Removal of soil polycyclic aromatic hydrocarbons derived from biomass fly ash by plants and organic amendments

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1 Plnt Soil Environ. Removl of soil polyyli romti hydrorons derived from iomss fly sh y plnts nd orgni mendments Zdeněk KOŠNÁŘ*, Pvel TLUSTOŠ Deprtment of Agroenvironmentl Chemistry nd Plnt Nutrition, Fulty of Agroiology, Food nd Nturl Resoures, Czeh University of Life Sienes Prgue, Prgue, Czeh Repuli *Corresponding uthor: kosnrz@f.zu.z ABSTRACT Košnář Z., Tlustoš P. (218): Removl of soil polyyli romti hydrorons derived from iomss fly sh y plnts nd orgni mendments. Plnt Soil Environ., 64: Phytoremedition using mize (Ze mys L.) ssisted y the ompost or vermiompost mendments ws the most pproprite strtegy for ioremedition of soil ontminted y polyyli romti hydrorons (PAHs) derived from iomss fly sh. Higher removl of low moleulr weight PAHs thn medium nd high moleulr weight PAHs within the sme tretment were oserved. The totl PAH ontent in plnted soil with ompost or vermiompost ws deresed in rnge etween %. There were no signifint differenes (P <.5) etween the ompost nd vermiompost mendments on the totl removl of sh-pahs. The ontent of PAH derived y sh did not hve dverse effet on mize ultivtion nd iomss yield. The ontriution of PAH redution y mize roots on the soil totl PAH removl ws negligile. Therefore, mize signifintly oosted the PAH removl in soil. The hrvested mize shoots did not represent ny environmentl risk. Keywords: rinogeni ompound; omustion residues; ontmintion; degrdtion; soil mendments Polyyli romti hydrorons (PAHs) re hydrophoi orgni ompounds with two or more enzene romti rings. Some PAHs re onsidered s potentilly rinogeni ompounds to humns; they n e formed minly during the inomplete omustion (Pris et l. 218). The relesed PAHs tend to e persistent e.g. in soils, sediments nd sewge sludge (Váh et l. 25, Dvořák et l. 217, Grí-Sánhez et l. 218). The unfvourle onditions of iomss omustion in power plnts n lso led to the umultion of PAHs in resulting shes (Msto et l. 215). The iomss shes usully lso ontin high mounts of minerl nutrients suh s C, K, P nd Mg, nd therefore there is n effort to reyle them s soil mendments nd/or fertilizers (Oheová et l. 217). The possile PAH ontent in shes pplied in soil hve not reeived onsiderle ttention. The inresed ontent of PAHs in shes n limit the soil sh pplition nd elevte the griulturl soil ontmintion (Enell et l. 28). Phytoremedition using mize (Ze mys L.) ould e suitle strtegy for len-up of sh-pahs ontminted soils euse mize signifintly enhned the degrdtion of ged PAHs in soil from wstewter-irrigted re (Guo et l. 217). Moreover, the ompost or vermiompost pplition into soil mended y PAH-ontminted shes ould improve the removl similrly s in the se of ioremedition of rtifiilly nd ged PAHs ontminted soil desried y Wng et l. (212) nd Feng et l. (214). Supported y the Ministry of Agriulture of the Czeh Repuli, Projet No. QK171379, nd y the Czeh University of Life Sienes Prgue, Projets No. CIGA nd

2 Plnt Soil Environ. Vol. 64, 218, No. 2: The min ims of this study were: (i) to determine the removl of PAHs derived from iomss fly sh in non-plnted/plnted sh-soil in omprison to non-plnted/plnted sh-soil mended with ompost or vermiompost; (ii) to determine the ontriution of mize on the PAH removl from soil. MATERIAL AND METHODS PAHs. In this study, 16 individul US EPA priority PAHs were investigted. The PAHs were sorted into four groups s follows: LMW PAHs low moleulr weight PAHs (the sum of nphthlene, enpthylene, enphtene, fluorene, phennthrene, nthrene); MMW