If you're like me you had at one time connected one of your Reporting Services instances to a report server database that was already in use by another instance. This allows the instance to show up in the Scale-out Deployment section of the Reporting Services Configuration Manager. My problem was that the server that got joined to the original server was no longer available as it had been repurposed, and when I clicked Remove Server to remove it from my scale-out it would fail because it couldn't contact the server. After searching for a solution for quite some time I decided to look around in the report server database tables, and voila! All I had to do was remove the old server from the Keys table. I can't guarantee there won't be any side effects to this method, but it worked like a charm for me.