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Bioresource Technology 99 (2008) 33543364

Anaerobic co-digestion of mechanically biologically treated municipal waste with primary sewage sludge A feasibility study
Ole Pahl
a

a,*

, Anna Firth b, Iain MacLeod a, Jim Baird

Caledonian Environment Centre, School of the Built and Natural Environment, Glasgow Caledonian University, Glasgow G4 0BA, UK b Scottish Water, 55 Buckstone Terrace, Edinburgh EH10 6XH, UK Received 18 May 2005; received in revised form 23 May 2007; accepted 14 August 2007 Available online 27 September 2007

Abstract This bench scale study investigated the suitability of MBT material for treatment by anaerobic digestion and the impacts of co-digestion of these wastes with sewage sludge. The results suggest that MBT material is amenable to anaerobic digestion with sewage sludge. The main problems for scale-up are related to the physical composition of the MBT material, the accumulation of heavy metals and other inert contaminants and the impact of both of these factors on nal sludge quality. Full-scale trials would be required to assess the long-term impacts of MBT waste on anaerobic digestion, if this form of co-digestion were to be pursued. The material contamination that presents a barrier to the direct recycling of MBT material in land-applications is also a major hurdle in commercial co-digestion. Better quality input material would be likely to result in higher methane yields and fewer restrictions on the utilisation of the product in recycling. 2007 Elsevier Ltd. All rights reserved.
Keywords: Anaerobic digestion; Biowaste; Mechanical biological treatment (MBT); Co-digestion; Sewage

1. Introduction The Landll Directive (1999/31/EC; EU, 1999), the Scottish National Waste Plan and corresponding Area Waste Plans have fundamental implications for the development of integrated waste management strategies throughout Scotland. Of particular signicance is the statutory requirement derived from the Landll Directive to achieve a number of targets including quantied and phased diversion of biodegradable waste from landll disposal by 2020, and pre-treatment of waste prior to nal disposal by landll. The specied quantities of biodegradable municipal waste to be diverted from landll are based on recorded 1995 waste arisings and are phased over the following timescales:

reduction to 75% of baseline by 2010; reduction to 50% of baseline by 2013; reduction to 35% of baseline by 2020. These targets were supplemented by a 2006 Scottish domestic target of a reduction to 85% of baseline quantities, equivalent to 1.5 million tonnes of biodegradable municipal solid waste (MSW) being landlled, and a combined recycling and composting rate of 25%. Whilst this initial domestic target was achieved, the increasingly stringent Landll Directive targets may pose a real problem for the Scottish waste management sector. Strategies designed to maximise the diversion and treatment of biodegradable waste from the municipal waste stream have the potential to deliver these targets, and generally are based on 60% biodegradable waste content in a typical MSW sample. Against this background, a number of local authorities have been committed to mixed waste composting technologies via mechanical biological treatment (MBT). This covers a range of technologies designed to process mixed

Corresponding author. Tel.: +44 141 331 3572; fax: +44 141 331 3570. E-mail address: o.pahl@gcal.ac.uk (O. Pahl).

0960-8524/$ - see front matter 2007 Elsevier Ltd. All rights reserved. doi:10.1016/j.biortech.2007.08.027

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wastes by composting; the primary purpose is to reduce and stabilise the organic fraction within the municipal solid waste (MSW). Specications for the use of biostabilised waste have been the subject of various reviews in recent years (Brinton, 2000; EU, 2001; GET, 2003; SEPA, 2004), and an important distinction is drawn between source-segregated green-wastes and residual or mixed waste which is subject to MBT. One particular feature of MBT systems in place in Scotland is a short but intense in-vessel composting phase followed by longer-term maturation in open windrows. As a consequence, the material retains a considerable amount of biodegradable material after the initial intensive aerobic treatment. Alternatives to this long-term aerobic maturation could be possible depending on the residual biodegradability. Whilst aerobic treatment via composting or MBT is aimed mainly at reduction in biomass and concentration and enhancement of fertiliser/soil improver value, there is also use of anaerobic digestion (AD) in the treatment of organic (fraction of) wastes. The benet of AD is that some of the energetic value of the removed biomass can be utilised in the form of biogas (Rao and Singh, 2004). AD also allows for cost-eective control of pathogens (Held et al., 2002; Termorshuizen et al., 2003) through the use of the generated biogas as a fuel for pasteurisation. Given these potential benets, the use of anaerobic digestion should not be overlooked in the development of Scottish wastetreatment strategies. However, the current emphasis in infrastructure development is clearly on the composting of green waste and the mechanical biological treatment of MSW so that a short- or medium-term change-over to AD systems is unlikely. At the same time, there are currently more outlets and treatment options in place for digestate such as sewage sludge than there are for MBT material. Consequently, this study was carried out, as part of a suite of research programmes to identify the best way forward, in order to determine the suitability of MBT material for treatment by anaerobic digestion and the impact of co-digestion of sewage sludge with this material. In light of a potential future phasing out of the composting element of the MBT treatment, two types of material were tested in co-digestion, namely the mechanically pre-sorted MSW before aerobic treatment (denoted MBT educt), and the material after aerobic treatment prior to long-term maturation in open windrows (denoted MBT product). 2. Methods This study consisted of a series of tests including rapid treatability tests and bench scale co-digestion of waste with sewage sludge. 2.1. Origin and preparation of organic material The sewage sludges used for the tests were collected from Scottish Waters wastewater treatment plant at Boness, West Lothian. Primary sedimentation sludge and

