Considering human exposure to pesticides in food products: Importance of dissipation dynamics

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1 Considering human exposure to pestiides in food produts: Importane of dissipation dynamis Peter Fantke 1,*, Ronnie Juraske 2, Olivier Jolliet 3 1 Quantitative Sustainability Assessment Division, Tehnial University of Denmark, Kgs. Lyngby, Denmark 2 Dr. Knoell Consult GmbH, Mannheim, Germany 3 Shool of Publi Health, University of Mihigan, Ann Arbor (MI), USA Corresponding author. ABSTRACT The general publi is ontinuously onerned about effets from pestiide exposure via residues in food rops. However, impats from pestiide exposure are mostly negleted in food produt-related LCAs. Time-to-harvest and dissipation from rops mainly drive residue dynamis with dissipation as the most unertain aspet in haraterization modeling. We analyzed measured half-lives (n=4513) with 95% falling between 0.6 and 29 days. With ~500 pestiides authorized alone in the EU for several hundred rops, however, experimental studies only over few possible pestiide-rop ombinations. Therefore, we estimated dissipation from measured data and provide referene half-lives for 333 pestiides applied at 20 C under field onditions. Our framework allows for detailed explorations of dietary hoies in LCA with respet to health impats from pestiide exposure via rop onsumption. The next step is to inlude pestiide exposure via rop onsumption along with improved pestiide dissipation data into existing LCIA methodologies for onsideration in future LCA studies. Keywords: Pestiides, human exposure, rop onsumption, dissipation half-lives, life yle impat assessment 1. Introdution A main onern of the general publi in various regions inluding Europe and the U.S. is related to long-term or hroni effets from low-level exposures to pestiides (Pretty 2005; Slovi 2010). Human population-level exposure predominantly ours from residues in food rops, supplemented by exposure from pestiide frations lost from agriultural fields after appliation (European Commission 2006; MKinlay et al. 2008). However, in almost all existing food produt-related life yle assessment (LCA) studies human and eosystem impats from exposure to pestiides (or other potentially toxi hemials) are not onsidered at all or onsidered negligible (Heller et al. 2013). This is partly due to the pereived high unertainty assoiated with impats from exposure to toxi hemials (Finnveden et al. 2009). A framework to haraterize human health impats of individual pestiides applied to different agriultural food rop types grown in Europe has been reently published (Fantke et al. 2011, 2012a). This framework is based on a set of interonneted ompartments, for whih pestiide fate and residues are alulated by solving s flexible set of differential mass balane equations with assumed first order kinetis by means of matrix algebra. In this study, time between pestiide appliation and rop harvest along with pestiide dissipation half-lives in rops have been identified as key aspets driving residue dynamis, whih is onsistent with similar assessments fousing on rop residue dynamis (Juraske et al. 2009; Rein et al. 2011). Whereas the influene of time to harvest has been analyzed and parameterized for existing life yle impat assessment (LCIA) models, pestiide dissipation in food rops remains one of the most unertain aspets in haraterizing human toxiologial impats of pestiides via food rop onsumption (Juraske et al. 2008; Fantke et al. 2012b). In the present study, we aim at reduing unertainty assoiated with pestiide dissipation in rops, thereby also failitating a feasible starting point for inluding human health impats from pestiide exposure via food rop onsumption in future LCA studies. 2. Methods We start from following the framework proposed by Fantke et al. (2012a) to alulate human health impat sores for pestiides applied to agriultural fields in Europe. This approah is based on estimated agriultural appliation data for the five most extensively used pestiides per rop and ountry in 2003 for 24 member states of the EU as of 2004 (EU24) from a ollaboration report between Eurostat and the European Crop Protetion Assoiation (European Commission 2007). Health impat sores of pestiide i applied to rop in a speifi year, IS i, (DALY/year), are alulated from the total mass applied in this speifi year, m i, (kg applied /year), the 390

