Eco-Efficiency Analysis of Biomethane Production - Industrial

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Eco-Efficiency Analysis of Biomethane Production Piotr Biernacki, S. Steinigeweg, Wilfried Paul, and Axel Brehm Ind. Eng. Chem. Res., Just Accepted Manuscript • DOI: 10.1021/ie502800r • Publication Date (Web): 25 Nov 2014 Downloaded from http://pubs.acs.org on November 26, 2014

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Industrial & Engineering Chemistry Research

Eco-Efficiency Analysis of Biomethane Production Piotr Biernackiab*, Sven Steinigewega, Wilfried Paula, Axel Brehmb. a

EUTEC Institute, University of Applied Sciences Emden/Leer,

Constantiaplatz 4, 26723 Emden, Germany. b

Technische Chemie, Fk.V, Carl von Ossietzky Universität Oldenburg, D-26111 Oldenburg.

KEYWORDS Eco-Efficiency; Biomethane power plants; Biogas upgrading technology; Electrolyte NRTL model; 2-(Ethylamino)ethanol; ABSTRACT This work was concentrated on upgrading an existing biogas plant, located in Wittmund (Germany; biogas volume flow of 3167.361 l min-1; CH4: 67,51 Mol. %; CO2: 29,87 Mol.%; N2: 1.98 Mol.%; O2: 0.65 Mol.%; H2S: 5.99 mgS m-3), operated by EWE GmbH, to a biomethane plant. Scrubbing with alkanoalmine solutions was chosen as carbon dioxide capturing method, since it has proven to be an efficient method of removing carbon dioxide and to obtain high methane slippage. Hence, this research was concentrated on a model based upon economical, social and ecological assessment of the alkanolamines, used only for capturing the carbon dioxide, which include monoethanolamine (MEA), diethanolamine (DEA), 2(Ethylamino)Ethanol (EAE), and diglycolamine (DGA). In the economical evaluation the energy

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consumption for the desorption step was evaluated, whereas the environmental assessment included marine toxicity and biodegradability. In order to complete the sustainability evaluation, the social aspects were evaluated with use of the reduced inherent safety index method. The environmental evaluation indicated, that three amines, MEA, DEA and EAE, fulfilled the criteria of the low toxicity to marine organisms and high biodegradability. The DGA was recognized to be dangerous for the environment. Furthermore, the social assessment revealed, that the evaluated amines have similar social acceptance, reflected by the similar chemical safety. Finally, the economical evaluation slightly favors 3.2 mass % EAE aqueous solution (energy efficiency of 0.262 MW per each mol of carbon dioxide recovered; 100% CO2 removal) and 30 mass % EAE aqueous solution (energy efficiency of 0.214 MW mol-1; 100% CO2 removal) over 30 mass % MEA aqueous solution (efficiency of 0.307 MW mol-1; 94.209% CO2 removal). As a consequence, 2-(Ethylamino)Ethanol and monoethanolamine were proved to be sustainable alkanolamines for biogas upgrading. Introduction The mathematical modeling was intended to precisely predict behavior of a system, concurrently significantly reducing amount of experiments necessary prior to accurate description of the system like e.g. phase equilibrium or anaerobic digestion1,2. Therefore a new experimental data, determination of parameters’ values, models’ optimizations, along with further proving of the mathematical modeling against existing plants was required for precise and efficient application of the numerical simulations1,2,3,4. Attributable to growing environmental consciences, the renewable energy sources are extensively evaluated and concurrently optimization attempts are conducted. An interesting case


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is an anaerobic digestion of organic waste, which is a waste management method, and simultaneously formed gas (biogas) may be utilized in combined heat and power (CHP) units to obtain energy and heat. This biogas may also be upgraded to biomethane by removal of carbon dioxide (30-50 volume %), leaving the valuable methane (50-70 volume %). Afterwards it satisfies requirements for natural gas send to the grid or may be utilized as a fuel for vehicles5. Furthermore, carbon dioxide could be used as a substrate in efficient energy storage Power2Gas6 method. This research was concentrated on upgrading an existing biogas plant, located in Wittmund (Lower Saxony, Germany), operated by EWE GmbH7, to a biomethane plant. As an upgrading method, thanks to which efficient carbon dioxide removal and high methane slippage is possible, but also efficient carbon dioxide recycling is achievable, scrubbing with aqueous alkanolamine solution was chosen8. Moreover, this technique is already proven to be mature method, simple for retrofitting to an existing plant9, and it is predicted by Rochelle to be the dominant method in year 203010. As a consequence, this research was concentrated on a model based upon economical, social and ecological assessments. of upgrading the biogas obtained from an existing plant. The economical efficiency included the analysis of the CO2 removal and the energy consumption during the desorption step. This was prepared with use of the ASPEN® Plus 8.0. In order to make sure that recommended alkanolamine will not harm environment, even at applying it on an industrial scale, an ecological assessment is included in this research, where marine toxicity and biodegradability were taken into account. In order to complete the sustainability evaluation, the social aspects were evaluated with use of the reduced inherent safety index method11, as proposed by other authors12,13.

