Dielectrophoresis (DEP) has been extensively used in lab-on-a-chip systems for trapping, separating, and manipulating of micro particles suspended in a liquid medium. The most widely used analytic model, the dipole model, provides an accurate prediction on the crossover frequency of submicron particles, but cannot explain the significant drop in crossover frequency of larger particles. Here, we present numerical simulations using the Maxwell stress tensor (MST) and finite element method to study the size effect of the DEP crossover frequency of spherical polystyrene particles suspended in de-ionized water. Our results show that the surface conductance due to the electrical double layer plays a key role, and the size dependency of crossover frequency obtained by the MST method agrees reasonably well with published experimental data. The exponents of the power law are approximately -1.0 and -4.3 for smaller (diameter < 4.6 μm) and larger particles (diameter > 4.6 μm), respectively. The free surface charge distribution reveals that the charge begins accumulating on the particle equator for particle diameters larger than a critical diameter of 4.6 μm, a result not captured by the dipolar approximation. This method may be extended to analyze bioparticles with complex shapes and composition, and provides new insights into the interpretation of dielectrophoresis applications using lab-on-a-chip systems.