Nickele al. En i on Sci Eu (2018) 30:53
h ps://doi.o g/10.1186/s12302-018-0183-8
RESEARCH
Modelling spa ial pa e ns o co ela ions
be weenconcen a ions o hea y me als
inmosses anda mosphe ic deposi ion in2010
ac ossEu ope
S e an Nickel1*, Win ied Sch öde 1, Roman Schmal uss1, Maike Saa ho 1, Ha y Ha mens2, Gina Mills2,
Ma ina V. F on asye a3, Lambe Ba ando ski4, Oleg Blum5, Alejo Ca ballei a6, Ludwig de Temme man7,
Ana oly M. Dunae 8, An oane a Ene9, Hilde Fage li10, Ba ba a Godzik11, Ilia Ilyin12, Sande Jonke s13,
Z onka Je an14, P an e a Lazo15, Sebas ien Leblond16, Sii i Lii 17, Blanka Manko ska18,
Enca nación Núñez‑Oli e a19, Juha Piispanen20, Ja mo Poikolainen20, Ion V. Popescu21, Flo a Qa i22,
Jesus Miguel San ama ia23, Ma ijn Schaap13, Mi ja Skudnik24, Zd a ko Špi ić25, T ajce S a ilo 4, Eili S einnes26,
Claudia S ihi21, I an Sucha a27, Hilde Thelle Ugge ud28 and Ha ald G. Zechmeis e 29
Abs ac
Backg ound: This pape aims o in es iga e he co ela ions be ween he concen a ions o nine hea y me als in
moss and a mosphe ic deposi ion wi hin ecological land classes co e ing Eu ope. Addi ionally, i is examined o wha
ex en he s a is ical ela ions a e a ec ed by he land use a ound he moss sampling si es. Based on moss da a col‑
lec ed in 2010/2011 h oughou Eu ope and da a on o al a mosphe ic deposi ion modelled by wo chemical ans‑
po models (EMEP MSC‑E, LOTOS‑EUROS), co ela ion coe icien s be ween concen a ions o hea y me als in moss
and in modelled a mosphe ic deposi ion we e speci ied o spa ial subsamples de ined by ecological land classes o
Eu ope (ELCE) as a spa ial e e ence sys em. Linea disc iminan analysis (LDA) and logis ic eg ession (LR) we e hen
used o sepa a e moss sampling si es ega ding hei con ibu ion o he s eng h o co ela ion conside ing he a eal
pe cen age o u ban, ag icul u al and o es y land use a ound he sampling loca ion. A e e i ica ion LDA models
by LR, LDA models we e used o ans o m spa ial in o ma ion on he land use o maps o po en ial co ela ion le els,
applicable o u u e ne wo k planning in he Eu opean Moss Su ey.
Resul s: Co ela ions be ween concen a ions o hea y me als in moss and in modelled a mosphe ic deposi ion
we e ound o be speci ic o elemen s and ELCE uni s. Land use a ound he sampling si es mainly in luences he
co ela ion le el. Small adiuses a ound he sampling si es examined (5 km) a e mo e ele an o Cd, Cu, Ni, and Zn,
while he a eal pe cen age o u ban and ag icul u al land use wi hin la ge adiuses (75–100 km) is mo e ele an o
As, C , Hg, Pb, and V. Mos alid LDA models pa e n wi h e o a es o < 40% we e ound o As, C , Cu, Hg, Pb, and V.
Land use‑dependen p edic ions o spa ial pa e ns spli up Eu ope in o in es iga ion a eas e ealing po en ially high
(= abo e‑a e age) o low (= below‑a e age) co ela ion coe icien s.
Conclusions: LDA is an eligible me hod iden i ying and anking bounda y condi ions o co ela ions be ween
a mosphe ic deposi ion and espec i e concen a ions o hea y me als in moss and ela ed mapping conside ing he
in luence o he land use a ound moss sampling si es.
© The Au ho (s) 2018. This a icle is dis ibu ed unde he e ms o he C ea i e Commons A ibu ion 4.0 In e na ional License
(h p://c ea i eco mmons .o g/licen ses/by/4.0/), which pe mi s un es ic ed use, dis ibu ion, and ep oduc ion in any medium,
p o ided you gi e app op ia e c edi o he o iginal au ho (s) and he sou ce, p o ide a link o he C ea i e Commons license,
and indica e i changes we e made.
Open Access
*Co espondence: s e an.nickel@uni‑ ech a.de
1 Chai o Landscape Ecology, Uni e si y o Vech a, Vech a, Ge many
Full lis o au ho in o ma ion is a ailable a he end o he a icle
Page 2 o 17
Nickele al. En i on Sci Eu (2018) 30:53
Backg ound
The Uni ed Na ions Economic Commission o Eu ope
(UNECE) Con en ion on Long- ange T ansbounda y
Ai Pollu ion (CLRTAP) o 1979 and i s eigh p o ocols
a e aimed a limi ing and educing ai pollu an s. Unde
he LRTAP con en ion, he Eu opean moni o ing and
e alua ion p og amme (EMEP) ga he s in o ma ion on
emission om i s pa ies, collec s da a on ai and p e-
cipi a ion quali y and models a mosphe ic anspo and
deposi ion o ai pollu an s [1]. Beyond his, biomoni-
o ing p og ammes p o ide da a on concen a ions in
a ious biological ma ices po en ially co ela ed wi h
a mosphe ic deposi ion o hea y me als (HM). Wi hin
he LRTAP con en ion, Eu opean Moss Su ey (EMS) is
conduc ed using na u ally g owing mosses as biomoni-
o s o a mosphe ic deposi ion o ai pollu an s. Since
1990, moss specimens ha e been sampled e e y 5yea s
a up o 7300 sampling si es in up o 35 coun ies [2–4]
o de e mine he concen a ions o hea y me als (HM),
ni ogen (N, since 2005) and pe sis en o ganic pollu an s
(POPs, since 2010) [4, 5]. The EMS is coo dina ed by he
ICP Vege a ion, an in e na ional coope a i e p og amme
(ICP) epo ing on impac s o ai pollu ion on ege a ion
o he LRTAP con en ion [3].