PAHs medium moleulr weight PAHs (the sum of fluornthene, pyrene, enzo[]nthrene, hrysene); HMW PAHs high moleulr weight PAHs (the sum of enzo[]fluornthene, enzo[k]fluornthene, enzo[]pyrene, indeno[l,2,3-,d]pyrene, dienz[,h]nthrene, enzo[g,h,i]perylene); totl PAHs the sum of ll 16 individul PAHs. Soil. The experimentl soil originted from long-term tril site lose to the ity of Humpole in the Czeh Repuli (49 33'15''N, 15 21'''E). The soil ws otined y mixing different susmples olleted from the field site t depth of 2 m. The non-sterilized soil ws homogenized, ir-dried t room temperture nd pssed through 5 mm stinless steel sieve. The min physiohemil hrteristis of the experimentl soil (Cmisol sndy lom ording to the FAO soil lssifition) re listed in Tle 1. Compost nd vermiompost. The ompost ws otined from the omposting of iowste mixture following the methodology desried y Hrt et l. (21). Briefly, the ompost prodution ws rried out in 7 L plsti lortory fermenter. The mixture ws prepred from livestok mnure, fresh grss, strw nd wste pper in rtio of 9:9:1:1 (w/w). The fermenter ws pled in lortory t 25 C nd the omposting proess ws rried out with fored ertion. After 18 dys, the ompost ws onsidered s mture nd suffiiently stilized to e used. The vermiompost ws otined from the vermiomposting of the sme iowste mixture mentioned ove following the methodology desried y Hnč et l. (217). Briefly, vermiomposting ws onduted in plsti vermiompost retors (Ekodomov, Prgue, Czeh Repuli) pled in lortory. 5 kg of the iowste mixture ws inoulted with.5 kg of sustrte ontining erthworms of the genus Eiseni. This mixture ws pled into 12 L plsti owl of vermi-retor nd left 18 dys for vermiomposting. The min physio-hemil hrteristis of the redy to use ompost nd vermiompost re shown in Tle 1. Ash. The experimentl iomss fly sh ws otined from ommeril iomss power plnt operted in the Czeh Repuli using 2 MW grte oiler. The tested sh ws derived from the Tle 1. Physio-hemil hrteristis of soil, ompost nd vermiompost Prmeter Soil Compost Vermiompost ph CCl2 5.2 ±. 8.4 ±. 8.7 ±.1 C tot (g/kg) 18.3 ± ± ± 1.8 N tot (g/kg) 1.35 ± ± ±.1 P vil (mg/kg) 1 / tot (g/kg) ± ± ±.4 K vil (mg/kg)/ tot (g/kg) 19 ± ± ±.6 C vil (mg/kg)/ tot (g/kg) 1586 ± ± ±.7 Mg vil (mg/kg)/ tot (g/kg) 153 ± ± ±.2 Totl PAHs (µg/kg) nd nd nd 1 Avil. ville element ontents (P, K, C nd Mg) in soil (mg/kg) were determined using Mehlih 3 extrtion; 2 tot. totl element ontents (P, K, C nd Mg) in ompost nd vermiompost (g/kg) were determined ording to the method used y Hnč et l. (217). nd not deteted (individul polyyli romti hydrorons (PAHs) were lower thn the detetion limit in the rnge etween µg/kg dry weight) 89

3 Plnt Soil Environ. omustion of whet strw in the temperture rnge 6 7 C. The olleted sh ws omposite of four rndom su-smples tken from ontiner with fly sh from eletrostti preipittor. The sh ws ir-dried t room temperture nd thoroughly mixed in lortory. The min physio-hemil hrteristis of the experimentl sh determined ording to Merl et l. (216) nd Košnář et l. (216) were: prtile size frtion <.25 mm, 67.8%; frtion mm, 32.2%; ph H2, 1.3; eletril ondutivity, O 9.9 ms/m; loss on ignition, 52.6%; P tot,.1%; K tot, 9.5%; C tot, 1.8%; Mg tot,.57%; totl PAHs, 16.2 mg/kg DW (dry weight). Pot experiment. The experiment ws onduted in n outdoor, tmospheri preipittion-ontrolled, vegettion hll with nturl temperture nd light using series of 6 L polypropylene pots: open top, 21 m; se, 18 m; height, 2 m. The pot experiment ws rried out in 9 tretments eh in four seprted pots for replition s follows: S soil (ontrol); C