Accurate
density data and a predictive equation of state (EoS)
for the CO2–CH4 system are significantly
important for the application of natural gas purification and carbon
capture, utilization, and storage (CCUS). In this work, densities
of the CO2–CH4 binary system with CO2 mole fractions ranging from 0.0998 to 0.8988 were measured
at temperatures of 313–353 K and pressures of 3–18 MPa
using a magnetic suspension balance, and the compressibility factors
and the relative combined standard uncertainties were also calculated
correspondingly. The PC-SAFT EoS was employed for the density modeling,
and the PR EoS was used for comparison. The measured density data
in this work and experimental density data from the literature were
used to optimize the binary interaction parameter k
ij
in the PC-SAFT EoS and PR EoS. The
predicting abilities of PC-SAFT and PR EoS with the optimized k
ij
were compared to the case
without binary interaction (k
ij
= 0). The PC-SAFT EoS with the optimized k
ij
had better performance than the PR
EoS with optimized k
ij
, and it could predict the density properties of the CO2–CH4 system accurately, with an average absolute
deviation (AAD) of 1.16%. Modelings from PC-SAFT with and without
the optimized k
ij
were
then compared with the measured densities obtained in this work. The
relative deviations for the calculation from PC-SAFT with the optimized k
ij
were within the range from
−3.93 to 2.94%. Moreover, the CO2–CH4 binary systems with CO2 mole fractions of 0.7985
and 0.8988 in this work can be regarded as CO2-rich fluids,
and their density reductions compared with pure CO2 were
evaluated for the measured density data and the values calculated
from the modified PC-SAFT.