Based on EMS da a om 2005, a mosphe ic deposi-
ion has been iden i ied as he main ac o de e mining
he spa ial a ia ion o concen a ions o cadmium (Cd)
and lead (Pb) in moss specimens collec ed h oughou
Eu ope [6–8]. Ha mens e al. [9] ound signi ican co -
ela ions be ween Cd and Pb concen a ion in moss and
espec i e a mosphe ic deposi ion modelled by EMEP
o mo e han wo- hi ds o he coun ies pa icipa ing
in he Eu opean Moss Su ey. Sch öde e al. [10] co e-
la ed Cd, me cu y (Hg), and Pb concen a ions in deposi-
ion and moss da a om he EMS 2005 wi hin a spa ial
amewo k o ecologically de ined land classes by use o
he nume ic chemical anspo model (CTM) o EMEP
MSC-Eas [11]. In u he s udies, also land use a ound
he sampling si es is shown o be an impo an ac o
a ec ing elemen concen a ions in moss [12–14].
The abo e-men ioned indings we e e i ied in he
in es iga ion p esen ed in his pape using da a collec ed
in he EMS 2010. The p esen s udy add esses he ollow-
ing objec i es.
1. Co ela ion analysis Examina ion o co ela ions
be ween concen a ions o HM in moss om he
EMS 2010/2011 and espec i e a mosphe ic deposi-
ion as modelled by use o he CTMs EMEP MSC-
Eas and LOTOS EUROS (LE), and o which ex en
he co ela ions a e speci ic o ecological land
classes o Eu ope (ELCE) [15].
2. S a is ical modelling Calcula ion, o which ex en he
amoun o ELCE-speci ic co ela ion coe icien s is
a ec ed by he a eal pe cen age o land use a ound
he sampling si es po en ially indica ing in luences
o local emission sou ces as o ins ance ag icul u al
and u ban land use o poin sou ces o ai pollu an s.
Hence, he eason o di e en ELCE-speci ic co e-
la ion coe icien s was in es iga ed.
3. P edic i e mapping Land use-dependen p edic ions
and mapping o co ela ion pa e ns ac oss Eu ope
(si e- ela ed/a ea- ela ed) and, inally, agg ega ion o
p edic ed spa ial pa e ns o decision suppo (e.g.
moss su ey ne wo k planning).
Fo his in es iga ion, da a on a mosphe ic deposi ion
o HM de i ed om he EMEP MSC-Eas [11] we e sup-
plemen ed by deposi ion da a calcula ed by use o he
chemical anspo model LOTOS-EUROS (LE) [16].
Me hods
Da a on elemen concen a ion in moss we e co ela ed
wi h espec i e modelled a mosphe ic deposi ion spe-
ci ically o ecological land classes o Eu ope (ELCE)
and majo land use ca ego ies a ound he sampling si es
de i ed om CORINE land co e 2006 and Global land
co e 2000 [17, 18] (Table1).
Da a onelemen concen a ions inmoss
In 2010/2011, moss specimens we e collec ed a 4499
sample si es in 26 coun ies ac oss Eu ope ollowing a
s anda dized expe imen al p o ocol [19]. Fu he coun-
ies like Ge many, I eland and Uni ed Kingdom who
pa icipa ed in o me moss su eys did no pa icipa e
in 2010. To p o ide ield-based e idence o he ex en o
long- ange ansbounda y pollu ion in Eu ope he moni-
o ing si es a e loca ed in backg ound a eas, e.g. sam-
pling si es we e a leas 300m away om majo oads
and 100 m away om any oad o houses. P ima ily,
Pleu ozium sch ebe i (B id.) Mi ., Hylocomium splen-
dens (Hedw.) Schimp., Hypnum cup essi o me Hedw.
s.s . and Pseudoscle opodium pu um (Hedw.) M. Fleisch
(synonym Scle opodium pu um Hedw. Limp .) [20] we e
sampled, bu also 32 o he species (7% o he samples).
Fo each si e, a leas i e indi idual moss samples o he
Keywo ds: Biomoni o ing, Chemical anspo models, Co ela ion analysis, Ecological classi ica ion, Linea
disc iminan analysis, Logis ic eg ession
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Nickele al. En i on Sci Eu (2018) 30:53
same species we e collec ed. Only he 2- o 3-yea -old
shoo s o he mosses we e used o he analyses. Concen-
a ions o nine HMs: a senic (As), cadmium (Cd), ch o-
mium (C ), coppe (Cu), me cu y (Hg), nickel (Ni), lead
(Pb), anadium (V), and zinc (Zn) we e de e mined [4, 9].
Da a ona mosphe ic deposi ion
S a is ical ela ions be ween elemen concen a ions in
moss and a mosphe ic deposi ion o HM de i ed om
he nume ic chemical anspo models (CTMs) LOTOS-
EUROS (LE) [16, 21] and EMEP [11] we e examined.
