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Page 1: Effects of micro-nano and non micro-nano MSWI ashes addition on MSW anaerobic digestion

Bioresource Technology 114 (2012) 90–94

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Bioresource Technology

journal homepage: www.elsevier .com/locate /bior tech

Effects of micro-nano and non micro-nano MSWI ashes addition on MSWanaerobic digestion

H.M. Lo a,⇑, H.Y. Chiu a, S.W. Lo a, F.C. Lo b

a Department of Environmental Engineering and Management, Chaoyang University of Technology, 168, Gifeng E. Rd., Wufeng District, Taichung 41349, Taiwan, ROCb Department of Occupational Safety and Health, China Medical University, 91 Hsueh-Shih Rd., Taichung 40402, Taiwan, ROC

a r t i c l e i n f o a b s t r a c t

Article history:Received 3 December 2011Received in revised form 29 February 2012Accepted 2 March 2012Available online 9 March 2012

Keywords:MSWMSWI ashesAnaerobic digestionMicro-nano scaleMetals

0960-8524/$ - see front matter � 2012 Elsevier Ltd. Ahttp://dx.doi.org/10.1016/j.biortech.2012.03.002

⇑ Corresponding author. Tel.: +886 4 23323000x44E-mail address: [email protected] (H.M. Lo).

This study aims at investigating the effects of micro-nano municipal solid waste (MSW) incinerator(MSWI) fly ash (FA) and bottom ash (BA) on the MSW anaerobic digestion. Results showed that suitablemicro-nano and non micro-nano MSWI ashes addition (FA/MSW 3, 6, 18 and 30 g g�1 VS and BA/MSW 12,36, 60 and 120 g g�1 VS) could enhance the biogas production compared to the control. It was particularlyfound to have the highest biogas production at the micro-nano MSWI BA/MSW ratio of 36 g g�1 VS(�193 mL g�1 VS MSW, �3.5 times to the control). Micro-nano MSWI FA and BA added bioreactorshad the higher biogas production than the corresponding non micro-nano MSWI FA and BA added ones.Suitable MSWI ashes addition could improve the biogas production due to the released metals levels suit-able for the MSW anaerobic digestion particularly found in the micro-nano added bioreactors.

� 2012 Elsevier Ltd. All rights reserved.

1. Introduction

Municipal solid waste (MSW) has been mainly treated by MSWincinerator (MSWI) while partly treated by landfilling, resourcerecovery, composting and gasification in Taiwan. The MSWI couldreduce the MSW volume and have the potential co-generation ben-efit of the steam and electricity while it also produces the residuessuch as bottom ash (BA) and fly ash (FA). MSWI BA and FA were re-ported to contain various metals and recalcitrant organic com-pounds such as polycyclic aromatic hydrocarbons (PAHs) andpolychlorinated dibenzodioxins/furans (PCDD/Fs). Both BA and FAcould be used as aggregate, backfill, soil amendment and cementadditives after careful pretreatment, toxicity and TCLP test (Linand Chen, 2006).

Studies on BA or FA on co-disposal or co-digestion with MSWwere few (Lo et al., 2010, 2009; Lo and Liao, 2007; Boni et al.,2007). MSWI BA and FA addition might release various metals lev-els resulting to the potentially beneficial or detrimental effects onthe MSW anaerobic digestion (Lo et al., 2009). However, beneficialfacilitation of MSW biodegradation by ash addition was still notwell understood. Similar investigations were also reported thatmetals of different levels might stimulate or inhibit the organicsubstrate anaerobic digestion and fermentation process (Fermosoet al., 2009; Chen et al., 2008; Yuan et al., 2009; Tan et al., 2009;Altas�, 2009; Li and Fang, 2007; Lin and Shei, 2008; Yue et al.,

ll rights reserved.

69; fax: +886 4 23742365.

