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Energies 2021, 14, 387 19 of 32 Energies 2021, 14, x FOR PEER REVItEhWeoretical calculation that, at a temperature below 10 ◦C, the equilibrium pressures o2f0tohfe33 CO2 hydrates are lower than those of CH4 hydrate. Figure 11. Phase diagram (equilibrium temperature as a function of pressure) for pure CO2 and Figure 11. Phase diagram (equilibrium temperature as a function of pressure) for pure CO2 and pure CH4 gas hydrates [50]. Reprinted from Applied Energy, Vol 280/edition number 115,843, pure CH4 gas hydrates [50]. Reprinted from Applied Energy, Vol 280/edition number 115,843, Quang-DuLe et al. Influence of the initial CH4-hydrate system properties on CO2 capture kinetics, Quang-DuLe et al. Influence of the initial CH4-hydrate system properties on CO2 capture kinetics, Copyright (2020), with permission from Elsevier. Copyright (2020), with permission from Elsevier. CO2 and CH4 molecules form both the type SI of crystal-structure hydrate that con- CO2 and CH4 molecules form both the type SI of crystal-structure hydrate that consists sists of six medium cages and two small cages. During the hydrate formation, the CO2 of six medium cages and two small cages. During the hydrate formation, the CO2 molecule, molecule, which is slightly larger than the CH4 molecule, only occupies the medium cages, which is slightly larger than the CH4 molecule, only occupies the medium cages, while the while the methane molecule occupies both medium and small cages. As a result, more methane molecule occupies both medium and small cages. As a result, more CH4 can form CH4 can form in the early stages. The heat of CO2 hydrate formation (−57.9 kJ/mol) is in the early stages. The heat of CO2 hydrate formation (−57.9 kJ/mol) is greater than the greater than the heat of dissociation of CH4 hydrates (54.5 kJ/mol). Therefore, a replace- heat of dissociation of CH4 hydrates (54.5 kJ/mol). Therefore, a replacement reaction occurs ment reaction occurs in the later stages due to the favorable exothermic process [51]. The in the later stages due to the favorable exothermic process [51]. The exothermic nature of exothermic nature of the CO2 hydrates formation provides the heat of methane dissocia- the CO2 hydrates formation provides the heat of methane dissociation and increases the tion and increases the storage temperature. Therefore, the storage’s temperature is a crit- storage temperature. Therefore, the storage’s temperature is a critical parameter that has to ◦ ical parameter that has to remain below 10.5 °C to avoid CO2 dissociation and CH4 hydrate remain below 10.5 C to avoid CO2 dissociation and CH4 hydrate re-formation. re-formation. Lee et al. have examined CH4 and CO2 molecule distribution over the two cage sites 13 Lee et al. have examined CH4 and CO2 molecule distribution over the two cage sites (i.e., S and M) by Magic Angle Spinning Carbon-13 Nuclear Magnetic Resonance (MAS C (i.e., S and M) by Magic Angle Spinning Carbon-13 Nuclear Magnetic Resonance (MAS NMR) into a hydrated sample. This analysis shows a limit to the CO2 replacement degree. 13 ItwCaNseMstRim)aintetodtahahty6d4r%ateodfmsaemthpalnee.cTahnisbeanreacloyvsiesrasbhloewfrsomaltihmeiNttGoHthresCerOv2oirre,prelascueltminegn,t adftegrroeen.lyItvwiasthesetiemxachteadngtheaotf64C%Oo,fma petrhoadnuecctahnybderarteecowvietrhabaleCfOrom/CtHheNraGtiHo orefs1e.r8voirr, 224 gresauteltrinagt,eaqfuteilriborniluymvicaotnhdeiteioxcnh.aOntgheeorwf CisOe,2,aakpinreotdicuctetshtysdhroawteedwitthatatCheOr2/eCpHla4ceramtieonotf re1a.8ctoiorngriesaatlemr aotsteqcoumilipblreiutemincolensdsithioan.fiOvtehehrowuirsse,,ankdintheeticptreosdtuschtohwyeddrathteartetshueltrsepwlaitche- amCeOnt/reCaHctiornatisoaolmf 1o.stCconmsepqleutenitnlyl,e5ss0%thaonf mfiveethaonuersin, acnluddtehdeipnrothdeurcetsheyrvdorairtecarensublets 24 rewpiltahcaedCbOy2/COH4 rantidotohfe1re.fCoorensaecqoumenptlleyt,e5m0%ethoafnmeertehcaonveeirnycilsundoetdpinostshibelree[s5e2rv].oircanbe 2, replTachedmbiyxCtuOre2,oafncdatrhbeornefdoiroexaidceomanpdlemteemtheatnheangeasreicsopvrersyenistninotthpeoshsyibdlrea[t5e2r]e.servoir whenTthe CmOixtuisreinojefcctaerdbointoditohxeidNeGaHnd. Amdeitshaasmneitgoaestiaslp. rpersoepnotsiendththeehfyodllroawteinregsperovloyi-r nwomheinaltehqeuCaOtio2nisfiinttjedctteodtihnetoexthperNimGeHn.taAldiastasmtoitmoeatsaulr.eptrhoepogsaesdmthixetuforell’osweqinugilipborliyunmo- condition in hydrate form [53]. mial equation fitted to the experimental data to measure the gas mixture’s equilibrium (8) Theequilibriumpressure ismeasuredinMPa,thetemperatureisin°K,andy is the mole percent of carbon dioxide in the vapor phase. The above equation was fitted for a temperature between 273 K and 288 K, while the maximum pressure of the CO2 was 2 7 ln Peq = 175.3− 89009 +0.07392× y+ 1.1307× 10 − 23.392× y +3.9566×10−5 × y2 (8) condition in hydrate form [53]. T T2T ln=175.3−89009+0.07392× +1.1307× 10 −23.392× +3.9566×10 × T PDF Image | Energies 14
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