CTMs a e based on ma hema ical desc ip ions o el-
e an physical and chemical p ocesses in he a mosphe e
and a e mos ly used o la ge-scale, a ea-wide es ima es
o a mosphe ic deposi ion [21]. The accu acy o deposi-
ion modelling basically depends on he quali y o he
inpu da a (emission, me eo ology, land use, o he condi-
ions) used o modelling a mosphe ic anspo and dep-
osi ion p ocesses as well as in insic model unce ain ies.
The EMEP deposi ion da a we e supplied by he
me eo ological syn hesizing cen es MSC-Eas (Mos-
cow) o EMEP ope a ing unde he LRTAP con en ion.
T a niko and Ilyin [11] used emission da a o calcula e
a mosphe ic deposi ion o Cd, Hg, and Pb. To e i y
hese model calcula ions, he esul s we e compa ed o
Cd and Pb measu emen da a om up o 66 EMEP si es
and o Hg da a collec ed a up o 22 EMEP si es [22].
The e i ied model esul s we e hen mapped on g ids o
50km × 50km [11].
Following Ha mens e al. [9], in his in es iga ion he
3-yea sum o HM deposi ion modelled by EMEP (on a
50km by 50km g id) co esponds o he HM concen-
a ion in he sampled 3-yea -old shoo s o he mosses.
He e, he deposi ion da a om 2008 o 2010 was assigned
o he da a collec ed in EMS 2010/2011. The 3-yea sums
o deposi ion 2009–2011 om LE [16, 21] we e assigned
o he concen a ions o HM in moss collec ed in EMS
2010/2011. LE p o ides deposi ion a es o As, Cd, C ,
Cu, Ni, Pb, V, and Zn on a 25km by 25km g id co e ing
Eu ope. Addi ional in o ma ion abou he CTM is gi en
in Addi ional ile1: TableS2.
Ecological land classi ica ion o Eu ope
The da a on elemen concen a ions in moss and a mos-
phe ic deposi ion we e spa ially joined o he map o eco-
logical land classes o Eu ope (ELCE) (Addi ional ile1:
Figu e S1, TableS1) de i ed om Ho nsmann e al. [15].
Acco ding o he le el o spa ial di e en ia ion, he eco-
logical classi ica ion encompasses 40 (ELCE40) o 200
(ELCE200) classes iden i ied by 48 geo-da a laye s on
po en ial na u al ege a ion [23], al i ude abo e sea le el
[24], soil ex u e [25], and mon hly a e ages o p ecipi a-
ion and ai empe a u e (1961–2002) [26]. ELCE40 and
ELCE200 we e calcula ed and mapped by means o clas-
si ica ion and eg ession ees [27]. To ensu e he bes
possible compliance wi h minimum sample size speci ied
o each eco egion [28, 29], ELCE40 was used, whe eby
ELCE uni s occu ing spo adically and wi h a o al spa-
ial ex en below 4.2% we e summa ized o one class
(“o he s”).
S a is ical analysis
Co ela ion analysis
The s a is ical design comp ises he calcula ion o Spea -
man ank co ela ion coe icien s ( s) o quan i ying he
ela ion be ween concen a ions in mosses and modelled
a mosphe ic deposi ion o HM and N (Fig.1). The meas-
u ed concen a ions o As, Cd, C , Cu, Hg, Ni, Pb, V, and
Zn in moss we e co ela ed wi h espec i e o al a mos-
phe ic deposi ion da a as modelled by EMEP and LE.
The eby, ecological land classes (ELCE40) wi hin pa ici-
pa ing Eu opean coun ies we e used as coding a iable
o calcula ing ELCE-speci ic co ela ions. Due o a non-
no mal dis ibu ion in mos o he subsamples, Spea man
ank co ela ion coe icien s ( s) we e de e mined. The
co ela ion coe icien s we e classi ied acco ding o B o-
sius [30] as e y weak (< 0.2), weak (0.2–0.4), mode a e
(0.4–0.6), s ong (0.6–0.8), and e y s ong (> 0.8).