Materials and Methods ACS Paragon Plus Environment

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Sustainability assessment Categories for sustainability assessments were based on the concept already introduced in the literature12,13. However, because this research was concentrated on the evaluation of the carbon dioxide absorption by different aqueous solutions of alkanolamines, the sustainability assessment was modified as graphically presented (figure 1). Moreover, because the same plant design was used for each of the alkanolamines, the economical evaluation of the associated investment costs was not applicable. The economical evaluation was carried out using the running costs because the energy consumption during the desorption stage is a crucial part. Consequently, in the environmental impact assessment bioaccumulation and marine toxicity were only analyzed, since energy evaluation was already included in the economical part. On the other side, other authors12,13 proposed to include chemical safety and plant safety as indicators of the social acceptance, which were obtained with use of the inherent safety index11. However, in this research only the subindices for hazardous substances of the chemical inherent safety index11 were recognized as applicable for this assessment. Analyzed system The chemical equilibrium for R2NH – H2O – CO2 system was already presented in the literature, and it is based on the work of

4,14,15,16

, where R2NH is a secondary amine. The

following reactions describe ionization of water (Reaction 1), formation of bicarbonate (Reaction 2) and its’ dissociation (Reaction 3). Additionally carbon dioxide absorption (Reaction 4), amine protonation (Reaction 5) and carbamate reversion to bicarbonate (Reaction 6), only possible for secondary and primary amines, were included 4,14,15,16. 2 ⇌ +

(Reaction 1)


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2 + ⇌ +

(Reaction 2)

+ ⇌ +

(Reaction 3)

NH + + ⇌ +

(Reaction 4)

+ ⇌ +

(Reaction 5)

+ ⇌ +

(Reaction 6)

Carbon dioxide dissociation (Reaction 2) and carbamate formation (Reaction 4) are expressed as kinetic reactions with use of power law expression, in accordance to the literature4,15,14,16: + →

(Reaction 7)

→ +

(Reaction 8)

+ + → +

(Reaction 9)

+ → + +

(Reaction 10)

Model used in this research In this research no thermodynamic model was developed, thus already published models were employed for describing the physical and chemical absorption of carbon dioxide in different aqueous alkanolamine solutions:

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Monoethanolamine (MEA, CAS: 141-43-5): prepared by Austgen4, implemented in the ASPEN Plus® V 8.0 Simulation Software

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Diethanolamine (DEA, CAS: 111-42-2): prepared by Austgen4, implemented in the ASPEN Plus® V 8.0 Simulation Software

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Diglycolamine (DGA, CAS: 929-06-6): prepared by Austgen4, implemented in the ASPEN Plus® V 8.0 Simulation Software


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2-(Ethylamino)ethanol (EAE, CAS: 110-73-6): prepared by Biernacki et al.14

Pure component properties Parameters for CO2, H2O, DGA, DEA, MEA were acquired from ASPEN Plus® databases (APV80.PURE27 and APV80.Binary), and for EAE from NIST database17. Case study EWE Wittmund Biogas Power Plant (Wittmund, Lower Saxony, Germany)7, in details describe in18, commissioned in 1996, was chosen as a source of biogas in this research. Manure (180 m3 d1

) and organic waste (100 m3 d-1), thus a residues mixture from restaurants, slaughter house,

kitchens, hospital, and food processing, were mixed to feed the biodigesters. The substrate input was mixed in a mixing tank (620 m3), send to the hygienisation tank for at least 1hour at minimum 70°C (30 m3), and finally divided into two 3500 m3 reactors. The averaged cumulative biogas production in March and April 2012 were equaled to 4561 m3 d-1, with an average temperature of 38.6°C, with such a composition: CH4: 67.51 Mol. %; CO2: 29.87 Mol.%; N2: 1.98 Mol.%; O2: 0.65 Mol.%; H2S: 5.99 mgS m-3. Process design The plant’s design is based on the work of Desider and Paolucci19, later applied by Luyben20, as presented in scheme 1. In this research for each of the analyzed amines the plant’s design was exactly the same, to allow comparison, as describe below. The plant consists of absorber, stripper, heat exchanger, and pumps. However, also an additional heater was included, because the heat exchanger was not sufficient. The absorber, a RadFrac column, consists of 11 stages, operated at 101.325 kPa pressure with 1.38 kPa pressure drop. The feed biogas was compressed


