Ci a ion: Pe ile, E.; D o ský, T.;
Václa ík, V.; Sy o á, L.; Cha á , J.;
Máˇcalo á, K.; Balcaˇ ík, L. The Use o
Cons uc ion Was e o Remedia e a
The mally Ac i e Spoil Heap. Appl.
Sci. 2023,13, 7123. h ps://doi.o g/
10.3390/app13127123
Academic Edi o : Ra ael
López Núñez
Recei ed: 27 Feb ua y 2023
Re ised: 22 May 2023
Accep ed: 12 June 2023
Published: 14 June 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/).
applied
sciences
A icle
The Use o Cons uc ion Was e o Remedia e a The mally
Ac i e Spoil Heap
E a Pe ile , Tomáš D o ský* , Voj ˇech Václa ík , Lucie Sy o á, Jakub Cha á , Ka eˇ ina Máˇcalo á
and Lukáš Balcaˇ ík
Depa men o En i onmen al Enginee ing, Facul y o Mining and Geology, VSB—Technical Uni e si y o
Os a a, 17. Lis opadu 15/2172, 708 00 Os a a, Czech Republic; [email p o ec ed] (E.P.);
[email p o ec ed] (V.V.); [email p o ec ed] (L.S.)
*Co espondence: [email p o ec ed]; Tel.: +420-597-323-593
Abs ac :
This a icle p esen s he esul s o expe imen al esea ch on he possible use o cons uc ion
and demoli ion was e (CDW) o imp o e he p ope ies o unbu n ailings o igina ing om he
he mally ac i e spoil heap in Heˇ manice (Os a a, Czech Republic). Mining ac i i y anywhe e in
he wo ld gene ally en ails a lo o nega i e impac s on he en i onmen , which a e o a long- e m
na u e. One o he mos p essing challenges in he emedia ion o he consequences o mining ac i i y
is he he mal ac i i y o spoil heaps associa ed wi h he high acidi y o he ailings. Ac i e acidi y
(pH/H
2
O), exchangeable acidi y (pH/CaCl
2
), hyd oly ic acidi y (H
a
), and elemen al composi ion o
ailings and CDW ha e been moni o ed. Based on an acidi y s udy, i has been p o en ha compa ed
o bu n ailings (pH/H
2
O = 8.4, pH/CaCl
2
= 8.9 and H
a
= 1.4 mmol kg
−1
), unbu n ailings show
acidic p ope ies (pH/H
2
O = 3.7, pH/CaCl
2
= 3.6 and H
a
= 205 mmol kg
−1
). The bioa ailabili y
o wo selec ed po en ially oxic elemen s (PTEs), namely Al and Fe, was examined based on he
elemen al composi ion. BCR sequen ial ex ac ion analysis was used o de e mine hei bioa ailabili y.
I has been p o en ha mixing CDW wi h ailings has a posi i e e ec on he pH alue, which has a
posi i e e ec on he u he de elopmen o he en i e si e. The inc ease in he pH alue is p o ably
dependen on he amoun o cons uc ion was e added, so i can be said ha he inc easing amoun
o cons uc ion was e will esul in imp o ed pa ame e s o he bu n ailings. The esul s o he
BCR analysis show ha aluminum om he ailings will be eleased bo h om he educible and
oxidisable ac ions, whe e i will be mainly bound o sulphides. The ela i ely high concen a ion o
Fe in he oxidisable ac ion (2002 mg Fe kg
−1
) sugges s ha Fe is bound o sulphides in he ailings,
and i is due o he high esidual py i e and sulphide con en in he dumped ma e ial, as expec ed.
This wo k has ound no limi s whe e CDW no longe posi i ely a ec s he acidi y o unbu n ailings.
Fo p ac ical applica ion, howe e , i is impo an ha he mix u e o CDW and ailings is p ope ly
mixed and hen used o emedia ion.
Keywo ds:
he mally ac i e spoil heap; mine was e; cons uc ion demoli ion was e; emedia ion;
mining ac i i y; sequen ial ex ac ion analysis
1. In oduc ion
Coal mining and he ecen mass closu e o mines a e associa ed wi h a nega i e
impac on na u al objec s and echnical s uc u es. In addi ion o he ex ac ion o mine al
aw ma e ials, he mining ac i i y also p oduces a la ge amoun o was e ma e ial, which is
gene a ed du ing all he phases o de elopmen and mining ac i i y in he mines, as well
as all he echnological ope a ions ela ed o he p ocesses o en ichmen and pu i ica ion
o he ex ac ed aw ma e ial. In he pas , mos o hese was e ma e ials we e deposi ed
on he su ace. Tha is why nume ous spoil heaps we e c ea ed nea coal mines o in hei
immedia e icini y. A huge amoun o ailings and o he ypes o was e ma e ials we e
deposi ed in hese spoil heaps. In coal basins a ound he wo ld, he e a e s ill hund eds o
Appl. Sci. 2023,13, 7123. h ps://doi.o g/10.3390/app13127123 h ps://www.mdpi.com/jou nal/applsci
Appl. Sci. 2023,13, 7123 2 o 19
objec s ep esen ing he loca ions wi h was e om coal mining [
1
–
3
]. Fo example, he e a e
app oxima ely 281 spoil ips and 46 spoil heaps in he Os a a-Ka ina Coal ield. These a e
an h opogenic ailing spoil heaps o med a di e en imes du ing he nea ly 200-yea long
adi ion o coal mining in he Czech pa s o he Uppe Silesian Coal Basin [
4
]. Howe e ,
he e a e coun ies in which his numbe is e en highe . Fo example, in neighbou ing
Poland, he e a e app oxima ely 250 such objec s, and in China, he numbe o si es whe e
ailings a e s o ed exceeds 1700 [2].