2007; Kuo and Genthner, 1996; Gikas, 2007; Kida et al., 2001;Ma et al., 2009; Worm et al. 2009). Recently, Lo et al. (2012) haveincorporated the above research and reported the new results thatsuitable levels of several individual metals could enhance the MSWanaerobic digestion. On the other hand, PAHs and PCDD/Fs ofMSWI ashes and their release were investigated by severalresearchers and their adsorption by adsorbents and biodegradationby microorganisms were also reported (Wyrzykowska et al., 2009;Lin et al., 2008; Yasuhara and Katami, 2007; Wang et al., 2010;Ham et al., 2008; Liu et al., 2008; Nam et al., 2005; Shitamuraet al., 2005; Oleszczuk, 2009).

Nanotechnology has been evolved to be an attractive option inengineering and environmental science. Mu and Chen (2011) hasreported that the presence of 1 mg g�1-TSS of ZnO nanoparticles(NPs) did not affect methane production of waste activated sludge,but 30 and 150 mg g�1-TSS of ZnO NPs induced 18.3% and 75.1% ofinhibition, respectively. Mu et al. (2011) has also investigated themetal oxide nanoparticles (TiO2, Al2O3, SiO2 and ZnO) on wasteactivated sludge anaerobic digestion. Nano-TiO2, nano-Al2O3 andnano-SiO2 in doses up to 150 milligram per gram total suspendedsolids (mg g�1-TSS) showed no inhibitory effect, whereas nano-ZnO showed inhibitory effect with its dosages increased. The meth-ane generation was the same as that in the control when in thepresence of 6 mg g�1-TSS of nano-ZnO, however, which decreasedrespectively to 77.2% and 18.9% of the control at 30 and150 mg g�1-TSS. The released Zn2+ from nano-ZnO was an impor-tant reason for its inhibitory effect on methane generation. Luna-delRisco et al. (2011) found that particle size of CuO and ZnO could

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Table 1Elemental values and carbon to nitrogen ratios between synthetic, Taichung city and Taiwan MSW.

Analyzed items C (%) H (%) O (%) N (%) S (%) Cl (%) P (%) K (%) C/N ratio

Synthetic MSW 46 6 41 1.4 – – – – 32.86Taichung city MSW 20.55 3.06 18.53 0.50 0.47 0.0625 0.1402 0.125 41.1Taiwan MSW 17.38 – – 0.47 0.5 0.07 – – 39.68

Table 2Basic characteristics of organic MSW and anaerobic sludge seeding.

Organic MSW Anaerobic sludge seeding

pH 7.90 ± 0.22 6.86 ± 0.09ORP (mV) 72.70 ± 4.52 17.25 ± 1.34EC (mS/cm) 0.34 ± 0.01 1.96 ± 0.05TS (%) 5.59 ± 0.19 2.78 ± 0.39VS (%) 3.96 ± 0.34 0.74 ± 0.40Ca (mg g�1) 110.03 ± 0.30 12.99 ± 0.55Mg (mg g�1) 7.84 ± 0.13 2.25 ± 0.15K (mg g�1) 65.31 ± 0.01 2.20 ± 0.07Na (mg g�1) 14.98 ± 0.80 0.69 ± 0.03Cd (mg g�1) 0.10 ± 0.05 0.01 ± 0.00Cr (mg g�1) 0.28 ± 0.04 0.11 ± 0.02Cu (mg g�1) 0.12 ± 0.03 0.20 ± 0.04Ni (mg g�1) 0.07 ± 0.00 0.06 ± 0.00Pb (mg g�1) 2.53 ± 0.10 0.07 ± 0.00Zn (mg g�1) 5.16 ± 0.35 1.34 ± 0.12

H.M. Lo et al. / Bioresource Technology 114 (2012) 90–94 91

affect the cattle manure anaerobic digestion. Biogas productionwas severely affected at concentrations of bulk and nanoparticlesover 120 and 15 mg L�1 for CuO and 240 and 120 mg L�1 for ZnO,respectively. EC50 concentrations for methane inhibition were esti-mated to be 129 mg Cu L�1 for bulk CuO, 10.7 mg Cu L�1 for nanoCuO, 101 mg Zn L�1 for bulk ZnO and 57.4 mg Zn L�1 for nano ZnO.

So far the investigations using BA or FA (containing metal oxi-des and other compounds) for co-digestion or co-disposal withMSW have rarely undertaken (Lo et al., 2009; Lo and Liao, 2007;Boni et al., 2007). Using metal oxides for co-digestion with organicsubstrate are also few. Only some anaerobic digestion of sludgeand manure with metal oxide addition were reported (Mu andChen, 2011; Mu et al., 2011; Luna-delRisco et al., 2011).

