Usually when you lift cargo, the volume of the cargo is tiny compared to the volume of the lifting gas. Picture a huge blimp with a tiny gondola underneath.

With an aerogel infusion, the volume of the aerogel is the same as the volume of the lifting gas. Picture a huge blimp lifting a huge-blimp-sized lump of something underneath. Even aerogel, light as it is, adds up.

In other words - it's barely useful, and the only reason it works is because of the square-cube law: the weight of the envelope goes up as the square of the dimension, while the lifting power goes up as the cube. If you want to fill the volume with something, you lose the scaling advantage.

The fact that an aerogel-filled blimp might still conceivably be neutrally buoyant is actually testament to how incredibly light aerogel is. If you filled the Hindenburg with water, it would be more than half the weight of the Empire State Building.