Ci a ion: Sz amowia -Sala, K.;
S yszko, K.; Samek, L.; Kis le , M.;
Mache zy´nski, M.; Ryša ý, J.; K pec,
K.; Ho ák, J.; Kaspe -Giebl, A.; Goła´s,
J. Compa a i e Analysis o
Real-Emi ed Pa icula e Ma e and
PM-Bound Chemicals om
Residen ial and Au omo i e Sou ces:
A Case S udy in Poland. Ene gies
2023,16, 6514. h ps://doi.o g/
10.3390/en16186514
Academic Edi o : Huichao Chen
Recei ed: 30 July 2023
Re ised: 2 Sep embe 2023
Accep ed: 5 Sep embe 2023
Published: 9 Sep embe 2023
Copy igh : © 2023 by he au ho s.
Licensee MDPI, Basel, Swi ze land.
This a icle is an open access a icle
dis ibu ed unde he e ms and
condi ions o he C ea i e Commons
A ibu ion (CC BY) license (h ps://
c ea i ecommons.o g/licenses/by/
4.0/).
ene gies
A icle
Compa a i e Analysis o Real-Emi ed Pa icula e Ma e and
PM-Bound Chemicals om Residen ial and Au omo i e Sou ces:
A Case S udy in Poland
Ka a zyna Sz amowia -Sala 1, Ka a zyna S yszko 1,* , Lucyna Samek 2, Magdalena Kis le 3,
Ma iusz Mache zy´nski 1, Jiˇ íRyša ý4, Kamil K pec 4, Jiˇ íHo ák4, Anne Kaspe -Giebl 3and Janusz Goła´s 1
1Depa men o Coal Chemis y and En i onmen al Sciences, Facul y o Ene gy and Fuels,
AGH Uni e si y o K akow, Al. Mickiewicza 30, 30-059 K aków, Poland;
[email p o ec ed] (K.S.-S.); [email p o ec ed] (M.M.); [email p o ec ed] (J.G.)
2Facul y o Physics and Applied Compu e Science, AGH Uni e si y o K akow, Al. Mickiewicza 30,
30-059 K aków, Poland; [email p o ec ed]
3Ins i u e o Chemical Technologies and Analy ics, TU Wien, Ge eidema k 9, 1060 Vienna, Aus ia;
[email p o ec ed].a (M.K.); anneliese.kaspe [email p o ec ed] (A.K.-G.)
4
Ene gy Resea ch Cen e, Ene gy and En i onmen al Technology Cen e, VSB–Technical Uni e si y o Os a a,
17. Lis opadu 2172/15, Po uba, 708-00 Os a a, Czech Republic; [email p o ec ed] (J.R.);
[email p o ec ed] (K.K.); [email p o ec ed] (J.H.)
*Co espondence: [email p o ec ed]
Abs ac :
The awa eness o en i onmen al pollu ion has been con inuously g owing in ecen decades
and is cu en ly eaching i s maximum. Eu ope and mos de eloped coun ies a e de e mined o
ensu e sa e b ea hing ai o hei ci izens, and he measu es o do so a e s ic e han e e be o e.
Combus ion p ocedu es emain he p ima y means o p oducing ene gy and wa m h in Poland.
Among he no able cons i uen s o lue gases p oduced as a esul o uel combus ion, solid pa icles
(o pa icula e ma e ) hold signi ican p ominence. The pape p esen s he chemical cha ac e isa ion
o pa icula e ma e emi ed om s a iona y and au omo i e emission sou ces. S a iona y emission
sou ces included he combus ion p ocess o ossil uels (so wood, bi uminous coal, ecopea coal,
culm) in domes ic hea ing uni s and he p ocess o combus ion o bi uminous coal in a powe plan .
Au omo i e emission sou ces included ligh du y and medium du y ehicles uelled by diesel.
Exhaus oxici y es s we e ca ied ou main aining he eal condi ions o PM emission. In all ield
measu emen s pa icula e ma e was g a ime ically measu ed and collec ed on qua z o glass ib e
il e s. Subsequen ly, he con en o ca bonaceous ac ion, ino ganic ions, and me als and me alloids
was analyzed using di e en analy ical echniques. The chemical composi ion o he pa icula e
ma e di e ed depending on he emission sou ce. Wi h espec o s a iona y combus ion sou ces, he
main ac o s de e mining solid pa icle emission a e ela ed p ima ily o he uel quali y. The du y
o ehicles was also a ac o ha in luenced he chemical cha ac e isa ion o he pa icula e ma e
emi ed om he engines.
Keywo ds:
pa icula e ma e ; s a iona y emission sou ces; mobile emission sou ces; combus ion
p ocesses; solid uels; liquid uels
1. In oduc ion
A mosphe e p o ec ion is one o he mos impo an ac ions unde aken by go e n-
men s in he en i e wo ld. Ai pollu ion is he la ges isk ha a ec s bo h en i onmen
and human heal h. Pa icula e ma e and PM-bound chemicals inhaled in o he lungs
des oy he na u al an ioxida i e ba ie in an o ganism, causing se ious damage o cells,
which, in u n, esul in ca dio ascula and in lamma o y diseases and, some imes, e en in
p ema u e dea hs [
1
]. Despi e many p og ammes owa d cleane a mosphe e se up by he
Eu opean Union, le els o pa icula e ma e concen a ion abo e EU s anda ds a e seen
Ene gies 2023,16, 6514. h ps://doi.o g/10.3390/en16186514 h ps://www.mdpi.com/jou nal/ene gies
Ene gies 2023,16, 6514 2 o 16
ac oss he Old Con inen . Acco ding o da a p esen ed by he Eu opean En i onmen al
Agency, Poland ( oge he wi h I aly) is s ill he coun y mos pollu ed by pa icula e ma -
e [
2
]. This p o es ha mul idisciplina y ac ions owa d dec easing human exposu e o
pollu an s and owa d limi a ion hei nega i e impac on ecosys ems a e s ill easonable.
