1. Introduction - Firenze University Press

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4. Conclusions In the present paper, a novel apparatus for gas hydrate production is illustrated and results of a first set of experimental applications of the reactor for CO2 hydrate formation are presented. Improvements on reactor design allowed to overcome issues relating to thermal effects and mass transfer barriers, resulting in a rapid CO2 hydrate formation with reaction times of even 15 minutes with additive promotion. Carbon dioxide hydrate formation was carried out in mild operating conditions, such as pressure values of 30 bar and temperature of 2-3 °C. The maximum value of storage capacity was 62.3 Nm 3 /m 3 in presence of SDS with a reaction time of 30 minutes. Gas storage capacity values are consistent with or rather greater - in case of SDS - than that observed by other authors. Results on CO2 hydrate formation are preparatory to investigation on other applications of industrial interest. In particular, our research activities will focus on CO2 separation from gas mixture, especially in case of biogas upgrading, and CO2 replacement in methane hydrates. Acknowledgments The authors would like to thank Consorzio IPASS Scarl, Italy for providing laboratory personnel and materials. References [1] A. Scondo, A. Sinquin, Effect of additives on CO2 capture from simulated flue gas by hydrates formation in emulsion –Proceedings of the 7th International Conference on Gas Hydrates (ICGH 2011), Edinburgh, Scotland, United Kingdom, July 17-21, 2011. [2] Davison J, Thambimuthu K, Technolgies for Capture of Carbondioxide. In: 7th International Conference on Greenhouse Gas Control Technologies (GHGT-7); Vancouver, 2004. [3] E.S. Kikkinides, R.T. Yang, S.H. Cho, Concentration and recovery of CO2 from flue-gas by pressure swing adsorption, Ind. Eng. Chem. Res. 1993;32:2714–2720. [4] R. Sivaraman, The Potential Role of Hydrate Technology in Sequestering Carbon Dioxide. Gas Tips, 2003 [5] C.A. Hendriks, K. Blok,W.C. Turkenburg, The Recovery of Carbon Dioxide from Power Plants in Climate and Energy, Kluwer Academic Publishers, Dordrecht, The Netherlands, 1989. [6] A. Chakma, A.K. Mehrotra, B. Nielsen, Comparison of chemical solvents for mitigating CO2 emissions from coal-fired power-plants, Heat Recovery Syst 1995; 15:231–240. [7] Herzog HJ, Drake E, Adams E, CO2 Capture, Reuse, and Storage Technologies for Mitigating Global Climate Change, White Paper Final Report 1997 DOE: 66. [8] Aaron D, Tsouris C, Separation of CO2 from flue gas: A review. Separation Science and Technology 2005; 40:321-348. [9] Nguyen Hong Duc, F. Chauvy, J.M. Herry - CO2 capture by hydrate crystallization – A potential solution for gas emission of steelmaking industry – Energy conversion and management 2007, 48:1313-1322. [10] Sum, A. K., Koh, C. A., Sloan, E. D. Clathrate Hydrates: From Laboratory Science to Engineering Practice. Ind. Eng. Chem. Res. 2009; 48: 7457-7465. [11] S. Arca, L. Poletti, R. Poletti, E. D’Alessandro. Upgrading of biogas technology through the application of gas hydrates. Proceedings of the 7th International Conference on Gas Hydrates (ICGH 2011), Edinburgh, Scotland, United Kingdom, July 17-21, 2011. [12] Sloan, E. D., Koh, C.A., 2008. Clathrate hydrates of natural gases, third ed. CRC Press, Taylor &Francis Group, Boca Raton. 81
[13] Kang S.P., Lee H., Lee C.S., Sung W.M. Hydrate phase equilibria of the guest mixtures containing CO2, N2 and tetrahydrofuran. Fluid Phase Equilibria, 2001;85(1-2):101-109. [14] H. Tajima, A. Yamasaki, F. Kiyono, Energy consumption estimation for greenhouse gas separation processes by clathrate hydrate formation, Energy 2004; 29:1713–1729 [15] Linga P., Adeyemo A. and Englezos P. Medium-pressure clathrate hydrate/membrane hybrid process for postcombustion capture of carbon dioxide. Environmental Science & Technology, 2008;42(1):315-320. [16] Di Profio, P., Arca, S., Germani, R., Savelli, G., 2005. Surfactant promoting effect on clathrate hydrate formation: are micelles really involved? Chemical Engineering Science 60, 4141-4145. [17] Kalogerakis N, Jamaluddin AKM, Dholabhai PD, Bishnoi PR. Effect of surfactants on hydrate formation kinetics. (SPE 25188). Proceedings of SPE International Symposium on Oilfield Chemistry, New Orleands, 1993. [18] Zhong, Y., Rogers, R.E., 2000. Surfactant effects on gas hydrate formation. Chemical Engineering Science 55, 4175-4187. [19] Ganji, H., Manteghian, M., Sadaghiani Zadeh, K., Omidkhah, M.R., Rahimi Mofrad, H., 2007. Effect of different surfactants on methane hydrate formation rate, stability and storage capacity. Fuel 86, 434-441. [20] L. Brinchi, B. Castellani, M. Filipponi, F. Rossi, G. Savelli – Investigation on a novel reactor for gas hydrate production - Proceedings of the 7th International Conference on Gas Hydrates (ICGH 2011), Edinburgh, Scotland, United Kingdom, July 17-21, 2011. [21] Liu N, Gong G, Liu D, Xie Y. Effect of additives on carbon dioxide hydrate formation. Proceedings of the 6th International Conference on Gas Hydrates (ICGH 2008); Vancouver, 2008. [22] Torré JP, Dicharry C, Ricaurte M, Daniel-David D, Broseta D. CO2 capture by hydrate formation in quiescent conditions: in search of efficient kinetic additives. Energy Procedia 2011;4:621-628. [23] M. Mork, Gudmundsson. Hydrate crystallization rate in a continuous stirred reactor: experimental results and a bubble-to-crystal model. In: Proceedings of the 4th international conference on gas hydrates, vol. 2; 2002. p. 813–8. [24] Iwasaki et al. Continuous natural gas hydrate pellet production by process development unit. - Proceedings of the 5th international conference on gas hydrates, vol. 4; 2005. p. 4003. [25] Hideo Tajima, et al. Continuous gas hydrate crystallization process by static mixing of fluids. - Proceedings of the 5th international conference on gas hydrates, vol. 1; 2005. p. 1010. [26] Dwain F. Spencer. US Patent: methods of selectively separating CO2 from a multicomponent gaseous stream; 2000. [27] G. K. Anderson, Enthalpy of dissociation and hydratation number of carbon dioxide hydrate from the Clapeyron equation – J. Chem. Thermodynamics 2003;35:1171-1183 82
