Applied Energy 111 (2013) 11721182

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Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Bioethanol production from various waste papers: Economic feasibility and sensitivity analysis
Lei Wang a,d, Mahdi Sharifzadeh c, Richard Templer b,d, Richard J. Murphy a,d,
a

Department of Life Science, Imperial College London, London SW7 2AZ, UK Department of Chemistry, Imperial College London, London SW7 2AZ, UK c Centre for Process System Engineering (CPSE), Department of Chemical Engineering, Imperial College London, London SW7 2AZ, UK d Porter Institute, Imperial College London, London SW7 2AZ, UK
b

h i g h l i g h t s
" Bioethanol produced from waste papers can be economically competitive with petrol. " Biomass feedstock cost is the main contributor to bioethanol cost. " Pre-treatments reduce the cost of bioethanol made from newspaper and ofce paper. " Increasing solids loading and enhancing fermentation can reduce bioethanol cost. " Plant capacity affects the bioethanol cost signicantly.

a r t i c l e

i n f o

a b s t r a c t
As a signicant fraction of municipal solid waste, waste paper is a potential source for producing bioethanol. In the present paper, bioethanol production from various waste papers (newspaper, ofce paper, cardboard and magazine) using an enzyme complex (Cellic Ctec 1) was evaluated from an economic standpoint. Four bases cases without pre-treatment and two state-of-the-art cases (including dilute acid pre-treatment for ofce paper and oxidative lime pre-treatment for newspaper) were constructed using laboratory experimental data, literature values, expert consultations and simulation using AspenPlus. Several scenarios were also carried out to assess the sensitivity of various technology parameters (i.e. solids loading in saccharication, anaerobic digestion and fermentation efciency, and sugar yields in pretreatment). The sensitivity analysis suggested that the economic performance of bioethanol produced from waste paper could be improved signicantly with an up to 25% reduction in minimum ethanol selling price (MESP) by increasing solids loading in saccharication and with a 6% reduction in MESP by enhancing fermentation efciency. The comparison of the bioethanol selling price at pump (reference year 2009) and the petrol price showed bioethanol produced from newspaper, ofce paper and cardboard were economically competitive with petrol. 2012 Published by Elsevier Ltd.

Article history: Received 19 January 2012 Received in revised form 24 August 2012 Accepted 26 August 2012 Available online 28 November 2012 Keywords: Waste papers Bioethanol Economic High-solids loading Enzyme production

1. Introduction Concerns over climate change effects and energy security have become prominent in public life in recent years. World energy consumption is predicted to increase by 50% to 2030 according to a prediction from the United States Energy Information Agency [1] and US retail gasoline prices have soared from 0.83 $/gallon in 2000 to 3.49 $/gallon in 2011 [2]. Such factors have stimulated the search for viable, alternative transport fuels. The UK is the third
Corresponding author at: Department of Life Science, Imperial College London, London SW7 2AZ, UK. Tel.: +44 (0)20 7594 5389; fax: +44 (0)20 7584 2056. E-mail address: r.murphy@imperial.ac.uk (R.J. Murphy).
0306-2619/$ - see front matter 2012 Published by Elsevier Ltd. http://dx.doi.org/10.1016/j.apenergy.2012.08.048

largest consumer of energy amongst the EU 27 countries, albeit with a relatively low dependency (25%) on energy imports in 2010 due to its large domestic energy production (mainly oil and gas) [3,4]. However, the share of renewable energy in the total energy consumption for the UK is relatively low as 3.3% in 2010 though progresses has been made toward the EUs Renewable Energy Directive (RED) target of 15% by 2020 [5]. Compared with the rst generation (1G) biofuel produced from food crops, second generation (2G) biofuels from lignocellulosic biomass or agricultural wastes have many advantages. For instance, most second generation biofuels are considered to be able to deliver substantial GHG emissions reductions when compared with petrol [6,7]. However, the development of 2G biofuels is also

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challenging, for example securing a low-cost and stable feedstocks, minimising land use changes caused by demand for biomass feedstocks and optimising bioethanol production technologies. Considering these challenges, waste papers as part of the degradable fraction in municipal solid waste (MSW) have potential to be a promising feedstock for bioethanol production. The reasons for this include: (1) waste papers are relatively abundant in the UK, reaching 8.8 million tons in 2008 due to reasonably efcient MSW collection and sorting systems, (2) they are economically competitive with other biomass feestocks because of the relatively low costs (average 40/ton), (3) they contain relatively high levels of carbohydrates that are potential convertible to bioethanol, (4) they are likely to be easily digestible without aggressive physical or chemical pre-treatments, (5) utilisation of waste papers for bioethanol production may offer a useful and valuable alternative route to managing these papers in addition to/as a complement to recycling. There is also a potentially available resource of waste papers in the UK because only 45% of recovered papers were recycled domestically while the remaining were exported overseas (in 2008) and in parallel the UK imported approximately 4.9 million tonnes of pulp and paper products. This reects the fact that not all recovered paper is demanded by UK paper mills because paper quality specications mean there are limits to increasing the recycled content in paper products [8] and, furthermore, (6) paper recycling technology itself has limitations, for example, effective deinking technology is needed to produce high quality paper products, paper bres can only be recycled through a limited number of cycles and recycling to paper is very difcult for waste paper that has been mixed with other organic waste (kitchen/garden waste etc.). Economic analysis has been used as a promising tool to assist the biofuels research community in identifying key cost drivers, evaluating novel technologies and assessing new process congurations. The National Renewable Energy Laboratory (NREL) in the US has developed a detailed techno-economic model for corn stover-based bioethanol production process design, to evaluate new developments and technologies [911]. The NREL model has been adapted in several studies, including the present research [1218]. In a previous study, we reported composition and high-solids loading saccharication results for various waste papers [18]. These laboratory-derived primary data have been used here to adapt the NREL corn stover-based model to a suitable process design for bioethanol production from waste papers [18]. The effects of varied feedstock, process and technology parameters on the economic analysis of ethanol from waste papers as reected in the calculated minimum ethanol selling price (MESP) are investigated in the present study. This work aims to provide a detailed economic assessment for waste papers-derived bioethanol production with sensitivity analysis and discussion on the robustness of this approach to biofuel production. 2. Materials and methods 2.1. Composition of waste papers Waste papers were collected locally in London, UK. They are (1) newspaper The London Paper previously distributed in the central London area, (2) printed ofce paper and packaging cardboard locally from Imperial College London, and (3) glossy magazine (supermarket catalogue). Their compositions were analysed in our previous study [19] in accordance with Sluiter et al. [20] and are listed in Table 1. 2.2. Saccharication of waste papers The enzyme complex used in this study, Cellic Ctec 1 (cellulolytic enzyme cocktail) was donated by Novozymes A/S, Demark.