In Sou h Poland, esiden ial hea ing and a ic- ela ed emission oge he wi h indus-
ial emission, soil emission, and seconda y ino ganic ae osols ha e been epo ed as he
main sou ces o a mosphe ic pollu ion [
3
–
7
]. Acco ding o he new nomencla u e p oposed
by he En i onmen al P o ec ion Agency o he Uni ed S a es, esiden ial hea ing is an
example o a non-poin emission sou ce, indus ial emission is a poin emission sou ce,
and au omo i e emission belongs o on- oad sou ces. All o hem may be classi ied as
low-s ack emission, wha e e s o he emission o ha m ul gases and pa icula e ma e a
a le el lowe han 40 m abo e he g ound [
8
,
9
]. The low-s ack ela ed pollu an s di ec ly
a ec human bodies and heal h. The e o e, i is essen ial o keep hese sou ces con inuously
examined and con olled.
Pa icula e ma e is an ac i e ca ie o many chemical compounds, bo h o ganic
and ino ganic. An ac i e cha ac e o PM is ela ed o he numbe o p ocesses ha a e
ongoing in he lue gas duc o in exhaus sys em o engine ca s. Reac ions o nuclea ion,
condensa ion, and agglome a ion occu which cause con inuous changes in he chemical
composi ion o PM and in size o ae odynamic diame e (AD) o pa icles [
10
]. PM
10
and
PM
2
.
5
a e classi ica ions o pa icula e ma e by AD ac o , commonly used o measu e
ai quali y and po en ial heal h isks. PM
10
e e s o pa icula e ma e wi h a diame e o
10
µ
m o smalle . These pa icles a e small enough o be inhaled in o he uppe espi a o y
sys em. PM
2
.
5
, on he o he hand, e e s o pa icula e ma e wi h a diame e o 2.5
µ
m o
smalle . These pa icles a e e en ine and can pene a e deepe in o he espi a o y sys em
and lungs and e en en e he bloods eam, posing a g ea e heal h isk [11].
The emission a ios o pa icula e ma e di e depending on uel and s o e o en-
gine applied, as well as on he ope a ion condi ions o he combus ion p ocess [
12
]. The
implemen a ion o exhaus a e ea men sys ems, such as h ee-way ca alys s o diesel
oxida ion ca alys s in au omo i e solu ions [
13
] and desulphu iza ion plan s and elec o-
s a ic p ecipi a o s [
14
,
15
] in indus ial u ili ies (i.e., he mal powe plan s) imp o es he
quali y o exhaus s eleased o he a mosphe e. Simila ly, many wo ks a ound he wo ld
a e conduc ed on exhaus a e ea men sys ems o he pu poses o esiden ial hea ing,
i.e., honeycomb P -based ca alys s [16,17].
Rega ding esiden ial hea ing, coal and wood a e usually used o hea and elec ici y
gene a ion. Despi e many p og ammes o he ins alla ion o cogene a ion sys ems and
eco-design ecommenda ions o he a chi ec u e o domes ic hea ing uni s, due o cu en
geopoli ical si ua ion wo ldwide, ossil uels o doub ul quali y a e equen ly used. The
usage o such uels in s o es no adap ed o he equi emen s o eco-design di ec i e c ea es
he p ocess o combus ion ine icien . This esul s in high emission ac o s o pa icula e
ma e and o he PM-bound componen s [12,18].
In Poland, he e exis 19 powe plan s and 23 he mal powe acili ies uelled by bo h
bi uminous and ligni e coal as well as biomass. Acco ding o da a om 2022 [
19
], he col-
lec i e usage o coal o gene a ing hea and elec ici y exceeded 70% in 2021. Fu he mo e,
he p ospec s o ansi ioning away om coal as he p edominan p ima y ene gy sou ce
a e conside ably ex ensi e [
20
]. The combus ion o ossil uels in indus ial p ocesses
also gi es ise o pa icula e ma e emissions. The quan i ies o pollu an s emana ing
om powe and he mal plan s a e unde cons an su eillance. Indus ial es ablishmen s
a e manda ed o cleanse lue gases be o e eleasing hem in o he a mosphe e, achie ed
h ough he ins alla ion o pos - ea men sys ems like deni i ica ion, dus ex ac ion, o
desul u iza ion uni s. Emissions o igina ing om coal- i ed powe and he mal acili ies
aise subs an ial conce ns due o hei capaci y o long-dis ance anspo , ad e se impac
on human heal h, isibili y in he a mosphe e, and ha m o ege a ion [21–24].
Au omo i e emissions a e one o he leading sou ces o ai pollu ion wi h a signi ican
sha e in o al pa icula e emissions du ing hea ing and non-hea ing seasons, pa icula ly
Ene gies 2023,16, 6514 3 o 16
in u ban a eas [
25
]. Acco ding o he la es da a p esen ed by he Eu opean Au omobile
Manu ac u e s Associa ion (ACEA) in 2020 he e we e mo e han 246 million ehicles in
use in he Eu opean Union [
26
]. In 2021 app oxima ely 60% o newly egis e ed passenge
ehicles we e diesel (20%) and gasoline- uelled (40%) ca s. In u n, new ucks and ans
a e mos ly uelled by diesel, sha ing mo e han 96% and 90%, espec i ely, o he o al
egis e ed medium- and hea y-du y ehicles. As he sha e o ligh -du y ehicles (LDVs)
equipped wi h gasoline engines is highe han ha o LDVs wi h diesel engines, i is
ob ious ha cu en esea ch ends in au omo i e b anch a e di ec ed owa d gasoline-
uelled and hyb id ca s. Fu he mo e, he Volkswagen emissions scandal, popula ly known
as he ‘diesel ga e’, caused, as he main a e ma h, a dec easing popula i y o ligh -du y
diesel ehicles among Eu opean d i e s. Howe e , i is ue ha “diesel ga e” un he
machine y o imp o emen s in au omo i e legisla ion and diesel pa icula e il e s (DPFs)
o elimina e PM emission and selec i e ca aly ic educ ion o elimina e NO
x
emission was
inally implemen ed [
27
]. Di icul ies wi h a e bu ning and egene a ion p ocess o DPFs
ha e caused hese ca aly ic eac o s o be illegally emo ed om exhaus sys ems e en in
2–3 yea s old ca s.