Table 1 Da a used o s a is ical analysis
a HM da a p o ided by MSC-Eas (No embe 2013)
Da a Commen andsou ce Uni
Elemen concen a ion in moss As, Cd, C , Cu, Hg, Ni, Pb, V, and Zn conc. in moss om he Eu opean Moss Su ey 2010/2011 μg/g
A mosphe ic deposi ion Modelled o al deposi ion o As, Cd, C , Cu, Ni, Pb, V, Zn summed o e 3 yea s (LOTOS‑EUROS
2009–2011, [21]) µg/m2
Modelled o al a mosphe ic deposi ion o Cd, Hg, Pb (EMEP MSC‑Eas ) summed o e 3 yea s (EMEP
2008–2010)aµg/m2
ELCE40 Ecological land classes o Eu ope [15] 40 land classes
Spa ial densi y o land use
a ound moss sampling si es A eal pe cen age o u ban, ag icul u al, and o es y land use, each wi hin a 1, 5, 10, 25, 50, 75, and
100 km adius a ound he moss sampling si es, de i ed om CORINE land co e 2006 [17] and
global land co e 2000 [18] o Russia, Uk aine and Bela us
%
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Nickele al. En i on Sci Eu (2018) 30:53
Linea disc iminan analysis/logis ic eg ession
The second s ep is o in es iga e he eason o he di -
e ence o ELCE-speci ic co ela ions. LDA models we e
used o ind linea sepa a ion lines as bes disc imi-
na e o sampling si es in ELCE egions e ealing high
o low elemen -speci ic co ela ion coe icien s. LDA
a emp s o ind a mul i a ia e disc iminan unc ion
Y = b0 + b1X1 + b2X2 + ⋯ desc ibing a linea combina ion
o wo o mo e p edic o s (X1, X2, …) and espec i e coe -
icien s (b0, b1, b2, …). The aim is o sepa a e g oups o
da a in a sca e plo so ha he a ia ion in da a wi hin
each g oup is minimized [31–33] and exp ess he con-
ibu ion o each p edic o in he selec ed disc iminan
model. Fo bina y classi ica ion o ELCE and hei allo-
ca ed sampling si es showing high (= A) o low (= B)
co ela ions, medians o he ELCE-speci ic Spea man
coe icien s we e aken o de ining elemen -speci ic
class bounda ies be ween high and low co ela ion le -
els. ELCE wi h coe icien s abo e he class bounda ies in
e ms o elemen -speci ic medians we e classi ied as ‘A’
and ELCE below he class bounda ies as ‘B’. Twen y-one
a iables o spa ial densi y o ag icul u al, o es y, and
u ban land use wi hin a 1, 5, 10, 25, 50, 75, and 100km
adius a ound he sampling si es (Table1) we e aken
as po en ial p edic o s o HM concen a ions in moss
samples. As he a ge a iable is al eady de e mined by
a mosphe ic deposi ion, i was no conside ed as a p e-
dic o . Fu he po en ial in luencing ac o s like ele a-
ion, p ecipi a ion, popula ion densi y as in es iga ed by
Nickel e al. [34] we e examined in a p e-analysis using
LDA, bu we e excluded due o low ele ance. Since he
alues o each o hese p edic o s ange be ween 0 and
100%, da a did no need o be s anda dized as ecom-
mended o LDA by Schönwiese [35]. O e all, wel e
LDA models we e buil wi h ega d o a ailable EMEP
deposi ion alues o (Cd, Pb, Hg) and LOTOS-EUROS
deposi ion es ima ions o (As, Cd, C , Cu, Ni, Pb, V, and
Zn). I was examined whe he he a iance could be su -
icien ly explained by jus wo o he po en ial 21 linea
disc iminan s (= spa ial densi y [%] o u ban, ag icul-
u al, and o es y land use, each wi hin a 1, 5, 10, 25, 50,
75, and 100km adius a ound he moss sampling si es,
Table1) o keep he models as simple as possible and
allowing o a be e in e p e a ion and isualiza ion o
he esul s. He e, nea -ze o coe icien s (linea combina-
ion coe icien anges be ween − 1 and 1) and co ela ed
p edic o s ha e been emo ed o a oid mul icollinea i y.
Fo example, i he coe icien o u ban land use wi hin a
10km adius was close o ze o han he 5km coe icien ,
he la e was aken.
Logis ic eg ession (LR) is simila o LDA, as i also
explains a ca ego ical a iable by he alues o con inu-
ous independen a iables. LR is p e e able in applica-
ions whe e he independen a iables a e no no mally
dis ibu ed. Since LR is less conc e e, LDA in he p esen
s udy was used o model building and LR o e i ica ion
o LDA esul s.
P edic ions
LDA models we e i s ly applied on he Eu ope-wide
da ase o moss sampling si es wi h in o ma ion on land
use densi y a ound he sampling si es. Model-speci ic
e o a es (%) we e calcula ed by means o con usion
ma ix alues (ac ual s. p edic ed alues). Cha s o he
linea disc iminan unc ions we e used o plausibili y
checks. Logis ic eg ession models we e buil using he
same p edic o s om he LDA models. Con usion ma i-
ces and e o a es (%) speci ied o each LR model we e
calcula ed and compa ed wi h he s a is ical cha ac e is-
ics o he LDA models.
To e i y o which ex en he models eally sepa a e
sampling si es showing high o low co ela ions be ween
elemen concen a ions in moss and espec i e a mos-
phe ic deposi ion, bi a ia e Spea man coe icien s o
he co ela ions be ween elemen concen a ions in moss
and a mosphe ic deposi ion we e again calcula ed o he
ollowing subsamples: sampling si es loca ed wi hin all
ELCE classes, ELCE classes showing co ela ions abo e
and below he elemen -speci ic class bounda ies be ween
high and low co ela ion le els de ined in Table1. Each
subsample was u he di ided in o g oups o sampling
si es classi ied by LDA in o ca ego y A o B. The mo e B
sampling si es modelled by LDA show low o , ice e sa,
A si es e eal high co ela ions, he mo e e icien he
be ween-class sepa a ion h ough he modelling and hus
he ele ance o p edic o s.
Geog aphic in o ma ion on he spa ial densi y o ag i-
cul u al, o es y, and u ban land use wi hin a 1, 5, 10,
Fig. 1 Design o s a is ical analysis (LDA linea disc iminan analysis,
LR logis ic eg ession)
Page 5 o 17
Nickele al. En i on Sci Eu (2018) 30:53
25, 50, 75, and 100km adius a ound he sampling si es
a ailable wi h blanke co e age o Eu ope was aken as
p edic o s o es ima ing ca ego ies o co ela ions (A, B)
be ween a mosphe ic deposi ion o nine HM in Eu ope
using LDA models and o ans o m spa ial in o ma-
ion on he land use o spa ial co ela ion pa e ns ac oss
Eu ope. Finally, spa ial pa e ns es ima ed by he bes
LDA models we e agg ega ed by calcula ing he numbe
o elemen -speci ic A classi ica ions (= abo e elemen -
speci ic class bounda ies be ween high and low co ela-
ion le els as de ined in Table2) o educe complexi y
which is mo e app op ia e o decision suppo . All s a-
is ical analyses we e pe o med using R p og amming
language [36], in pa icula unc ions o LDA as imple-
men ed in he ‘MASS’ package ex ending R’s co e unc-
ionali y [37].
