2 Thermodynamics of Solutions of CO2 with Effects of Pressure and Temperature 5 Sara Spilimbergo and Ireneo Kikic

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1 1 Introduction to Dense Phase Carbon Dioxide Technology 1 Giovanna Ferrentino and Murat O. Balaban 2 Thermodynamics of Solutions of CO2 with Effects of Pressure and Temperature 5 Sara Spilimbergo and Ireneo Kikic 2.1 Introduction Thermodynamics of liquid vapour phase equilibria Calculation of g Calculation of f Calculation of the liquid vapour phase equilibria Application to CO2 H2O system model Non-electrolyte models Electrolyte models Thermodynamics of solid vapour equilibria List of symbols 31 3 Experimental Measurement of Carbon Dioxide Solubility 37 Giovanna Ferrentino, Thelma Calix, Massimo Poletto, Giovanna Ferrari, and Murat O. Balaban 3.1 Introduction Solubility of carbon dioxide in water Definition and brief review of early studies Physical properties associated with the phase diagram of carbon dioxide Effect of pressure and temperature on carbon dioxide solubility in water Experimental methods for carbon dioxide solubility measurement Analytical methods Synthetic methods Review of experimental results Conclusions 66

2 4 Effects of Dense Phase Carbon Dioxide on Vegetative Cells 67 Osman Erkmen 4.1 Introduction Gases used for inactivating microorganisms Effect of DPCD on vegetative microorganisms Effect of DPCD on bacterial cells Effect of DPCD on vegetative forms of fungi, pests and viruses Factors affecting the sensitivity of microorganisms to DPCD Effect of CO2 physical states Effect of temperature and pressure Effect of CO2 concentration Effect of agitation Effect of water content Effect of pressurization and depressurization rates Effect of pressure cycling Effect of microbial type Effect of initial microbial number Effect of physical and chemical properties of suspension Effect of culture conditions and growth phases Injured microorganisms Effect of combination processes Effect of type of system Treatment time and inactivation kinetics Mechanisms of microbial inactivation by DPCD Solubilization of CO2 under pressure into suspension Cell membrane modification 88

3 4.5.3 Cytoplasmic leakage Intracellular ph decrease Key enzyme inactivation Inhibitory effect of molecular CO2 and HCO3 - on metabolism Intracellular precipitation and electrolyte imbalance Extraction of vital cellular constituents Physical cell rupture Characterization of CO2 states and survival curves Quantifying inactivation Conclusions 96 5 Effects of Dense Phase Carbon Dioxide on Bacterial and Fungal Spores 99 Patricia Ballestra 5.1 Introduction Inactivation of bacterial spores by DPCD Effect of temperature Effect of pressure Effect of ph and aw of the treatment medium Susceptibility of different bacterial spores Effects of combination treatments Mechanisms of bacterial spore inactivation Inactivation of fungal spores by DPCD Conclusion Effects of DPCD on Enzymes 113 Murat O. Balaban 6.1 Introduction Effects of gas bubbling 118

4 6.3 Alteration of the protein structure Studies with multiple enzymes Effects on specific enzymes Alpha-amylase Acid protease Alkaline protease Gluco-amylase Lipase Pectinesterase (PE) Pectin methyl esterase (PME) Polyphenol oxidase (PPO) Tyrosinase Lipoxygenase Peroxidase Alkaline phosphatase Myrosinase Hydrolases Conclusions and suggestions The Kinetics of Microbial Inactivation by Carbon Dioxide under High Pressure 135 Maria G. Corradini and Micha Peleg 7.1 Introduction The survival curve Primary models Secondary models the effect of pressure alone The temperature effect and that of other auxiliary factors 143

5 7.2.4 Dynamic treatments Application of the models to published experimental data Primary model derivation Concluding remarks List of symbols Applications of DPCD to Juices and Other Beverages 157 Murat O. Balaban and Xiaojun Liao 8.1 Introduction Juices processed with DPCD Orange juice Apple juice Mandarin juice Grapefruit juice Watermelon juice Coconut water Guava puree Grape juice Pear Carrot Carrot juice Peach Kiwi Melon Other beverages processed with DPCD Beer Kava kava 173

6 8.3.3 Jamaica beverage Conclusions Use of Dense Phase Carbon Dioxide in Dairy Processing 177 Giovanna Ferrentino and Giovanna Ferrari 9.1 Introduction Carbon dioxide in milk Enzymes and microorganisms in milk Application of carbon dioxide to milk Carbon dioxide addition to raw milk Carbon dioxide addition during thermal pasteurization of milk Effect of carbon dioxide addition on sensory properties of milk Dense phase carbon dioxide process Application of carbon dioxide for enzyme inactivation Application of carbon dioxide to cottage cheese production Application of carbon dioxide to yogurt and fermented products Application of carbon dioxide to casein production Casein properties Casein production by high-pressure carbon dioxide Comparison between continuous and batch systems for casein production by carbon dioxide Economic comparison between high-pressure carbon dioxide and a conventional process for casein production Conclusions Particle Engineering by Dense Gas Technologies Applied to Pharmaceuticals 199 Neil R. Foster, Raffaella Mammucari, Luu Thai Danh, and Wen Hui Teoh 10.1 Introduction Dense gas as a solvent 201

7 Rapid expansion of supercritical solutions Rapid expansion of supercritical solutions Rapid expansion of supercritical solutions with a nonsolvent Particles from gas-saturated solutions Dense gases as antisolvents Gas antisolvent process Aerosol solvent extraction system Solution-enhanced dispersion by supercritical fluids Atomized rapid injection for solvent extraction SCFs as co-solvents Depressurisation of an expanded liquid organic solvent Dense gases as aerosolisation aids (spray-drying assistance) Carbon dioxide assisted nebulisation with a bubble dryer Supercritical fluid assisted atomisation Conclusion Industrial Applications Using Supercritical Carbon Dioxide for Food 227 James T.C. Yuan and John S. Novak 11.1 Overview Past development Mechanism of microbial inactivation Effect of other gases on microbial inactivation scco2 commercialization activities Porocrit process Impact on juice quality Impact on nutrient values Impact on microbial inactivation 233

8 Impact on microbial inactivation for solid foods scco2 processing efficiencies Conclusions Outlook and Unresolved Issues 239 Luc Van Ginneken, Linsey Garcia-Gonzalez, Kathy Elst, and Frank Devlieghere 12.1 Introduction Unresolved issues Inactivation mechanism of DPCD Food quality and storage Target foods Process equipment and intellectual property Fouling, cleaning, and disinfecting Occurrence of DPCD-resistant mutants Industrial implementation and process economics Future outlook and conclusions Acknowledgements 264 References 265 Index 309