ompost-soil; V vermiompost-soil; A sh-soil; CA ompostsh-soil; VA vermiompost-sh-soil; PS plnted soil (ontrol for plnts); PC plnted ompost-soil; PV plnted vermiompost-soil; PA plnted sh-soil; PCA plnted ompostsh-soil; PVA plnted vermiompost-sh-soil. Eh tretment (S nd PS) ontined 5 kg soil DW per pot nd rest of the tretments ontined 5 kg of mended soil per pot. The sh, ompost nd vermiompost in mended soil of the respetive tretment represented 1% (w/w), 1% (w/w) nd 1% (w/w), respetively. The initil PAH ontents of experimentl tretments re shown in Tle 2 exluding the tretments without the sh ddition euse the PAHs were not deteted in them initilly. As the experimentl plnt ws tested mize (Ze mys L. vr. Colisee). The mize seeds were gined from the KWS (Einek, Germny). Before sowing, eh pot reeived 5 mg N in NH 4 NO 3 wter solution, 32 mg P nd 8 mg K in K 2 HPO 4 wter solution. The mize seeds were sown diretly in soil t depth of 2 3 m, t rte of 8 seeds per pot. The plnts were thinned to 3 per pot t the ge of the third lef emergene. The pots were mnully wtered with deminerlized wter regulrly in order to keep soil moisture t 6 7% of the mximum wter holding pity. Soil smples were olleted t the end of the 12-dys experiment. Eh soil smple ws omposite of five su-smples from different zones of eh pot. The plnt smples (roots nd shoots seprtely) were otined fter the hrvest. Roots were wshed with distilled wter to remove the tthed soil prtiles. Before the PAH nlysis the smples were seprtely ir-dried t lortory temperture, homogenized nd plnt smples were pulverized to fine powder with mill (Retsh, Hn, Germny). PAH nlysis. The extrtion of PAHs from soil nd plnt smples ws rried out ording to the US EPA (27) using n ultrsoni th (Bndelin eletroni, Berlin, Germny) with ontinuous re-extrtion yles followed y the sili gel len-up proess in onordne to the US EPA (1996). The PAH identifition followed y the PAH quntifition ws sed on gs Tle 2. Initil polyyli romti hydroron (PAH) ontents (µg/kg dry weight) in experimentl tretments Tretment LMW PAHs MMW PAHs HMW PAHs Totl PAHs A CA VA PA PCA PVA All vlues represent mens (n = 4). There were no signifint differenes (P <.5) in initil PAH ontents etween the tretments: A sh-soil; CA ompost-sh-soil; VA vermiompost-sh-soil; PA plnted sh-soil; PCA plnted ompost-sh-soil; PVA plnted vermiompost-sh-soil; LMW PAHs low moleulr weight PAHs; MMW PAHs medium moleulr weight PAHs; HMW PAHs high moleulr weight PAHs; totl PAHs the sum of ll 16 individul PAHs 9

4 Plnt Soil Environ. Vol. 64, 218, No. 2: hromtogrphy/mss spetrometry method desried y US EPA (214) using 689N-gs hromtogrph with 5975-mss detetor (Agilent Tehnologies, Snt Clr, USA). The seprtion of PAHs ws rried out using pillry olumn (2 m.18 mm inner dimeter,.14 μm film thikness) (Agilent J&W Sientifi, Snt Clr, USA). The detiled hromtogrphi regime nd nlytil preision of the method were desried elsewhere y Košnář et l. (216). Dt proessing nd sttistil nlysis. The totl soil PAH removl (%) in Figures 1 nd 2 ws lulted s follows: Totl soil PAH removl = 1 (PAH residul PAH initil )/PAH initil Where: PAH residul residul ontent of PAHs in soil (µg/kg DW) t the end of the 12-dys experiment; PAH initil initil ontent of PAHs in soil (µg/kg DW) t dys. The plnt PAH removl (%) in Tle 3 ws lulted s follows: plnt yield PAHonentrtion Plnt PAH removl = 1 [ ] PAH initil /pot Where: plnt yield mize roots yield (kg roots DW/pot); PAH onentrtion PAH onentrtion in mize roots (µg PAH/kg plnt DW); PAH initil /pot initil PAH ontent in soil t dys per eh pot (µg PAH/pot). The one-wy ANOVA t P <.5 followed