Diesel engines a e cha ac e ised by signi ican ly highe o que han gasoline engines
as hey ha e la ge cylinde s and longe s okes. Fu he mo e, diesel engines a e able o
ex ac mo e ene gy om uel as hey ope a e a highe comp ession a io [
28
]. The e o e,
hey a e success ully used in ehicles o medium and hea y du y. Fu he mo e, i is no
p edic ed ha he numbe o medium-du y ehicles (MDV) and hea y-du y ehicles (HDV)
will dec ease. Fo hese easons, i seems o be adjus able o con inue he examina ions on
emission o pollu an s, especially o pa icula e ma e , om diesel- uelled ehicles as well.
He e we p esen he chemical cha ac e isa ion o pa icula e ma e gene a ed in
combus ion p ocesses o di e en ypes o uel in bo h s a iona y and au omo i e sou ces.
Field measu emen s a all emission sou ces we e ca ied ou unde eal condi ions ‘as i is’.
Hence, he esul s p o ide aluable in o ma ion on eal exposu e o PM and PM-bound
chemicals and allow us o unde s and he na u e o emi ed pollu an s. The inal goal
o his wo k was o iden i y cha ac e is ic componen s pe each emission sou ce, o he
pu poses o u he wo k conce ning he op imisa ion o mac o ace se ing as a PM
sou ce appo ionmen echnique.
2. Ma e ials and Me hods
2.1. Collec ing o Samples o Real-Emi ed Pa icula e Ma e om Di e en
Combus ion-Rela ed Sou ces
2.1.1. Sampling o Pa icula e Ma e Emi ed om Residen ial Solid Fuels Combus ion
Samples o pa icula e ma e emi ed du ing esiden ial coal combus ion we e g a i-
me ically measu ed using a specialised p obe equipped wi h a 47 mm diame e il e
holde and a 1 kW lue gas pump. The low o lue gas h ough he p obe was cons an and
equal as 2.3 m
3
h
−1
. The ac ion o o al suspended pa icles was collec ed. The pa icles
we e sampled on qua z ib e il e s (Pall lex
®
) du ing combus ion o ecopea, bi uminous
coal, so wood and culm. Once he PM is collec ed, he samples we e hen condi ioned
o 48 h o s abilize he mass in condi ions o cons an empe a u e and humidi y. All uels
we e combus ed h ee imes in domes ic hea ing uni s (DHU) main aining simila eal
condi ions in he combus ion p ocess. Table 1summa ises he pa ame e s cha ac e izing
he domes ic hea ing uni s used in expe imen s.
2.1.2. Sampling o Pa icula e Ma e Emi ed om Indus ial Coal Combus ion
As an example o indus ial dus samples, he ly ash o he coal combus ion p ocess was
aken om he 220 MW powe uni , equipped wi h he OP-650 pul e ised boile (Ra ako,
Poland). Samples we e collec ed om a lue gas duc a e he sys ems o selec i e ca aly ic
educ ion, elec os a ic p ecipi a ion and we lue gas desul u iza ion. Ash pa icles we e
collec ed on 110 mm diame e qua z ib e il e s (Wha man
®
QM-A), applying he au oma ic
g a ime ic dus measu ing sys em (ZAM K˛e y, Poland) equipped wi h a hea ed p obe and
Ene gies 2023,16, 6514 4 o 16
il e ing sys em, d ye , cen al con ol uni , and a egula ed sucking pump (4–10 m
3
h
−1
). The
sampling ime was 90 o 120 min.
Table 1. The cha ac e isa ion o domes ic hea ing uni s u ilised du ing expe imen s.
Fuel Kind DHU Type Sampling Time
So wood S o e, nominal powe : 24 kW, e iciency: 83.4% 480–1800 s
Culm S eel hea ing boile wi h wa e -cooling wa e , nominal powe 30 kW, e iciency 84% 600 s
Ecopea coal Cen al hea ing uni wi h a s o e dedica ed o ecopea coal uelling 600 s
Bi uminous coal Cen al hea ing uni a cas i on s o e, nominal powe 18 kW, e iciency 77% 600 s
The sampling was ca ied ou acco ding o EN 132841:2001 [
29
] and PN-Z-04030-
7:1994 [
30
]. S anda ds egula e he me hod o measu emen o dus mass concen a ion,
which desc ibes, among o he s, he loca ion demands o measu ing poin s, he size and
shape o p obes, and he way o sampling in a speci ic c oss sec ion. Fu he mo e, he
sampling and measu emen a e o be pe o med in an isokine ic way, since he lue gas
eloci y in he p obe has o be he same as in he lue gas duc .
2.1.3. Sampling o Pa icula e Ma e Emi ed om Diesel-Type Engines
Samples o pa icles emi ed om diesel engines we e collec ed basing on he g a ime ic
il a ion me hod acco ding o he Regula ion No. 83 o he Economic Commission o Eu ope
o he Uni ed Na ions (UN/ECE)–Uni o m p o isions conce ning he app o al o ehicles
wi h ega d o he emission o pollu an s acco ding o engine uel equi emen s. The pa icles
we e sampled om ligh and medium du y ehicles on glass ib e il e s (Wha mann
®
) o ,
espec i ely, 47 mm and 70 mm in diame e . The glass ib e il e s we e weigh ed be o e and
a e sampling using a Sa o ius weigh wi h an accu acy o 0.0001 mg. The samples we e
weigh ed and condi ioned a a weigh ing chambe in cons an empe a u e (22
±
3
◦
C) and
humidi y (45 ±8%).
Pa icle samples emi ed om a medium du y ehicle we e collec ed using he AVL
Sma Sample 478 equipped wi h a pa ial lue gas dilu ion unnel on he engine es bed
wi h powe b ake. AVL Sma Sample 478 con ains a sampling p obe, cyclone sepa a o ,
and il e package o a g a ime ic measu emen o solid pa icles. The samples we e
collec ed du ing he Eu opean S eady Cycle d i ing es , which is made up o 13 s eps
e lec ing a ied le els o engine load. Each es was 1000 s long. Each ime, 54.8 m
3
o lue
gas was pumped h ough he glass ib e il e .
Pa icles emi ed om a ligh du y ehicle we e sampled on a chassis es bed AVL Zoellne
4WD using he cons an olume sampling sys em wi h a dilu ion unnel and a sys em o
g a ime ic measu emen o pa icle emission. In o de o main ain he eal cha ac e o s udies,
he emission es s we e conduc ed o pe o m bo h calm u ban d i ing s yle (low speeds wi h
an a e age speed a 26 km h
-1
, low engine loads and low empe a u e o exhaus s) and mo e
agg essi e d i ing s yle in ex a-u ban mode wi h a e age speed o 69 km h−1.