Table 1 Concentrations tested using rapid test method (ml) # 1 2 3 4 5 6

a

MBT product slurrya 0 100 200 300 400 800

Primary sludge 400 300 200 100 0 0

Digested sludge 400 400 400 400 400 0

1.5 kg of dried MBT product mixed with 1000 ml tap water.

return sludge from the aeration basins was used in the rapid treatability tests (Table 1) whereas the bench scale tests used return sludge only for seeding (3:1 return and primary sludge) followed by additions of primary sludge. The sludges were refrigerated prior to use. The MBT material was collected from Levenseat landll site, where MSW is subjected to a dry screening process employing a bag splitter, 60 mm trommel, over-band magnet and Eddy current. The remaining fraction (denoted MBT educt) is then composted in a bunker system for about 2 weeks (at this stage denoted MBT product) and subsequently moved to large, open windrows of around 3 m height, where it matures for 6 months. The matured MBT product at Levenseat undergoes a nal screening process prior to further use but, for the purpose of this study, any inert contaminants larger than approximately 5 mm were removed by hand. In preparation for particle size reduction and subsequent production of a slurry of a consistency that could be handled by the laboratory set-up, the material was partially dried at 35 C in a fan-assisted oven in layers of no more than 20 mm thickness for 24 h and reduced in particle size to pass a sieve of 2 mm mesh size (Retsch cutting mill SM100) prior to being stored; the drying temperature was limited to 35 C in order to avoid volatilisation of fatty acids. Stored material was made into a slurry with water at a ratio of 1.5 kg of partially dried material mixed with 1000 ml of tap water. The mixtures were made up in batches in sucient volume for the rapid treatability tests and the bench scale trials, and frozen until needed. This was in order to limit variability in the feedstock during preparation. The feedstock was defrosted and incubated in a water bath at 35 C before use. 2.2. Sampling routine Analysis for determinants was carried out on feedstock-, interim- (half-way through the 3 HRT digestion period) and nal sludge-samples. All analyses were conducted in accordance with the guidance on methods of sampling and analysis for determining the quality of environmental matrices given by the UK Environment Agencys National Laboratory Service (Blue Books; EA, 2007): heavy metals cadmium, copper, chromium, nickel, lead, zinc (nitric acid/atomic absorption spectrophotometry; Blue Book 49) and mercury (ameless atomic absorption spectrophotometry; Blue Book 10);

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ammonia (Nessler/spectrophotometry; Blue Book 48); total solids (gravimetric; Blue Book 83 and 105); volatile solids (gravimetric; Blue Book 83); volatile fatty acids (gas chromatography; Blue Book 21); pH (electrode; Blue Book 149).

Wasted sludge was analysed twice a week in a similar fashion but excluding heavy metal analysis. Manual particle size analysis using soil sieves of various graduations was carried out on both MBT product and educt. Biogas production rate (ml/h) and quality (CH4 and CO2 content) was measured twice/three times per week. Daily measurements of temperature were also taken to ensure optimum operating conditions of the digesters. After completion of the digestion period, samples of the residual sludge were collected for analysis of inert material. 2.3. Rapid treatability tests An initial set of rapid anaerobic digestion tests was carried out in order to assess the suitability of the MBT product for anaerobic co-digestion with sewage sludge. Suitability was assessed by comparison of gas production rates with those of sewage sludge only. A number of concentrations of MBT product were assessed against the controls (Table 1) in two consecutive runs. Anaerobic digestion was carried out in 1 l plastic bottles. Each bottle was lled to 800 ml with a mixture of biowaste and sewage sludge, as detailed above. Digested sludge was used in the mixture to provide a quicker start-up period than primary sludge alone. Each bottle was shaken to mix the contents thoroughly and then tted with an airtight lid and a tube to carry biogas to a collecting tube. The volume of gas collected was measured by the displacement of water from the collecting tube. The test vessels were incubated in a water bath at approximately 35 C for 5 h and the volume of gas produced recorded every hour, after gently shaking each bottle to release any gas trapped in the sludge. At this initial stage of the project (rapid treatability tests) detailed analysis of the feed material was not undertaken. 2.4. Bench scale trials The bench scale trials were carried out using 5 l Quickt vessels with 4 port lids. Each vessel was tted with a stainless steel stirrer, which was powered by a motor and stirred continuously at 60 rpm, a thermometer and a gas collection system. The fourth port was used to add and remove sludge. Due to its thick consistency, sludge additions were administered manually through the port, with a exible tube and clamp acting as gas lock. Heating tapes wrapped around the outside of each vessel were used to maintain the temperature of the digesting sludge at 35 C 3 C. Fig. 1 shows the experimental set-up, which is similar to that described by Wilkie et al. (2004).
Fig. 1. Schematic of bench scale digester set-up.