Table 1 Composition of waste papers (All results are presented as percentages of as-received waste paper) [19]. Newspaper Moisture Glucan Xylan Galactan Mannan Arabinan Lignin Extractives CaCO3 Ash 7.25 43.78 6.59 1.76 6.78 1.73 16.82 3.65 1.98 9.49 Ofce paper 4.90 55.69 13.91 0.00 0.00 0.00 5.78 1.87 7.71 7.57 Magazine 4.40 34.35 4.51 1.89 5.42 1.74 14.19 3.30 2.52 28.83 Cardboard 5.90 49.56 7.75 1.78 4.78 1.46 14.86 2.40 3.96 9.32

Its activity was measured to be 120 FPU/ml of liquid product as supplied [21]. Waste papers were blended with water at 15% (w/w) for 10 min in a bench-top blender. Sulphuric acid was used to adjust the pH of slurry to 5.2 due to its alkalinity. High-solids loading (15% w/w) saccharications for the four types of paper were performed at laboratory scale at 50 C for 72 h using an overhead stirred reactor. Monomer sugars concentrations were detected by HPLC with a Biorad Aminex HPX-87P column operating at 80 C, water mobile phase and a ow rate of 0.6 ml/min. Sugar yields in terms of the percentage of monomer sugar released from carbohydrates were calculated. 2.3. Processes conguration Process congurations for four base cases (waste paperto-bioethanol processes) and two state-of-the-art cases (ofce paper-to-bioethanol with dilute acid pre-treatment and newspaper-to-bioethanol with oxidative lime pre-treatment) are given in Sections 2.3.1 and 2.3.2. The process parameters and the values applied in sensitivity analysis are presented in Section 2.3.3. 2.3.1. Base cases Fig. 1 shows the process design for the waste papers-to-bioethanol base cases [18]. Waste papers are unloaded, unwrapped and go through a metal removal process in the feedstock handling area (A100). In the blending area (A200), waste papers are pulped at 15% w/w solids loading in pulpers with a cycle time of 15 min (10 min blending, 5 min feeding time). The maximum capacity for this high solid content blending is 10.43 dry tonne per batch at an energy consumption of 30 kW/dry tonne [22,23]. The pulped paper slurry is then saccaharied enzymatically at 50 C for 72 h in reactors arranged as a continuous train (A300). The sugar yield data obtained experimentally was applied in developing the output from the saccharication reactor design. A recombinant bacterium Zymomonas mobilis which both ferments pentose and hexose is used in the fermentation (A400). The hydrolysate from saccharication and nutrients of corn steep liquor and diammonium phosphate (DAP) are then sent to seed incubation and fermentation tanks operated at 40 C for 36 h [9]. The conditions and nutrients loadings in seed incubation and fermentation tanks are adopted from the NREL process [9]. The bioethanol yield from glucose in the fermentation is 95% [9]. Total sugar lost due to contamination in the fermentation process was assumed to be 7% according to NREL [9]. Bioethanol from fermentation is then puried to 99.5% (w/w) using distillation, rectication and molecular sieve adsorption processes (A500). The solid cake with a moisture content below 50% obtained from the distillation bottoms via a series of press lter separations is sent to the combustion area (A800) and the liquid fraction is sent to the waste water treatment (WWT) area (A600) where biogas is produced in anaerobic digestion and water is further cleaned in

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Diammonium phosphate (DAP) Recycled water Purchased enzyme Corn steep liquor (CSL) Recycled water Z.mobilis CO2

H 2 SO4

A200 Blending
Recycled water

A300 Enzymatic hydrolysis

Steam

A400 Fermentation

Feedstock

A500 Product recovery A600 Waste water treatment

Filter separation
Liquid from distillation bottom

A100 Feedstock handling

Distillation

Biogas

Cell mass

Solid fuel

Ethanol

A900 Utilities

A800 Combustor/Boiler/Turbine

A700 Storage

Fig. 1. Schematic process ow diagram of base cases (bioethanol production from waste papers using Cellic Ctec 1, dashed boxes indicate the detailed unit processes) [18].

aerobic digestion. 37 g Of nutrients containing 90% of sodium dioxide and 10% of urea are added per kg of COD (chemical oxygen demand) [12]. The produced biogas, the solid fraction from the distillation bottoms and cell mass generated in the aerobic digestion (30 g/kg COD removed) are sent to a circulating uidized bed combustor (CFBC) operated at 870 C [9]. The heat generated is used to produce steam and electricity supplying the plant. The additional surplus electricity is sold to the National Grid. 2.3.2. Two state-of-the-art cases In the two state-of-the-art process designs, dilute acid (DA) pretreatment for ofce paper and oxidative lime (OL) pre-treatment for newspaper were selected as the relatively efcient methods after reviewing a variety of pre-treatments on paper or paperderived materials [18]. Fig. 2a and b present these two process designs with detailed illustrations in pre-treatment area (A200) and product recovery area (A500). In the ofce paper-to-bioethanol with DA pre-treatment process, shredded ofce paper is heated to 100 C in a pre-heater by the low pressure steam (4.4 atm) at an initial solids loading of 30%. The DA pre-treatment is carried out with 0.5% (w/w) H2SO4 at 220 C for 2 min [24]. Specic sugar yields data for ofce paper in DA pre-treatment was not available and, therefore, those in for DA pre-treatment of corn stover by NREL were used as surrogates. Seven percent of glucan and 75% of xylan were assumed to be converted to monomer sugars and 8% of the xylan degradated to by-products [25]. The liquid fraction from the treated slurry is detoxied by overliming and re-acidied with H2SO4 to pH 5 and then re-combined with the solid fraction and transferred to the saccharication area (A200). According to Capekmenard et al.s study [24], the sugar yields at an enzyme loading of 12.5 FPU/g glucan (equivalent to 120 mg Cellic Ctec 1 liquid product as supplied/g glucan) is increased to 91% with DA pre-treatment from 69% without pre-treatment. The process design in the product recovery area (A500) is different from that in base case. The liquid fraction from the distillation bottoms is sent to a series of evaporators (due to its relatively high content of organics), concentrated to a syrup and then sent to the combustor for heat and electricity generation. In the newspaper-to-bioethanol with OL pre-treatment, shredded newspaper is heated to 100 C at 30% solids loading prior to pre-treatment. The OL pre-treatment is operated at 140 C with 1.875% (w/w) lime (Ca(OH)2) solution under compressed air at