y the Tukey s test ws performed to evlute the sttistil differenes etween the tretments. The dt were evluted using the Mirosoft Exel 21 (Mirosoft Corportion, Redmond, USA) nd Sttisti 12. (SttSoft, Tuls, USA). RESULTS AND DISCUSSION The influene of sh-pahs in the development of ioremedition pprohes ws ssessed y ompring of mize iomss yield in Tle 3. The ompost nd vermiompost mendments in PC nd PV tretments signifintly inresed (P <.5) the yield of mize roots in omprison to the plnted ontrol tretment (PS). The mize shoots yields were the sme in ll the tretments. The soil ontminted y sh-pahs hd no dverse effets on mize iomss (roots nd shoots) yield s there were no signifint differenes (P <.5) etween the respetive tretments. Our results of iomss yield were omprle with 12 dys experiment with mize grown in soil ontminted y pyrene nd phennthrene rtifiilly (Lio et l. 215). In our study, the PAHs were found only in mize roots ultivted on sh-mended soil (Tle 3). The ompost nd vermiompost mendments ould enhne () LMW PAHs removl (%) 1 5 d () MMW PAHs removl (%) d () 8 HMW PAHs removl (%) Figure 1. Removl of () low moleulr weight polyyli romti hydrorons (LMW PAHs); () medium moleulr weight PAHs (MMW PAHs), nd () high moleulr weight PAHs (HMW PAHs) from soil t the end of the 12-dy experiment. Eh olumn shring different lower se letters indite signifint differenes (P <.5) etween the tretments: A sh-soil; CA ompost-sh-soil; VA vermiompost-sh-soil; PA plnted sh-soil; PCA plnted ompost-sh-soil; PVA plnted vermiompost-shsoil. Error rs indite stndrd devition vlues of n = 4 91

5 Plnt Soil Environ. Totl PAHs removl (%) d the iovilility of soil sh-pahs euse signifintly inresed PAH ontent ws oserved in roots of PCA nd PVA tretments thn in PA tretment. The PAH ontent in mize shoots ws not deteted nd trnslotion of sh-pahs found in roots to the shoots remined unonfirmed. This ws in line with the study y Go et l. (211) who indited tht the spiked PAHs re umulted in roots rther thn trnsported through the xylem flow to the shoots. In this study, the PAH removl of sh origin from soil y mize roots ws negligile in rnge Figure 2. Removl of totl polyyli romti hydrorons (PAHs) from soil t the end of the 12-dy experiment. Eh olumn shring different lower se letters indite signifint differenes (P <.5) etween the tretments: A sh-soil; CA ompostsh-soil; VA vermiompost-sh-soil; PA plnted sh-soil; PCA plnted ompost-sh-soil; PVA plnted vermiompost-sh-soil. Error rs indite stndrd devition vlues of n = 4 etween.2.4% (Tle 3). This ould indite tht the ontriution of PAH umulted in mize roots on the totl PAH removl from soil of PCA nd PVA tretments ws miniml. This finding is onsistent to the study y Kálková nd Tlustoš (211) who reported signifintly lower thn 1% umultion of ged PAHs y mize from soil. The removl of individul PAH groups is shown in Figures 1 nd 2 exluding the tretments without the ddition of sh euse the PAHs were deteted in them neither t the eginning nor in the end of the experiment. Different LMW, MMW nd totl PAH removl from soil of ll investigted tretments ws determined s follows: PCA ~ PVA > PS > CA ~ VA > A, nd followed y PCA ~ PVA > PS ~ CA ~ VA > A for the HMW PAH removl. The phytoremedition of sh-soil ssisted y ompost or vermiompost (PCA nd PVA) ws the most pproprite strtegy in the PAH removl. Cultivtion of mize on sh-soil in omintion with ompost mendment in PCA tretment removed 79.