Spoil heaps o mine ailings signi ican ly a ec he cha ac e o he landscape and a e
pe cei ed as a nega i e aes he ic elemen ha s ands ou om he su ounding elie o
he landscape. Whe he hey a e o e g own wi h in asi e ege a ion o e ime o hey
a e a e mo e o less success ul emedia ion, hese a e s ill a eas wi h limi ed op ions o
u he use. In addi ion o he ad e se e ec on he landscape, he p esence o su ace coal
was e dumps is closely ela ed o hei impac on he en i onmen [
2
,
5
,
6
]. F om he poin
o iew o hei en i onmen al bu den, spoil heaps can be pa icula ly p oblema ic due o
hei he mal ac i i y, and also he chemical composi ion o he deposi ed ma e ial which,
as a esul o he age o he spoil heap and i s he mal ac i i y, canno be clea ly de e mined
o mo e p ecisely es ima ed.
In he pas , a signi ican impac o ca bon ailings s o ed in spoil heaps on he indi id-
ual componen s o he en i onmen was no assumed. Ca boni e ous ailings as such do
no con ain any con aminan s, bu unde ce ain condi ions hese can be uncon ollably
eleased om he ailings. The main isk ac o ha is closely associa ed wi h ca boni e ous
ailings is he possibili y o endogenous combus ion [
7
]. The chemical eac i i y o ocks
deposi ed in spoil heaps is mainly de e mined by he amoun o uns able mine als p esen
(e.g., py i e, ca bona es, and eldspa s). Py i e wea he s e y easily. I occu s due o he
in il a ion o p ecipi a ion o he pene a ion o ai olume in o he spoil heap, esul ing
in he o ma ion o sulphu ic acid, o sulpha es. This acidi ica ion p ocess is mo e isible
especially in places o endogenous combus ion. The deg ee o he mal ans o ma ion o
he was e a ec s he leachabili y o me als. Signi ican ly mo e elemen s (Al, Co, C , Cu, Ni)
a e leached om he deeply he mally ans o med samples (sin e s) han om samples o
he mally in ac (unbu n ) was e and sligh ly he mally ans o med (bu n ) was e. This
is due o he p esence o a la ge amoun o glaze in sin e , and his glaze is subjec o
de i i ica ion and he elease o me als con ained in i [
8
]. Changes in empe a u e also
a ec he chemical s a us o o ganic subs ances ound in he coal was e dump. This leads o
he o ma ion o phenols and hei de i a i es, which can pass in o wa e and subsequen ly
cause i s pollu ion [
9
–
11
]. The ma e ial deposi ed on spoil heaps is also cha ac e ized by
di e en pa icle sizes [
12
]. I he ma e ial is po ous, he hea sp eads mo e easily and much
as e . Wi h ine-g ained ma e ials, ai mo emen is slowe and he empe a u e he e o e
inc eases g adually. The geo echnical condi ion o he spoil heap o o he ypes o was e o
sludge ma e ials ha migh ha e been deposi ed on he spoil heaps in he pas mus also
be aken in o conside a ion. They can ep esen a seconda y sou ce o con amina ion o he
ock en i onmen [8,11,13].
Spon aneous combus ion usually igge s he p ocess o long-las ing subsu ace i es.
Due o he con en o sulphide sulphu and o he combus ible subs ances (deb is o con-
eyo bel s, wooden pa s o mine suppo s, e c.), ca boni e ous ailings ep esen a cons an
isk o combus ion (e.g., by inapp op ia e in e en ion in old spoil heaps). Tha is why
he emedia ion wo k also plays an impo an ole, because i should lead o he mal
phenomena inhibi ion on he spoil heap, and should be adap ed o he local mo phology,
echnology, composi ion and olume o he deposi ed was e ma e ial [
7
,
11
]. An inc ease in
he empe a u e o he subsoil and he su ace is a e y signi ican nega i e ac o ela ed o
he mal p ocesses, and i leads o changes in he opog aphy, soil co e , and plan co e , as
well as he a mosphe e [
2
,
14
]. I i es occu in he ailing dumps, he emission o pollu an s
in o he ai will inc ease signi ican ly. As a esul o he inc eased empe a u e and mo e
in ense e apo a ion, he ma e ial on he spoil heap sheds i s mois u e, and d y pa icles
ge in o he ai mo e easily. I he coal con ained in he was e u ns in o ash du ing i e, i s
Appl. Sci. 2023,13, 7123 3 o 19
endency o be ca ied away by he wind inc eases, especially du ing he ope a ions ela ed
o i e ex inguishing, emo al, and anspo o bu n ma e ial, o du ing emedia ion
wo ks. Since he was e ma e ial con ains sulphu , SO
2
and H
2
S a e gene a ed. This is
e idenced by he yellow e lo escence on he su ace o he spoil heap body (Figu e 1). As
a esul o wind e osion, spoil heaps a e he e o e a seconda y sou ce o ai -bo ne dus
(including espi able PM10 pa icles) [15,16].
Appl.Sci.2023,13,xFORPEERREVIEW3o 20

pa iclesge in o heai mo eeasily.I  hecoalcon ainedin hewas e u nsin oashdu ‐
ing i e,i s endency obeca iedawayby hewindinc eases,especiallydu ing heop‐
e a ions ela ed o i eex inguishing, emo al,and anspo o bu n ma e ial,o du ing
emedia ionwo ks.Since hewas ema e ialcon ainssulphu ,SO2andH2Sa egene a ed.
Thisise idencedby heyellowe lo escenceon hesu aceo  hespoilheapbody(Figu e1).
Asa esul o winde osion,spoilheapsa e he e o easeconda ysou ceo ai ‐bo nedus 
(including espi ablePM10pa icles)[15,16].

Figu e1.Heřmanicespoilheap.
