First, "not equal" operator in Construct is "<>", so change event 30 to "Pick Sprite by evaluating Sprite.AnimationFrame<>3". Or you can use "Sprite compare frame =3" and then invert this condition.
Once you picked all sprites with frame<>3, you can't pick another sprite with frame=3 in the same event. To do this, you need a family which will act as a different object. Add Sprite to a family, then use "Pick Family with animation frame=3" in event 31, and pin Sprite to the Family.