Resul s
Co ela ions be weenHM concen a ions inmoss
anda mosphe ic deposi ion o ELCE ca ego ies
ac ossEu ope and o Eu ope asawhole
All analyses wi h HM concen a ion in moss we e based
on a easonably la ge sample size o a leas 3274 (As) ou
o 3965 (Zn) sample poin s. The minimum sample sizes
o elemen s and ELCE40 classes we e calcula ed and p e-
sen ed by Sch öde e al. [28, 29]. As he numbe o moss
sampling si es was e y low (> 10 in he classes D_16,
D_21, L_2, M_5, and M_6), he co ela ions o hese
classes a e no conside ed eliable and a e no desc ibed
below. Howe e , hese ou classes al oge he ep e-
sen only 2.3% (= 69,600km2) o he sampled a ea in he
coun ies pa icipa ing in he EMS (= 3,083,500km2).
Cadmium
S ong co ela ions be ween elemen concen a ions
measu ed in moss and modelled deposi ion (EMEP,
LE) wi h coe icien s ( s) anging om 0.6 o 0.8 we e
achie ed o 7% (EMEP) up o 10.5% (LE) o he a ea o
ELCE40 co e age o all coun ies pa icipa ing in he EMS
2010 oge he (Table2). These ELCE40 ca ego ies (D_13,
F1_1, S_0, and “o he s”) a e loca ed in Poland, Swi ze -
land and Aus ia (Fig.2). The s eng h o he Eu ope-wide
co ela ion is also high ( s = 0.65, p < 0.01). Mode a e s
alues occu ed o ELCE40 uni s co e ing 47.0–49.6%
o he landmass. Moss da a om each 5 ELCE40 ( o LE
in pa s o he han o EMEP) a e weakly co ela ed wi h
he modelled Cd deposi ion (EMEP: 15.0%; LE: 17.5%). 7
(EMEP) up o 9 (LE) ou o 27 ELCE40 uni s e eal non-
signi ican o e y weak co ela ions (23.5–31.1%).
Lead
Fo Pb, in 4 (EMEP) up o 6 (LE) ou o 27 ELCE40 uni s
he s alues we e no signi ican (12.0–20.3% o a ea o
ELCE uni s co e ed by moss sampling si es) (Table2).
F om he emaining ELCE40 classes, 6 (in case o LE,
26.3%) and 7 (EMEP, 28.9%) ELCE uni s show Spea -
man’s ank coe icien s be ween 0.2 and 0.4. Fo ano he
10 ELCE ca ego ies (LE) and, espec i ely, 11 ELCE ca -
ego ies (EMEP), co ela ion coe icien s came ou o be
be ween 0.4 and 0.6. The a ea comp ises 36.6–43.5% o
he o al a ea co e ed by moss samples mainly loca ed
in Finland, Sweden and F ance (Fig.2). Highes co ela-
ions (0.6 > s > 0.8) we e ound o max. 5 ELCE classes:
D_13 (only EMEP), S_0 (only LE), B_2, C_0, F1_1, “o h-
e s” (bo h EMEP and LE) (15.6–16.8% o he landmass)
p edomina ely dis ibu ed in No way. Wi h ega d o he
samplings ac oss Eu ope, Spea man’s ank coe icien s
a e 0.64 (LE) and 0.7 (EMEP).
Me cu y
Fo Hg, in 21 ou o 27 ELCE uni s, he s alues we e
no signi ican , below 0.02 o e en nega i e (82.5% o
a ea o ELCE classes co e ing all pa icipa ing coun ies
oge he ). I is clea ha he co ela ion be ween moss
da a om he EMS 2010 and EMEP modelled deposi-
ion is e y low ( s = 0.14, Table2). Abo e-a e age co -
ela ions wi h coe icien s be ween 0.4 and 0.6 we e only
ound o ELCE uni s B_1, D_14, F4_1, and J_2 (9.2%
o he a ea), spa sely loca ed in Fennoscandia, Es onia,
Poland, F ance and Spain (Fig.2). Fo ano he 2 ELCE
classes (D_7, F1_1), co ela ion coe icien s we e be ween
0.2 and 0.4, comp ising 8.3% o he a ea co e ed by moss
samples.
A senic
Fo Eu ope as a whole, low co ela ions be ween As con-
cen a ions in moss and espec i e modelled a mosphe ic
deposi ion (LOTOS-EUROS) we e ound ( s = 0.3). 14
ou o 27 ELCE40 uni s e eal non-signi ican co ela ions
wi hin 41.1% o he sampled ELCE40 a ea (Table2). In 5
ou o he emaining 13 ELCE40 uni s, a iables we e neg-
a i ely co ela ed (30.1%). Th ee ELCE40 classes e eal
signi ican weak co ela ions wi h s alues be ween 0.2
and 0.4 (13.1%). Me ely 4 ELCE40 uni s show mode a e
coe icien s be ween 0.4 and 0.6 (C_0, D_17, D18, and
F1_1). The ELCE40 uni wi h he highes co ela ion was
U_1 ( s = 0.72, p < 0.01) comp ising dispe sed small a eas
wi hin he pa icipa ing coun ies (1%) (Fig.3).