Initially, all the digesters were lled with 4 l of sewage sludge (3:1 digested and primary sludge). This was followed by a 2-week stabilisation period, during which time 500 ml of sludge was rst removed and a further 500 ml of fresh primary sludge added every 2 days. This allowed time for the experimental set-up to be checked, i.e. to ensure gas seals were intact and temperature controls were correct, and for the microbiological activity to stabilise. Following the stabilisation phase, biowaste slurry was mixed with primary sludge at dierent concentrations before the mixed sludge was added to each digester: concentrations of 0%, 12.5% and 25% MBT material were tested in duplicate, plus an extra two controls using primary sludge. Every 2 days, 500 ml of sludge was removed from each digester, before a further 500 ml of fresh sludge/sludge-biowaste mix was added. Using the feeding pattern of 500 ml feed every 2 days (excluding Saturdays and Sundays), the hydraulic retention time (HRT) of the sludge was 18.7 days. The trials were run for 3 HRTs in total. Following analysis of interim results, taken after 1.5 HRTs, it was thought that the control digesters were not performing as well as anticipated and that this was due to low-solids content of the primary sludge. Therefore, from day 12 of the second HRT onwards, feedstock mixes were made up using thicker primary sludge from alternative sources (Dalderse and Galashiels wastewater treatment works). At the end of the rst HRT, due to an accumulation of volatile fatty acids and increasing acidity in the digesters (setpoint: pH 6), 2 M Na2CO3 was added to each digester in sucient quantity to adjust the pH to within the range 6.87.8 and to increase buering capacity. Subsequently, the pH of the feed to be added was checked before addition and corrected to within this range if necessary, also using 2 M Na2CO3. At the end of the nal HRT the resultant sludge was analysed. Once the stirrers had been turned o, the

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contents were left to settle overnight. The supernatant was then removed and discarded, and the remaining sludge was mixed before composite samples from each set were collected. 2.5. Gas measurements Gas production rates were measured daily via the volume of water displaced in an inverted graduated tube lled with water (Fig. 1; amended from Blue Book #5, EA, 2007). The tube was lled under vacuum and the volume of gas collected in the tube measured after 1 h. The main purpose of the gas measurement, for this project, was to identify whether there were any dierences in gas production rates for dierent feed make-ups, rather than to assess absolute gas production rates. Given that the process was operated continuously, measurement of an hourly rate was deemed sucient to compare between dierent set-ups. Similarly, the eect of biogas solution in the liquid phase was considered negligible as it aected all vessels. Following gas volume measurement, the collecting tubes were detached from the digesters and gas collecting bags attached. Gas was collected overnight and analysed for methane and carbon dioxide content the following day using a Geotechnical Instruments GA45 Plus Infrared gas analyser. Such gas analysis was carried out 23 times per week. 3. Results and discussion 3.1. Rapid tests In both test runs, the control digesters produced the highest volume of biogas (Table 2). The second test run showed a better correlation between reduction in gas production and increase in biowaste concentration. On the basis of these results it was decided that bench scale tests would be carried out at 12.5% and 25% concentrations of
Table 2 Results of rapid test biogas production Feedstock MBT product content (%) Biogas produced (ml/h) 1st hour 50 10 0 20 5 15 65 35 30 20 15 15 2nd hour 30 25 30 20 0 15 30 10 15 10 10 10 3rd hour 0 30 15 10 0 0 30 10 15 5 5 5 4th hour 10 10 10 20 0 0 25 5 5 5 10 0 5th hour 10 10 5 5 5 5 30 5 10 0 15 0 Total (ml/5 h) 100 85 60 75 10 35 180 65 75 40 55 30

biowaste. Higher concentrations of biowaste were deemed unlikely to be suitable for co-digestion, not least due to the increasingly paste-like consistency of the mixed slurry. 3.2. Bench scale trials 3.2.1. Feedstock analysis Following initial preparation of feedstock materials, analyses were carried out for volatile solids content and heavy metal concentration of the feedstock. 3.2.1.1. Volatile solids (VS) content. Assessment of volatile solids loading rate during anaerobic digestion is important to maintain a stable digester, as an overload of organic material can lead to excessive acid production, which inhibits the activity of methanogenic bacteria. It was shown (Table 3) that the MBT waste feedstocks (both MBT product and educt) contained higher concentrations of volatile solids than the primary sludge, despite the presence of a greater proportion of total solids present as VS in primary sludge. This was due to the low concentration of total solids in the primary sludge in comparison with the sludge/ MBT mixtures. It is interesting to note that there was less dierence in the volatile solids content between MBT product and educt mixed slurries than was expected after the intense aerobic pre-treatment during the MBT process. The VS content and loading rates utilised during this project (Table 3) ranged from 36% to 71% TS and 1.9 to 3.8 g l1 d1, respectively, and were comparable to those reported in related studies on the co-digestion of the organic or source-segregated organic fraction of municipal solid waste: 5095% TS and 0.74.5 g VS l1 d1 (Davidsson et al., 2007; Angelidaki et al., 2006; Gomez et al., 2006; Hartmann and Ahring, 2005; Krupp et al., 2005; Sosnowski et al., 2003; Vogt et al., 2002). 3.2.1.2. Heavy metal concentration. For all metals except copper, metal concentrations in the mixtures containing MBT material exceeded the levels in the primary sludge but were of similar magnitude to those reported as average for the European Union (Table 4). Copper in both the 12.5% and 25% mixes of MBT was less than in primary sludge. The relatively high copper level in the primary sludge may have been due to copper pipes used for water supply and this is not an unusual level for sewage sludge.
Table 3 Volatile solids contents of feedstocks Feedstock % TS % VS (of TS) 72.4 59.1 50.6 50.5 42.6 VS content (g VS l1) 35.9 56.7 70.2 53.7 70.7 VS loading rate (g l1 d1) 1.9 3.0 3.8 2.9 3.8