32 bar for 3 h [26]. According to a kinetic model of the OL pretreatment of poplar wood, 20% of lignin is estimated to be dissolved and 10% of xylan and less than 1% of glucan are estimated to become monomer sugars [27]. The liquid fraction separated from the treated slurry is injected with carbon dioxide (CO2) to precipitate CaCO3 at a recovery rate of 21% for calcium [26]. The recovered lime is modelled to go to landll and CaCl2 efuent is released to the environment after an appropriate dilution. The sugar yields from saccharication at an enzyme loading of 7.5 FPU/g glucan (equivalent to 72 mg Cellic Ctec 1 liquid product as supplied/g glucan) reach 78% with the OL pre-treatment (33% without the pretreatment) [26]. Similarly to the DA pre-treatment process, evaporators are used to produce a syrup which is sent to the combustor. 2.3.3. Sensitivity analysis on process parameters A main aim of the sensitivity analysis was to investigate the inuence of varied process parameters on the MESP calculated in the economic analysis. The process parameters considered were: (1) solids loading in saccharication, fermentation efciency, anaerobic digestion efciency for waste paper-to-bioethanol base cases without pre-treatment; (2) xylan conversion efciency in the DA pre-treatment in the state-of-the-art process for ofce paper-to-bioethanol and, (3) xylan conversion efciency and the fraction of lignin dissolved in the OL pre-treatment in the stateor-the-art process for newspaper-to-bioethanol. The process parameters and their ranges are listed in Table 2. For solids loading in saccharication, 15% (w/w) was used in the baseline scenarios. A higher level of 20% (w/w) was set in the sensitivity analysis (maximum solids loading of the pulper (18% 2% w/w)). The pulping time for this solids loading is reported as 30 min and energy consumption is 15 kW/dry tonne [22]. Ten percent (w/w) is used as a lower level of solids loading in sensitivity analysis. Sugar yields in saccharication achieved at these various solid loadings were assumed to be unchanged. For fermentation, xylose conversion efciency is reported varying from 76% to 80% while those for mannose, galactose and arabinose vary from 0% to 40% [25]. The data used in the baseline scenarios are the higher of these experimental data ranges. The minimum values used in the sensitivity analysis were the lower levels of these data range while the maximum values were all 85% release which is projected by NREL to be achievable in 2012 [9].

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(a)
A100 Feedstock handling
Steam
Office paper

A200 Dilute acid pre-treatment

Recycled H2 SO 4 water Pre-treatment Liquid Filtration Solid cake Overliming

Gypsum

Diammonium phosphate (DAP) Corn steep liquor (CSL) Recycled water Purchased enzyme Z.mobilis

CO2

Pre-steam

Filtration

A300 Enzymatic hydrolysis

A400 Fermentation

Recycled water

A900 Utilities

A600 Waste water treatment

Biogas Cell mass

Condensate

A500 Product recovery

Steam Evaporation Syrup Filtration Solid fuel Distillation Ethanol

A800 Combustor/Boiler/Turbine

A700 Storage

(b)
A100 Feedstock handling
Pre-steam
Newspaper

Recycled water

Diammonium phosphate (DAP) Corn steep liquor (CSL) Recycled water Purchased enzyme Z.mobilis

CO2

A200 Oxidative lime pre-treatment

Solid cake Pre-treatment Recycled water Lime Neutralisation HCl Filtration Re-slurry

Liquid Lime recovery Lime CaCl2

A300 Enzymatic hydrolysis

A400 Fermentation

Steam

CO2 from fermentation

Recycled water

A900 Utilities

A600 Waste water treatment

Biogas Cell mass

Condensate

A500 Product recovery

Steam Evaporation Syrup Filtration Solid fuel Distillation Ethanol

A800 Combustor/Boiler/Turbine

A700 Storage

Fig. 2. Schematic process ow diagram of state-of-the-art cases ((a) ofce paper-to-bioethanol with dilute acid pre-treatment and (b) newspaper-to-bioethanol with oxidative lime pre-treatment, dashed boxes indicate the detailed unit processes).

Table 2 Process parameters studied in sensitivity analysis. Parameter Value Min Saccharication Solid loading Fermentation Xylose fermentation efciency (%) Other sugars fermentation efciency (%) Anaerobic digestion COD removal (%) Biogas L/kg COD removed Ofce paper with dilute acid pre-treatment Xylan conversion efciency to xylose in pre-treatment (%) Newspaper with oxidative lime pre-treatment Xylan conversion efciency to xylose in pre-treatment (%) Fraction of lignin dissolved (%) 0 10 10 20 20 30 [26,27] 10 76 0 85.5 230 33 Baseline scenarios 15 80 40 87 279 75 Max 20 85 85 90 313 90 [22,28] [9,25] Reference

[2931]

[9,25]

For anaerobic digestion, efciency data from literature is summarised in Table 3. The average values of these ranges for the COD removal efciency and the biogas production rate are used in the baseline scenarios. Biogas is assumed to comprise 75% methane and 25% carbon dioxide on dry molar basis [9].