2.2. De e mina ion o he Con en o PM-Bound Chemicals
The ba ch o samples o pa icula e ma e samples om esiden ial, indus ial and
au omo i e sou ces was analy ically measu ed o he p esence o me als and me alloids,
including hea y me als like me cu y (Hg) and a senic (As). The con en o o ganic and
elemen al ca bon (OC, EC) and ino ganic ions was also measu ed.
Rega ding me als and me alloids he concen a ion o Cl, K, Ca, Ti, V, C , Mn, Fe, Ni,
Cu, Zn, B , S , Rb, and Pb was measu ed using a mul i unc ional ene gy dispe si e X- ay
luo escence spec ome e acco ding o Samek e al., 2015 and Samek e al., 2016 [
31
,
32
]. The
QXAS package allowed o quan i a i e analysis acco ding o Vekemans e al., 1994 [33].
To de e mine he concen a ion o PM-bound me cu y, a MA-3000 me cu y au o-
ma ic analyze (NIC, Japan), equipped wi h an au o sample , was used. The p inciple
Ene gies 2023,16, 6514 5 o 16
o measu emen is based on he mal decomposi ion, gold amalgama ion, and a omic
abso p ion. The me hod ollows he ecommenda ions o US EPA 7473 [
34
] and ASTM
D-6722-01 [
35
]. The de ailed p ocedu es o sample ea men we e ou lined in p e ious
pape s o Au ho s [14,36].
Ca bonaceous mass ac ion (OC, EC) was de e mined using a he mal op ical me hod
(Sunse Lab OC/EC ae osol analyze , Sunse Lab. Inc.) de eloped o a mosphe ic samples,
using he qua z.pa empe a u e p o ocol and lase in he ansmission mode. De ails o
sample ea men we e desc ibed in a p e ious wo k o Au ho s [
37
]. The o al ca bon (TC)
in au omo i e pa icula e ma e was de e mined using a ca bon analyze equipped wi h
an in a ed adia ion de ec o . The PM sample on a glass ib e il e was bu ned a 1000
◦
C
unde oxygen condi ions. The in a ed senso iden i ied he p oduced CO
2
esul ing om
he sample combus ion. The esul s we e hen calcula ed on he basis o he calib a ion
cu e p epa ed o he TC mass ange o 5 o 500
µ
g. S anda d solu ions we e p epa ed on
he basis o a a a ic acid dilu ion [38].
The isoc a ic ion ch oma og aphy (IC) was applied o de e mine he con en o ino -
ganic ions as ollows: Na
+
, K
+
, Mg
2+
, Ca
2+
, NH
4+
, NO
3−
, NO
2−
, Cl
−
, SO
42−
. IC analysis
was pe o med on an ICS-1100 ins umen (The mo Scien i ic) equipped wi h an AS-DV
au osample and ion exchange columns: Ion Pac AS22 (4
×
250 mm) o anions, mobile
phase: 4.5 mM Na
2
CO
3
+ 1.4 mM NaHCO
3
; CS16 (5
×
250 mm) o ca ions, mobile phase:
12 mM MSA. A e elec ochemical supp ession (AERS 500 (4 mm) and CERS 500 (4 mm)
supp esso s): quan i ica ion was pe o med wi h a conduc i i y de ec o . The injec ion
olume was 25
µ
L and he low a e was 1.2 mL min
−1
. The de ails o me hodology applied
was p e iously desc ibed in Sz amowia -Sala e al., 2019 and Pacu a e al., 2022 [12,39].
3. Resul s and Discussion
3.1. Real-Emission o Pa icula e Ma e om Di e en Combus ion-Rela ed Sou ces
Figu e 1p esen s he esul s o g a ime ic analysis and mass econs uc ion o pa ic-
ula e ma e emi ed om se en combus ion- ela ed sou ces. WOOD e e s o so wood
combus ion in a DHU, CULM– o culm combus ion in a DHU, ECOPEA– o ecopea coal
combus ion in a DHU. COAL
(In)
– o indus ial bi uminous coal combus ion, COAL– o
bi uminous coal combus ion in a DHU, LDDV– o low-du y diesel ehicles and MDDV– o
medium-du y diesel ehicles.
The g a ime ic measu emen s o mass concen a ion o pa icula e ma e eal-emi ed
om combus ion- ela ed sou ces demons a ed ha he highes PM emission in lue gas
was epo ed o bi uminous coal combus ion in a domes ic hea ing uni and was equal o
464.7 mg m−3
. The emission o PM om combus ion o o he solid uels was se e al imes
lowe and complied wi h a dec easing end CULM > WOOD > COAL
(In)
> ECOPEA e e -
ing o concen a ions equal o: 36.7, 20.9, 5.9 and 5.3 mg m
−3
, espec i ely. The eco ded
mass concen a ion o pa icula e ma e esul ing om indus ial coal combus ion adhe es
o he h esholds ou lined in Bes A ailable Techniques conclusions [
40
], which es ablish a
PM emission ange o 5–50 mg pe no mal m
3
o lue gases. I is clea ha he employed
elec os a ic p ecipi a o , u ilized wi hin he powe plan whe e PM samples we e ga he ed,
e ec i ely elimina ed he dus p oduced du ing he combus ion p ocess, con ibu ing o
he elease o cleane lue gases in o he a mosphe e. The elease o pa icula e ma e om
au omo i e sou ces exhibi ed no ably lowe igu es when con as ed wi h he combus ion
o esiden ial and indus ial uels. I was eco ded a 592.5
µ
g m
−3
o low-du y and
101.9 µg m−3
o medium-du y diesel ehicles, which ansla es o emission a es o 0.0003
and 0.0005 g km
−1
, espec i ely. These indings align wi h, o ma ginally su pass in he
case o MDDV, he PM emission limi s s ipula ed by EURO 6 egula ions, which ha e been
es ablished a 0.0045 g km−1.