Control: 0.0 12.5 25.0 38.0 50.0 100.0 Control: 0.0 12.5 25.0 38.0 50.0 100.0

Control (primary sludge) 12.5% MBT educt 25.0% MBT educt 12.5% MBT product 25.0% MBT product

5.0 9.6 13.9 10.6 16.6

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Table 4 Heavy metal contents of feedstocks (all in mg/kg TS) Feedstock type Control (primary sludge) 12.5% MBT educt 25.0% MBT educt 12.5% MBT product 25.0% MBT product EU sewage sludge (AROMIS, 2005) Cd 0.8 0.6 0.7 0.8 0.8 2.0 Cr 29 59 57 54 40 73 Cu 197 127 163 536 253 330 Pb 69 94 98 188 184 36 Ni 18 35 43 68 79 104 Zn 331 369 377 533 558 811

MBT educt, the largest proportions were glass and stones (21% and 22%, respectively). 3.2.2. Gas production and gas quality The production of biogas (Table 6) was variable throughout the duration of the trial and this may indicate that the gas collection periods should have been longer. However, average absolute gas production rates were shown to be higher for mixed substrate than for the control in all cases, except for the 25% MBT product. Here, despite containing higher levels of volatile solids, gas production was less than for the control. However, when expressed as a ratio of gas produced per mass unit of volatile solids entering the digesters (Table 6) it is clear that the control achieved the highest levels of gas production. The additions of MBT material at 12.5% resulted in a reduction in gas production of similar proportions for both MBT product and educt, and a further drop in gas production rate was observed at 25% addition of MBT material, which was more pronounced for the MBT product. The observed drop in gas production in line with increased MBT concentration could be explained by the resultant increase in TS and VS content; Rao and Singh (2004) observed a similar drop with a comparable increase in solids concentration. However, it also has to be noted that the increasing concentration of MBT material (both product and educt) used in this project led to a signicant introduction of heavy metals into the digesters (Section 3.2.4), which may have contributed to the reduced gas production rates. Overall, the gas production rates achieved (Table 6) ranged from 0.13 m3 kg1 VS (25% MBT product) to

In all cases heavy metal levels in the mixes containing MBT product were higher than in those containing MBT educt. A particularly high result of 536 mg/kg was obtained for copper concentration in the 12.5% MBT product. As the biowaste contained large quantities of solid material, this may have been due to a slug of copper present in the particulate matter. 3.2.1.3. Particle size analysis. Particle size analysis of the MBT product and educt (Table 5) showed that the MBT product contained a higher proportion of physical contaminants (75%) than the MBT educt (64%), and that around a third of physical contaminants of the MBT product were retained on a 20 mm sieve, compared with almost half of the physical contaminants for the MBT educt. It is assumed that the relatively higher content of physical contaminants in the MBT product was due to a concentration eect arising from the loss of organic material during the MBT process. The largest proportion, by weight, of the physical contaminants retained in the MBT product was glass (52% of the total sample tested). However, in the
Table 5 Result of fractionation analysis Sieve size (mm) Retained absolute (g) Sample MBT product 37.5 20.0 10.0 5.0 2.36c Panc Total Total (%) MBT educt 37.5 20.0 10.0 5.0 2.36c Panc Total Total (%)
a b c

Type of physical contaminants retained absolute (g) Physical 24.4 187.0 203.6 67.1 34.4 64.7 581.2 74.5 Glass 0.0 141.0 171.4 58.6 371.0 47.6 Metal 2.7 6.2 2.4 0 11.3 1.4 Plastic 1.1 3.9 19.4 2 26.4 3.4 Stone 20.6 35.9 10.4 6.5 73.4 9.4
b

Retained accumulative (%) Organica 0.2 8.6 21.1 50.1 67.4 100.0 Physical 4.2 36.4 71.4 82.9 88.9 100.0

Organic 0.4 16.7 24.7 57.6 34.4 64.7 198.5 25.4

24.8 203.7 228.7 124.9 68.8 129.3 780.2

22.9 278.1 211.8 100.2 46.3 49.6 708.9

16.8 62.5 79.0 48.1 23.2 24.8 254.4 35.9

5.8 215.5 132.0 52.0 23.2 24.8 453.3 63.9

0.0 97.1 38.0 15.7 150.8 21.3

0.0 54.1 3.9 16.8 74.8 10.6

0.2 15.2 10.7 0.6 26.7 3.8

5.6 49.1 79.4 18.9 153 21.6

6.6 31.2 62.2 81.1 90.3 100.0

1.3 48.8 77.9 89.4 94.5 100.0

Paper, wood, compost and dirt. Also contains ceramics and other consolidated mineral contaminants. Due to the ne nature of this material an assumption is made that it was 50% organic.