For the ofce paper with DA pre-treatment, the data range of xylan conversion efciency was adopted from the 2011 updated NREL report [25]. For newspaper with the OL pre-treatment, the data predicted by the kinetic model are in the range of 10% of experimental data [27] and this range was used in sensitivity

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Table 3 Anaerobic treatment of distillation bottoms from distilling fermented liquor from cellulosic feedstock. Biomass Wood (Eucalyptus) Wood (Eucalyptus) Wood (Pinus radiata) Wood (Pinus radiata) Average Temperature (C) 35 35 37 37 % of COD removal 86.6 85.5 86 90 87 Methane yield L/kg COD removed 270 230 302 313 279 Reference [29] [29] [31] [30]

analyses of the xylan conversion efciency and the fraction of lignin solubilised. 2.4. Economic analysis The economic analysis (with 2009 as the reference year) was performed to evaluate the four base cases (waste paper-tobioethanol without pre-treatment) and the two state-of-the-art cases (ofce paper-to-bioethanol with DA and newspaper-tobioethanol with OL pre-treatments). The MESP was used as a main economic indicator to compare processes and as input to pump prices of bioethanol from waste papers for comparison with petrol pump prices and for comparison with other studies where the MESP has been applied [10,16,32]. The MESP is the selling price of bioethanol that makes the net present value of biomass to bioethanol process equal to zero with a 10% discounted cash ow rate of return over a 20 year plant life [9]. The MESP does not include any fuel duty or government subsidy. The MESP is calculated by a discounted cash ow method based on the estimated total project cost as well as variable operating, xed operating costs, revenues and income tax etc. 2.4.1. Total project cost The total project cost comprises of other costs (e.g. start-up cost and land fees etc.) and the total capital cost (which contains the total installed cost and indirect cost). The total installed cost consists of total installed equipment cost, warehouse cost and site development cost. The installed equipment cost is either estimated by Aspen Economic Analyzer or an approach that scaled up or down the same equipment from the NREL process with known cost but of a different size using the following equation [10]:

ne km) [35]. The cost for the enzyme complex Cellic Ctec 1 (3.421 /107 FPU) is estimated based on the cost of the traditional enzyme Celluclast 1.5L (1.416 /106 FPU) with an expected reduction in the cost for Cellic Ctec 1 [32,36]. The xed operating costs including labor costs (Table A.3), overhead items and general expenses are listed in Table A.4. 2.4.3. Discounted cash ow method The discounted cash ow method was applied to calculate MESP using parameters dened in Table A.5. In the cost breakdown, the capital recovery charge (CRC) is dened as a proxy for the ownership costs of assets with a productive life greater than one year and calculated from the following equation [37]:

Capital Recovery Charge CRC V 0 V n i1 in Vn i 1 in 1 2

where V0 is the total project cost at the beginning of year 1, n is the plant life time, Vn is the value at the end of useful life, i is the interest rate that is set as 10%. 2.4.4. Sensitivity analysis on cost parameters The MESP estimation is inuenced by assumptions about process parameters (e.g. solids loading in saccharication, fermentation efciency, anaerobic digestion efciency, etc.) and cost parameters (e.g. plant capacity, raw material cost, capital cost, etc.). The state-of-the-art newspaper-to-bioethanol process was selected as an example to explore the effects of varied cost parameters on its MESP. The cost parameters studied in the sensitivity analysis and their variation ranges are listed in Table 4. 2.5. Supply chain model In order to compare with petrol, the supply chain of bioethanol production from waste papers was modelled as shown in Fig. 3 [40]. Bioethanol cost at pump (excluding tax) includes raw material transportation cost, bioethanol production cost and distribution expense. The starting point is the market price of waste papers ready to be transferred to the bioethanol plant. This price reects the costs of collection of waste papers, sorting and storage and market effects on price due to demand (e.g. for recycling). The transportation cost of the waste papers to the bioethanol plant was determined in Section 2.3.2. The bioethanol production was modelled in-house. The transport and distribution cost of bioethanol is estimated as 0.032 $/L by Slade et al. [40]. The bioethanol price at pump is determined by adding fuel duty (0.352 /L in 2009) and 15% vat tax to the bioethanol cost at pump. Thus, if the bioethanol price at pump is lower than that for petrol, it can be concluded that bioethanol is economically competitive with petrol. All cases (and scenarios in the sensitivity analyses) are modelled at a commercial scale of 2000 dry tonne waste paper per day. However, knowledge in pilot scale (100 dry tonne/day) and demonstration scale (200 and 500 dry tonne/day) also attracts interests before investing at a commercial scale. An investigation

Costunknown Costknown

 f Sizeunknown scale Sizeknown

where fscale is the scale exponent adopted from Aden [10]. The calculated cost of purchased equipment from Eq. (1) was transformed to the reference year (2009) using the Chemical Engineering Index [33]. The average exchange rate in 2009 of 1.443 was used to convert USD costs to GBP where appropriate. Total capital costs and the total project costs were calculated based on the factors in Appendix A (Table A.1). 2.4.2. Operating cost The operating cost includes variable and xed operating costs. Variable costs include raw material costs, waste disposal and purchased utilities etc. Table A.2 in Appendix A summarizes the feedstock and chemical costs, purchased energy as well as cooling water costs. Feedstock cost includes the cost for transporting waste papers by truck to the assumed bioethanol plant which was modeled as being 50 km away from Greenwich, London which was the location of the material recycling facility (MRF) assumed for the waste papers sourcing [34]. The transportation cost was estimated to be 0.08 /tonne km, an average value of the costs for full load truck (0.04 /tonne km) and less-than-truck load (0.11 /ton-

L. Wang et al. / Applied Energy 111 (2013) 11721182 Table 4 Cost parameters considered in sensitivity analysis. Parameters % Variation related to baseline scenario Min Total capital cost Cost of waste papers Enzyme cost Surplus electricity price 0.7 0.5 0.5 0.9 Max 1.3 1.5 1.5 1.2 A A A A range range range range of of of of 30% was considered sufcient to cover uncertainties in capital cost 50% obtained in the survey of waste papers price in the UK 50% was considered reasonable given the uncertainties in the costs of enzyme production 10% to +20% obtained in the survey of the electricity price for the UK [38] [8] [38] [39] Remark

1177

Reference

Waste paper price /L

Transportation cost /L

Feedstock cost at plant /L

Bioethanol production cost /L

Bioethanol cost at plant /L

Distribution cost /L

Fuel duty /L

Bioethanol cost at pump /L

Tax VAT /L

Bioethanol price at pump /L

Fig. 3. The elements of bioethanol price at pump (Unit: /L).