The o ma iono  ege a iong oupsisalwaysaposi i ephenomenon,because he
decomposi iono phy omasssuppo s he o ma iono humus.Inplaceswi h ege a ion,
endogenouscombus ioncan u nin oanopen i eand huscon ound hein es men s
spen  o  ecul i a ion.Thiswas hecase, o example,in he mallyac i eHeřmaniceo 
Hed ikaspoilheaps(Os a a,Mo a ian‐SilesianRegion,CzechRepublic).I is he e o e
no anisola edcasewhenal eady eclaimedandadap eda easo  o me spoilheapss a 
ospon aneouslyhea up[2].I is e ydi icul  odealwi hho spo sandp e en endog‐
enouscombus iono oldspoilheaps ha con ainla geamoun so coaldeb isandwe e
o enplacedinaloose,unconsolida edcon igu a ion ha allowsoxygen oeasilyin e ac 
wi h hewas e.Regula moni o ingmakes hei iden i ica ionpossible,bu appa en ly,
heonlyway odealwi h hemis oin ensi y hecombus ionbyimp o ing heaccesso 
ai and husallowing he ailings obu n h ough[17].Thisis he easonwhymanyen i‐
iesdecided o ecul i a ecoalwas edumpsonlya e  heyhadbeenbu ned,ex in‐
guished,o pa iallyexca a ed.Resea chhasshown ha in hecaseo bu ningcoalwas e
dumps, hein oduc iono  ege a ionhasnoe ec unless heobjec issu icien lyp o‐
ec edagains  i e.Insuchsi ua ions,spon aneoussuccessionis heonlysolu ion[2].
The emo alo damagescausedbyminingac i i iesisno  ela ed o heOs a a‐
Ka inaCoal ieldonly.Inanumbe o legisla i eandlegalmeasu eso o he coun ies,
he eisanobliga ion o ecul i a edamageda eason hesu ace.Thisisaglobalp oblem
andalong‐ e mp ocess[18].Thesean h opogenicgeomo phologicalbodiesa e,on he
onehand,abu den o  heen i onmen ;bu on heo he hand, heycanbeanimpo an 
asou ceo cheapanda ailableagg ega es.Thecu en p essu e olimi  heuseo p i‐
ma y awma e ials, heex ac iono whichcausesaddi ionalunpleasan impac son he
landscapeand heen i onmen ,necessa ilyleads o heuseo was easseconda y aw
ma e ials.In heCzechRepublic, hisp oblemwassol edlegisla i elyin2001,because
miningwas eisno classi iedaswas e,bu asap oduc usedinland eclama iono  oad
cons uc ion.
Figu e 1. Heˇ manice spoil heap.
The o ma ion o ege a ion g oups is always a posi i e phenomenon, because he
decomposi ion o phy omass suppo s he o ma ion o humus. In places wi h ege a ion,
endogenous combus ion can u n in o an open i e and hus con ound he in es men s
spen o ecul i a ion. This was he case, o example, in he mally ac i e Heˇ manice o
Hed ika spoil heaps (Os a a, Mo a ian-Silesian Region, Czech Republic). I is he e o e
no an isola ed case when al eady eclaimed and adap ed a eas o o me spoil heaps s a o
spon aneously hea up [
2
]. I is e y di icul o deal wi h ho spo s and p e en endogenous
combus ion o old spoil heaps ha con ain la ge amoun s o coal deb is and we e o en
placed in a loose, unconsolida ed con igu a ion ha allows oxygen o easily in e ac wi h
he was e. Regula moni o ing makes hei iden i ica ion possible, bu appa en ly, he
only way o deal wi h hem is o in ensi y he combus ion by imp o ing he access o ai
and hus allowing he ailings o bu n h ough [
17
]. This is he eason why many en i ies
decided o ecul i a e coal was e dumps only a e hey had been bu ned, ex inguished, o
pa ially exca a ed. Resea ch has shown ha in he case o bu ning coal was e dumps, he
in oduc ion o ege a ion has no e ec unless he objec is su icien ly p o ec ed agains
i e. In such si ua ions, spon aneous succession is he only solu ion [2].
The emo al o damages caused by mining ac i i ies is no ela ed o he Os a a-
Ka ina Coal ield only. In a numbe o legisla i e and legal measu es o o he coun ies,
he e is an obliga ion o ecul i a e damaged a eas on he su ace. This is a global p oblem
and a long- e m p ocess [
18
]. These an h opogenic geomo phological bodies a e, on he
one hand, a bu den o he en i onmen ; bu on he o he hand, hey can be an impo an
a sou ce o cheap and a ailable agg ega es. The cu en p essu e o limi he use o
p ima y aw ma e ials, he ex ac ion o which causes addi ional unpleasan impac s on
he landscape and he en i onmen , necessa ily leads o he use o was e as seconda y aw
ma e ials. In he Czech Republic, his p oblem was sol ed legisla i ely in 2001, because
mining was e is no classi ied as was e, bu as a p oduc used in land eclama ion o
oad cons uc ion.
In Eu ope, he wo economic sec o s p oducing he la ges olume o was e a e
mining and qua ying (28.1%), and building indus y and demoli ion (34.7%) [
19
]. In
he
Czech Republic
, cons uc ion and demoli ion was e cons i u es a signi ican pa o he
Appl. Sci. 2023,13, 7123 4 o 19
o al amoun o was e p oduced in e ms o weigh . In he yea s 2014–2020, he p oduc ion
o cons uc ion was e accoun ed o mo e han hal o he o al p oduc ion o was e (see
Table 1). On he con a y, wi h ega d o he decline in mining ac i i y, was e om mining
and qua ying accoun ed o only 0.05% o he o al amoun o was e p oduced in 2020 [
20
].
Table 1. P oduc ion o was e in he yea s 2014–2020 [20].
