Thesis (MScEng)--Stellenbosch University. / ENGLISH ABSTRACT: Carbon dioxide (CO2) is classified as the main greenhouse gas (GHG) contributing to global warming. Estimates by the Intergovernmental Panel on Climate Change (IPCC) suggest that CO2 emissions must be reduced by between 50 to 85% by 2050 to avoid irreversible impacts. Carbon capture and storage (CCS) strategies can be applied to de-carbonize the emissions from fossil-fueled power plants. Compared to other CCS techniques, post-combustion capture (PCC) is most likely to be implemented effectively as a retrofit option to existing power plants. At present however CCS is not yet commercially viable. The main challenge with CCS is to reduce the inherent energy penalty of the CO2 separation stage on the host plant. Seventy-five to eighty percent of the total cost of CCS is associated with the separation stage. There are several technologies available for separating CO2 from power plant flue gas streams. Reactive absorption with aqueous amine solutions has the ability to treat low concentration, low pressure and large flux flue gas streams in industrial-scale applications. It is most likely to be the first technology employed commercially in the implementation of CCS. The energy required for solvent regeneration however, is high for the standard solvent used in reactive absorption processes, i.e. MEA. This leads to a reduction in thermal efficiency of the host plant of up to 15%. Alternative solvent formulations are being evaluated in an attempt to reduce the energy intensity of the regeneration process. The main objective of this study was to establish a novel, simplified thermodynamic method for solvent screening. Partial solubility parameters (PSPs) were identified as the potential basis for such a method. The major limitation of this approach is that the model doesn’t account for effects from chemical reaction(s) between materials, e.g. CO2 reacting with aqueous alkanolamine solutions; considering only the effects from dissolution. The EquiSolv software system was developed based on PSP theory. The Hansen 3-set PSP approach was used to describe the equilibrium behaviour of CO2 absorbing in task specific solvents. The Hansen theory was expanded to a 4-set approach to account for contributions from electrostatic interactions between materials. The EquiSolv program was used successfully to screen large sets of solvent data (up to 400 million formulations) in the search for suitable alternative solvent formulations for CO2 absorption. The secondary objective of this study was to evaluate the ability of the proposed PSP model to accurately predict suitable alternative solvents for CO2 absorption through preliminary experimental work. A series of CO2 absorption experiments were conducted to evaluate the absorption performance of predicted alternative solvent formulations. The predicted alternative solvent formulations exhibited a significant improvement in absorption performance (up to a 97% increase in the measured absorption capacity) compared to conventional solvent formulations. Statistical analysis of the experimental results has shown that there is a statistically significant concordant relationship between the predicted and measured rankings for the absorption performance of the predicted solvent formulations. Based on this it was concluded that PSP theory can be used to accurately predict the equilibrium behaviour of CO2 absorbing in task specific solvents. Recently ionic liquids (ILs) have been identified as potential alternatives to alkanolamine solutions conventionally used for CO2 absorption. Absorption experiments were conducted as a preliminary assessment of the absorption performance of ILs. Results have shown ILs to have significantly improved performance compared to conventional alkanolamine solvents; up to a 96% increase in the measured absorption capacity compared to conventional solvents. Future work should focus on developing task specific ionic liquids (TSILs) in an attempt to reduce the energy intensity of solvent regeneration in CO2 absorption processes. / AFRIKAANSE OPSOMMING: Koolsuurgas (CO2) word geklassifiseer as die vernaamste kweekhuis gas (GHG) wat bydra to globale verwarming. Beramings