2 pestiide residue fration in rop harvest, hf i, (kg residue /kg applied ), the food proessing fator, PF (kg intake /kg residue ) aounting for redution of residues in rop harvest due to e.g. washing or ooking, the dose-response slope fator, ß i (inidene risk/kg intake ), and the severity fator expressed in disability-adjusted life years as a omposite measure for overall population health impats, SF (DALY/inidene): IS i, m i, hf i, PF SF i Eq. 1 Fantke et al. (2012a) reported an overall model output unertainty range, i.e. a variane in health impat sores, assoiated with ontributing input variables along the impat pathway (Eq. 1) between 4.75 and 838,505 DALY/year aross EU24 in Main soure of unertainty in the mass balane resulting in residual frations of pestiides in rop harvest is the first order rate oeffiient representing dissipation from rops. Hene, we fous in this study to redue unertainty related to dissipation in rops. Unertainty of any model input and output variable x an be haraterized by its squared geometri standard deviation GSD 2 (x) and related probability of 95% = {x/ GSD 2 (x) < x < x GSD 2 (x)}. We use GSD 2 (x k ) for input variables x k {m i,, hf i,, PF, ß i, SF} as provided by Fantke et al. (2012a) to obtain GSD 2 (IS i, ) of model output (health impat sores IS i, ): GSD ( IS i ) exp 1 (ln[gsd ( x )]), k k Eq. 2 The unertainty related to the alulation of pestiide residues in rop harvest is reported to be GSD 2 (hf i, ) = 27 and to orrespond to a ontribution of 29.6% to the output-related unertainty of GSD 2 (IS i, ) = To redue GSD 2 (hf i, ) and thereby also GSD 2 (IS i, ), we systematially built an inventory database of existing experimental studies providing dissipation half-lives in agriultural food rops and other plants (Fantke and Juraske 2013). Measured dissipation half-lives from 811 sientifi studies (>99% peerreviewed) were available or alulated from onentration-time urves for 346 pestiides applied to 183 rops (n = 4513) with 95% of all half-lives falling between 0.6 and 29 days. However, with almost 500 pestiides authorized alone in the European Union for use on several hundred rops, analyzed experimental studies still over only a small fration of possible pestiide-rop ombinations. In response to this need, we developed models to estimate dissipation in rops based on the review from Fantke and Juraske (2013). We first haraterized measured pestiide dissipation half-lives by desribing their distribution and by determining the influene of temperature from a subset of 1030 data points with reported study ondition average air temperatures. We then provided reommended geometri means of dissipation halflives at 20 C and 95% onfidene intervals for 333 reported pestiides, and used multiple imputations for substituting missing temperature data. Next, we proposed a regression-based model to predit dissipation half-lives for pestiides as a funtion of temperature, substane hemial lass, seleted substane properties and plant harateristis for all pestiides where reported data were not available. We finally evaluated model predition performane using sums of squares of predition residuals for exluded data. Results of these models for pestiide dissipation in rops were ompared with previously used dissipation data in the assessment model framework proposed in Eq. 1 and ompared in terms of model input and output unertainty expressed in terms of GSD Results Referene half-lives for 333 pestiides with reported temperatures applied at 20 C under field onditions range from 0.2 days for pyrethrins and 0.3 days for hlorsulfuron to 31 days for dalapon with 95% of all halflives falling in the range between 1 and 18 days. Parameter estimates orret these half-lives for speifi rops, temperatures, and study onditions. On average over all substanes, temperature imputation only ontributes with 5.1% to standard errors of half-lives. Standard errors of substane and plant parameter estimates approximately follow a derease proportional to the inverse of the square root of the number of data points. With a minimum of 20 data points, we get a standard error of 0.08, implying a 95% onfidene interval on geomean halflives of a fator 1.5. For pestiides without reported data, we developed our final preditive model aims at estimating dissipation half-lives of pestiides as a funtion of their hemial lass and properties. Substane lass, plant speies, old storage onditions, temperature, substane moleular weight, otanol/water partition oeffiient and saturation vapor pressure were taken into aount as final preditor variables. All other tested substane properties (air/water and soil organi arbon/water partition oeffiients, half-lives in air and soil) either 391