Yea To al P oduc ion o Was e
P oduc ion o Cons uc ion
and Demoli ion Was e
Sha e o Cons uc ion and
Demoli ion Was e on he To al
P oduc ion
%
2014 32,028,422 19,124,592 59.7
2015 37,338,298 24,916,868 65.1
2016 34,242,076 20,669,215 60.4
2017 34,553,461 20,153,879 58.3
2018 37,940,560 21,498,561 56.7
2019 37,310,939 23,551,255 63.1
2020 38,486,186 24,955,252 64.8
In compliance wi h he EU communica ion COM/2014/398 “Towa ds a ci cula econ-
omy: A ze o was e p og am o Eu ope”, which in oduces he main objec i es and mea-
su es in he ield o ci cula economy, he land illing o ecyclable was e will no be allowed
om he yea 2025, and i will be comple ely p ohibi ed om he yea 2050 [
21
]. As a
co ec i e measu e, i is ecommended o inc ease he neu aliza ion po en ial by liming,
especially in loca ions wi h an inc eased concen a ion o py i e, o wi h he occu ence
o ja osi e, which can be an impo an indica o in his ega d. An inc ease in he neu al-
iza ion po en ial can also slow down he kine ics o py i e oxida ion. Howe e , a dec ease
in ailings acidi y by su ace applica ion o lime can be e y di icul and ime-consuming
gi en he limi ed mo emen o lime h ough he spoil heap body.
The aim o his a icle is o assess he e ec o he admix u e o cons uc ion and
demoli ion was e (CDW) on he p ope ies o ailings wi h an acidic cha ac e . Acco ding
o he cu en p ac ices o he applica ion o CDW o he mal was e, i is used o ill up
he dep essions c ea ed, o example, by bu ning h ough ho spo s, bu his does no
achie e he ul ima e goal ha would lead o a pH adjus men . One o he objec i es was
he e o e o check whe he a g ea e e ec could be achie ed by mixing CDW and unbu n
ailings, and o check whe he he pe cen age o unbu n ailings and CDW would ha e an
e ec on he inal si ua ion. In addi ion, unbu n mine was e could be used in line wi h
he 3Rs (Reduce, Reuse, and Recycle) concep o he ci cula economy, hus emo ing old
en i onmen al bu dens.
2. Ma e ials and Me hods
2.1. Desc ip ion o he Mining Si e
Tailings om he la ges and mos he mally ac i e complex (Figu e 2) in he en i e
Os a a-Ka ina Coal ield, he Heˇ manice spoil heap (a ea o 881,993 m
2
, olume o
20,106 m3
, epose heigh
20–30 m
), ha e been chosen o he expe imen s. This is he
younges he mally ac i e spoil heap o a e aced cha ac e , which was c ea ed om he
mid-19 h cen u y, when ailings om he Ida Mine we e deposi ed he e. In ense he mal
ac i i y was eco ded in he body o he spoil heap in 2004, when he e we e open i es a
he oo s o ees plan ed as pa o emedia ion. In 2005, a g ou ing wall was buil he e
o p e en hese he mal p ocesses, bu he combus ion p ocess is s ill aking place he e
a his ime. In 2009, he p ocess o emo al was s a ed in o de o build an ai ba ie
be ween he ock and he bu ning ma e ial. Cons uc ion was e was also deposi ed he e in
an uncon olled manne , bu i was no inco po a ed in o he ailings in any way.
Appl. Sci. 2023,13, 7123 5 o 19
Appl.Sci.2023,13,xFORPEERREVIEW5o 20

his ime.In2009, hep ocesso  emo alwass a edino de  obuildanai ba ie be‐
ween he ockand hebu ningma e ial.Cons uc ionwas ewasalsodeposi edhe ein
anuncon olledmanne ,bu i wasno inco po a edin o he ailingsinanyway.

Figu e2.The malac i i yinHeřmanicespoilheap.
2.2.SamplingandP e‐Analy icalS eps
Samplingo  ailings om hesu aceo  hespoilheapbodywasca iedou o e i s
en i ea ea(30samplingpoin s)whe e he malac i i yis akingplace.Fi s ,app ox.10–
20cmo  heuppe laye o  hespoilheap,whichwasno pa o  hesample aken,was
emo ed.Tailingsamplesweighingapp ox.5kgwe e aken om hedep ho 20–50cm.
Byca e ulmixing, he ailingsamples omall hesamplingpoin s(seeFigu e3)we e
homogenizedin oonecomplexsample,whichwass o edinaclosableplas iccon aine 
a e cooling.The ailingsampleswe e i s d iedinalabo a o ya labo a o y empe a‐
u e(±23°C)and henhomogenizedusingaRe schjawc ushe  ypeBB200WC(Haan,
Ge many).A e homogeniza ion, he ailingswe esie ed h oughaRe schs ainlesss eel
sie ewi h hemeshsizeo 2mmandsubsequen lyd ied oacons an weigh ina acuum
d ye VO29MEMMERT(Schwabach,Ge many).Thed ied ailingsampleswe ekep in
adesicca o .
Thesampleso bu n  ailingswe e aken om heplacewhe e he ailingsa e e‐
mo ed(poin sma kedwi ha iangle) o  hepu poseo compa isono  hechemical
composi iono bu n andunbu n  ailings;seeFigu e3.Thep ocedu e o  ea ingbu n 
ailingsamplesisiden ical o hep ocedu e o  ea ingunbu n  ailingsamples,whichis
desc ibedabo e.
Figu e 2. The mal ac i i y in Heˇ manice spoil heap.
2.2. Sampling and P e-Analy ical S eps
Sampling o ailings om he su ace o he spoil heap body was ca ied ou o e
i s en i e a ea (30 sampling poin s) whe e he mal ac i i y is aking place. Fi s , app ox.
10–20 cm o he uppe laye o he spoil heap, which was no pa o he sample aken, was
emo ed. Tailing samples weighing app ox. 5 kg we e aken om he dep h o 20–50 cm.