This work investigated the effects of various dose of micro-nanoand non micro-nano MSWI FA and BA on the anaerobic co-diges-tion of MSW and MSWI ashes that might provide the useful infor-mation for the MSW anaerobic digestion.

2. Methods

2.1. Materials

MSWI FA and BA were obtained from an incinerator located incentral Taiwan. Micro-nano (ground by ball mill, RETSCH, PM100) and non micro-nano MSWI ashes properties of metal com-pounds and image by XRD (PANalytical X’Pert Pro MRD) andFE-SEM (JEOL JSM-6700F) and micro-nano MSWI ashes distribu-tion by high performance particle sizer (HPPS, HPP5001, Malvern)can be found from Fig. S-1–S-5, respectively. Figure S-1 showed theXRD plot of MSWI FA, micro-nano MSWI FA, MSWI BA and micro-nano MSWI BA. XRD plot of Figure S-1 showed to contain Al2O3,CaCO3, Ca(OH)2, SiO2, Ca3SiO5, CaMg(CO3)2, Ca2SiO4, PbO and ZnSfor all MSWI BA and FA. CaO, Al2O3, SiO2 were mostly found inMSWI FA and BA. Figure S-2 showed the FE-SEM image of un-ground MSWI FA and BA while Figure S-3 showed the FE-SEM im-age of ground micro-nano MSWI FA and BA. Results of FE-SEMshowed that ground micro-nano MSWI BA (Fig. S-3f) had the po-tential to agglomerate compared to unground ones (Fig. S-2f).Ground micro-nano MSWI FA (Fig. S-3c) had more needle shapethan unground ones (Fig. S-2c). Figure S-4B showed that particle

size distributions of micro-nano MSWI FA were 83, 2 and 15% for0.4–106, 106–1110 and 1110–10000 nm after immediate measure-ment respectively. Figure S-4D indicated that particle size distribu-tions of micro-nano MSWI FA were 75%, 0% and 25% for 0.4–106,106–1110 and 1110–10000 nm after one day settlement respec-tively. As to micro-nano MSWI BA, Figure S-5B showed that parti-cle size distributions of micro-nano MSWI BA were 68%, 0% and32% for 0.4–106, 106–1110 and 1110–10000 nm after immediatemeasurement respectively while Figure S-5D indicated that thoseof micro-nano MSWI BA were 55, 8% and 37% for 0.4–106, 106–1110 and 1110–10000 nm after one day settlement respectively.MSWI FA had higher amount of 0.4–106 nm than MSWI BA.

Particle size distribution and chemical compositions such asmetal element, metal compounds and PAHs/PCDD(Fs) can be seenin Table S-1 and Table S-2. Table S-1 showed the particle size range(lm) and individual ratio (%) of BA and FA from some reports (Loet al., 2005; Wey et al., 2006; Huang and Huang, 2008). It also pre-sented the particle size distribution of micro-nano MSWI BA andMSWI FA investigated in this study. Table S-2 presented the metalscontent, LOI (loss of ignition), pH and PAHs by this investigationand dl-PCBs, PBDD/Fs, PCDD/Fs, PAHs and metals oxides from liter-atures as indicated in superscript number. Table S-3 indicated thebioreactors type, analyzed items and frequency and the requiredbioreactors for experiment. Table S-4 reported the metals levelsin the various ashes and control bioreactors that might affect theinhibition or stimulation of MSW anaerobic digestion.

