Newtonian Gravity:
Your biggest effect after the monopole term and $J_2$ will be all of the other multipole terms representing the realistic gravitational field of the Earth expressed in spherical harmonics. $J_2$ is the largest of them by far (order 1E-03), but certainly not the only one. I believe the next three in line include $J_{22}$ which represents/includes the lowest azimuthal (longitudinal) term. See for example the Wikipedia subsection The deviations of Earth's gravitational field from that of a homogeneous sphere where you will see where $J_2$ fits in. You will find the coefficients of the multipole terms for the scalar potential field expressed in various places, out to different orders. You will then have to do the math to find the vector gradient of the field which will give you the acceleration terms as you've shown for $J_2$. Or, you might find tables with the expressions and coefficients already evaluated for you.
Some approximate values just to give you an idea (copied from 1, 2 and 3):
J2 = 1.1E-03
J3 = -2.5E-06
J4 = -1.6E-06
J22 = -1.8E-06
I've written more about using the Geopotential coefficients in the as-yet unanswered question For the mathematical relationship between J2 (km^5/s^2) and dimensionless J2 - which one is derived from the other?.
General Relativity:
I've extracted this bit about a commonly used expression for corrections due to General Relativity from this answer, which includes several sources/references where you can read more about this kind of calculation.
Remember that your coordinates for oblateness are for the Earth, and the ecliptic (where you find the Sun and Jupiter for example) is tilted by roughly 23 degrees, and the Moon's orbit has it's own plane and complex orbital motion.
You either need to treat at least the Sun (which also moves!), Earth and Moon (next in line would come Jupiter and Venus) as additional bodies whose motion needs to be integrated numerically (you can do that first, store it, then interpolate from it) or you can interpolate their positions from an existing ephemeris. You can search this site for references to spice
or Skyfield
for interpolators of the NASA JPL Development Ephemerides for example.
Although I'm not so familliar with GR, I'm going to recommend an equation that seems to work well and seems to be supported by several links. It is an approximate relativistic correction to Newtonian gravity that is used in orbital mechanics simulations. You will see various forms in the following links, most with additional terms not shown here:
The following approximation should be added to your Newtonian gravity terms, where $\mathbf{r}$ and $\mathbf{v}$ represent the distance and velocity vectors between each object who's acceleration you are evaluating and each object for which the GR term you feel has a strong-enough gravitational field to consider. Or you can do it for all pairs if you don't want to bother with the housekeeping.
$$\mathbf{a_{GR}} = GM \frac{1}{c^2 |r|^3}\left(4 GM \frac{\mathbf{r}}{|r|} - (\mathbf{v} \cdot \mathbf{v}) \mathbf{r} + 4 (\mathbf{r} \cdot \mathbf{v}) \mathbf{v} \right).$$
jpl-horizons
, spice, pyephem and skyfield for starters. $\endgroup$