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to 125.64 kPa at 336 K, as specified by Luyben20. The amines were feed at 101.325 kPa pressure and with temperature of 313 K. The rich solvent’s temperature (amine + absorbed carbon dioxide) was with use of heat exchanger and an additional heater increased to 380 K prior to feeding it to the stripper. The stripper column, also the RadFrac, was specified to have 10 stages, and it was operated at 202.65 kPa pressure, whereas 151.99 kPa operating pressure was set in the reflux drum. The bottom of the stripper was estimated to reach 400 K, while in the condenser the temperature was set to 343 K, to remove most of the water. Both, absorber and stripper, were described with use of the equilibrium and kinetic reactions. For each amine stripper specification was set to:

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Distillate rate of 20 kmol hr-1

•

Reflux ration of 0.75 (mole basis)

•

Water was additionally removed from condenser, and mixed with recycled hot solvent, coming from the bottom

Results and Discussion Ecological assessment Marine biodegradability and ecotoxicity of 43 different amines were measured and evaluated by Eide-Haugmo et al.21, and 10 interesting for this research amines are summarized in table 3. Following the Norwegian Activities Regulation22, the minimum recommended value of ecotoxicity, represented by lethal concentration to 50% of the population (EC50/LC50), should be equal or higher than 10 mg l-1. The marine biodegradability, represented in percentage of the theoretical oxygen demand, should be higher than 20%, but preferably it should be above 60%.


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As a consequence amines like DIPA (Diisopropanolamine) , MDEA (N-methyldiethanolamine), AMP (2-Amino-2-methylpropanol) or PZ (Piperazine) do not fulfill the marine biodegradability requirements, and also Piperidine do not meet the minimal recommended value for ecotoxicity. Despite DGA also did not satisfy the marine biodegradability requirements, it was further evaluated and compared to EAE since some parameters used in modeling EAE, were set equal to parameters for DGA14. On the other side, amines like MEA, DEA, EAE, where all three are natural substances, are above limit values. DEA was recognized to have the lowest toxicity to marine organisms, whereas EAE was classified as a substance with slight acute toxicity (10 – 100 mg l-1), but it is still not found to be a problematic substance or its‘ application should be limited21. Concerning the marine biodegradability all three substances achieved high biodegradability (>60% Theoretical Oxygen Demand (ThOD) levels, with leading EAE (70.4 %ThOD). As a consequence, DEA, EAE and MEA were found to have the best ecological profile, therefore they were used for the economical assessment. Social analysis According to the subindices for hazardous substances in the inherent safety index, there are four parameters were evaluated to ensure safety of the chemicals applied, which according to the literature12,13 satisfies the social analysis11:

•

Flammability Subindex IFL: 0-4

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Explosiveness Subindex IEX: 0-4

•

Toxic Exposure Subindex ITOX: 0-6

•

Corrosiveness Subindex ICOR: 0-2


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The scale described the severity of the parameter, thus the lower the value the lower the e.g. toxicity. The parameters, characteristic of the amines, along with the result for the amines are included on table 2. The parameters IFL and IEX were determined with the use of the flash point value, the lower and higher explosive limit value respectively, as proposed in by Heikkila11. Unfortunately, due to lack of information about the Threshold Limit Values and clear information about required construction material, the approach of Heikkila11 was modified. As a consequence, an example of the subindices for hazardous substances in the inherent safety index for methanol was found in the literature12, and the determination of the ITOX was based on it. Methanol was classified according to the Regulation (EC) No 1272/2008 as a category 3 acute toxic substance (acute toxicity: inhalation, dermal and oral) and also it is recognized as a category 1 toxic substance: specific target organ toxicity – single exposure 23. Therefore, it was decided to compare the toxicity of the evaluated amines to the toxic character of methanol, which its toxic exposure subindex was determined to be 2 12. As a consequence, since MEA and DGA are classified as a category 4 acute toxic substances24, 27, both were in this work recognized as a ITOX = 1. On the other side, since EAE is classified as a category 3 acute toxic substance26, and DEA is classified as category 1 acute toxic substance for specific target organ toxicity – single exposure 23, both were here recognized as ITOX = 2 just as methanol was by Li et al.12. Furthermore, the corrosiveness subindex was also determined in an indirect way, with assumptions due to lack of experimental data. According to the database of European Chemicals Agency (ECHA) EAE was not found to be corrosive to metals29, therefore ICOR = 1. On the other side, according to the literature30,31 EAE is less corrosive than MEA, and according to Rawat et al. DEA and MEA are significantly corrosive32, therefore ICOR = 2 for MEA and DEA. Moreover, according to the