Physical and chemical components of MSW and anaerobicsludge seeding from Fu-Tien located in Taichung city were as de-scribed by Lo et al. (2009). Major elements of organic MSW suchas C, H, O, N etc. were measured by elemental analyzer (HeraeusvarioIII-NCH). C, H, O and N were measured to be about 46%, 6%,41% and 1.4% (C38.3H60O25.63N) respectively. MSW and sludge seed-ing were measured to have TS �5.5% (VS �4%) and TS �3% (VS�1%) respectively. Table 1 and Table 2 showed the basic character-istics of MSW and sludge seeding. Table 1 showed that Taichungcity and Taiwan MSW had the close C(%), N(%), S(%), Cl(%) valuesof about 20.55 and 17.38, 0.50 and 0.47, 0.47 and 0.5, 0.0625 and0.07 respectively. C (46%) and N (1.4%) of synthetic MSW showedhigher compared to those of Taichung city and Taiwan MSW. How-ever, C/N ratios of Taichung city, Taiwan and synthetic MSW werefound to have close values in the order of 41.1, 39.68 and 32.86suitable for anaerobic digestion.

3. Experimental

Anaerobic reactors were 500 mL plastic bottle each containing350 mL MSW and 150 mL anaerobic sludge seeding admixture.Adding ratios for MSWI FA (FA) and micro-nano FA (MNFA) were0.12, 3, 6, 18 and 30 g g�1 VS while those for MSWI BA (BA) and mi-cro-nano BA (MNBA) were 0.6, 12, 36, 60 and 120 g g�1 VS respec-tively. Anaerobic reactors without ashes addition were conductedas the control. All anaerobic reactors were carried out with dupli-cate. Briefly speaking, 2 reactors (1�2 = 2) were used to measurethe biogas production per day while 12 reactors (6�2 = 12) for eachadded ratio were sacrificed to analyze the pH, ORP, EC, salinity, VSand metals in filtrate at day 0, 10, 20, 30, 50 and 90. Detailed anal-ysis frequency can be seen in Table S-3. All anaerobic reactors were

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Various ashes added and control anaerobic reactors

MNFA0.12MNFA3

MNFA6

MNFA18

MNFA30FA0.12

FA3FA6

FA18FA30

MNBA0.6

MNBA12

MNBA36

MNBA60

MNBA120BA0.6

BA12BA36

BA60BA120

Control

Biog

as a

ccum

ulat

ion,

mL

g-1 V

S

0

50

100

150

200

250Day 10Day 30Day 50Day 70Day 90

Fig. 1. Biogas accumulation in various ashes added anaerobic reactors at day 10, 30, 50, 70 and 90.

92 H.M. Lo et al. / Bioresource Technology 114 (2012) 90–94

performed by batch mode without stirring and were maintained at35 �C oven suitable for anaerobic process.

Biogas production was measured by gas collector with waterreplacement method. pH, ORP, EC, salinity, VS and metals in filtrate(after 100 mL admixture membrane filtration) were measured(Table S-3) according to standard methods for the examination ofwater and wastewater (AWWA, 1995). pH, ORP and EC and salinitywere measured by pH 207 (Lutron), pH meter SP-2300 (SUNTEX)and Con 400 series (SUNTEX) respectively. TS and VS were mea-sured by 105 �C oven (DS45, Deng Yng) and 550 �C furnace (CMF304, Cheng Jang). Metals were analyzed by ICP-OES (IRIS IntrepidII, Thermal Electron Corporation). ICP-OES was set at the requiredoperational conditions. Incident energy was 1100 W and reflectiveenergy was <5 W. Observational mode of plasma was side on andthe plasma height was 14 mm. Argon was used to produce the de-sired high temperature with RF power (1150 W). Nebulizer flow(25 PSI) and auxiliary flow rate were set at 0.75 and 0.5 L min�1

respectively. Data acquisition was obtained with TEVA software(Thermo Elemental).

4. Results and discussion

4.1. Biogas production accumulation

Biogas accumulation was found higher at adding ratios of 3, 6,18 and 30 g g�1 VS for FA and MNFA while those of 12, 36, 60and 120 g g�1 VS for BA and MNBA compared to the control respec-tively (Fig. 1). It was particularly found to have the highest biogasproduction at the micro-nano MSWI BA/MSW ratio of 36 g VS�1

(�193 mL g�1 VS MSW, �3.5 times to the control). MNFA addedanaerobic reactors had the higher biogas accumulation than thecorresponding FA added ones. Similarly, MNBA added anaerobicreactors showed the higher biogas accumulation than the corre-sponding BA added ones. It is also noted that MNBA 36, MNBA60 and BA 36 g g�1 VS added anaerobic reactors showed to havecomparative higher biogas accumulation than other ashes addedones. MSW at most anaerobic reactors were found almost to reachits highest biodegradation after 50 days operation.