3 did not signifiantly improve model auray or showed strong orrelation with another variable. This model yields standard errors on the parameter estimates of 0.07 to 0.16 for substane lasses and 0.06 to 0.15 for plant speies. Implementing the new estimated dissipation half-lives into the model assessment framework proposed in Eq. 1 yields a redued model input unertainty in terms of a redued GSD 2 (hf i, ) = 12, whih orresponds to a redution in variane of residues in rop harvest aross pestiides and rops. Thereby, we redued overall output-related unertainty in terms of a redued GSD 2 (IS i, ) = and the ontribution of residues in rop harvest (represented by hf i, ) from initially 29.6% to now 19.5% (see Figure 1). With this, we redued unertainty in haraterizing human exposure to pestiides via food rop onsumption. Figure 1. GSD 2 (x) of input variables along the pathway from pestiide appliation to severity of health impats to obtain impat sores (DALY/year) due to the use of pestiides in EU24 in Human health impat sores for use of pestiides in the EU24 ountries in 2003 as applied in Fantke et al. (2012a) were re-alulated based on the newly obtained dissipation data. Overall, pestiides ontributed annually to 1950 DALY/year in EU24 in 2003, to whih only 13 substanes applied to grapes/vines, fruit trees, and vegetables aounted for 90% of total annual health impats. Impat sores thereby range from 0.34 DALY/year for sugar beet and 1.35 DALY/year for ereals to 724 DALY/year for grapes/vines and 1100 DALY/year for vegetables (Figure 2). The total burden per person in hours lost over lifetime was 1.5. Compared with figures for the burden from exposure to fine partiulate matter in the air with 195 days or seond-hand smoke in the air with 24 days (Hänninen et al. 2014), this figure is relatively low. However, unertainties in our results even though redued for dissipation data in food rops highlight the figure ould be somewhat higher, ranking pestiides with other important environmental stressors in health impat terms when omparing with our upper end 95% onfidene interval limit of 17.4 days burden per person over lifetime (see Figure 2). Figure 2. Mean and 95% onfidene interval of impat sores (DALY/year) due to the five most extensively used pestiides on eah rop lass as well as sum over rops aross EU24 in

4 4. Disussion We developed a set of 333 omparative pestiide dissipation half-lives in food rops under referene onditions represented by an average plant, field onditions, and a temperature of 20 C (Fantke et al. 2014). These half-lives have been orreted to aount for rop type, onditions, and temperature in the underlying experimental studies. This omprehensive approah, where we orret for measured temperature, reported rop speies, and reported study onditions for prediting dissipation, and where we impute missing temperatures and finally study the variability of reported half-lives for eah pestiide signifiantly redues the unertainty around eah estimated dissipation half-life, thereby muh better refleting referene study onditions. Our additional preditive model is designed to estimate dissipation half-lives from properties of individual pestiides belonging to 14 substane lasses, for whih no half-lives representing referene onditions ould be obtained in our study due to missing experimental data. Considering the high variability between substanes and rops, and data availability, our reommended referene half-lives along with the preditive model estimates onstitute a first step towards reduing unertainty in our assessment framework with respet to pestiide degradation in food rops. However, we aknowledge that for LCA studies, the underlying data also need to be available aross pestiides and rops. Therefore, additional researh is required to systematially assess the relationship between overall pestiide dissipation and degradation in rops, sine typially degradation is onsidered as separate proess in LCIA models, to further understand the influene and importane of degradation in rops as one of the main drivers of subsequent human exposure and related health impats to be inluded in future LCA studies. Furthermore, reporting guidelines for measuring dissipation from food rops need to be improved with respet to providing suffiient information on environmental study onditions (e.g. reporting temperature, humidity, soil type) and residues in rops (providing enough data points to aount for measurement variability and to effetively perform urve fitting for estimating dissipation kinetis). This will further inrease LCIA input data quality when using experimentally-derived half-lives. 5. Conlusion Our pestiide- and rop-speifi assessment framework allows for detailed explorations of dietary hoies in a LCA ontext with respet to human health impats from pestiide exposure via food rop onsumption. Furthermore, we redue unertainty related to one of the key drivers of pestiide residue dynamis in food rops in support of improving the reliability of impat assessment results. The next step is to inlude human exposure via rop onsumption along with improved pestiide dissipation data into existing LCIA methodologies for onsideration in future LCA studies. We further aknowledge that impats from pestiides in LCAs are often dominated by impats on biodiversity (Geiger et al. 2010) and on groundwater (Arias-Estévez et al. 2008). Hene, we emphasize the need to inlude pestiides into food-related LCA studies and reommend overing all relevant impat ategories related to pestiides inluding human toxiity, eosystem toxiity and groundwater ontamination to provide an improved basis for LCA-based deision support. 6. Referenes Arias-Estévez M, López-Periago E, Martínez-Carballo E, Simal-Gándara J, Mejuto J-C, Garía-Río L (2008) The mobility and degradation of pestiides in soils and the pollution of groundwater resoures. Agr Eosyst Environ 123: European Commission (2006) Speial Eurobarometer 238, Wave 64/1 - Risk Issues. Brussels European Commission (2007) Eurostat Statistial Books: The use of plant protetion produts in the European Union Data , Brussels Fantke P, Juraske R, Antón A, Friedrih R, Jolliet O (2011) Dynami multirop model to haraterize impats of pestiides in food. Environ Si Tehnol 45: Fantke P, Friedrih R, Jolliet O (2012a) Health impat and damage ost assessment of pestiides in Europe. Environ Int 49: 9-17 Fantke P, Wieland P, Juraske R, Shaddik G, Sevigné E, Friedrih R, Jolliet O (2012b) Parameterization models for pestiide exposure via rop onsumption. Environ Si Tehnol 46:

5 Fantke P, Juraske R (2013) Variability of pestiide dissipation half-lives in plants. Environ Si Tehnol 47: Fantke P, Gillespie B, Juraske R, Jolliet O (2014) Estimating half-lives for pestiide dissipation from plants. Environ Si Tehnol. DOI: /es500434p Finnveden G, Haushild MZ, Ekvall T, Guinée J, Heijungs R, Hellweg S, Koehler A, Pennington D, Suh S (2009) Reent developments in Life Cyle Assessment. J Environ Manage 91: 1-21 Geiger F et al. (2010) Persistent negative effets of pestiides on biodiversity and biologial ontrol potential on European farmland. Basi Appl Eol 11: Hänninen O, Knol AB, Jantunen M, Lim T-A, Conrad A, Rappolder M, Carrer P, Fanetti A-C, Kim R, Buekers J, Torfs R, Iavarone I, Classen T, Hornberg C, Mekel OCL (2014) Environmental Burden of Disease in Europe: Estimates for nine stressors in six ountries. Environ Health Persp: doi: /ehp Heller MC, Keoleian GA, Willett WC (2013) Toward a life yle-based, diet-level framework for food environmental impat and nutritional quality assessment: A ritial review. Environ Si Tehnol 47: Juraske R, Antón A, Castells F (2008) Estimating half-lives of pestiides in/on vegetation for use in multimedia fate and exposure models. Chemosphere 70: Juraske R, Castells F, Vijay A, Muñoz P, Antón A (2009) Uptake and persistene of pestiides in plants: Measurements and model estimates for imidaloprid after foliar and soil appliation. J Hazard Mat 165: MKinlay R, Plant JA, Bell JNB, Voulvoulis N (2008) Endorine disrupting pestiides: Impliations for risk assessment. Environ Int 34: Pretty JN (2005) The Pestiide Detox: Towards a More Sustainable Agriulture. Earthsan, London, UK Rein A, Legind CN, Trapp S (2011) New onepts for dynami plant uptake models. SAR QSAR Environ Res 22: Slovi P (2010) Pereptions of pestiides as risks to human health. In: Krieger R (ed) Hayes Handbook of Pestiide Toxiology, 3rd edn. Aademi Press, London, UK, pp

6 This paper is from: Proeedings of the 9th International Conferene on Life Cyle Assessment in the Agri-Food Setor 8-10 Otober San Franiso Rita Shenk and Douglas Huizenga, Editors Amerian Center for Life Cyle Assessment

7 The full proeedings doument an be found here: It should be ited as: Shenk, R., Huizenga, D. (Eds.), Proeedings of the 9th International Conferene on Life Cyle Assessment in the Agri-Food Setor (LCA Food 2014), 8-10 Otober 2014, San Franiso, USA. ACLCA, Vashon, WA, USA. Questions and omments an be addressed to: ISBN:

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