% of LMW PAHs, 51.5% of MMW PAHs nd 48.1% of HMW PAHs from soil. These PAH removls were not sttistilly (P <.5) different to those rehed in the PVA tretment using mize on vermiompost mended sh-soil. The higher LMW PAH removl thn the MMW nd HMW PAH removl in the sme tretment indited tht the LMW PAHs of sh origin re suseptile to e iodegrdle similrly to the ged PAHs s ws desried y Feng et l. (214). The results of totl PAH removl in Figure 2 showed tht the totl PAHs derived from iomss Tle 3. Yield of mize roots nd shoots, polyyli romti hydroron (PAH) onentrtion in roots nd PAH removl y roots Tretment Root (g/pot DW) Shoot (g/pot DW) Totl PAHs in roots (µg PAH/kg roots DW) Plnt PAH removl (%) PS nd nd PC nd nd PV nd nd PA PCA PVA nd not deteted (individul PAHs were lower thn the detetion limit in the rnge etween µg/kg dry weight (DW)). All vlues represent mens (n = 4). Different lower se letters within the sme olumn indite signifint differenes (P <.5) etween the tretments: PS plnted soil (ontrol for plnts); PC plnted ompost-soil; PV plnted vermiompost-soil; PA plnted sh-soil; PCA plnted ompost-sh-soil; PVA plnted vermiompost-sh-soil 92

6 Plnt Soil Environ. Vol. 64, 218, No. 2: fly sh in non-mended re soil (A tretment) were removed negligily. The ompost or vermiompost whih were pplied into the soil of non-plnted tretments (CA nd VA) seprtely deresed the totl PAH ontent in soil signifintly in omprison to the non-mended tretment (A) in the rnge etween %. The phytoremedition of PAHs in sh-soil (PA tretment) showed tht the mize hs signifintly higher ility to remove sh-pahs thn the CA nd VA tretments euse the sum of totl PAH ontent ws removed y 26.7%. The totl PAH ontent in the plnted soil mended with ompost nd vermiompost (PCA nd PVA tretments) deresed y 62.9% nd 64.9%, respetively. However, there were no signifint differenes (P <.5) etween the ompost nd vermiompost mendment on the removl of totl sh-pahs. The higher PAH removl in PCA nd PVA tretments thn in other tretments indited tht the mize plnts ould stimulte the growth nd tivity of soil utohthonous miroorgnism involved in PAH degrdtion due to the prodution of exudtes relesed in mize rhizosphere s ws reported y Nnekr et l. (215). Moreover, the ompost or vermiompost used together with mize ould stimulte the tivity of soil utohthonous PAH degrders whih ould e supported y PAH degrders ugmented to soil from the mendments. Furthermore, the inorportion of these orgni mterils ould support the PAH removl y the irreversile trpping proesses of PAHs in soil s ws desried y Ouvrrd et l. (214). This study showed tht the mize ultivtion on PAH ontminted soil mended with the ompost nd vermiompost s seprtely pplied mendments were the most effiient ioremedition pprohes of soil ontminted y PAHs of sh origin. The resulted residul PAH ontents in PCA (587.4 µg/kg DW) nd PVA (565.6 µg/kg DW) were signifintly lower thn the limit of totl PAHs (1 µg/kg DW) for soils required y the Ministry of the Environment of the Czeh Repuli (216). Moreover, the hrvested oveground iomss of mize did not represent ny environmentl risk. REFERENCES Enell A., Fuhrmn F., Lundin L., Wrfvinge P., Thelin G. (28): Polyyli romti hydrorons in sh: Determintion of totl nd lehle onentrtions. Environmentl Pollution, 152: Dvořák T., Száková J., Vondráčková S., Košnář Z., Holečková Z., Njmnová J., Tlustoš P. (217): Content of inorgni nd orgni pollutnts nd their moility in ottom sediment from the Orlík wter reservoir (Vltv river, Czeh Repuli). Soil nd Sediment Contmintion: An Interntionl Journl, 26: Feng L.J., Zhng L.Q., Feng L. (214): Dissiption of polyyli romti hydrorons in soil mended with sewge sludge ompost. Interntionl Biodeteriortion nd Biodegrdtion, 95 (Prt A): Hrt J., Tlustoš P., Hnč A., Švehl P., Váň J., Tluk