deur die Interregeringspaneel oor Klimaatsverandering (IPKV) toon aan dat CO2 emissies teen 2050 verminder moet word met tussen 50 en 85% om onomkeerbare invloede te vermy. Verskeie koolstof opvangs en bergings (KOB) strategieë kan toegepas word ten einde die koolstof dioksied konsentrasie in die emissies van kragstasies wat fossielbrandstowwe gebruik, te verminder. Naverbranding opvangs (NVO) is die mees aangewese KOB tegniek wat effektief toegepas kan word op bestaande kragstasies. Tans is KOB egter nog nie kommersieël lewensvatbaarvatbaar nie. Die hoof uitdaging wat KOB in die gesig staar is om die energie boete inherent aan die CO2 skeidingstap te verminder. Tussen vyf-en-sewentig en tagtig persent van die totale koste van KOB is gekoppel aan die skeidingstap. Daar is verskeie metodes beskikbaar vir die skeiding van CO2 uit die uitlaatgasse van kragstasies. Reaktiewe absorpsie met waterige oplossings van amiene kan gebruik word om lae konsentrasie, lae druk en hoë vloei uitlaatgasstrome in industriële toepassings te behandel. Dit is hoogs waarskynlik die eerste tegnologie wat kommersieël aangewend sal word in die toepassing van KOB. Die oplosmiddel wat normalweg vir reaktiewe absorpsie gebruik word (d.w.s. MEA) benodig egter ‘n groot hoeveelheid energie vir regenerasie. Dit lei tot ‘n afname in die termiese doeltreffendheid van die voeder aanleg van tot 15%. Alternatiewe oplosmiddelstelsels word tans ondersoek in ‘n poging om the energie intensiteit van die regenerasieproses te verminder. Die hoof doelwit van hierdie studie was om ‘n nuwe, ongekompliseerde termodinamiese metode te vestig vir die keuring van alternatiewe oplosmiddels. Parsiële oplosbaarheidsparameters (POPs) is geïdentifiseer as ‘n moontlike grondslag vir so ‘n metode. Die model beskryf egter slegs die ontbindings gedrag van materiale. Die effekte van chemise reaksie(s) tussen materiale, bv. die tussen CO2 en waterige oplossings van alkanolamiene, word nie in ag geneem nie. Die POP teorie het gedien as grondslag vir die ontwerp van die EquiSolv sagteware stelsel. Die Hansen stel van drie POPs is gebruik om die ewewigsgedrag te beskryf van CO2 wat absorbeer in doelgerig-ontwerpte oplosmiddels. Die Hansen teorie is verder uitgebrei na ‘n stel van vier POPs om die bydrae van elektrostatiese wisselwerking tussen materiale in ag te neem. Die EquiSolv program is verskeie kere met groot sukses gebruik vir die sifting van groot stelle data (soveel as 400 miljoen formulasies) in die soektog na alternatiewe oplosmiddels vir CO2 absorpsie. Die sekondêre doelwit van die studie was om die vermoë van die voorgestelde POP model om geskikte alternatiewe oplosmiddels vir CO2 absorpsie akkuraat te voorspel, te ondersoek deur voorlopige eksperimentele werk. ‘n Reeks CO2 absorpsie eksperimente is gedoen ten einde die absorpsie werkverrigting van die voorspelde alternatiewe oplosmidels te ondersoek. ‘n Verbetering in absorpsie werkverrigting van tot 97% is gevind vir die voorspelde oplosmiddels vergeleke met die van oplosmiddels wat tipies in die industrie gebruik word. Statistiese ontleding van die eksperimentele resultate het getoon dat daar ‘n beduidende ooreenstemming tussen die voorspelde en gemete rangskikking van die voorspelde oplosmiddels se werkverrigting bestaan. Dus kan POP teorie gebruik word om die absorpsie van CO2 in doelgerig-ontwerpte oplosmiddels akkuraat te beskryf. Ioniese vloeistowwe (IVs) is onlangs geïdentifiseer as moontlike alternatiewe oplosmidels vir die alkanolamien oplossings wat normaalweg gebruik word vir CO2 absorpsie. Absorpsie eksperimente is gedoen ten einde ‘n voorlopige raming van die absorpsie werkverrigting van IVs te bekom. Daar is bevind dat IVs ‘n beduidende verbetering in werkverrigting toon in vergelyking met die alkanolamien oplosmiddels wat normaalweg gebruik word. ‘n Verbetering in absorpsie werkverrigting van tot 96% is gevind vir die voorspelde IV-bevattende oplosmiddels vergeleke met die van oplosmiddels wat tipies in die industrie gebruik word. Die fokus van toekomstige navorsing moet val op die ontwikkeling van doelgemaakte ioniese vloeistowwe (DGIVs) in ‘n poging om die energie intensiteit van oplosmiddel regenerasie in CO2 absorpsie prosesse te verminder.