4.2. Anaerobic parameters

Anaerobic parameters of pH, ORP, EC and salinity for MSWanaerobic digestion in the bioreactors were measured (Fig. 2).Results showed that most pH, ORP, EC and salinity were found inthe range of �4.8 to �10.1, ��190 to �110 mV, �1.8 to�7.8 ms cm�1, �0.6 to �4.2 respectively.

Most pHs in all bioreactors were found to be suitable for anaer-obic digestion (pH 6.5–7.5) although the higher pHs were found inthe initial higher MNBA 120, BA 60 and BA 120 g g�1 VS addedanaerobic reactors. On the other hand, ORPs had lower values atMNBA 120 and BA 60 and BA 120 g g�1 VS added anaerobic reac-tors. EC and salinity showed to have similar trends at all bioreac-tors. Higher ashes added bioreactors were found to have higherEC and salinity. This result might be attributed to the higher ashesaddition leading to the higher metals and anions release causingthe higher EC and salinity.

4.3. Metals levels effects on MSW anaerobic digestion

Apart from anaerobic parameters, released metals such as alkalimetals, heavy metals and trace metals in leachate from ashesadded and control bioreactors were analyzed (Fig. S-6, Table S-4).Most alkali metals of Ca, Mg, K and Na were found to have higherreleased levels particularly found in the higher ashes added biore-actor. This phenomenon reflected the facts that higher ashes dosecould release higher amount of alkali metals and anions leading toa potential higher EC and salinity values. In addition, those re-leased alkali metals levels appeared to show MSW anaerobic diges-tion stimulation rather than inhibition compared to the literaturedata (Table S-4). Except Ca, Mg, K and Na, the Fe, Si, Mn, B, Al,Ta, Ba and W were found to show comparatively higher levelsaccounting for fifth to twelfth order compared to all other metals.All other 17 metals showed to have lower levels less than 1 mg/L(Fig. S-6, Table S-4).

Suitable levels of alkali metals, heavy metals and trace metalswere reported to have the potential to enhance the microbial activ-ity and stimulate the anaerobic digestion and fermentation process

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Various ashes added and control anaerobic reactors

MNFA0.12MNFA3

MNFA6

MNFA18

MNFA30FA0.12

FA3FA6

FA18FA30

MNBA0.6

MNBA12

MNBA36

MNBA60

MNBA120BA0.6

BA12BA36

BA60BA120

Control

pH

4

5

6

7

8

9

10

11

Various ashes added and control anaerobic reactorsMNFA0.12

MNFA3MNFA6

MNFA18

MNFA30FA0.12

FA3FA6

FA18FA30

MNBA0.6

MNBA12

MNBA36

MNBA60

MNBA120BA0.6

BA12BA36

BA60BA120

Control

OR

P, m

V

-250

-200

-150

-100

-50

0

50

100

150

Various ashes added and control anaerobic reactors

MNFA0.12MNFA3

MNFA6

MNFA18

MNFA30FA0.12

FA3FA6

FA18FA30

MNBA0.6

MNBA12

MNBA36

MNBA60

MNBA120BA0.6

BA12BA36

BA60BA120

Control

EC

, mS

/cm

0

2

4

6

8

10

Various ashes added and control anaerobic reactors

MNFA0.12MNFA3

MNFA6

MNFA18

MNFA30FA0.12

FA3FA6

FA18FA30

MNBA0.6

MNBA12

MNBA36

MNBA60

MNBA120BA0.6

BA12BA36

BA60BA120

Control

Sal

inity

0

1

2

3

4

5

Fig. 2. pH, ORP, EC and salinity in various ashes added anaerobic reactors at day 0, 10, 20, 30, 50 and 90.