By ca e ul mixing, he ailing samples om all he sampling poin s (see Figu e 3) we e
homogenized in o one complex sample, which was s o ed in a closable plas ic con aine
a e cooling. The ailing samples we e i s d ied in a labo a o y a labo a o y empe a-
u e (
±
23
◦
C) and hen homogenized using a Re sch jaw c ushe ype BB200 WC (Haan,
Ge many). A e homogeniza ion, he ailings we e sie ed h ough a Re sch s ainless s eel
sie e wi h he mesh size o 2 mm and subsequen ly d ied o a cons an weigh in a acuum
d ye VO29 MEMMERT (Schwabach, Ge many). The d ied ailing samples we e kep
in a desicca o .
The samples o bu n ailings we e aken om he place whe e he ailings a e emo ed
(poin s ma ked wi h a iangle) o he pu pose o compa ison o he chemical composi ion
o bu n and unbu n ailings; see Figu e 3. The p ocedu e o ea ing bu n ailing samples
is iden ical o he p ocedu e o ea ing unbu n ailing samples, which is desc ibed abo e.
A sample o a mix u e o cons uc ion and demoli ion was e was aken du ing he
demoli ion o a ci ic ameni y building, and i con ained he emains o b icks, plas e , and
iles wi hou admix u e o he e ogenous ma e ials ( emains o cables, pape , plas ics). The
samples we e ea ed in he same way as he ailing samples.
A mix u e o ailings and cons uc ion was e in di e en a ios was used o p epa e
samples o he de e mina ion o he physical-chemical pa ame e s and sequen ial ex ac-
ion analysis (SEA). The mixed samples con ained ailings and a mix u e o cons uc ion
was e in he a ios o 9:1 (90% ailings + 10% cons uc ion mix), 7:3 (70% ailings + 30% con-
s uc ion mix) and 8:2 (80% ailings + 20% cons uc ion mix). A highe a io o cons uc ion
was e was no examined. The e o was o main ain a highe a io o ailings, which is he
main ea ed ma e ial.

Appl. Sci. 2023,13, 7123 6 o 19
Appl.Sci.2023,13,xFORPEERREVIEW6o 20


Figu e3.Samplingpoin so Heřmanicespoilheap.
Asampleo amix u eo cons uc ionanddemoli ionwas ewas akendu ing he
demoli iono aci icameni ybuilding,andi con ained he emainso b icks,plas e ,and
ileswi hou admix u eo he e ogenousma e ials( emainso cables,pape ,plas ics).The
sampleswe e ea edin hesamewayas he ailingsamples.
Amix u eo  ailingsandcons uc ionwas eindi e en  a ioswasused op epa e
samples o  hede e mina iono  hephysical‐chemicalpa ame e sandsequen ialex ac‐
ionanalysis(SEA).Themixedsamplescon ained ailingsandamix u eo cons uc ion
was ein he a ioso 9:1(90% ailings+10%cons uc ionmix),7:3(70% ailings+30%
cons uc ionmix)and8:2(80% ailings+20%cons uc ionmix).Ahighe  a ioo con‐
s uc ionwas ewasno examined.Thee o was omain ainahighe  a ioo  ailings,
whichis hemain ea edma e ial.
2.3.Calcula ionsandIns umen alCondi ions
To ecalcula e he esul s,i wasnecessa y ode e mine hed yma e .Thede e mi‐
na ionwasmadeusing heg a ime icme hod.Thecalcula iono d yma e andwa e 
con en wasca iedou acco ding oEqua ions(1)and(2).
Calcula iono massmois u econ en :
𝑤 󰇛󰇜∙
,(1)
whe e:
w—massmois u econ en in%,
m1—o iginalsampleweigh ing,
m2—sampleweigh a e d yinging.
Calcula iono d yma e :
s=100−w,(2)
whe e:
s—d yma e in%,
w—massmois u econ en in%.
Figu e 3. Sampling poin s o Heˇ manice spoil heap.
2.3. Calcula ions and Ins umen al Condi ions
To ecalcula e he esul s, i was necessa y o de e mine he d y ma e . The de e mi-
na ion was made using he g a ime ic me hod. The calcula ion o d y ma e and wa e
con en was ca ied ou acco ding o Equa ions (1) and (2).
Calcula ion o mass mois u e con en :
w=(m1−m2)·100
m2, (1)
whe e:
w—mass mois u e con en in %,
m
1—o iginal sample weigh in g,
m
2—sample weigh a e d ying in g.
Calcula ion o d y ma e :
s= 100 −w, (2)
whe e:
s—d y ma e in %,
w—mass mois u e con en in %.
De e mina ion o he pH alue in he aqueous leacha e was ca ied ou acco ding o
ˇ
CSN ISO 10390 (836221) Soil quali y—De e mina ion o pH.
Exchangeable acidi y was de e mined acco ding o ˇ
CSN EN ISO 14254 (836223) Soil
quali y—De e mina ion o exchangeable acidi y in calcium chlo ide leaching. The po en ial
exchange eac ion also includes adso bed H
+
p o ons and Al
3+
and Fe
3+
ions. An inoLab
®
pH 7110 labo a o y pH me e om Xylem Analy ics Ge many Sales GmbH (Weilheim,
Ge many) was used o measu e bo h pa ame e s. When leaching p o ons om ailing
samples using a neu al sal solu ion (CaCl
2
), i is no possible o displace all H
+
p o ons
om he so p ion complex. Hyd oly ically alkaline sodium ace a e sal s we e he e o e
used o displace all bound p o ons.