O. Pahl et al. / Bioresource Technology 99 (2008) 33543364 Table 6 Biogas production rates and quality during bench scale trials Average production of biogas l h1 (StdDev) Control (primary sludge) 12.5% MBT educt 25.0% MBT educta 12.5% MBT product 25.0% MBT product
a

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m3 kg1 VS 0.29 0.23 0.19 0.24 0.13

% CH4 (StdDev) 35 (17) 40 (20) 42 (17) 47 (11) 43 (17)

Biogas recoveryb % v/v (StdDev) 86 (13) 88 (9) 96 (6) 89 (10) 92 (9)

0.115 (81) 0.147 (120) 0.148 (108) 0.146 (93) 0.100 (101)

One of the replicates failed at an early stage in the trials. The reasons for this are not established and the data have been excluded from the results presented here. b Sum of concentration (%) of carbon dioxide and methane as an indication of analytical capture of main biogas constituents.

0.29 m3 kg1 VS (control) and are therefore comparable to similar data reported elsewhere, which range from 0.1 to 0.7 m3 kg1 VS (Davidsson et al., 2007; Hartmann and Ahring, 2005; Rao and Singh, 2004; Sosnowski et al., 2003). It should be noted that the data reported here relate to anaerobic digestion of aerobically pre-treated material and utilised mechanical sorting where reference data was obtained using source-separated organic fraction only of MSW (OF-MSW), and this may explain why gas production rates observed here were at the lower end of the range observed elsewhere. However, the methane content of the biogas was variable and low in all cases: 4050% methane in biogas compared to 5570% reported elsewhere (Davidsson et al., 2007; Hartmann and Ahring, 2005; Rao and Singh, 2004; Sosnowski et al., 2003). The methanogenic bacteria, which convert acetate and carbon dioxide to methane, are the most sensitive group of bacteria in the process. The results seem to suggest that the high concentrations of heavy metals (Section 3.2.4) may have caused the poor gas quality due to the eect on methanogenic bacteria, while the relatively low level of overall gas production may be explained by the high solids loading and the pre-digested make-up of the feedstock.

in both buering capacity and pH, from the end of the rst HRT onwards. Average concentrations of VFAs in a fullscale, healthy sewage-sludge digestion process are expected to be less than 500 mg l1 (MacBrayne, 2004); VFA concentrations observed during these trials were on average up to 10 times this value, or more. However, VFA levels in the digestion of the organic fraction of MSW have been reported in the region of several thousand mg l1 (Angelidaki et al., 2006; Gallert et al., 2003; Rao and Singh, 2004). There are conicting reports on the causes and eects of elevated levels of VFA; Burton and Turner (2003) report that VFA levels up to 10,000 mg l1 have little inhibitory eect on methanogenic activity at neutral pH levels, possibly with the exception of propionate at levels above 1000 mg l1 (McCarty and McKinney, 1961). Gallert and Winter (1999) attribute inhibitory eects to elevated levels of acetate, in addition to the eect of elevated hydrogen concentrations on syntropic metabolisms. However, hydrogen inhibition of fermentative bacteria appears not to have occurred during this project because the formation of acetic acid was similar to that of the controls. Some build-up of propionic acid was observed towards the end of the trials, so that a long-term inhibition of fermentative bacteria could not be excluded. Overall, it appears most likely that the observed accumulation of VFAs and the sub-normal methane concentrations in the biogas indicate a reduction in the activity of methanogens, most likely caused by heavy metal inhibition (Section 3.2.4). 3.2.4. Sludge quality heavy metals An accumulation of zinc, lead and nickel in the digesters was observed as the trials progressed (Table 7). This eect was most pronounced in the digesters containing MBT product (70, 250 and >220% increase, respectively) and it is suggested that metals were concentrated in the MBT product due to loss of organic material. A similar trend is also apparent for cadmium, although less pronounced. Relatively high levels of copper were detected in the initial samples and this is assumed to have been due to high concentrations present in the sewage sludge following initial set-up. Copper concentrations in the digesters containing MBT product were higher than the control in the interim and nal samples, again suggesting a concentration eect in the MBT product. Accumulation of mercury and chromium did not follow a similar pattern to that of the other metals tested. In the case of mercury, interim concentrations were lowest and initial concentrations larger than those in both interim and nal samples. High initial concentrations may suggest that most of the mercury present was contributed by the primary sludge rather than by the biowaste. For chromium, evidence of accumulation is shown as, in all cases, there was an increase in content from initial to interim and nal samples. Relative toxicities of heavy metals for anaerobic digestion have been reported (Codina et al., 1998) as Zn > Cr > Cu > Cd > Ni > Pb and absolute EC50 values (50% inhibition of microbiological activity), respectively,

3.2.3. Sludge quality volatile fatty acids Reduced activity of the methanogenic bacteria can lead to an increase in the levels of volatile fatty acids (VFAs) as well as a reduction in methane production. Although average fatty acid levels varied considerably (Fig. 2), a general trend was apparent in all digesters as concentrations of VFAs increased from low levels to higher levels through the middle period of the trials and decreased again to lower levels towards the end of the period. The reduction in VFA concentration from the mid period onwards was slightly oset by the addition of Na2CO3, and resultant increase

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Acid conc. [mg/l]

Control

20

30

40

50

60

Acid conc. [mg/l]

10000 8000 6000 4000 2000 0

0 10 20 30 40 50 60

12.5% MBT educt

Acid conc. [mg/l]

10000

25% MBT educt

8000 6000 4000 2000 0 0 10 20 30 40 50 60

Acid conc. [mg/l]