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Hazardous Substance Fact Sheet DGA is not allowed to be stored in metal containers33, therefore the ICOR for DGA was decided also to be 2, following the original description of the inherent safety index1. Summing the four parameters, which are the subindices for hazardous substances in the inherent safety index, application of MEA, EAE or DGA during the carbon dioxide capture at a biomethane power plant would be safer than DEA. However, since the results were very close, and the simplified parameters’ determination methodology was applied, before the final decision a full chemical safety analysis with use of inherent safety index is recommended. Economic analysis The 10.156 kmol hr-1 (for this section only those two components of the biogas were of interest: 6.789 kmol CH4 hr-1 and 3.367 kmol CO2 hr-1) of biogas formed at EWE Wittmund biogas power plant was purified with four different alkanolamines. At the beginning the biogas was upgraded with 3.2 mass % EAE aqueous solution and 30 mass % EAE aqueous solution, and then compared to DGA, DEA and MEA. The goal was to obtain high purity biomethane (>96 mass%), which can be, after drying, send to the natural gas grid. However, due to the possible fluctuations of the biogas composition, it was decided to achieve 100% carbon dioxide removal. Additionally, the energy consumption of the condenser and reboiler were used for the final economical evaluation, where energy consumption per each mole of CO2 recovered was analyzed. The calculation results are presented on table 3. Despite the lowest amine flow of 2(Ethylamino)ethanol (4.593 kmol hr-1), biomethane of a very high purity (100 vol.% CO2 removal efficiency) along with the highest carbon dioxide recovery efficiency (3.246 kmol CO2 hr-1). The same 100 vol.% efficiency removal of carbon dioxide removal could only be achieved


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by DGA. The satisfactory result of 94.209 vol.% carbon dioxide removal of was achieved with 30 mass % aqueous solution of MEA, as proposed by Luyben20. Higher concentration of EAE ( 30 mass % aqueous solution; 8.657 kmol hr-1) also delivers very good energetical efficiency of 0.214 MW mol-1, and 100 vol.% carbon dioxide removal efficiency, however it is important to mention that this calculation is an extrapolation of the model, because the binary energy interaction parameters were determined based on experimental results with carbon dioxide solubility in 2,5 and 5 mass % aqueous solutions of EAE14. Unfortunately, the DEA result of 42.66 kmol hr-1 amine flow is recognized to be unrealistic, and application of the 2,5 mol of DEA per mol of CO2 (mole flow of 7.901 kmol hr-1) also did not deliver the expected results. Therefore, it can be stated, that DEA model implemented in ASPEN® V8.0 is not applicable for biogas upgrading (content of carbon dioxide in incoming gas was equal to 30 mass %) and future research will focus on optimization of the model. Conclusion An economical, social and ecological assessment of the alkanolamines was prepared, where the main goal was purification of the biogas coming from an existing biogas power plant, thus after removal of H2S. The ecological assessment, where marine ecotoxicity and biodegradability were evaluated21, revealed that Diethanolamine (DEA), Monoethanolamine (MEA) and 2(Ethylamino)ethanol (EAE) fulfilled the requirements for a chemical to be used on an industrial scale. Furthermore, the subindices for hazardous substances in the inherent safety index used for evaluation of the chemical safety, which is directly linked to social acceptance, were also prepared. As a consequence, MEA, EAE, and DGA had better results than DEA, however due to the simplified methodology applied, and similar results, it is recommended to conduct the full chemical safety analysis with use of inherent safety index before the final decision. On the other