Ene gies 2023,16, 6514 6 o 16
Ene gies 2023, 16, 6514 6 o 17
o pa icula e ma e om au omo i e sou ces exhibi ed no ably lowe igu es when con-
as ed wi h he combus ion o esiden ial and indus ial uels. I was eco ded a 592.5 µg
m−3 o low-du y and 101.9 µg m−3 o medium-du y diesel ehicles, which ansla es o
emission a es o 0.0003 and 0.0005 g km−1, espec i ely. These indings align wi h, o ma -
ginally su pass in he case o MDDV, he PM emission limi s s ipula ed by EURO 6 egu-
la ions, which ha e been es ablished a 0.0045 g km−1.
Figu e 1. Mass concen a ion o eal-emi ed pa icula e ma e om diffe en combus ion- ela ed
sou ces (columns—PM mass econs uc ion on he base o PM-bound componen s mass; ▬— he
g a ime ically measu ed mass o PM).
The analysis o pa icle sizes wi hin pa icula e ma e o igina ing om indus ial
combus ion e ealed ha he pa icles con ained 22.9% wi hin he PM2.5 ac ion and
74.9% wi hin he PM10 ac ion [14]. This dis ibu ion migh be in luenced by chemical and
physical eac ions occu ing wi hin ume gas duc s, leading o an al e a ion in pa icle
dimensions. Simila indings ha e been epo ed by o he esea che s who obse ed ha
pa icle size dis ibu ion esul ing om he combus ion o solid uels ypically ollows a
bimodal pa e n. In he case o coal combus ion, i gene a es a g ea e p opo ion o coa se
pa icles compa ed o ine pa icles [41,42]. Biomass combus ion, con e sely, o en p o-
duces a highe quan i y o ine pa icles compa ed o coal [43]. Howe e , ollowing ca -
boniza ion o o e ac ion p e ea men , emissions o ine pa icles ypically expe ience a
subs an ial educ ion [44]. The size dis ibu ion o pa icles o au omo i e o igin has been
al eady widely s udied. I was epo ed ha he majo i y o PM om diesel- uelled ehi-
cles is in he nanopa icle ange [45] wi h peak concen a ions wi hin he ange 16–124 nm
[46–48]. This ein o ces he ac ha indi iduals a e p ima ily exposed o he ine ac-
ions o pa icula e ma e de i ed om combus ion- ela ed sou ces, which p esen
g ea e heal h haza ds han hei coa se coun e pa s.
The PM samples collec ed du ing he combus ion o a ious uels unde wen de-
ailed analy ical ea men , enabling he de e mina ion o he majo chemical cons i uen s
Figu e 1.
Mass concen a ion o eal-emi ed pa icula e ma e om di e en combus ion- ela ed
sou ces (columns—PM mass econs uc ion on he base o PM-bound componen s mass;
Ene gies 2023, 16, 6514 6 o 17
o pa icula e ma e om au omo i e sou ces exhibi ed no ably lowe igu es when con-
as ed wi h he combus ion o esiden ial and indus ial uels. I was eco ded a 592.5 μg
m−3 o low-du y and 101.9 μg m−3 o medium-du y diesel ehicles, which ansla es o
emission a es o 0.0003 and 0.0005 g km−1, espec i ely. These indings align wi h, o ma -
ginally su pass in he case o MDDV, he PM emission limi s s ipula ed by EURO 6 egu-
la ions, which ha e been es ablished a 0.0045 g km−1.
Figu e 1. Mass concen a ion o eal-emi ed pa icula e ma e om di e en combus ion- ela ed
sou ces (columns—PM mass econs uc ion on he base o PM-bound componen s mass; ▬— he
g a ime ically measu ed mass o PM).
The analysis o pa icle sizes wi hin pa icula e ma e o igina ing om indus ial
combus ion e ealed ha he pa icles con ained 22.9% wi hin he PM2.5 ac ion and
74.9% wi hin he PM10 ac ion [14]. This dis ibu ion migh be in luenced by chemical and
physical eac ions occu ing wi hin ume gas duc s, leading o an al e a ion in pa icle
dimensions. Simila indings ha e been epo ed by o he esea che s who obse ed ha
pa icle size dis ibu ion esul ing om he combus ion o solid uels ypically ollows a
bimodal pa e n. In he case o coal combus ion, i gene a es a g ea e p opo ion o coa se
pa icles compa ed o ine pa icles [41,42]. Biomass combus ion, con e sely, o en p o-
duces a highe quan i y o ine pa icles compa ed o coal [43]. Howe e , ollowing ca -
boniza ion o o e ac ion p e ea men , emissions o ine pa icles ypically expe ience a
subs an ial educ ion [44]. The size dis ibu ion o pa icles o au omo i e o igin has been
al eady widely s udied. I was epo ed ha he majo i y o PM om diesel- uelled ehi-
cles is in he nanopa icle ange [45] wi h peak concen a ions wi hin he ange 16–124 nm
[46–48]. This ein o ces he ac ha indi iduals a e p ima ily exposed o he ine ac-
ions o pa icula e ma e de i ed om combus ion- ela ed sou ces, which p esen
g ea e heal h haza ds han hei coa se coun e pa s.
The PM samples collec ed du ing he combus ion o a ious uels unde wen de-
ailed analy ical ea men , enabling he de e mina ion o he majo chemical cons i uen s
— he
g a ime ically measu ed mass o PM).
The analysis o pa icle sizes wi hin pa icula e ma e o igina ing om indus ial com-
bus ion e ealed ha he pa icles con ained 22.9% wi hin he PM
2
.
5
ac ion and 74.9% wi hin
he PM
10
ac ion [
14
]. This dis ibu ion migh be in luenced by chemical and physical eac-
ions occu ing wi hin ume gas duc s, leading o an al e a ion in pa icle dimensions. Simila
indings ha e been epo ed by o he esea che s who obse ed ha pa icle size dis ibu ion
esul ing om he combus ion o solid uels ypically ollows a bimodal pa e n. In he case
o coal combus ion, i gene a es a g ea e p opo ion o coa se pa icles compa ed o ine
pa icles [
41
,
42
]. Biomass combus ion, con e sely, o en p oduces a highe quan i y o ine
pa icles compa ed o coal [
43
]. Howe e , ollowing ca boniza ion o o e ac ion p e ea -
men , emissions o ine pa icles ypically expe ience a subs an ial educ ion [
44
]. The size
dis ibu ion o pa icles o au omo i e o igin has been al eady widely s udied. I was epo ed
ha he majo i y o PM om diesel- uelled ehicles is in he nanopa icle ange [
45
] wi h peak
concen a ions wi hin he ange 16–124 nm [
46
–
48
]. This ein o ces he ac ha indi iduals a e
p ima ily exposed o he ine ac ions o pa icula e ma e de i ed om combus ion- ela ed
sou ces, which p esen g ea e heal h haza ds han hei coa se coun e pa s.