H.M. Lo et al. / Bioresource Technology 114 (2012) 90–94 93

(Lo et al., 2012, 2010, 2009; Fermoso et al., 2009; Chen et al., 2008;Yuan et al., 2009; Tan et al., 2009; Altas�, 2009; Li and Fang, 2007;Lin and Shei, 2008; Yue et al., 2007; Ma et al., 2009; Worm et al.,2009) as listed in Table S-4. Those levels in the control and ashesdosed bioreactors were found to have potential stimulation ratherthan inhibition particularly occurred in the ashes dosed bioreactors(MNFA3, MNFA6, MNFA18, MNFA30, FA3, FA6, FA18, FA30,MNBA12, MNBA36, MNBA60, MNBA120, BA12, BA36, BA60,BA120) (Fig. 1, Table S-4). The biogas accumulation and VS reduc-tion can also be found in Fig. S-7.

Some studies were reported that metal oxides nanoparticlessuch as TiO2, Al2O3, SiO2, ZnO and CuO could affect the activatedsludge and cattle manure anaerobic digestion (Mu and Chen,2011; Mu et al., 2011; Luna-delRisco et al., 2011). Mu and Chen(2011) reported that 30 and 150 mg g�1-TSS of ZnO nanoparticlescould induce 18.3% and 75.1% anaerobic digestion inhibition ofwaste activated sludge, respectively. However, it showed no inhib-itory effect at 1 mg g�1-TSS of ZnO. Mu et al. (2011) also reportedthat nano-TiO2, nano-Al2O3 and nano-SiO2 in doses up to150 mg g�1-TSS and nano-ZnO 6 mg g�1-TSS had no effect onanaerobic digestion. However, nano-ZnO 30 and 50 mg g�1-TSS de-creased biogas production respectively to 77.2% and 18.9% of thecontrol. Released Zn level from nano-ZnO was thought to be thekey factor for the methane generation inhibition. Luna-delRiscoet al. (2011) indicated that biogas production was severely affectedat concentrations of bulk and nanoparticles over 120 and15 mg L�1 for CuO and 240 and 120 mg L�1 for ZnO, respectively.EC50 concentrations for methane inhibition were estimated to be129 mg Cu L�1 for bulk CuO, 10.7 mg Cu L�1 for nano CuO,

101 mg Zn L�1 for bulk ZnO and 57.4 mg Zn L�1 for nano ZnO. Inthis study, released levels (Fig. S-4) from MSWI ashes (micro-nanoand non micro-nano scale) containing Al2O3, CaCO3, Ca(OH)2, SiO2,Ca3SiO5, CaMg(CO3)2, Ca2SiO4, PbO and ZnS by XRD analysisappeared to show stimulation (Fig. 1) rather than inhibition atthe ashes dosed bioreactors (MNFA3, MNFA6, MNFA18, MNFA30,FA3, FA6, FA18, FA30, MNBA12, MNBA36, MNBA60, MNBA120,BA12, BA36, BA60, BA120) (Table S-4). Micro-nano ashes addedbioreactors also showed to have the higher biogas production thanthe corresponding non micro-nano ashes added ones. This resultmight be attributed to be the micro-nano ashes agglomerationsuitable for more microorganisms’ habitat therefore enhancingthe biogas production. It is noted that individual and combinedmetals effects on anaerobic digestion might be conducted for fur-ther detailed understanding of MSWI ashes and metal oxides onsludge and MSW anaerobic digestion.

5. Conclusions

Biogas production was enhanced by suitable MSWI ashes addi-tion that might release suitable metals levels beneficial for the in-crease of biogas production particularly found at same ratios ofmicro-nano ashes addition compared to control. MNBA 36 anaero-bic reactors were found to have the highest biogas productioncompared to other ones. Trace compounds such as PAHs andPCDD/Fs were reported to be adsorbed onto MSW and sludgeadmixture indicating no harm for the anaerobic digestion. It is con-cluded that suitable MSWI ashes addition could stimulate the

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94 H.M. Lo et al. / Bioresource Technology 114 (2012) 90–94

anaerobic digestion and enhance the biogas production particularfound in the micro-nano MSWI ashes addition.

Acknowledgements

The authors are grateful to The National Science of Council ofTaiwan (R.O.C) for providing research grant No. NSC 94-2211-E-324-003.

Appendix A. Supplementary data

Supplementary data associated with this article can be found, inthe online version, at http://dx.doi.org/10.1016/j.biortech.2012.03.002.

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