of the economic performance of a smaller plant capacity was therefore also studied in the sensitivity analysis. 3. Results and discussion 3.1. High-solids loading saccharication Table 5 shows the sugar yields obtained experimentally by enzymatic hydrolyses at 160 mg Cellic Ctec 1 liquid product as supplied/g glucan (equivalent to 16.8 FPU/g glucan) after 72 h from four types of waste papers. Ofce paper has the highest glucose and xylose yields probably due to its low lignin content of 5.78% and shorter bres compared with the other types of paper (resulting from the feedstock and pulping process used for ofce paper manufacture). Similarly, cardboard has lower lignin content (14.86%) than newspaper (16.82%) therefore a potential higher accessibility for enzyme. The lowest sugar yields were from magazine due to its relatively high content of impurities (e.g. paper llers and coatings etc.). These experimental results were applied in the base cases modelling. 3.2. Energy efciency In this study, the energy efciencies were determined as the ratio of the energy contained in products (ethanol and electricity) to

that in the biomass feedstocks (lower heating value). According to the production data summarised in Table 6, the energy efciencies for the four baseline cases are in the range of 20% (magazine) to 45% (ofce paper). The higher energy efciencies for conversions to biofuel in the present study for ofce papers is due to its more favourable composition than other typical biomass feedstocks, especially its higher carbohydrates content. Most of the energy content in the ofce paper feedstock is contained in its carbohydrates and these are largely converted to ethanol. Twenty percent or more of the energy content in other biomass feedstocks remains in the lignin-rich residues after ethanol production due to their higher feedstock lignin contents (e.g. 17% for newspaper and 18% for wheat straw [41]) compared with the ofce paper (less than 6%).

3.3. Economic analysis results 3.3.1. Cost breakdown analysis A cost breakdown of the newspaper-to-bioethanol process at 160 mg Cellic Ctec 1 liquid product as supplied/g glucan is shown as a percentage of the MESP (0.35 /l) in Fig. 4. Biomass cost is the single biggest cost contributor, accounting for 63.5% of the MESP, while only a small contribution is made by enzyme cost due to the relatively low price of Cellic Ctec 1. The capital recovery charge for the combustor and the electricity generator represents 16.7% of

Table 5 Sugar yields (% of component present) of waste papers by enzymatic hydrolyses for 72 h at enzyme loading of 160 mg/g glucan. Glucose (%) Newspaper Ofce paper Cardboard Magazine 55.5 76.1 62.2 49.8 Xylose (%) 57.7 62.8 61.8 41.8 Cellobiose (%) 3.3 5.4 2.2 2.1 Galactose (%) 57.0 62.4 44.8 Mannose (%) 56.2 60.1 46.7 Arabinose (%) 28.3 31.7 19.6

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Table 6 Economic analysis results for four base cases and two state-of-the-art cases. Newspaper Conditions Initial solid loading Pre-treatment Enzymatic hydrolysis Bioethanol yield (l/dry ton feedstock) Bioethanol production (million l/year) Cost Installed equipment cost breakdown (million ) Blending/Pre-treatment Saccharication and fermentation Product recovery Waste water treatment Combustor/boiler/ turbogenerator Utilities Total installed equipment cost (million ) Total project investment (million ) Non-feedstock material costs (million ) Waste disposal (including gypsum) (million ) Surplus electricity (/l) Imported steam (kg/l) Bioethanol MESP (/l)
a

Newspaper with OL pre-treatment

Ofce paper

Ofce paper with DA pretreatment 30% Dilute acid, 0.5% (w/w) H2SO4, 220 C, 2 min 120 mg/g glucan, 72 h 419 294

Cardboard

Magazine

20% 160 mg/g glucan, 72 h 212 148

30% Oxidative lime, 1.875% (w/w) Ca(OH)2, 7.1 bar (absolute) O2, 140 C, 3 h 96 mg/g glucan, 72 h 290 203

20% 160 mg/g glucan, 72 h 343 240

20% 160 mg/g glucan, 72 h 247 173

20% 160 mg/g glucan, 72 h 136 96

1.4 23.5 18.8 6.5 42.7 9.8 105.8 184.4 5.6 3.6 0.184 0.35

27.3 17.4 22.3 4.3 38.3 19.9 128.8 224.7 9.2 1.9 0.129 0.31

1.3 23.4 17.7 7.4 29.9 6.7 90.2 157.3 8.7 4.9 0.009a 0.32

16.5 19.1 18.5 6.1 24.6 13.7 103.8 181.1 8.3 12.1 0.006a 3.84 0.31

1.4 23.5 18.6 5.7 40.9 8.6 102.1 178.0 6.9 3.7 0.127 0.33

1.4 22.9 20.6 5.7 37.2 7.3 98.0 170.1 4.9 6.4 0.167 0.66

Negative value means purchasing electricity.

Capital recovery charge Raw materials Fixed cost Process Electricity Grid electricity Total plant electricity
MESP=0.35/l

Biomass Feedstock handling Blending Enzyme Saccharification Fermentation Product recovery Waste water treatment
1.9% 4.4% 3.6% 16.9% 10.9% 18..1% 10.0% 1.4% -42.7% (Net)

63.5%

Combustor & electricity generator Storage Utilities

-100% -80% -60% -40% -20% 0%

13.2%

20%

40%

60%

80%

Contributions to MESP %
Fig. 4. Cost distributions from each process as a percentage of the MESP for the newspaper-to-bioethanol process (160 mg/g glucan, 72 h, Cellic Ctec 1).

the total costs of this area. However, the credits from electricity sold to the National Grid results in a negative net cost contribution (42.7%). In other words, the utilisation of the biomass residue for export of surplus electricity generated to the UK National Grid can offset 42.7% of cost of producing the bioethanol. Further potential savings in the capital costs could be achieved if saccharication and fermentation were combined, as these two processes account for 16.9% and 10.9% of MESP, respectively. Table 6 summarises the economic analysis results for the four base cases and the two state-of-the-art cases. For the base cases, ofce paper is the most favourable feedstock due to its high bioethanol production of 343 l/dry tonne feedstock and lowest MESP of

0.32 /l. Cardboard-derived bioethanol has a yield of 247 l/dry ton feedstock and the second lowest MESP of 0.33 /l. Bioethanol produced from magazine paper has the highest MESP of 0.66 /l and the lowest yield of 96 l/dry ton feedstock. By comparing the installed equipment cost for each area in the base cases, it is found that variations in the product recovery area are due to the different ethanol concentrations in the feeding streams to the distillation column and differences in the combustion area are because of the varied amounts of solid fuel feed. For example, ofce paper-to-bioethanol has the lowest installed equipment cost in the product recovery and combustion areas because of its relatively high ethanol concentration in the distillation column

