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THERMAL PROPERTIES OF SC CO2 BY MC SIMULATIONS 411 FIGURE 7 Speed of sound vs. density diagram for carbon dioxide. Legend as in Fig. 2. is regarded as a sensitive test since it involves not only the correct representation of heat capacities, but also of the first derivatives of the volume. The overall predictions can be considered excellent. The largest deviations are once more found for the lower temperature high-density region. These deviations are consistent with the deviations found in density. The largest error in the speed of sound is approximately 5%, which is considerably lower than the errors found in the properties involved in its definition, CP and k [see Eq. (11)], in the extended critical region, possibly due to a compensation of errors in the quotient of these two quantities. This suggests that speed of sound as a single property may provide a less sensitive test than heat capacity and isothermal compressibility, each by itself, particularly in the near-critical region. For instance, CO2 at 330 K is sufficiently close to critical conditions that a clearly defined peak is observed in k (Fig. 4) and CP (Fig. 5), yet there is no equivalent minimum in u (Fig. 7), which requires a lower temperature to appear. CONCLUSIONS The parameters for the 2CLJQ model for CO2 were o b t a i n e d b y M o ̈ l l e r a n d F i s c h e r [ 2 ] b y fi t t i n g experimental saturation properties. It has been shown that these parameters give good predictions of VLE properties [2]. In this work, the transfer- ability of the parameters to the supercritical region has been studied through a comprehensive comparison between calculated values of several thermodynamic properties for CO2 and their experimental values (represented by the Span – Wagner EOS) as well as against the 2CLJQ EOS. We have presented simulation results for the isobaric heat capacity, volume expansivity, isother- mal compressibility and combinations of these quantities such as the speed of sound and the Joule – Thomson coefficient for which experimental data are available. It has been shown that these parameters can be used with confidence for the prediction of thermodynamic properties, including those of industrial interest such as the speed of sound or Joule – Thomson coefficient, for CO2 in the supercritical region, except in the extended critical region. This region is larger than usual due to the differences between the critical point predicted for the 2CLJQ model for CO2 and the experimental critical point. Unfortunately, this region is extre- mely important for the so-called CO2-driven process where the tunability of CO2 plays a key role. Therefore, care must be taken when using this potential to model CO2 in this extended critical region. We also show that the agreement of calculated and experimental values for speed of sound does not necessarily guarantees good agreement in the isobaric heat capacity and the first derivatives of the volume. Deviations between the 2CLJQ EOS and simu- lations, which can be quite large in the two-phase region [22], appear to become less important at higher supercritical temperatures and pressures. The present results, however, are limited to CO2 only. More extensive testing with a wider range of fluids will be required before the predictive capabilities of the 2CLJQ can be fully assessed in the supercritical region.PDF Image | Thermal Properties of Supercritical Carbon Dioxide
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