Ch omium
O all elemen s examined, C e eals he weakes Eu ope-
wide co ela ion be ween concen a ions in moss and
o al deposi ion modelled by LE ( s = 0.03, Table 2). Fo
16 ou o 27 ELCE40 uni s, he s alues we e no signi i-
can (49.5% o a ea o ELCE uni s co e ed by moss sam-
pling si es), and o 37.3%, he s alues we e below 0.02

Page 6 o 17
Nickele al. En i on Sci Eu (2018) 30:53
Table 2 Co ela ions be weenelemen concen a ions inmoss andmodelled a mosphe ic deposi ion speci ied o ecological land classes o Eu ope
EMEP/LOTOS-EUROS = chemical anspo models used o calcula ing a mosphe ic deposi ion; ELCE40 = ecological land classes o Eu ope [15] and o he ELCE which we e summa ized o one class (“o he s”); co ela ion
coe icien s acco ding o Spea man (*p < 0.05, **p < 0.01); (n) in b acke s = sample size; ELCE-speci ic co ela ions abo e he elemen -speci ic class bounda y be ween low and high co ela ion le els (= ca ego y A) a e in
i alic p in
ELCE40 EMEP LOTOS-EUROS
Cd Hg Pb As Cd C Cu Ni Pb V Zn
All 0.65** (3777) 0.14** (3313) 0.70** (3604) 0.30** (3274) 0.65** (3633) 0.03** (3820) 0.50** (3465) 0.09** (3772) 0.64** (3490) 0.19** (3832) 0.17** (3965)
B_1 0.39** (73) 0.48** (67) 0.54** (73) 0.23 (67) 0.45** (73) − 0.13 (73) 0.22 (73) − 0.24 (73) 0.67** (73) − 0.09 (73) 0.29* (73)
B_2 0.51** (110) − 0.18 (110) 0.63** (110) − 0.11 (111) 0.17 (110) − 0.52** (111) − 0.20 (110) − 0.67** (110) 0.27 (110) 0.13 (34) 0.09 (111)
C_0 0.52** (253) 0.19** (239) 0.62** (252) 0.45** (246) 0.52** (253) 0.16* (258) 0.51** (252) − 0.04 (258) 0.65** (252) 0.27** (227) 0.11 (259)
D_7 0.13 (186) 0.29** (135) − 0.01 (186) − 0.14 (134) 0.19* (186) 0.22** (186) 0.05 (186) − 0.23** (186) 0.25** (186) − 0.54** (186) − 0.04 (186)
D_8 0.37* (42) − 0.10 (34) 0.49** (42) 0.10 (34) 0.31* (42) − 0.10 (42) 0.52** (42) − 0.20 (42) 0.44** (42) 0.07 (42) − 0.03 (42)
D_10 − 0.08 (11) 0.20 (11) 0.22 (11) 0.05 (11) − 0.23 (11) − 0.11 (11) 0.08 (11) − 0.25 (11) 0.12 (11) − 0.27 (11) 0.09 (11)
D_13 0.72** (99) 0.18 (76) 0.61** (99) − 0.26** (114) 0.74** (99) − 0.48** (139) 0.40** (99) − 0.21* (121) 0.44** (255) − 0.20* (156) 0.10 (139)
D_14 0.39** (82) 0.43** (77) 0.46** (78) 0.15 (83) 0.57** (82) − 0.2* (119) 0.36** (94) − 0.04 (119) 0.55** (78) − 0.21* (136) 0.33** (137)
D_17 − 0.03 (115) 0.12** (71) 0.36** (89) 0.46** (127) 0.29** (115) 0.69** (147) 0.46** (93) 0.33** (148) 0.40** (89) 0.19* (153) 0.17 (154)
D_18 0.22** (255) 0.14* (248) 0.29** (255) 0.47** (201) 0.33** (255) 0.08 (255) 0.37** (255) 0.43** (255) 0.44** (255) 0.22** (253) 0.21** (255)
D_19 0.47** (258) 0.18* (165) 0.54** (258) 0.24** (165) 0.47** (258) 0.06 (258) 0.39** (258) 0.03 (258) 0.53** (258) 0.27** (258) 0.19** (258)
D_22 0.21** (168) 0.09 (166) 0.36** (168) 0.06 (167) 0.29** (168) 0.43** (171) 0.29** (168) 0.04 (171) 0.42** (168) 0.28** (171) 0.05 (171)
F1_1 0.72** (87) 0.37** (87) 0.62** (87) 0.57** (42) 0.76** (87) 0.06 (95) 0.48** (87) − 0.01 (94) 0.65** (87) − 0.14 (91) 0.39** (95)
F1_2 0.17** (308) − 0.15** (308) 0.38** (192) − 0.19** (289) 0.20** (308) − 0.11 (191) 0.31** (191) − 0.07 (192) 0.43** (192) 0.14 (191) 0.17 (154)
F2_5 0.53** (66) 0.19 (65) 0.33** (66) − 0.51 (12) 0.72** (66) − 0.12 (77) 0.27* (66) − 0.11 (71) 0.40** (66) 0.01 (37) 0.38** (77)