10000 8000 6000 4000 2000 0

0 10 20 30 40 50 60

12.5% MBT product

Acid conc. [mg/l]

10000 8000 6000 4000 2000 0

0 10 20 30 40 50 60

25% MBT product

Total VFA

acetic acid

propionic acid

Time [days]

Fig. 2. Average VFA levels observed in the digesters.

as 50, 50, 100, 200 and 350 mg/l (Pb not reported). With the exception of cadmium and nickel, these EC50 values were exceeded in all digesters. Zinc has the lowest EC50 and was present at high levels in all digesters. This may have inhibited the methanogenic bacteria, which are the most sensitive group of bacteria in the process, and may

be the reason for the poor gas quality results reported above. 3.2.5. Sludge quality particle size analysis Analysis of the sediment collected over the duration of the trials (Table 8) showed total solids contents in the

Table 7 Accumulation of heavy metals during bench scale digestion (all concentrations are provided in mg kg1 TS) Zinc S Control 12.5% MBT educt 25.0% MBT educta 12.5% MBT product 25.0% MBT product 566 568 563 512 532 I 487 577 500 821 766 E 595 641 671 883 912 D (%) 5 13 19 73 71 Lead S 103 111 109 96 99 I 130 176 144 288 260 E 180 199 215 337 343 D (%) 75 80 98 253 246 Nickel S 27.8 27.2 31.8 32.6 30.8 I 28.5 53.2 48.6 78.4 83.9 E 33.9 66.5 73.4 106.5 116.0 D (%) 22 144 131 227 277 Cadmium S 1.10 1.10 1.00 1.05 1.20 I 0.98 1.10 0.85 1.40 1.05 E 1.05 1.30 1.30 1.65 1.60 D (%) 5 18 30 57 33 Copper S 269 290 314 240 220 I 233 229 176 377 374 E 334 202 191 402 426 D (%) 24 30 39 67 93 Mercury S 1.51 1.58 1.74 1.09 1.57 I 1.02 1.05 0.81 0.83 0.68 E 1.07 1.04 1.45 0.90 1.13 D (%) 30 34 16 18 28 Chromium S 46.3 46.3 50.9 48.5 49.8 I 51.1 83.8 66.5 62.8 48.8 E 69.2 115.0 117.0 95.0 104.1 D (%) 49 148 130 96 109 O. Pahl et al. / Bioresource Technology 99 (2008) 33543364

Concentration of heavy metals as measured at: S = start, I = interim, E = end date; D = accumulation of heavy metals compared to start date. a End value based on single measurement only.

Table 8 Total solids, organic matter (OM) and OM-normalised heavy metal contents of digester sediment Feedstock type Control 12.5% MBT educt 25.0% MBT educt 12.5% MBT product 25.0% MBT product SEPA Limit Total solids (%) 7.2 15.3 16.2 23.1 24.3 Organic matter (% TS (StdDev)) 56.7 (0.12) 41.1 (2.12) 53.5 (12.1) 30.0 (2.75) 39.0 (2.00) Cadmium (mg kg1 OM) 1.5 1.3 1.7 1.4 1.6 <3 Chromium (mg kg1 OM) 96 117 151 81 102 <400 Copper (mg kg1 OM) 463 206 246 345 419 <200 Lead (mg kg1 OM) 249 203 277 289 337 <200 Mercury (mg kg1 OM) 1.5 1.1 1.9 0.8 1.1 <1 Nickel (mg kg1 OM) 47 68 95 91 114 <100 Zinc (mg kg1 OM) 824 653 866 757 897 <1000

Note: heavy metal limits normalised to 40% organic matter content.

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MBT digesters of between 2 and 3 times that of the control digesters, for MBT educt and product, respectively. There appeared to be little eect of the mixture MBT content (12% or 25%) on the total solids concentration in the nal sediment, whereas there was a marked dierence in organic matter content of total solids between the dierent mixtures. Surprisingly, lower levels of organic content were recorded for the 12.5% mixtures than for the respective 25% mixtures, and this may indicate more eective digestion of organic matter in the more dilute mixtures. Overall, up to 70% of total solids were found to be made up of inorganic material, and the highest inorganic content was present in the sediment of mixes containing MBT product, with less elevated levels of inorganic content found in the sediment of mixes containing MBT educt. The occurrence of physical contaminants was higher in all digesters containing biowaste than in the control digesters. This was apparent, also, from visual inspection of the accumulated sediment. 3.3. Summary of results and discussion 3.3.1. Stabilisation and biogas production During these trials there appeared to be an increase in the absolute volume of biogas produced after the addition of MBT material, with the exception of the larger addition of MBT product at 25%. However, the addition of 12.5% MBT product and educt reduced the biogas production rate, normalised to VS-added, by about 20%, while the addition of 25% MBT material resulted in signicantly reduced gas production rates: down to less than 50% of the control in the case of 25% MBT product. The gas quality data was limited, but there appeared to be no improvement or detriment to the methane content resulting from the addition of biowaste. In general, methane content was lower than that usually produced by full-size sewage-sludge digesters, which would be expected to be around 65% (MacBrayne, 2004), and also lower than that reported in other studies using OFMSW. In combination, the results (Table 6) show that comparatively poor further stabilisation of the MBT organic matter was achieved during the anaerobic digestion process, which could be expected given that the material had already been put through an aerobic treatment process. Interestingly, the observed reduction in gas production ratios (m3 kg1 VS) is equivalent to the percentage addition of MBT material (except for 25% MBT product, where it is even lower). In terms of absolute gas production, the results show that the co-digestion of MBT material with sewage sludge resulted in a higher absolute biogas yield per available digester volume for all but the 25% MBT product mixes, although feed conversion and methane production were poor compared to the control. 3.3.2. Total solids and heavy metals During the short duration of these trials two major issues were encountered: solids content and contamination with heavy metals.