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Proceedings e report 90
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ECOS 2012 : the 25 th International
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Advisory Committee (Track Organizer
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The 25 th ECOS Conference 1987-2012
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VOLUME VI CONTENT VI. 1 CARBON CAPT
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-----------------------------------
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» Personal transportation energy c
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» Excess enthalpies of second gene
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VOLUME IV IV . 1 - FLUID DYNAMICS A
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» Exergy analysis and genetic algo
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» Optimal lighting control strateg
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» Stability and limit cycles in an
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PROCEEDINGS OF ECOS 2012 - THE 25 T
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Fig. 2. The exergy destruction of M
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ineffectiveness of the catalyst, in
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[ P EXmth EX SNG] ESR F where EXm
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Fuel inputkW 728221 203771 237719 3
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Not only at desined Rc (the ratio o
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4. DISCUSSION The graphic exergy an
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Figure 9(a) illustrates the energy
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Engineering Technical Conferences &
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generally there are four kinds of m
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However, even under the off-design
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Fig. 3. 600MW supercritical coal-fi
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CO2 rich loading(molCO2/molMEA) 0.4
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Net efficiency (%) 40.28 30.29 26.4
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Fig. 11. Schematic diagram of heat
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Page 60 and 61: Applied Thermal Engineering 2010;30
Page 62 and 63: Abstract: PROCEEDINGS OF ECOS 2012
Page 64 and 65: Fig. 1. Solution diagram of „four
Page 66 and 67: K ~ K 1 eK 1a p K 1a iK mK
Page 68 and 69: Oxygen recovery rate, % 105 95 85 7
Page 70 and 71: Calculated optimal compressor press
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Page 74 and 75: The net amount of the flue gas leav
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Page 78 and 79: Energy efficiency, % 34,00 33,00 32
Page 80 and 81: points efficiency increase related
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Page 86 and 87: Figure A4. Thermoflex flow sheet of
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Page 92 and 93: these factors. A sensitivity analys
Page 94 and 95: methane slip contributes to 13% of
Page 96 and 97: As can be seen in Fig. 5 the impact
Page 98 and 99: References [1] Eurobserv’er, The
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Page 102 and 103: in which CO2 is separated from H2,
Page 104 and 105: dimensions of water droplets and wa
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Page 116 and 117: 3.3 - Utilising waste heat All exis
Page 118 and 119: 4.5 - Suomusjärvi olivine deposits
Page 120 and 121: material will change from a few % t
Page 122 and 123: Fig. 5 Schematic diagram of the PFB
Page 124 and 125: 8. Combined SO2 capture and CO2 min
Page 126 and 127: Fig. 10 Carbonate- (left) and sulph
Page 128 and 129: [13] Ekdahl, E., Idman, H. Statemen
Page 132 and 133: HEAT Fig. 1. Scheme and main reacti
Page 134: (raw) materials pre-heating and AS
Page 137 and 138: Fig 3- Aspen Plus® model 110
Page 139 and 140: Table 4. Elemental and XRD analysis
Page 141 and 142: the ÅA CSM route. The content of M
Page 145 and 146: moisture - 0,2237 ash - 0,0876 LHV
Page 147 and 148: 2.2 CFB plant For the current momen
Page 149 and 150: The CO2 emission factor which indic
Page 151 and 152: The CO2 emission factor calculated
Page 153 and 154: Appendix A Fig A.1. Simulation mode
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Page 157 and 158: Table A.1. Calculated parameters at
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References [1] Pfaff I., Oexmann J.