L. Wang et al. / Applied Energy 111 (2013) 11721182

1179

Variaton in MESP related to base case

feeding stream (4.6% w/w) and its relatively small amount of fuel fed to the combustor. Applying a DA pre-treatment can increase the yield of bioethanol from ofce paper from 240 to 294 million litres per year but with a small reduction in MESP (0.01 /l). For the process with pre-treatment, capital costs are increased by 15% mainly because of the extra equipment costs in the pre-treatment area and the utility area where more heat exchangers are required. In addition, extra electricity and high pressure steam are also required because less energy is recovered from the combustor with the decreased amount of lignin and polymerised sugar in its feed stream. Nonfeedstock material costs and waste disposal costs are higher in the process with DA pre-treatment due to the increased sulphuric acid consumption and consequently larger amount of gypsum sent to landll when compared with the process without pretreatment. However, the OL pre-treatment on newspaper can reduce MESP by 0.04 /l and increase the bioethanol yield by 55 million litres per year. For the process with OL pre-treatment, the additional installed equipment costs in the pre-treatment area together with those in the product recovery and utilities areas overcome the reduction in the installed equipment costs for other processes, resulting in a higher total installed equipment cost. In addition, non-feedstock material costs are signicantly increased by the utilisation of hydrochloride acid. However, the benets brought by the higher bioethanol yield and lower enzyme consumption counterbalance these increased expenses. Therefore, the OL pre-treatment can improve the economic feasibility of bioethanol produced from newspaper. Overall, the MESPs of bioethanol produced from waste papers are in the range of 0.31 /l (0.45 $/l) to 0.66 /l (0.95 $/l) which is consistent with and generally somewhat more favourable than those for bioethanol produced from other lignocellulosic biomass which range from 0.57 $/l to 1.17 $/l for the studies cited [16,25,32]. For example, the estimated MESPs of bioethanol from corn stover by NREL [25] are in the range from 3.404.44 $ (US)/ gallon (0.901.17 $/l) depending on the different technologies and congurations applied. The MESPs estimated for bioethanol potentially from willow was reported as 0.61 /l (0.88 $/l with an exchange rate of 1 US dollar = 0.69 GBP in 2009) for a UK scenario and 0.80 /l (1.15 $/l) for a Poland scenario [15]. Dutta et al. [16] indicated MESPs of bioethanol from corn stover between 2.68 3.30 $/gallon (0.710.87 $/l) with different conguration designs. Sassner et al. [32] estimated the MESPs for bioethanol from willow (Salix), corn stover and spruce in the range of 4.155.49 SEK/l (0.570.76 $/l with an exchange rate of 1 SEK = 0.14 US dollar in 2006). It should be noted that these MESPs cover a wide range due to variations in raw material costs, equipment expenses, labour costs, energy costs and tax rates which are location dependent, while enzyme costs and other model parameters (e.g. discounted rate and capital depreciation method) are also case specic.

Composition of bioethanol price at pump /L

1.80 1.60 1.40 1.20 1.00 0.80 0.60 0.40 0.20 0.00
CB-CT1 MG-CT1 OP-CT1 NP-CT1 OPAC NPOL

Petrol price at pump /L (2009)

Distribution cost

Fuel tax

MESP before tax

Fig. 5. A summary of the pump price of bioethanol produced from various waste papers. Note CB cardboard, OP ofce paper, MG magazine, NP newspaper, CT1 Cellic Ctec 1, and OPAC ofce paper with dilute acid pre-treatment, NPOL newspaper with oxidative lime pre-treatment.

3.4. Sensitivity analysis 3.4.1. Cost parameters Sensitivity analysis results for the MESP of the newspaperto-bioethanol process are shown in Fig. 6 spider diagram. The gradient indicates the extent of impacts of these cost parameters on results: the steeper the line, the greater changing that parameter will affect the result. It is shown that total capital costs, electricity price and biomass cost have the greatest inuences on the results. Capital costs affect the MESP signicantly; however, it is in a closer range of uncertainties when compared with enzyme and biomass costs. Conversely, the enzyme cost has a small impact on the MESP even with high uncertainties. This can be explained by the MESP breakdown shown in Fig. 4. Enzyme costs contribute relatively insignicantly; therefore, the inuence caused even by considerable change in enzyme price is small. The surplus electricity price correlates negatively with the MESP because the surplus electricity brings in credits lowering the MESP. This parameter varies over a limited range of values; however, it has a great impact on the MESP. These results suggest that it is important to secure a low cost supply of waste paper feedstocks, reduce the capital costs and also sell the surplus electricity at a high price.

40% 30% 20% 10% 0% -10% -20% -30% -40% 30% 60% 90% 120% 150%

3.3.2. Comparison of bioethanol with gasoline at pump Following the approaches for constructing the supply chain model dened in Section 2.5, the bioethanol selling price at pump derived from the four base cases and the two state-of-the-art cases are shown in Fig. 5 in comparison with the petrol price. The bioethanol price at pump has been converted to a petrol equivalent based on 1 l of bioethanol replacing 0.68 l of petrol due to their different energy densities (21.2 MJ/L for bioethanol and 31.2 MJ/L for petrol). With the exception of magazine paper, bioethanol produced from waste papers with or without pre-treatments are economically superior to petrol.

Relatvie parameter variation Capital cost Surplus electricity selling price Enzyme cost Waste paper cost

Fig. 6. The sensitivity of MESP to changes in cost parameters for the case of newspaper-to-bioethanol production (Cellic Ctec 1 at the enzyme loading of 160 mg/g glucan).