The PM samples collec ed du ing he combus ion o a ious uels unde wen de ailed
analy ical ea men , enabling he de e mina ion o he majo chemical cons i uen s p esen
wi hin he pa icula e ma e . Figu e 1illus a es a column cha ha depic s he econs uc-
ion o PM mass based on he summa ion o masses a ibu ed o analy ically measu ed
PM-associa ed subs ances, which encompass ca bonaceous compounds like o ganic and
elemen al ca bon, as well as me als, me alloids, and ino ganic ions, comp ising bo h ca ions
and anions. The ca ego y e med “Unde ined” was calcula ed as he di e ence be ween
he mass o g a ime ically measu ed PM and he cumula i e mass o PM componen s
de e mined analy ically. This ep esen s he po ion o PM ha eluded speci ica ion du ing
labo a o y analysis. Fo pa icula e ma e s emming om wood, culm, and coal combus-
Ene gies 2023,16, 6514 7 o 16
ion in domes ic hea ing uni s, as well as om diesel- uelled ehicles, he unde ined ac ion
did no su pass 15% o he o al PM mass. In con as , wi hin PM gene a ed om indus ial
coal combus ion, he unde ined ac ion domina ed, accoun ing o o e 60% o he PM.
This can be a ibu ed o he subs an ial con ibu ion o ino ganic PM componen s, o en
cha ac e ized by hei hyg oscopic na u e. I is also plausible ha ce ain cons i uen s o
PM, such as polycyclic a oma ic hyd oca bons ound in he o ganic ma e , me cu y bound
o PM, ni ic ions, ammonium ions, and sulpha e ions, migh ha e e apo a ed du ing
sample p epa a ion o ans e . The accu acy and ul ima e ou comes o PM measu emen s
can also be in luenced by he chosen me hodology. Nussbaume e al., 2008 [
49
] unde sco e
ha he selec ion o sampling me hods wa an s me iculous conside a ion o he physical
and chemical a ibu es o he PM, he eby minimizing measu emen inaccu acies. To
mi iga e e o s, i is ecommended ha pa icula e ma e samples be collec ed h ough
p e-dilu ion echniques, which p e en chemical condensa ion ha migh o he wise lead o
an o e es ima ion o PM mass concen a ions. Howe e , he au ho s’ in en in his con ex
was o cha ac e ize he eal isk posed by exposu e o combus ion- ela ed pa icula e ma e
in i s na u al s a e.
No ably, o pa icula e ma e o igina ing om combus ion o ecopea coal, he econ-
s uc ed mass exceeded he g a ime ically measu ed PM mass. This disc epancy could
be a ibu ed o a po en ial o e es ima ion in he analy ical da a due o he ela i ely low
masses o he PM samples being analyzed. The de ailed discussion ega ding PM-bound
componen s is p esen ed in 3.2–3.4 chap e s.
3.2. PM-Bound Ca bonaceous Compounds
The p edominan sha e o pa icula e ma e o igina ing om he combus ion o
di e en uels is a ibu ed o ca bonaceous compounds. This is pa icula ly p onounced
in he case o so wood combus ion (55.5%), culm combus ion (66.7%), and bi uminous
coal combus ion (58.9%) wi hin esiden ial hea ing uni s (Figu e 1). Speci ically, o ganic
ca bon cons i u ed 54% o he o al ca bon con en de i ed om so wood, 81% om culm,
and a subs an ial 96% om bi uminous coal. Con e sely, o pa icles s emming om
he combus ion o ecopea coal, ca bonaceous compounds made up 23% o PM, wi h a
cumula i e concen a ion as high as 1230
µ
g m
−3
. This concen a ion is no ably lowe
when compa ed o o al ca bon concen a ions a ising om so wood combus ion by a
ac o o 9, om culm combus ion by a ac o o 20, and om bi uminous coal combus ion
in domes ic hea ing uni s by a subs an ial ac o o 223.
Con e sely, indus ial combus ion o bi uminous coal exhibi ed he lowes le els o ca -
bonaceous compounds, accoun ing o a me e 1.6% o PM mass (as shown in Figu e 1). The con-
cen a ions o o ganic and elemen al ca bon we e co espondingly low a 72.1 and
20.1 µg m−3
,
espec i ely. This diminished p esence o ca bonaceous compounds in he PM emissions om
powe plan s likely s ems om he e ec i e ope a ion o exhaus a e ea men sys ems wi hin
he lue gas duc s, which e icien ly emo e hese compounds om he pa icula e ma e ,
lea ing behind mine al and me allic cons i uen s.
In he ealm o mobile sou ces, he mass o o al ca bon made up 45% o pa icula e
ma e emissions om medium-du y diesel ehicles (MDDV) and a mo e signi ican 70%
om ligh -du y diesel ehicles (LDDV). This aligns wi h he indings o He e al.’s s udy
in 2017, indica ing ha elemen al ca bon ypically cons i u es up o 56% o he o e all
ca bonaceous con en wi hin pa icula e ma e o igina ing om diesel sou ces. Fu he -
mo e, acco ding o he men ioned s udy, he emaining po ion, app oxima ely 44%, can be
a ibu ed o he low- ola ili y o ganic ac ion (de i ed om uel and lub ica ing oil) and
he high- ola ili y o ganic ac ion (associa ed wi h unconsumed uels) [48].
To comp ehensi ely cha ac e ize pa icula e ma e o igina ing om di e se combus ion-
ela ed sou ces, he analysis inco po a ed he compu a ion o mass a ios be ween o ganic
ca bon and elemen al ca bon (OC/EC). This pa ame e se es as a aluable indica o o he
ca bonaceous composi ion wi hin he pa icula e ma e . The highes OC/EC alue o 24.0
was iden i ied in PM de i ed om esiden ial combus ion o bi uminous coal. This heigh ened
Ene gies 2023,16, 6514 8 o 16
a io sugges s a p e alence o o ganic ca bon o e elemen al ca bon in his con ex . In he
case o domes ic ecopea coal combus ion, an OC/EC alue o 13.2 was eco ded, e lec ing a
subs an ial o ganic ca bon p esence ela i e o elemen al ca bon. No ably lowe OC/EC alues
we e obse ed o culm combus ion in domes ic hea ing uni s, egis e ing a 4.3. Simila ly,
indus ial coal combus ion in powe plan s yielded a ela i ely modes OC/EC alue o 3.6. Fo
pa icula e ma e a ising om he combus ion o so wood, an OC/EC alue o 1.2 was no ed.