Hyd oly ic acidi y H
a
(mmol kg
−1
) was de e mined by i a ion using sodium ace a e
solu ion. Sodium ions displace hyd ogen ions om he so p ion complex, which o m
ace ic acid in he ailing solu ion, he amoun o which is de e mined by i a ion wi h a
Appl. Sci. 2023,13, 7123 7 o 19
measu ed sodium hyd oxide solu ion. The hyd oly ic acidi y was hen calcula ed acco ding
o he equa ion (see Equa ion (3)):
Ha=a· ·cNaOH ·1000 ·K
g, (3)
whe e:
H
a—hyd oly ic acidi y in mmol kg−1,
a—consump ion o NaOH du ing i a ion in mL,
— ac o 0.1 M NaOH,
c
NaOH —concen a ion o NaOH,
1000
—con e sion o 1 kg o soil,
K—co ec ion o sodium ace a e,
g—weigh o soil in g.
2.3.1. Sequen ial Ex ac ion Analysis (SEA)
The eac i i y o mobili y o po en ially oxic elemen s (PTEs) in soils, sedimen s, o
o he ma e ials and hei po en ial oxici y depends on he phase in which he isk elemen
is con ained, as well as he physical and chemical p ocesses hese phases unde go. A a ie y
o sequen ial ex ac ion ypes ha e been de eloped o de e mine PTE mobili y. The numbe
o indi idual s eps in hese ypes o sequen ial ex ac ions is qui e he e ogeneous [
22
–
27
]. In
ou expe imen , he sequen ial ex ac ion analysis used was c ea ed by he Eu opean Com-
mission in he p og am called S anda ds, Measu emen and Tes ing P og amme, o mally
called he BCR (
Bu eau Communi y o Re e ence
). I is used in di e en modi ica ions
and consis s o h ee s eps [
28
–
35
]. A e each s ep, i.e., a e
16 h
, he samples we e cen-
i uged using an EBA 21 cen i uge om Schoelle Ins umen s (
P ague, Czech Republic
)
o sepa a e he solid and liquid phases. The cen i uga ion was ca ied ou o 20 min
a
3000×g pm
. The indi idual s eps o he sequen ial BCR ex ac ion analysis used a e
summa ized in Table 2.
Table 2. O e iew o ex ac ion agen s and condi ions o BCR analysis.
S ep Isola ed F ac ions Agen Volume
mL
Tempe a u e
◦CTime
1Exchangeable ac ion and ac ion
bound o ca bona es 0.11M CH3COOH 40 22 ±2 shaking 16 h
2F ac ion bound o Fe/Mn oxides and
hyd oxides ( educible ac ion)
0.1M NH2OH HCl
acidi ied 2.0M HNO340 22 ±2 shaking 16 h
3
F ac ion bound o o ganic ma e and
sulphides (oxidizable ac ion)
8.8M H2O2,pH=2
1.0M NH
4
OAc, pH = 2
10
50
22 ±2
85 ±2
22 ±2
leaching 1 h
leaching 1 h
shaking 16 h
2.3.2. Analy ical Me hods
The F-AAS (Flame a omic abso p ion spec ome y) me hod was applied o de e -
mine he concen a ion o selec ed haza dous me als in indi idual ac ions using an
AAS con AA
®
700 a omic abso p ion spec ome e om Analy ik Jena GmbH company
(Jena, Ge many).
The chemical composi ion o he samples was de e mined semi-quan i a i ely by X-
ay luo escence on he XEPOS (Spec o, Kle e, Ge many) ene gy dispe sion spec ome e .
A e i u a ion, he samples we e placed in a plas ic cu e e wi h a Myla p o ec i e oil
and hen analyzed in a p o ec i e a mosphe e (He).
The phase composi ion and mic os uc u al p ope ies we e de e mined using X- ay
powde di ac ion (XRD) echnique. XRD pa e ns we e ob ained using a Rigaku Sma Lab
di ac ome e (Rigaku, Tokyo, Japan) wi h a D/ eX Ul a 250 de ec o . The X- ay sou ce
Appl. Sci. 2023,13, 7123 8 o 19
was a Co ube (CoK
α
,
λ1
= 0.178892 nm,
λ2
= 0.179278 nm) ope a ing a 40 kV and 40 mA.
The powde samples we e inely g ound wi h aga e mo a and p essed wi h a mic oscope
glass in a o a ing sample holde and measu ed in he e lec ion mode (B agg-B en ano
geome y) p io o he analysis. The samples we e o a ed (30 pm) du ing he measu emen
o elimina e he p e e ed o ien a ion e ec . The XRD pa e ns we e collec ed wi hin he
ange o 2
θ
5
◦
–90
◦
wi h a s ep size o 0.01
◦
and a speed o 0.5
◦
deg.min
−1
. The measu ed
XRD pa e ns we e e alua ed using PDXL 2 so wa e ( e sion 2.4.2.0) and compa ed wi h
he PDF-2 da abase, 2015 elease (ICDD, New on Squa e, Wo ces e , MA, USA).
3. Resul s and Discussion
Tailings as a seconda y p oduc o coal mining a e no longe conside ed was e in he
Czech Republic, acco ding o Ac No. 185/2001 Coll., on was e and on he amendmen o
ce ain o he laws. The handling o ailings, hei s o age, and use a e mainly co e ed by
mining legisla ion (Ac No. 89/2016 Coll. Ac o he Fede al Assembly on he P o ec ion
and Use o Mine al Resou ces, he so-called “Mining Ac ” as amended). An op imal
p oposal o landscape egene a ion in he a ea a ec ed by mining ac i i y mus be based
p ima ily on in o ma ion desc ibing he impac o ailings om mining and coal p ocessing
on he en i onmen .