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3.4.2. Process parameters Fig. 7 shows the sensitivity analysis results for the MESPs of the four base cases and the two state-of-the-art cases on the varied range of process parameters in Table 2. The baseline scenario is shown as the top column for each case. The MESP of bioethanol in each case is found to be most sensitive to the variation in the solids loading of saccharication. The MESPs of bioethanol are decreased by up to 20% when the solids loading increases from 15% to 20%. This is because of (1) the reduction in energy consumption for distillation due to the more concentrated bioethanol stream fed to distillation column, and (2) the reduction in capital costs in the waste water treatment area due to the smaller required capacity. The MESPs of bioethanol increase by up to 40% when the solids loading is lowered to 10%. The MESPs of bioethanol from ofce paper without and with DA pre-treatment are not sensitive to changes in fermentation and anaerobic digestion efciencies. This is because ofce paper has negligible amount of mannose, arabinose and galactose and consequently the variations in fermentation efciencies of these sugars will not affect the MESPs. Similarly, due to the low contents of these sugars and the relative high fermentation efciencies of glucose and xylose, the amount of organics owing to anaerobic digestion is low. Therefore, the impact caused by variations in anaerobic digestion performance is insignicant. For the other three types of waste paper without pre-treatment and newspaper with OL pre-treatment, MESPs are relatively sensitive to fermentation efciency but not sensitive to the anaerobic digestion efciency. Overall, the fermentation efciency has the most signicant impact on the MESPs of magazine-derived bioethanol: its MESP is reduced by 8% when conversion efciencies of sugars
0.33 0.32 0.35 0.33 0.34

(except for glucose) reach 85%. The inuence of anaerobic digestion efciency on the MESP for all types of waste papers without pretreatment varies but over a small range of 3%. It is also apparent that variation in technologies affects the conclusion over which are the most preferable waste paper feedstocks for bioethanol production. Besides ofce paper, cardboard becomes an attractive feedstock when a higher solids loading in enzymatic hydrolysis can be achieved. For newspaper with OL pre-treatment, the MESP of bioethanol is more sensitive to the fraction of lignin removed when compared with the xylose yield in pre-treatment. This is because the fraction of lignin removed affects the amount of surplus electricity generated. In conclusion, the economic performance of bioethanol is highly sensitive to solids loading and is also reasonably sensitive to fermentation efciency. Improving these two elements has the potential to result in a reduction in the MESPs up to 25% and 6% respectively. 3.4.3. The plant capacity Fig. 8 shows the results of an exploration of different plant capacities on the bioethanol selling price at pump. Pump price increases sharply if plant capacity is reduced over the range of 500 to 100 dry tonnes per day. The trend of pump price attens when the plant capacity is over 500 dry tonne per day. Bioethanol from magazine paper is not economically competitive with bioethanol from other waste papers or petrol regardless of the plant capacity (at the same waste paper price of 40/tonne). When the plant capacity is over 1000 dry tonnes per day, ofce paper-derived bioethanol becomes economically competitive with petrol. However, the

0.27

0.44

Cardboard

0.55 0.61

0.66 0.82 0.66 0.67 0.72

Magazine

0.27

0.32 0.35 0.32 0.33 0.32 0.33

Office paper

0.28

0.35 0.33 0.48 0.38 0.35 0.36

Newspaper

Baseline scenario Solid loading (Max) Solid loading (Min) Fermentation (Max) Fermentation (Min) Anaerobic digestion (Max) Anaerobic digestion (Min) Xylose yield in pretreatment (Max) Xylose yield in pretreatment (Min) Lignin removal in OL pretreatment (Max) Lignin removal in OL pretreatment (Min)
0.50 0.60 0.70 0.80 0.90

0.31

Office paper with DA

0.31 0.32 0.31 0.32 0.31 0.31 0.31

Newspaper with OL

0.29

0.33 0.31 0.31 0.31 0.31 0.30 0.33

0.00

0.10

0.20

0.30

0.40

MESP /L
Fig. 7. The sensitivity analysis on process parameters for four base cases and two state-of-the-art cases (Note: saccharication conditions for cardboard, magazine, ofce paper, newspaper and ofce paper with dilute acid (DA) pre-treatment are 120 mg/g glucan enzyme loading and 72 h; that for newspaper with oxidative lime (OL) pretreatment is 72 mg/g glucan enzyme loading and 72 h).

L. Wang et al. / Applied Energy 111 (2013) 11721182

4.00 3.50 3.00

1181

MESPs /L

Cardboard Magazine Office paper Newspaper

Table A.1 Additional costs for determining total project investment [9]. Item Warehouse Site Development Indirect cost Prorateable cost Field expenses Home ofce and construction Project contingency Other costs Value 1.5% Of total installed equipment cost 9% Of total installed equipment cost 10% Of total installed cost 10% Of total installed cost 25% Of total installed cost 3% Of total installed cost 10% Of total capital cost

2.50 2.00 1.50 1.00 0.50 0.00 0 400 800 1200 1600 2000
Petrol price at pump (2009)

Plant capacity dry tonne/day

Fig. 8. The bioethanol price at pump produced from various waste papers using Cellic Ctec 1 at different plant capacity. Petrol price at pump is shown as reference. Table A.2 Materials, chemicals and energy cost. Biomass/chemicals/energy Cost 44 /ton (average) 34.65 /ton 83.17 /ton 71.94 /ton 48.51 /ton 244 /ton 3.421 /107 FPU 0.20.4 /ton 2062 /ton 1559 /ton 554 /ton 3000 /ton 0.144 /ton 0.152 /ton 24.5 /tonb 170 /tonc 0.09819 /kw h Reference [8,35] [45] [46] [47] [9,48] [9,49] [32,36] [50] [9] [9] [9] [9] [50] [50] [51] [15,52] [39]

methodology of pricing bioethanol will depend on the size of the total bioethanol market, political support (e.g. government subsidy) and the local availability and pricing of feedstocks. Consideration of these factors will also inuence the investors decision regarding the size/viability of a waste-paper-to-bioethanol project. 4. Conclusions Economic analyses of bioethanol production from various waste papers were conducted using experimentally generated data, literature data and AspenPlusTM simulation. It is concluded that, with the exception of magazine paper, bioethanol produced from newspaper, ofce paper and cardboard can be economically superior to petrol at pump prices. In addition, DA and OL pre-treatments can improve the economic feasibility of ofce paper-to-bioethanol and newspaper-to-bioethanol supply chains. A series of sensitivity analysis suggests that biomass feedstock cost, capital costs and surplus electricity selling price are dominant factors affecting the MESP. Therefore, securing a feedstock source at relatively low prices, reducing capital investment, and selling surplus electricity at high price can improve the economic performance of waste papers-to-bioethanol supply chains. The sensitivity analysis also suggests that increasing the solids loading in saccharication and enhancing fermentation efciency can reduce the minimum ethanol selling price. Overall, this work suggests that there is considerable potential from an economic perspective for using waste paper as feedstock for bioethanol production. These analyses provide an economic rationale and incentive for further environmental impact studies such as those of Shi et al. [42] and Wang et al. [43,44] (including consequential effects such as diversion, increased recovery in paper recycling etc.) on the potential for using waste papers as feedstocks for biofuel production. Acknowledgments The authors gratefully acknowledge the Porter Institute (Imperial College London) for part nancing this work. We are also most grateful to Novozymes A/S, Demark for supply of Cellic Ctec 1 and information regarding enzyme prices. Appendix A. Parameters used in economic analysis The factors used to determine the total project investments can be found in Table A.1. The operating costs including variable operating costs (materials, chemicals and energy costs) and xed operating costs (labour costs, overhead items and general expenses etc.) are listed in Tables A.2A.4. Parameters used in the discounted cash ow calculation are summarised in Table A.5.