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side, the economic analysis was assessed by upgrading an existing biogas plant, located in Wittmund (Germany; biogas volume flow of 190.42 m3 hr-1 (10 156 kmol hr-1); CO2 mol flow of 3.367 kmol hr-1; CH4 mol flow of 6.789 kmol hr-1), operated by EWE GmbH. The final results indicated, that the efficient energy consumption per each mole of carbon dioxide removed was achieved by 3.2 mass % EAE (energy consumption of 0.262 MW mol-1; with 100 vol.% CO2 removal efficiency), by 30 mass % EAE aqueous (energy consumption of 0.214 MW mol-1; with 100 vol.% CO2 removal efficiency) and DGA ( energy consumption of 0.249 MW mol-1; with 100 vol.% CO2 removal efficiency). The result with MEA (energy consumption of 0.307 MW mol-1; 94.209 vol.% CO2 removal efficiency) was slightly worse. Unfortunately, it was not possible to fully evaluate the CO2 removal using DEA. Consequently, in spite of DGA be promising in the economical viewpoint, due to its slow biodegradability in marine environments, it is not recommend to be used, in order to avoid high impact on the environment. As a consequence, taking under consideration ecological and economical profile, it can be stated that EAE and MEA are fulfilling the criteria of eco-efficiency analysis, and can be used in the future. AUTHOR INFORMATION Corresponding Author Tel.: +49 4921 807 1876 E-mail: [email protected] Funding Sources Funding for this study was provided by German Federal Ministry for Education and Research (BMBF): project FKZ 17N1710 ACKNOWLEDGMENT


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Discussions with Prof. Dr. Axel Borchert, Prof. Dr. M. Schlaak, Dr. Frank Uhlenhut from EUTEC Institute, Hochschule Emden/Leer are highly valued. REFERENCES 1). Gmehling, J.; Kolbe, B.; Kleiber, M.; Rarey, J. Chemical Thermodynamics for Process Simulation, Wiley-VCH Verlag & Co. KGaA. ISBN: 978-3-527-31277-1, 2012. 2). Schoen, M. Numerical Modelling of Anaerobic Digestion Processes in Agricultural Biogas Plants, Inssbruck: PhD Dissertation, University Inssbruck, 2009. 3). Novak, J. P.; Matous J.; Pick, J. Liquid - Liquid Equilibria, Amsterdam: Elsevier, 1987. 4). Austgen, D. M. A Model of Vapour - Liquid Equilibria for Acid Gas - Alkanolamine Water Systems, University of Texas at Austin, 1989. 5). Weiland, P. Biomass Digestion in Agriculture: A Successful Pathway for the Energy Production and Waste Treatment in Germany, Engineering Life Science. 2006, vol. 6, pp. 302309. 6). EUTEC. Hochschule Emden/Leer, 2012. [Online]. Available: http://www.hs-emdenleer.de/forschung-transfer/institute/eutec/laufende-projekte/klaeranlagen-alsenergiespeicher.html. [Accessed 22 03 2014]. 7). EWE Biogas GmbH & Co. KG. Wittmund biogas power plant: Important data at a glance, 2011. [Online]. Available: http://www.ewe-biogas.de/english/index_28.php. [Accessed 06 08 2011].


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5723-e044-00144f67d031/AGGR-6765098b-eb35-4ff8-a5c3-3f08fce063b9_DISS-dcee03afb431-5723-e044-00144f67d031.html#GEN_RESULTS_HD. [Accessed 16 05 2014]. 30). Sutar, P. N.; Jha, A.; Vaidya, P. D.; Kenig, E. Y. Secondary amines for CO2 capture: A Kinetic investigation using N-ethylmonoethanolamine, Chemical Engineering Journal. 2012, vols. 207-208, pp. 718-724. 31). Suda, T.; Iwaki, T.; Mimura, T. Facile Determination of Dissolved Species in CO2 Amine - H2O System by NMR Spectroscopy, Chemistry Letters. 1996, vol. 25, pp. 777-778. 32). Rawat, J.; Rao, P. V.; Choudary, N. V. Controlling corrosion in amine treatment units, Digital Refining, Crambeth Allen Media LLP., 2011. 33). New Jersey Department of Health, Right to Know; Hazardouse Substance Fact Sheet: 2(2-Aminoethoxy)Ethanol, October 2008. [Online]. Available: http://nj.gov/health/eoh/rtkweb/documents/fs/0073.pdf. [Accessed 16 05 2014].


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Sustainability assesment of chemical/energy processes

Economic

Environment

Energy consumption

Bioaccumulation & marine toxicology

Society

Hazardous substances/ chemical safety

Figure 1. Structure of the sustainability assessment applied in this research.


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Scheme 1. Typical chemical absorption plant.


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Table 1. Marine biodegradability and ecotoxicity of 10 amines .

Compound

Abbreviation

Biodegradability ThODNH3* BOD28*

Ecotoxicity EC50*

Natural

(95% confidence interval)

[%ThOD*] [mg l-1]

[mg l-1]

Minimum values

-

-

20/60

10

-

Monoethanolamine

MEA

1.31

68

198

(189-208)

Yes

Diglycolamine

DGA

1.52

Eco-Efficiency Analysis of Biomethane Production - Industrial

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