F2_6 0.41** (264) 0.01 (238) 0.48** (264) − 0.18** (250) 0.46** (264) − 0.39** (301) 0.31** (264) − 0.49** (291) 0.28** (264) − 0.14* (307) 0.18** (301)
F3_1 0.26** (201) 0.20** (189) 0.35** (201) 0.24** (173) 0.43** (201) − 0.09 (204) 0.13 (201) − 0.09 (203) 0.30** (201) − 0.05 (201) 0.20** (204)
F3_2 0.53** (115) − 0.21* (113) 0.45** (115) 0.17 (115) 0.53** (115) 0.13 (114) 0.13 (114) 0.17 (115) 0.47** 5 (115) 0.08 (114) 0.17 (114)
F4_1 0.28 (17) 0.57* (17) 0.51* (17) − 0.41 (11) 0.09 (17) 0.30 (17) − 0.12 (17) − 0.27 (17) 0.02 (17) 0.36 (17) 0.03 (17)
F4_2 0.53** (468) − 0.06 (394) 0.56** (468) − 0.09* (491) 0.46** (468) − 0.45** (540) 0.00 (467) − 0.14** (510) 0.01 (468) − 0.01 (571) − 0.08 (541)
G1_0 0.20* (126) 0.03 (63) 0.13 (126) 0.02 (137) 0.14 (126) − 0.04 (189) 0.01 (126) − 0.12 (189) 0.10 (126) − 0.17* (177) 0.29** (189)
G2_0 0.08 (186) 0.21** (174) 0.26** (162) − 0.12 (174) 0.32** (186) − 0.49** (152) 0.36** (151) 0.41** (162) 0.40** (162) 0.03 (152) − 0.14 (176)
J_2 0.43** (60) 0.50** (60) 0.51** (59) 0.02 (60) 0.54** (60) 0.25 (10) 0.49** (49) 0.60** (59) 0.55** (59) 0.21 (49) − 0.16 (50)
S_0 0.69** (54) − 0.04 (44) 0.58** (54) 0.13 (41) 0.64** (54) 0.18 (61) 0.37* (55) − 0.23 (61) 0.62** (54) − 0.15 (55) 0.42** (62)
U_1 0.47** (47) 0.05 (47) 0.51** (47) 0.72** (24) 0.57** (47) 0.23 (49) 0.49** (47) − 0.09 (49)0.48** (47) 0.31* (49) 0.35* (49)
U_2 − 0.01 (81) − 0.06 (73) 0.13** (80) − 0.24* (98) 0.16 (81) − 0.45** (102) 0.32** (79) − 0.01 (98) 0.18 (80) − 0.24* (102) 0.02 (103)
O he s 0.78** (45) 0.09 (42) 0.74** (45) 0.37* (40) 0.79** (45) − 0.01 (53) 0.17 (45) − 0.35* (53) 0.68** (45) 0.10 (50) 0.39** (53)
Class bounda y 0.35 0.10 0.43 0.00 0.44 0.05 0.32 0.00 0.40 0.10 0.15
Page 7 o 17
Nickele al. En i on Sci Eu (2018) 30:53
01.000500 Kilome e s
Co ela ions Cd (EMEP)
> 0.8
0.6 - 0.8
0.4 - 0.6
0.2 - 0.4
< 0.2
01.000500 Kilome e s
Co ela ions Cd (LE)
> 0.8
0.6 - 0.8
0.4 - 0.6
0.2 - 0.4
< 0.2
01.000500 Kilome e s
Co ela ions Hg (EMEP)
> 0.8
0.6 - 0.8
0.4 - 0.6
0.2 - 0.4
< 0.2
01.000500 Kilome e s
Co ela ions Pb (EMEP)
> 0.8
0.6 - 0.8
0.4 - 0.6
0.2 - 0.4
< 0.2
01.000500 Kilome e s
Co ela ions Pb (LE)
> 0.8
0.6 - 0.8
0.4 - 0.6
0.2 - 0.4
< 0.2
Fig. 2 ELCE‑speci ic co ela ions o Cd, Pb and Hg concen a ions in mosses and espec i e modelled a mosphe ic deposi ion. A mosphe ic
deposi ion was modelled by LE (2009–2011) o EMEP (2008–2010); concen a ion alues in mosses we e de e mined in 2010
Page 8 o 17
Nickele al. En i on Sci Eu (2018) 30:53
Fig. 3 ELCE‑speci ic co ela ions o As, C , Cu, Ni, V and Zn concen a ions in mosses and espec i e modelled a mosphe ic deposi ion. A mosphe ic
deposi ion was modelled by LE (2009–2011) o EMEP (2008–2010); concen a ion alues in mosses we e de e mined in 2010
Page 9 o 17
Nickele al. En i on Sci Eu (2018) 30:53
o e en nega i e (Fig.3). A s ong co ela ion ( s = 0.69)
could be shown o land class D_17, co e ing 2.4% o he
analysed a ea, loca ed in Sweden, Finland and Russia.
D_22 (5.4%) as a pa o Sweden e eals a leas mode -
a e co ela ions ( s = 0.43). The emaining su ace show-
ing low co ela ions is alloca ed o ELCE uni D_7, which
co e s 5.4% o he landmass.
Coppe
The la ges a ea co e ed by moss sampling si es (48.9%)
is alloca ed o low co ela ions ( s) be ween 0.2 and 0.4.