3.1. Mine alogical-Pe og aphic Cha ac e is ics o Tailings
The mine alogical-pe og aphic cha ac e is ics o ailings a e impo an o assessing
hei po en ial impac on he en i onmen . The ep esen a ion o di e en ypes o ocks
in he ailings is de e mined by he laye uni in which coal was mined. The con en o
combus ible subs ances in he spoil heap ma e ial a ec s bo h he pe og aphic composi ion
and he g anulome y. Du ing he s udy o spoil heap ma e ial in he Os a a-Ka ina
Coal ield (Czech Republic), i was p o en ha he pe og aphic composi ion o he ailings
is p ac ically iden ical wi hin he indi idual spoil heaps. The main ock ypes on he spoil
heaps a e a ious ypes o aleu opeli es (black and black-g ay o g ay sil s ones o e y
ine-g ained sands ones wi h oo soil con en ), which come om he immedia e icini y
o he coal seams. The decay o sil s one is ela i ely as . Fine-g ained, medium-g ained
o coa se-g ained sands ones a e also ep esen ed in he spoil heap ma e ial in la ge and
a iable quan i ies. These ocks a e somewha mo e esis an o wea he ing. In sands ones
especially, he cemen o hei sand g ains is co oded o o m sand elu ia. The a e o
disin eg a ion o sands ones, he e o e, depends on he na u e o hei cemen . Sands ones
wi h ca bona e and clay cemen a e especially less esis an , while silici ied sands ones a e
e y s able. The mos common ype o ca bona es is anke i e o a ep esen a i e o he
dolomi e-anke i e isomo phic se ies. As a ock- o ming mine al, anke i e occu s ela i ely
a ely in he cemen o some sands ones, while i s occu ence is mo e common in seam
pa ing. A signi ican pa o he so-called peloside i es is made up o anke i e a he han
side i e. Calci e is e y a e in Os a a-Ka ina Coal A ea (OKCA) ocks. Small amoun s
o clay mine als (o he illi e-smec i e mixed s uc u e ype) may show swelling when in
con ac wi h wa e [36].
The mining ma e ial is cha ac e ized p ima ily by ocks and ock ma e ial (clay s ones,
muds ones, sands ones, e c.). The e a e also la ge amoun s o silica (SiO
2
) in i , alumina
(Al
2
O
3
), i on oxides (Fe
x
O
y
), po assium oxide (K
2
O), ca bon (C) and calcium oxide (CaO),
sodium oxide (Na
2
O), o i anium oxide (TiO
2
) [
37
,
38
]. The mine alogical composi ion o
he ailings sample om he he mally ac i e Heˇ manice spoil heap is p esen ed in Table 3.
SiO2is also he mos abundan (43%), and he accompanying aluminosilica es a e p esen
in smalle amoun s.
3.2. Chemical Composi ion o Tailings
A he Heˇ manice spoil heap, which is he mally ac i e, bo h he ailings ound in
he uppe pa o he spoil heap body and he bu n ailings ha a e being emo ed ha e
been analyzed. In unbu n ailings, which we e in he cen e o a en ion, he p e ailing
Appl. Sci. 2023,13, 7123 9 o 19
elemen s included Si (27%), Fe (25%), and Al (11%). I cons i u ed he mos decisi e sha e
o ino ganic componen s. Conside ing he pe cen age p esence o silicon, i can be assumed
ha acidi ica ion does no occu due o he loss o Si, bu due o he lack o basic ca ions
du ing he decomposi ion o aluminosilica es. The con en o Si (48%) and Al (19%) in
bu n ailings inc eased, while he con en o Fe (15%) dec eased.
Table 3. Mine alogical composi ion o ailings using XRD me hod in %.
Mine al Fo mula W
Qua z SiO243
Musco i e KAl2(AlSi3O10)(F,OH)219
Clinochlo e
Mg
3.75
Fe
2+1.25
Si
3
Al
2
O
10
(OH)
813
Albi e NaAlSi3O88
Po assium K 2
Feldspa KAlSi3O8−CaAl2Si2O810.5
Mino i y 4.5
In unbu n ailings om he su ace o he Heˇ manice spoil heap body, he o al
sulphu con en was 3.5%. Racla skáe al. also s a es ha he o al sulphu con en o he
anhyd ous sample in OKC coal is gene ally low, and ha he a e age in he indi idual
laye s and a eas a e usually lowe han 1%, and each an a e age o 0.78% in wo king
seams [
36
]. Pešek p esen s a much la ge ange o o al sulphu alues o 0.4–4.8% wi h
a mean alue o 2.1% [
39
]. In bu n ailings, he o al sulphu con en is educed o 0.5%
due o endogenous combus ion. Pešek also s a es ha simila o sulphu con en , luo ide
and chlo ide con en is highly a iable bu gene ally low, and phospho us, luo ides, and
chlo ides a e bound o he occu ence o hyd oxylapa i e. Howe e , he chlo ide con en
in he black coal o he Uppe Silesian Basin is usually lowe han 0.025% [
39
]. Unbu n
ailings om he Heˇ manice spoil heap con ained 0.3% o P and 0.5% o chlo ides. Thei
highe ep esen a ion in ailings in he Heˇ manice spoil heap may be ela ed o seconda y
hali e con amina ion. The con en o elemen s such as Na (<0.01%), Ca (0.7%), Mg (0.2%)
in he unbu n ailings is e y low. Daniels, S ewa , and Zippe (2018) epo ha hea y
me als such as coppe , nickel, and zinc a e o en linked wi h py i e and o he sulphide
mine als. Inc eased le els o hea y me als in he soil solu ion can be oxic o plan oo s
and mic obes, and hey can also pose a isk o wa e quali y [40]. Howe e , he con en o
hea y me als in he OKCA ca boni e ous ocks is e y low and hei ep esen a ion does
no exceed he olume o o he indus ial emissions om an ecological poin o iew. Tha
is why i does no ep esen a se ious en i onmen al bu den (see Table 4).
Table 4. Elemen al analysis o samples using XRF me hod in %.
