Sorry for the late reply. I'm not sure which software you are using but this may be possible using keyboard shortcut commands. More details about his here:http://vectir.com/blog/2009/11/20/controlling-applications-with-keyboard-macros/
If keyboard shortcuts are available for adding/removing from your playlist this may be possible with a custom remote profile using this method.
If you need further assistance can you please supply more details about your setup?