Mode a ely s ong co ela ions we e ound o 6 ou o
27 ELCE40 uni s (C_0, D_8, D_17, F1_1, J_2, and U_2)
spa sely dis ibu ed in almos e e y pa icipa ing coun y
and comp ising 15.6% o he ELCE uni s. In compa ison,
Eu ope as a whole is also cha ac e ized by an in e medi-
a ely s ong co ela ion ( s = 0.5). All o he 10 ou o 27
ELCE40 uni s e eal non-signi ican co ela ions wi hin
35.5% o he sampled ELCE40 a ea.
Nickel
Fo Ni, mos o he ELCE40 uni s e eal nega i e co ela-
ions (28.5% o he analysed a ea) o non-signi ican al-
ues (53.8%). Signi ican posi i e co ela ions in ELCE40
classes we e ound o D_17 (0.2 > s > 0.4), D_18, G2_0
(0.4 > s > 0.6) and J_2 (0.6 > s > 0.8) (Table 2). Toge he ,
hese ou land classes comp ise only 13.1% o he ELCE
e i o y wi hin pa icipa ing coun ies, in pa icula
Sweden, Es onia and F ance (Fig.3). O e all, his co -
esponds o a e y low co ela ion o s = 0.09 ac oss
Eu ope.
Vanadium
Wi h espec o a mosphe ic V deposi ion modelled by
LE and espec i e concen a ion in moss, me ely 5 o 31
ELCE40 classes (plus “o he s”) e eal signi ican posi i e,
low Spea man’s ank coe icien s (C_0, D_18, D_19, D_22,
and U_1). They co e 25.7% o he sampled a ea and can
be p ima ily ound in Fennoscandia, no he n Spain and
F ance (Fig.3). 2.4% o he a ea analysed (D_17) shows
signi ican low co ela ions. The emaining ELCE uni s
(66.8%) e eal non-signi ican o nega i e co ela ions
(Table2). Fo V ac oss Eu ope, he Spea man coe icien
also has o be classi ied as low and amoun s o s = 0.19.
Zinc
On he Eu opean le el, he co ela ion be ween modelled
Zn deposi ion (LE) and concen a ions in moss is signi i-
can ly low wi h s = 0.17. The only ELCE40 uni wi h an
in e media ely high co ela ion is S_0, loca ed in pa s o
Es onia, Finland and Russia (1.4% o he sampled a ea).
The 7 ou o 26 ELCE40 classes wi h a leas low co ela-
ions we e he ollowing: D_18, F1_1, F2_5, F3_1, G1_0,
U_1, and “o he s”, loca ed in eas e n and no he n pa s
Eu ope. The coe icien s o he emaining ELCE uni s
a e e y low o non-signi ican (29.5% and 45.6% o he
landmass).
Linea disc iminan analysis/logis ic eg ession
The equency o he p edic o s used as disc iminan s in
he 11 LDA models anges be ween 1 and 3, which means
ha none o he ac o s in pa icula s ands ou (Fig.4).
Mo eo e , he ele ance o he p edic o s o sepa a -
ing sampling si es con ibu ing o high o low co ela-
ions is elemen speci ic. When aking a eal pe cen age o
u ban and ag icul u al land use as indica o s o po en-
ial in luences o a eal and poin emission sou ces, small
adiuses a ound he sampling si es (5km) a e ob iously
mo e ele an o Cd, Cu, Ni, and Zn han ha o he
o he elemen s examined. Vice e sa, a eal pe cen age
o u ban and ag icul u al land use wi hin la ge adiuses
(75–100km) is mo e ele an o As, C , Hg, Pb, and V.
LDA models wi h he highes quali y co esponding
o e o a es ≤ 30% we e ound o C and V ollowed
by As, Cu, Hg, and Pb (only LE) wi h e o a es ≤ 40%
(Table3), i.e. in 7 ou o 11 cases < 40% o he sampling
si es has been inco ec ly classi ied acco ding o hei
su ounding land use. Al hough all p edic o s we e no
no mally dis ibu ed, which is a undamen al assump-
ion o LDA, e o a es o he logis ic eg ession models
(LR) using he same p edic o s as he LDA models we e
e y simila .
F om Tables2 and 3, i is ob ious ha LDA models
a e app op ia e, pa icula ly in case o elemen s show-
ing low co ela ions be ween a mosphe ic deposi ion and
concen a ions in moss (C , Cu, Hg, V). Fo Cd and Pb
wi h s ong co ela ions, densi y o land use a ound he
sampling si es seems o be less ele an . This is also con-
i med by he s a is ical indica o s o he signi icance o
he p edic o s gi en om LR modelling: Densi y o u ban
land use (5km) o Cd (EMEP, LE) and ag icul u al land
use (100km) as a p edic o o Pb (EMEP) was bo h non-
signi ican , which may also explain he high e o a es o
41–44%.
Figu e4 shows he disc iminan lines ob ained om
LDA. The 11 sca e plo s exempli y he sepa a ion
be ween sampling si es con ibu ing o high and low co -
ela ion. Since he whole se o ELCE would lead in o
non- eadable g aphs, ELCE uni s wi h maximum and
minimum co ela ion coe icien s ha e been selec ed as
examples. E o a es o 26–44% (Table3) a e e lec ed
in disc iminan lines no eally sepa a ing g een and ed
poin s. Resul ing om his, LDA models o As, C , Cu,
Hg, Pb, and V p o e o be he mos app op ia e. The
loca ion o poin clus e s in case o Ni and Zn appea s
o be implausible, because low densi ies o u ban and
Page 16 o 17
Nickele al. En i on Sci Eu (2018) 30:53
Recei ed: 18 Oc obe 2018 Accep ed: 11 Decembe 2018
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