% Bu n Tailings Tailings % Bu n Tailings Tailings
Na <0.01 <0.01 Mo 0.0007 0.0011
Ag <0.0002 <0.0002 Nb 0.0066 0.0054
Al 19.04 11.16 Nd 0.0313 0.0292
As 0.001 0.020 Ni 0.03 0.03
Ba 0.2815 0.678 P0.19 0.30
Bi <0.00010 <0.00010 Pb 0.01142 0.0272
B 0.0006 0.0082 P 0.0066 <0.00020
Ca 1.99 0.68 Rb 0.0608 0.0543
Cd 0.0017 0.00047 S0.54 3.50
Ce 0.0342 0.011 Sb 0.0021 0.00043
Cl 0.01 0.49 Se <0.00005 0.0006
Co 0.01 0.005 Si 48.09 26.70
C 0.06 0.04 Sn 0.0036 0.00081
Cs 0.0110 0.014 S 0.0388 0.0532
Cu 0.02 0.03 Ta 0.0118 0.0115
Appl. Sci. 2023,13, 7123 16 o 19
and 30% o CDW, Fe loses i s a ini y o sulphu and will p obably be p e e en ially bound
in he o m o oxides and hyd oxides in he mix u e.
4. Conclusions
The use o a mine was e dump a e deep coal mining causes a numbe o p ac ical
p oblems. The mos impo an p oblem o be sol ed is he mal ac i i y. The pace and
dynamics o succession in bu ning coal was e dumps depends on he s age o he i e,
opog aphy, and cha ac e o he subs a e. Coal was e a ies in colou , om ligh g ay o
black. A la ge pa o he incoming sola adia ion is hus e ained as hea , and in sunny
wea he , he empe a u e on he su ace o he spoil heap o en exceeds he ai empe a u e
se e al imes, which is a al o plan s. Ano he p oblem ela ed o he he mal ac i i y
o he spoil heaps is hei bu ning empe a u e, which eaches up o 1300
◦
C in some ho
spo s, speci ically a he Heˇ manice spoil heap. The e apo a ed PTEs a e mos ly so bed on
he smalles pa icles o he gene a ed ash du ing subsequen cooling (a e en e ing he
ai ). This esul s in la ge pa icles being deple ed o oxic me als. The emaining me als
mainly en ich PM
x
due o so p ion and condensa ion o apou s on ine PM
x
pa icles.
Since he dus pa icle has he la ges speci ic su ace, he su ace o he pa icles also has
he highes concen a ion o oxic me als.
In he e en ha he body o he land ill con amina es i s su oundings (PM
x
, AMD)
and in ensi e he mal ac i i y occu s, such as in he case o he he mally ac i e Heˇ manice
spoil heap, i is mos o en ecommended o comple ely emo e i . I he spoil heap is
comple ely emo ed, hen he a ea can be conside ed as a pe ec ly no mal ounda ion soil
wi h ega d o he loca ion o he body and on he bed ock. Dynamically de eloping, mo e
lexible, and ad anced echnologies make i possible o apply he 3R p inciple ( educ ion,
euse, and ecycling) o he ci cula economy in p ac ice o he mining indus y as well. The
exca a ed bu n ailings, oge he wi h a la ge ac ion o unbu n ailings, can be used as
cons uc ion ma e ial o embankmen s, oads, ailways, and o he cons uc ions. They can
also be used as aw ma e ial o ci il enginee ing, indus y, and eclama ion.
Fo es eclama ion and he so-called con olled succession a e mainly used in he
Os a a-Ka ina Coal ield. The land can be used, o example, as ec ea ional a eas, gol
cou ses, hippod omes, ci y pa ks, cons uc ion si es, e c. In a ci cula economy, i is
impo an o iden i y all possible ways o euse o esou ces. Mixing alkaline cons uc ion
was e wi h unbu n ailings om he su ace o he spoil heap signi ican ly a ec ed i s
acidi y, which has a posi i e e ec on he inc ease o ac i e and exchangeable acidi y and
he dec ease o hyd oly ic acidi y. Cons uc ion and demoli ion was e (CDW) is also a
ich sou ce o a whole ange o basic ca ions, which can be used o en ich he ailings.
This can speed up and posi i ely a ec he eclama ion o moun ain landscapes. The
exca a ed a ea can hen be used, o example, o de elopmen in he o m o esiden ial
uni s, shopping cen es, manu ac u ing plan s and many o he s. The a ea can also be
used o build ec ea ional cen es, such as a ennis hall, oo ball ield, cul u al acili ies,
and o he s.
Au ho Con ibu ions:
Concep ualiza ion, E.P., T.D. and V.V.; me hodology, E.P. and T.D.; alida ion,
E.P., T.D. and V.V.; o mal analysis, K.M., V.V. and T.D.; in es iga ion, L.S., J.C., K.M. and L.B.;
esou ces, J.C.; w i ing—o iginal d a p epa a ion, E.P., V.V., T.D. and L.S.; w i ing— e iew and
edi ing, E.P. and T.D.; isualiza ion, T.D.; supe ision, E.P.; p ojec adminis a ion, V.V. and J.C.;
unding acquisi ion, J.C. All au ho s ha e ead and ag eed o he published e sion o he manusc ip .
Funding:
This esea ch was unded by: VSB-TUO, Facul y o Mining and Geology—g an s num-
be SP2022/57; VSB-TUO, Facul y o Mining and Geology—g an s numbe SP2023/017. P ojec
CZ.11.4.120/0.0/0.0/15_006/0000074 TERDUMP Coope a ion VŠB-TUO/GIG Ka owice on he su -
ey o bu ning dumps on bo h sides o he common bo de .
Ins i u ional Re iew Boa d S a emen : No applicable.
In o med Consen S a emen : No applicable.

Appl. Sci. 2023,13, 7123 17 o 19
Da a A ailabili y S a emen :
The da a p esen ed in his s udy a e a ailable upon eques om he
co esponding au ho .
Con lic s o In e es : The au ho s decla e no con lic o in e es .
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