Waste paper costa Sulfuric acid HCl 36% (w/w) Lime (Ca(OH)2) Corn steep liquor Diammonium phosphate (DAP) Cellic Ctec 1 Cooling water BFW chemicals Cooling water chemicals WWT chemicals WWT polymers Low pressure steam (4.4 bar) High pressure steam (13.2 bar) Ash landll Gypsum landll Electricity

a Includes waste paper price of 40 /ton (average of various type of waste papers) and transportation cost of 4 /ton. b Includes landll cost 22 /ton and tax 2.5 /ton. c Includes landll cost for classied as hazardous 130 /ton and tax 40 /ton.

Table A.3 Labour costs [53]. Annual salary (annual / personnel) Plant manager Plant engineer Maintenance supervisor Lab manager Shift supervisor Lab technician Maintenance technician Shift operators Yard employees General manager Clerks & secretaries Total salary 57000 49400 43900 38400 29300 22000 27500 22000 18000 61800 18000 1767000 Number of personnel 1 1 1 1 5 2 8 20 32 1 5

Table A.4 Fixed operating cost [9]. Item General overhead Maintenance fee Insurance and taxes Administrative cost Marketing cost Research and development (R&D) Value 60% Of total labour cost 2% Of total installed equipment cost 1.5% Of total installed cost 15% Of total labour cost 2% Of MESP 2% Of MESP

1182 Table A.5 Discounted cash ow method parameters [9]. Parameters Plant life Discounted rate General plant depreciation General plant recovery period Steam plant depreciation Steam plant recovery period Corporation tax rate Financing Construction period 1st 6 months expenditures Next 12 months expenditures Last 12 months expenditures Working capital Start-up time Revenues Variable costs Fixed costs
a

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Energy audit of the kerbside recycling services. The London Borough of Camden, 2008; 2010. <http://camden.gov.uk/ccm/content/ environment/policies-reports-and-data/energy-audit-of-the-kerbsiderecycling-services.en;jsessionid=F2423B19ED95A4F04FF0C09567CBEE07. node2>. [35] Madariaga J. Proling best practices: an explanatory analysis of box-plant trucking logistics in the paper industry (MSc). Atlanta: Georgia Institute of Technology; 2004. [36] Andersen L. Personal communication. Denmark: Novozymes A/S; 2010. [37] Frank G. Crop processor economics: partial budgeting its use corn silage. Center for dairy protability. University of Wisconsin, Madison; 1999. [38] Slade RB. Prospects for cellulosic ethanol supply-chains in Europe: a technoeconomic and environmental assessment (PhD). Univiersity of London; 2009. [39] Department of enegry and climate change. Industrail electricity prices in the EU and the G7 contries. Department of enegry and climate change, UK; 2011. [40] Slade R, Bauen A, Shah N. The commercial performance of cellulosic ethanol supply-chains in Europe. Biotechnol Biofuel 2009;2:3. [41] Ballesteros I, Negro MJ, Oliva JM, Cabanas A, Manzanares P, Ballesteros M. Ethanol production from steam-explosion pretreated wheat straw. Appl Biochem Biotechnol 2006;129132:196508. [42] Shi AZ, Koh LP, Tan HTW. The biofuel potential of municipal solid waste. Global Change Biol Bioenergy 2009;1:31720. [43] Wang L, Templer R, Murphy RJ. Environmental sustainability of bioethanol production from waste papers: sensitivity to the system boundary. Energy Environ Sci 2012;5:828193. [44] Wang L, Templer R, Murphy RJ. A life cycle assessment (LCA) comparison of three management options for waste papers: bioethanol production, recycling and incineration with energy recovery. Bioresour Technol 2012;120:8998. [45] ICIS. Sulfuric acid market seeks balance; 2011. <http://www.icis.com/Articles/ 2010/09/06/9390780/sulfuric-acid-market-seeks-balance.html>. [46] ICIS. Hydrochloric acid report, 2010; 2011. <http://www.icispricing.com/ il_shared/Samples/SubPage110.asp>. [47] Miller MM. 2009 Minerals yearbook US Lime. US department of the interior; 2010. guez N, Corte nguez JM. Development of s S, Domi [48] Salgado JM, Rodri cost-effective media to increase the economic potential for larger-scale bioproduction of natural food additives by Lactobacillus rhamnosus, Debaryomyces hansenii, and Aspergillus niger. J Agr Food Chem 2009;57: 1041428. [49] World Bank Commodity. World bank commodity price data; 2011. <http:// siteresources.worldbank.org/INTPROSPECTS/Resources/3349341304428586133/Pnk_0511.pdf>. [50] Ulrich GD, Vasudevan PT. Engineering practice. how to estimate utility costs. Chem Eng 2006;113:6670. [51] HM Revenue & Customs UK. Goverment response to modernising landll tax legislation, 2010; 2011. <http://www.2degreesnetwork.com/preview/ resource/government-response-modernising-landll-tax-legislation-hmtreasury/>. [52] WRAP. Gypsum, partial nancial impact assessment of a quality protocol for the production and use of gypsum from waste plaster board; 2010. p. 31. [53] Stalker M. IChemE salary survey 2008; 2010. <http://www.ceas.manchester. ac.uk/undergraduate/accreditation/cashing_in.pdf>. [54] HM Revenue & Customs UK. Income tax rates and allowances; 2011. <http:// www.hmrc.gov.uk/rates/it.htm>.

Values 20 Years 10% 200% Declining balance 7 Years 150% Declining balance 20 Years 28%a 100% Equity 2.5 Years 8% 61% 31% 5% Of total capital investment 6 Months 50% 75% 100%

From HM Revenue & Customs [54].

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