In e es ingly, his alue is no ably lowe —3.5 imes so—compa ed o he alue p oposed by
Sillanpää e al., 2006 [
50
], which s ood a 4.15. I is pe inen o men ion ha Sillanpää e al.,
2006 s udy epo ed a subs an ially low OC/EC a io o 0.8 o diesel ehicles. Con e sely,
signi ican ly highe OC/EC a ios we e documen ed o domes ic uel combus ion.
The p esence o a subs an ial amoun o o ganic ca bon ela i e o elemen al ca bon
could indica e ha he combus ion p ocesses a e no ope a ing op imally, which in u n
can lead o he emission o ha m ul and po en ially oxic subs ances. This unde sco es
he impo ance o e icien combus ion echniques, p ope uel p epa a ion, and adequa e
ai supply o minimize he o ma ion o hese haza dous compounds. The p onounced
p e alence o o ganic ca bon o e elemen al ca bon wi hin he pa icula e ma e com-
posi ion can likely be a ibu ed o incomple e combus ion p ocesses. This phenomenon
gi es ise o he o ma ion o po en ially haza dous compounds, such as polycyclic a o-
ma ic hyd oca bons (PAHs). Incomple e combus ion, cha ac e ized by insu icien oxygen
a ailabili y, ends o p oduce a highe p opo ion o o ganic ca bonaceous compounds.
These compounds a e o med when complex hyd oca bons in he uel a e no comple ely
b oken down in o simple componen s like ca bon dioxide. Ins ead, hey unde go pa ial
b eakdown, leading o he c ea ion o compounds like PAHs. These compounds a e o
conce n due o hei po en ial o pose heal h isks. PAHs a e known o ha e ca cinogenic
p ope ies and a e associa ed wi h a ious espi a o y and ca dio ascula ailmen s when
inhaled [12,39].
3.3. PM-Bound Ino ganic Ions
The p opo ion o anions wi hin he pa icula e ma e exhibi ed a ia ions con in-
gen on he speci ic uel subjec ed o combus ion. The pa icula e ma e s emming om
so wood combus ion exhibi ed he lowes anion con en , cons i u ing a me e 1.2% o pa ic-
ula e ma e . A sligh ly ele a ed concen a ion o anions, 5.7%, was eco ded o pa icula e
ma e esul ing om he combus ion o bi uminous coal in domes ic hea ing uni s (DHUs).
This 5.7% equa es o 26,643
µ
g m
−3
, a concen a ion ou old highe han he summed
anion concen a ion om culm combus ion. In he la e case, anions con ibu ed o 17.3%
o he pa icula e ma e ’s mass. The composi ion o PM o igina ing om indus ial coal
bu ning e ealed anionic con ibu ions o 11% o he PM mass. A no ably dis inc pa e n
eme ged in he case o ecopea combus ion wi hin DHUs, whe e anions ook he mos
subs an ial sha e, accoun ing o a s iking 67.5% o he mass (Figu e 1).
The concen a ion o ino ganic ions wi hin he pa icula e ma e exhibi ed dis inc pa -
e ns, wi h he highes concen a ions being obse ed o chlo ide ions (Cl
−
) and sulpha e
ions (SO
42−
). An o de ly examina ion o hese indings e eals se e al ends (Figu e 2A):
•
Wi hin pa icula e ma e s emming om so wood combus ion, sulpha e ions ook he
lead, con ibu ing a signi ican 60% o he o e all anion mass. Chlo ide ions, hough
sligh ly lowe , s ill held subs an ial p ominence, con ibu ing 28% o he anion mass.
•
The p esence o luo ine ions (F
−
) was iden i ied in pa icula e ma e a ising bo h om
esiden ial coal combus ion and he indus ial p ocess o coal bu ning. In he o me ,
he concen a ion o luo ine ions wi h a concen a ion o 500
µ
g m
−3
accoun ed o
1.5% o he o al anion mass, while in he la e , i ose o 25%. The simila con ibu ion
(21% and 24%) o F
−
mass was also no iced o low-du y and medium-du y diesel
ehicles, espec i ely.
•
In he con ex o esiden ial coal combus ion, chlo ine ions domina ed he anion
composi ion, con ibu ing a subs an ial 95% o he anion mass. In coal bu ning in a
DHU, sulpha es sha ed a smalle p opo ion, comp ising 2% o he anion mass.
Ene gies 2023,16, 6514 9 o 16
•
Ecopea coal combus ion and bi uminous coal combus ion in powe plan s displayed
he lowes con ibu ions o chlo ide ions. In pa icula e ma e om ecopea coal
combus ion, chlo ides con ibu ed a me e 25% o he anion mass. Meanwhile, he
anions balance leaned hea ily owa ds sulpha e ions, making up almos 100% o he
anion mass.
•
Chlo ines and sulpha es con ibu ed in 28% and 70%, espec i ely, o anions ac ions
o pa icula e ma e om culm combus ion.
•Ni a es we e obse ed only in PM de i ed om medium-du y diesel ehicles.
Ene gies 2023, 16, 6514 10 o 17
A.
WOOD
CULM
ECO-PEA
COAL
COAL(In)
MDDV
LDDV
0
10
20
30
40
50
60
70
80
90
100
The pe cen age sha e o anions in pa icula e ma e mass
[%]
B.
WOOD
CULM
ECO-PEA
COAL
COAL(In)
MDDV
LDDV
0
10
20
30
40
50
60
70
80
90
100
The pe cen age sha e o ca ions in pa icula e ma e mass
[%]
SO
42-
PO
43-
NO
3-
NO
2-
B
-
Cl
-
F
-
Ca
2+
K
+
Mg
2+
NH
4+
Na
+
Li
+
Figu e 2. The sha e o ino ganic ions ((A). anions, (B). ca ions) in pa icula e ma e eal-emi ed
om diffe en combus ion- ela ed sou ces.