An estimated 10% of the available operating capacity in the digester containing 25% MBT product was lost due to sediment build-up over the duration of the trial (51 days). The other digesters with co-digestion also showed signs of excessive sediment build-up, despite the fact that up to 50% of inorganic material in the MBT feedstock was removable by means of a 20 mm screen. Signicant improvement in the removal of this inert material prior to anaerobic digestion would be required to avoid its excessive accumulation, and wear and tear on pumps. This could be achieved via screening to 10 mm but this screen size may be too small to be feasible for application at full-scale. There was evidence of the accumulation of heavy metals in the digesters. This occurred most notably in the digesters receiving MBT product and may lead to increasing longterm toxicity to the digestion process. In particular, zinc and chromium, which are reported to have the highest levels of toxicity, were present in the MBT slurries at levels close to or in excess of reported EC50 values. There may also be concerns about nal sludge quality in terms of heavy metals, depending on the anticipated end-use of the sludge. The Scottish Environment Protection Agency position on the recycling of waste in land-application provides maximum limits for the heavy metal content of such material (SEPA, 2004). These values are normalised to 30% organic matter content in the waste material. MBT material has a lower organic matter content than sewage sludge and, ironically, this somewhat reduces the normalised concentration of heavy metals (Table 8) in cases where much of the heavy metal load originates from the sewage sludge, e.g. copper, even though this eect decreases with increasing ratio of MBT addition. For lead and nickel the addition of MBT material potentially increases the normalised concentration of heavy metals beyond the limits set by the regulator, and this means that land-application of the nal sludge is further restricted. 3.3.3. Feasibility of this form of co-digestion From the results described so far emerges an argument against the co-digestion of MBT material with sewage sludge in full-scale, commercially operated anaerobic digesters, as they are typically operated by water treatment works. The MBT material would need to be made into a slurry with water and/or sewage sludge, thus allowing the material to be conveyed in existing pipework and pumps. Still, the increasingly paste-like nature of the mixed slurry, in addition to the extra infrastructure requirement, would present a mechanical problem and, in combination with the danger of sediment build-up in the digesters, represents a major hurdle to the feasibility of this form of codigestion. The extra capital and running costs for the co-digestion of MBT material may be oset by gate fees and increases in absolute biogas yield achievable for a given digester volume. However, apart from these operational considerations, the results of this project indicate that the main

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hurdle to the feasibility of this form of co-digestion lies in the accumulation of heavy metals in the sediment. Following implementation of the Landll Directive, this material is likely to be applied to land in areas where facilities for advanced treatment such as incineration or gasication are not available (currently about 50% of Scottish sewage sludge falls into this category). The elevated level of heavy metals would eectively rule out this form of disposal or recycling and would therefore present a considerable problem for sewage treatment operators, who would have to nd other outlets for their nal sludge in an environment where the pre-existing concentrations of heavy metals already limit recycling. So, while it may be informative to collect further data on the digestibility of MBT material in co-treatment with sewage sludge and other organic waste streams, it would appear that the high level of heavy metals in the MBT material, together with the high load of inorganic material, would render commercial utilisation of this form of codigestion not feasible in practice. Signicant reductions in heavy metal concentrations are required before further investigation of this form of codigestion should be undertaken. Then, trials could include a comparison of the viability of anaerobic digestion of MBT material with that of pre-screened and pulped material, which has proved very successful in full-scale operating plants in Denmark (Evans, 2002). This would highlight the benets of screening processes on nal product quality and could tie in with other work on the design of pilot scale digesters that are suitable for the development of treatment schemes for future translation into full-scale treatment (Gallert et al., 2003). Until then, there is an urgent need to improve the quality of MBT material in terms of its heavy metal as well as inorganic content, for example via improved collection schemes, source segregation or improved mechanical treatment. However, this will take time and it can be argued that this improved MBT material should be treated directly either in composting or anaerobic digestion facilities, depending on desired end-use and material characteristics (e.g. green garden waste for composting or kitchen waste for anaerobic digestion). Thus, the co-digestion of MBT material with sewage sludge appears not to be feasible as an interim, short-term solution towards achieving the Scottish landll diversion targets. 4. Conclusions The results of this trial suggest that MBT waste is amenable to anaerobic digestion with sewage sludge at bench scale. The trial was of short duration (51 days) and the MBT material used may not have been truly representative of material which would be used at full-scale i.e. large contaminants had to be removed by hand and the remaining material milled to reduce particle size before use. The concentrations of heavy metals and inert material present a considerable barrier to commercial, full-scale