P., Jelínek F. (21): The role of ertion intensity, temperture regimes nd omposting mixture on gseous emission during omposting. Compost Siene nd Utiliztion, 18: Hnč A., Částková T., Kužel S., Cjthml T. (217): Dynmis of vertil-flow windrow vermiomposting system. Wste Mngement nd Reserh, 35: Go Y., Li Q., Ling W., Zhu X. (211): Arusulr myorrhizl phytoremedition of soils ontminted with phennthrene nd pyrene. Journl of Hzrdous Mterils, 185: Grí-Sánhez M., Košnář Z., Merl F., Arnd E., Tlustoš P. (218): A omprtive study to evlute nturl ttenution, myougmenttion, phytoremedition, nd miroil-ssisted phytoremedition strtegies for the ioremedition of n ged PAH-polluted soil. Eotoxiology nd Environmentl Sfety, 147: Guo M.X., Gong Z.Q., Mio R.H., Su D., Li X.J., Ji C.Y., Zhung J. (217): The influene of root exudtes of mize nd soyen on polyyli romti hydrorons degrdtion nd soil teril ommunity struture. Eologil Engineering, 99: Kálková L., Tlustoš P. (211): The uptke of persistent orgni pollutnts y plnts. Centrl Europen Journl of Biology, 6: Košnář Z., Merl F., Perná I., Tlustoš P. (216): Investigtion of polyyli romti hydroron ontent in fly sh nd ottom sh of iomss ininertion plnts in reltion to the operting temperture nd unurned ron ontent. Siene of the Totl Environment, : Lio C., Ling X., Lu G., Thi T., Xu W., Dng Z. (215): Effet of surftnt mendment to PAHs-ontminted soil for phytoremedition y mize (Ze mys L.). Eotoxiology nd Environmentl Sfety, 112: 1 6. Msto R.E., Srkr E., George J., Jyoti K., Dutt P., Rm L.C. (215): PAHs nd potentilly toxi elements in the fly sh nd ed sh of iomss fired power plnts. Fuel Proessing Tehnology, 132: Merl F., Tejneký V., Száková J., Tlustoš P. (216): Nutrient dynmis in soil solution nd whet response fter iomss sh mendments. Agronomy Journl, 18:

7 Plnt Soil Environ. Ministry of Environment of Czeh Repuli (216): Deree No. 153/216 Coll., out the Agriulturl Soil Qulity nd Protetion Requirements. Legl Code of the Czeh Repuli, (In Czeh) Nnekr S., Dhote M., Kshyp S., Singh S.K., Juwrkr A.A. (215): Miroe ssisted phytoremedition of oil sludge nd role of mendments: A mesoosm study. Interntionl Journl of Environmentl Siene nd Tehnology, 12: Oheová P., Merl F., Košnář Z., Tlustoš P. (217): Fertiliztion effiieny of wood sh pellets mended y gypsum nd superphosphte in the ryegrss growth. Plnt, Soil nd Environment, 63: Ouvrrd S., Leglize P., Morel J.L. (214): PAH phytoremedition: Rhizodegrdtion or rhizottenution? Interntionl Journl of Phytoremedition, 16: Pris A., Leduphin J., Poinot P., Gillrd J.L. (218): Polyyli romti hydrorons in fruits nd vegetles: Origin, nlysis, nd ourrene. Environmentl Pollution, 234: US EPA (1996): Method 363C: Sili Gel Clenup, prt of Test Methods for Evluting Solid wste, Physil/Chemil Methods. Wshinghton, EPA Pulition SW-846. US EPA (27): Method 355C: Ultrsoni Extrtion, prt of Test Methods for Evluting Solid wste, Physil/Chemil Methods. Wshinghton, EPA Pulition SW-846. US EPA (214): Method 827D: Semivoltile orgni ompounds y gs hromtogrphy/mss spetrosopy, prt of Test Methods for Evluting Solid wste, Physil/Chemil Methods. Wshinghton,EPA Pulition SW-846. Váh R., Horváthová V., Vysloužilová M. (25): The pplition of sludge on griulturlly used soils nd the prolem of persistent orgni pollutnts. Plnt, Soil nd Environment, 51: Wng K., Zhng J., Zhu Z.Q., Hung H., Li T.Q., He Z.L., Yng X., Alv A. (212): Pig mnure vermiompost (PMVC) n improve phytoremedition of Cd nd PAHs o-ontminted soil y Sedum lfreidii. Journl of Soils nd Sediments, 12: Reeived on Jnury 16, 218 Aepted on Jnury 29, 218 Pulished online on Ferury 6,