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with a CC installation could be avo
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2.3. Basic CHP plant indices. The b
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3. Off-design calculations The main
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Fig. 6. CHP plant efficiency Fig. 7
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amount of steam delivered to the he
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[5] Lukowicz H., Mroncz M.: Analysi
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water removal is feasible by coolin
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Figure 2. Sketch of the suggested P
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a b Figure 5. a) Exergy balance of
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The basis of comparison of each met
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Figure 7a. Impact of S/CATR on PCU
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However, more energy duty is requir
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Abstract: PROCEEDINGS OF ECOS 2012
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3.1. JACOBIAN-ASPEN Interface ASPEN
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Fig. 3. Triple Pressure Bottoming S
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As seen from Table 1, the mass flow
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4. Conclusion Fig. 5. Partial Emiss
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[19] Yantovski E., Shokotov M., Sho
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investigation and the developing of
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University of L’Aquila and German
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hydrogen combustion technology at d
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eversibility of a pre-treated synth
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Fig. 1. TG curves collected for spe
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(see Fig 5). Carbon dioxide uptake
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period is reduced to the first 15 c
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CO2 capture capacity up to 150 th c
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the way for biogas utilisation is t
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projectand is described in the foll
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4. Pilot plant tests In order to de
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Concerning the absorption reaction,
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with Regeneration (AwR), consists i
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[25] Aspen Plus 2004.1. Cambridge,
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systems for fuel drying waste strea
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heated in a heat exchanger placed i
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Fig. 2. Lower heating value of fuel
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Acknowledgements The results presen
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large amount of CO2 [1,5-7]. APCr a
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N 1 i ( x x i n 1 m ) 2.3. Carbon
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DTA analysis of the untreated APCrs
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Table 4. Relative Error (%) of the
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CaO HCl CaCl H O 193kJ / mol (
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[1] M. Fernández Bertos, S.J.R. Si
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2. Process development 2.1. Backgro
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to dissolve the chloride salts prec
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The remaining 25% (5 ml/min) of the
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Table 6. Experimental conversions o
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p p 1 1. 5 p H 1 1. 5 2O p mi
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Calculating from the Aspen Plus mod
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[11] Mattila, H.-P., Experimental s
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Mg2SiO4(s) + 2CO2(g) →2MgCO3(s) +
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(Mg/Fe) of the mineral rock, Mg-sil
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Figure 2. Effect of Mg/Fe ratio of
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Figure 4 shows that an increase in
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Figure 5. Process flow diagram of M
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2. Only cold utility is needed belo
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extraction process at 400 °C (~ 62
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Table A2. Extraction equations and
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[13] Teir S, Kuusik R, Fogelholm CJ
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In the area of coal technologies al
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Tabel 1. Characteristics quantities
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N m eT 4a ~ T cp T4a 1 ( K
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Auxiliary power rate of ASU, % 40 4
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[8] Buhre B.J.P., Elliott L.K., She
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1.1 - Cement Manufacturing The ceme
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2. Numerical model The purpose of t
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-0.309x15.77x2 2.085x3 240x4 12.53x
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Table 4 - Results of the optimizati
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1. Define the studied system (in th
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cycle) or a lignin extraction plant
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limiting factor for the maximum siz
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Table 5. Key data for the four ener
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Global CO 2 emissions [ktonnes/yr]
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for biofuels and the investment cos
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The possibility to capture CO2 from
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[17] Berglin N, Andersson L. Proces
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Therefore NL Agency (an agency of t
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2.2.2. Pinch analysis Pinch analysi
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3. Case study 3.1. Plant and proces
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Te 1000 mp era 900 tur 800 e [°C 7
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Application of the approach led to
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The advantage of dynamic models is
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e equal at both time intervals and
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2.5. Selecting the number of TSs Se
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A) Time Slices for solar thermal en
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The first step of procedure is to p
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cTSs demand TS solar TSs 0 2 4 6 8
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In the presented paper a framework
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[5] Erdil E, Ilkan M, Egelioglu F.
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district energy network simulation
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were decreased by 10°C.All scenari
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Site 3 Heat sources Heat load Site
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3.2.2. Input data and assumptions A
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Fig.7 shows the operation forecast
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[13] TERMIS Operation User Guide, 7
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Polygeneration is a term used to de
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The increase in energy utilization
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are available for an entire year, 8
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6. Extensions to core methodology 6
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thermal storage and possible suppor
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laterites. Ore Geology Reviews, v.
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gasification [15], hybrid biomass g
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the second reactor. In this unit, s
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The variables effect was evaluated
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atio, as well as the shift-syngas f
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Fig. 4. Effect of operating tempera
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SDG has slight effect on the syngas
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[26.] Castle WF. Air separation and
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1. Introduction - Firenze University Press

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