co-digestion of MBT material with sewage sludge in existing water industry installations. Improvements in collection or pre-treatment may reduce these barriers but they would also negate the need for co-digestion as an outlet route for poor quality MBT material. This form of codigestion is therefore unlikely to provide an interim solution towards achieving the Scottish landll diversion targets. Acknowledgements This research was initiated and funded by the Scottish Executive, via the Scottish REMADE project. References
Angelidaki, I., Chen, X., Cui, J., Kaparaju, P., Ellegaard, L., 2006. Thermophilic anaerobic digestion of source-sorted organic fraction of household municipal solid waste: start-up procedure for continuously stirred tank reactor. Water Research 40 (14), 26212628. AROMIS, 2005. Assessment and reduction of heavy metal input into agro-ecosystems. Final report of the EU-Concerted Action AROMIS. KTBL-Schrift 432. Kuratorium fu r Technik und Bauwesen in der Landwirtschaft e.V. (KTBL), Darmstadt, Germany, p. 47. Brinton, W.F., 2000. Compost Quality Standards and Guidelines. Woods End Research Laboratory, England, UK. Burton, C.H., Turner, C. (Eds.), 2003. Anaerobic treatment options for animal manures. In: manure management. Silsoe Research Institute, Bedford, UK, pp. 273282. ISBN 0953128261. Codina, J.C., Mun oz, M.A., Cazorla, F.M., Perez-Garcia, A., Morin igo, M.A., De Vicente, A., 1998. The inhibition of methanogenic activity from anaerobic domestic sludges as a simple toxicity bioassay. Water Research 32 (4), 13381342. ., Gruvberger, C., Christensen, T.H., Hansen, T.L., Jansen, Davidsson, A J. la C., 2007. Methane yield in source-sorted organic fraction of municipal solid waste. Waste Management 27 (3), 406414. EA, 2007. Methods for the examination of waters and associated materials (Blue Books). Standing Committee of Analysts (SCA), Environment Agency (National Laboratory Service), Rothley, Leicestershire, UK. EU, 1999. Council Directive 1999/31/EC of 26 April 1999 on the landll of waste. European Union. Ocial Journal L182, 16/07/1999, p. 0001 0019. EU, 2001. Working Document on the Biological Treatment of Biowaste, second draft. European Union, DG VII, Brussels. Evans, T., 2002. Anaerobic Digestion in Denmark. Tim Evans Environment, Ashtead, England, UK. Gallert, C., Winter, J., 1999. Bacterial metabolism in wastewater treatment systems. In: Winter, J. (Ed.), Biotechnology Environmental Processes I, 11(a). Wiley, pp. 1753. Gallert, C., Henning, A., Winter, J., 2003. Scale-up of anaerobic digestion of the biowaste fraction from domestic wastes. Water Research 37 (6), 14331441. GET, 2003. Cool Waste Management. Greenpeace Environmental Trust. ISBN 1-903907-04-7. Gomez, X., Cuetos, M.J., Cara, J., Moran, A., Garcia, A.I., 2006. Anaerobic co-digestion of primary sludge and the fruit and vegetable fraction of the municipal solid wastes. Conditions for the mixing and evaluation of the organic loading rate. Renewable Energy 31, 2017 2024. Hartmann, H., Ahring, B.K., 2005. Anaerobic digestion of the organic fraction of municipal solid waste: inuence of co-digestion with manure. Water Research 39 (8), 15431552. Held, C., Wellacher, M., Robra, K.-H., Gu bitz, G.M., 2002. Two-stage anaerobic fermentation of organic waste in CSTR and UFAFreactors. Bioresource Technology 81 (1), 1924.

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O. Pahl et al. / Bioresource Technology 99 (2008) 33543364 Sosnowski, P., Wieczorek, A., Ledakowicz, S., 2003. Anaerobic codigestion of sewage sludge and organic fraction of municipal solid wastes. Advances in Environmental Research 7 (3), 609616. Termorshuizen, A.J., Volker, D., Blok, W.J., ten Brummeler, E., Hartog, B.J., Janse, J.D., Knol, W., Wenneker, M., 2003. Survival of human and plant pathogens during anaerobic mesophilic digestion of vegetable, fruit, and garden waste. European Journal of Soil Biology 39 (3), 165171. Vogt, G.M., Liu, H.W., Kennedy, K.J., Vogt, H.S., Holbein, B.E., 2002. Super blue box recycling (SUBBOR) enhanced two-stage anaerobic digestion process for recycling municipal solid waste: laboratory pilot studies. Bioresource Technology 85, 291299. Wilkie, A.C., Smith, P.H., Bordeaux, F.M., 2004. An economical bioreactor for evaluating biogas potential of particulate biomass. Bioresource Technology 92 (1), 103109.

Krupp, M., Schubert, J., Widmann, R., 2005. Feasibility study for codigestion of sewage sludge with OFMSW on two wastewater treatment plants in Germany. Waste Management 25, 393399. MacBrayne, D., 2004. Operational parameters for Scottish Waters sewage sludge digesters, personal communication. McCarty, P.L., McKinney, R.E., 1961. Volatile acid toxicity in anaerobic digestion. Journal of Water Pollution Control Federation 33 (2), 223 232. Rao, M.S., Singh, S.P., 2004. Bioenergy conversion studies of organic fraction of MSW: kinetic studies and gas yieldorganic loading relationships for process optimisation. Bioresource Technology 95 (2), 173185. SEPA, 2004. Composting position September 2004. Scottish Environment Protection Agency Stirling, UK.