - precipitation

Methods - air

Air samples collected • At fixed, weekly, intervals using a high-

volume pump (ca 400 m3/day)• Using pre-cleaned cartridges with quartz

fiber filter and PUF/XAD/PUF• Ca 10-12 samples/season• Ca 100 pesticides analysed today• Started in 2009 at Vavihill

PUF-2 / XAD / PUF-1Airflow

0,0001

0,001

0,01

0,1

1

10

2001 2003 2005 2007 2009 2011 2013 2015

Tota

l con

cent

ratio

n (µ

g/l)

Vavihill (south) - Total concentration in precipitation/ sample 2002 - 2015

Max total concentration 3.9 µg/l in a sample from October 2015, with prosulfocarb constituting the major part (3.8 µg/l)

0,0001

0,001

0,01

0,1

1

10

2001 2003 2005 2007 2009 2011 2013 2015Tota

l con

cent

ratio

n (µ

g/l)

Vavihill (south) - Total concentration per sample 2002 - 2015

Max total concentration 3.9 µg/l in a sample from October 2015, with prosulfocarb constituting the major part (3.8 µg/l)

• During later years (2012-2015) 65 a.i. & 6 TP:s were detected

• Most detects at the low ng/l-level, though some were occasionally detected above 0.1 µg/l, mainly• prosulfocarb, protioconazole-destio,

MCPA, pendimethalin, and terbutyhazine-desethyl

Detection frequency in rainwater at Vavihill (south) during recent years 2012-2015

Of those pesticides detected in ≥ 20 % of the samples – ca 50 % were not used in Sweden during the investigation period (e.g. lindane, endosulfan, chlorpyrifos, terbuthylazine, metolachlor, epoxiconazole, flufenacet)

0% 25% 50% 75% 100%lindane

prosulfocarbpropamocarb

endosulfan-alphachlorpyrifos

terbuthylazine-desethylMCPA

metazachlorterbuthylazine

boscalidendosulfan-sulfate

prothiochonazole-desthioclomazone

endosulfan-betaisoproturonmetolachlorfluazinam

epoxiconazolediflufenicanazoxystrobin

fenpropimorphethofumesate

flufenacetHCH-alphacarbendazimpendimethalin

cyprodinildicamba

vinclozolinpyraclostrobin

2,4-D

Approved

0,1 1 10 100

prosulfokarbprothioconazole-desthioterbuthylazine-desethyl

metazachlorpropamocarbterbuthylazine

MCPAboscalid

bentazoneisoproturonmetamitronflufenacet

metolachlortrinexapac-acid

2,4-Depoxiconazole

chlomazonclopyralid

propiconazolediflufenicanethofumesat

pendimethalinfenpropimorph

Averagedeposi-on2012-2015(µg/m2*year)

0,001 0,01 0,1 1 10 100

terbuthylazine-desethylterbuthylazine

flufenacetmetolachlor

epoxiconazolependimethalin

tri-allatelindane

chlorpyrifosdiuron

quinoxyfenlinuronBAM

methabenzthiazuronatrazineHCH-alfa

dimethoateendosulfan-alfaendosulfansulfatendosulfan-beta

dichlobenilHCB

vinclozolin

Non-registredpes.cides

= not used in Sweden

Atmospheric deposition at Vavihill in southern Sweden 2012-2015 (April-October)• Herbicides

dominate, followed by fungicides

• Also pesticides not registered for use in Sweden (red bars) contribute to the total load

Yearly ∑ 3-month deposition (µg/m2) 2002-2017 for pesticides not used in SwedenBanned within the EU (left) and approved within EU (right)

Now registered in Sweden, with sale starting in 2015

Long-term trends - deposition

Yearly ∑ 3-month deposition (µg/m2) 2002-2017 Pesticides used in Sweden (left) and for pesticides banned during the period (right)

66 15

Long-term trends - deposition

Air samples - distribution between filter, PUF and XADfor 26 pesticides detected in >20% of the air samples (n = 34)

* Substances not approved for use within EU at the time of sampling

• PUF breakthrough (> 30%) for dichlobenil, HCH-a, HCB and trifluralin.

• However, only 4% of total pesticide concentration found in XAD and PUF-2

Pesticides in airApril 2017 – March 2018

• Some were primarily detected on filter

• Seasonal occurrence

Pesticides in airApril 2017 – March 2018

• Others were detected on PUF

• Year round

Detection frequency in air (adsorbent, PUF-1) 2012-2015

• A total of 31 a.i. and 5 TP:s • Majority of pesticides

detected in the gas phase are not approved for use within Sweden, many not even within the EU

• Most concentrations at low levels (< 0.1 µg/m3 air), mainly prosulfocarbdetected above this level (max. 30 µg/m3 air)

0% 20% 40% 60% 80% 100%

endosulfan-alphaHCH-alphachlorpyrifos

lindaneHCB

prosulfocarbDDE-p,pDDT-p,p

chlordane-gammachlordane-alfa

endosulfan-betaendosulfan-sulfat

terbutylazinependimethalin

terbuthylazine-desethyletofumesate

tolchlofos-methyl

Not approvedApproved

0% 20% 40% 60% 80% 100%

diflufenican

lambda-cyhalotrin

esfenvalerate

fenpropimorph

propiconazole

chlorpyrifos

azoxystrobin

tau-fluvalinate

aclonifen

terbuthylazine-…

cypermethrin

pendimethalin

terbuthylazine

cyprodinil

prosulfocarb

alfa-cypermethrin

isoproturon

Not approved

Approved

Detection frequency in air (filter) 2012-2015

• Majority of pesticides

detected in the

particulate phase are

approved for use within

Sweden

• Most concentrations at

low levels (< 0.1 µg/m3

air), mainly

fenpropimorph detected

above this level (max.

0.8 µg/m3 air)

Conclusions• Currently used pesticides are regularly detected at

ng/l-levels in rainwater, with occasional µg/l-level findings

• A larger number of pesticide detected during spring/early summer, however higher concentrations were detected during fall (mainly prosulfocarb)

• Deposited amount corresponds to ca 0.1 - 0.0001% of the applied dose in the field

• A significant contribution to atmospheric deposition in southern Sweden from pesticides not used within Sweden, i.e. a transboundary atmospheric transport of pesticides

Thank you! Questions?

Acknowledgement:• The national pesticide monitoring programme is funded by the Swedish

Environmental Protection Agency• Information about the pesticide monitoring program at

• Department of Aquatic Sciences and Assessment or• Centre for Chemical Pesticides