These indings co obo a e exis ing li e a u e, such as he s udy by Popo iche a e
al. in 2014 [51], ein o cing he consis ency o he esul s ob ained and enhancing he
b oade unde s anding o ca ion dis ibu ion ac oss a ious combus ion sou ces.
The ela ionship be ween anions and ca ions, cha ac e ized by he equi alen con-
cen a ions a io o anion o ca ion (A/K), exhibi ed dis inc beha iou s ac oss a ious
combus ion scena ios. No ably, only in he case o indus ial coal combus ion did he p o-
po ions o anions and ca ions achie e equilib ium, indica ed by an A/K alue o 0.95. In
he emaining ins ances in ol ing wood, culm, ecopea, coal, medium-du y diesel ehicles
(MDDV), and ligh -du y diesel ehicles (LDDV), he A/K a ios displayed speci ic alues
o 0.7, 1.6, 1.3, 4.0, 0.16, and 0.06, espec i ely. The mos no ewo hy ele a ion in A/K a io
was obse ed o coal bu n in domes ic hea ing uni s, egis e ing a alue o 4.0. This sub-
s an ial alue s emmed om an excess o anions, pa icula ly chlo ide ions. I is easona-
ble o assume ha hese chlo ides a e p edominan ly bound o NH4+ and Na+. Calcula ing
his su plus, he mass concen a ion o chlo ide excess eached 18,567 µg m−3. The in i-
guing aspec was he su p isingly low A/K a ios o mobile sou ces, unde sco ing a p o-
nounced excess o ca ion concen a ion wi hin pa icula e ma e . This de ia ion om bal-
ance could be a ibu ed o he p esence o ca ions in insoluble o ms, which limi s hei
abili y o main ain equilib ium wi h anions. he a ying A/K a ios unde line he in ica e
chemis y o ion in e ac ions and solubili y pa e ns wi hin emi ed pa icula e ma e . The
in ica e in e play be ween anions and ca ions in pa icula e ma e highligh s he com-
plex chemis y occu ing du ing combus ion p ocesses. This chemis y is p obably in lu-
enced by ac o s such as uel ype, combus ion empe a u e, and eac ion kine ics.
3.4. PM-Bound Me als and Me alloids
Among he a ious componen s o pa icula e ma e , me als and me alloids occu-
pied he lowes sha e, as depic ed in Figu e 1. The analysis o pa icula e emissions om
coal combus ion indica ed ha he cumula i e mass o he analyzed elemen s cons i u ed
less han 1% o he o al PM mass, despi e hei collec i e concen a ion being 4400 µg m−3.
Figu e 2.
The sha e o ino ganic ions ((
A
). anions, (
B
). ca ions) in pa icula e ma e eal-emi ed om
di e en combus ion- ela ed sou ces.
The dis ibu ion o ca ions wi hin he analyzed pa icula e ma e exhibi ed dis inc
a ia ions con ingen on he combus ed uel (Figu e 2B). The indings can be sys ema ically
elucida ed as ollows:
•
The cumula i e concen a ion o ca ions in pa icula e ma e om esiden ial coal
combus ion amoun ed o 3.600
µ
g m
−3
, while om ecopea coal bu ning, i s ood a
1.050
µ
g m
−3
. These igu es con ibu ed o 0.8% and 20.0% o he pa icula e ma e ’s
mass, espec i ely. No ably, ca ion mass o igina ing om combus ion exceeded ha
om ecopea coal bu ning by a ac o o 2.0, cons i u ing 6% o PM mass.
•
The lowes concen a ions o ca ions we e egis e ed in pa icles emi ed om so wood
combus ion (200
µ
g m
−3
) and bi uminous coal combus ion in powe plan s (346
µ
g m
−3
).
•Ino ganic ions con ibu ed 2% o PM mass o ligh -du y diesel ehicles (LDDV) and
8% o medium-du y diesel ehicles (MDDV). No ably, among he ca ions, sodium
ca ions held he highes con ibu ion, comp ising 76% o he ca ion mass o LDDV
and 55% o MDDV. Po assium and calcium also held subs an ial p opo ions wi hin
his ionic balance.
•
In PM om coal and ecopea coal combus ion in DHUs, ammonium ions (NH
4+
) we e
p edominan , con ibu ing o o e 80% o he ca ion mass. Lowe NH
4+
con en was
obse ed in PM om culm (10%), so wood (38%), and powe plan emissions (20%).
•
In he case o so wood combus ion, po assium ca ions (K
+
) exhibi ed a p e alence
simila o ha o ammonium ions. Sodium ca ions (Na
+
) sha ed abou 20% o PM
Ene gies 2023,16, 6514 16 o 16
29.
CSN EN 13284-1; S a iona y Sou ces Emissions—De e mina ion o Low Range Mass Concen a ion o Dus —Pa 1: Manual
G a ime ic Me hod. Eu opean S anda ds: Plzen, Czech Republic, 2017.
30.
PN-Z-04030-7:1994; Ai P o ec ion agains Pollu ion—Dus Concen a ion Measu emen —Measu emen o Concen a ion and
Mass Flow o Dus in Flue Gases by he G a ime ic Me hod. 1994.
31.
Samek, L.; S egowski, Z.; Fu man, L. P elimina y PM2.5 and PM10 F ac ions Sou ce Appo ionmen Complemen ed by S a is ical
Accu acy De e mina ion. Nukleonika 2016,61, 75–83. [C ossRe ]
32.
Samek, L.; Fu man, L.; Kawik, T.; Welnogo ska, K. Applica ion o X-Ray Fluo escence Me hod o Elemen al Analysis o PM2.5
F ac ion. Nukleonika 2015,60, 621. [C ossRe ]
33.
Vekemans, B.; Janssens, K.; Vincze, L.; Adams, F.; Van Espen, P. Analysis o X-Ray Spec a by I e a i e Leas Squa es (AXIL): New
De elopmen s. X-Ray Spec om. 1994,23, 278–285. [C ossRe ]
34.
EPA. Me hod 7473 (SW-846): Me cu y in Solids and Solu ions by The mal Decomposi ion, Amalgama ion, and A omic Abso p ion
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