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4.1 INTRODUCTION In 1869, Thomas Andrews (Andrews, 1869) first recognized the presence of the critical point, which gave birth to a new world of critical phenomena and supercritical fluid science. A SCF is defined as a substance above its critical temperature TC and critical pressure PC . This definition should arguably include the clause “but below the pressure required for condensation into a solid”, however this is commonly omitted as the pressure required to condense a SCF into a solid is generally impracticably high. However, we will refer to any fluid above its critical temperature as ‘supercritical’ regardless of its pressure or density. The critical point represents the highest temperature and pressure at which the substance can exist as a vapour and liquid in equilibrium. The phenomenon can be easily explained with reference to the phase diagram for pure carbon dioxide (Figure 4-1). This shows the areas where carbon dioxide exists as a gas, liquid, solid or as a SCF. The curves represent the temperatures and pressures where two phases coexist in equilibrium (at the triple point, the three phases coexist). The gas–liquid coexistence curve is known as the boiling curve. If we move upwards along the boiling curve, increasing both temperature and pressure, then the liquid becomes less dense due to thermal expansion and the gas becomes denser as the pressure rises (Licence et al., 2004). Eventually, the densities of the two phases converge and become identical, the distinction between gas and liquid disappears, and the boiling curve comes to an end at the critical point. The critical point for carbon dioxide occurs at a pressure of 7.38 MPa and a temperature of 304.128 K. The Table 4-1 and the Figure 4-2 lists the critical data of SCFs most frequently used in chemical reactions. A single supercritical fluid can be tuned to mimic the properties (dielectric constant, solubility) 46PDF Image | MOLECULAR SIMULATION STUDIES IN THE SUPERCRITICAL REGION
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