Thanks Doug, got that fixed, the server the CA server the DC was pointing to had been turned off. Installed one locally on that DC, so I no longer get that error. I configured the NPS to match the config in your screenshots.
The clients are now prompted to accept a new certificate, which makes sense.
But now instead I get "Connection failed." when trying to connect from a Mac.
If I log on to the controller and do a test of the radius, it returns Test Completed, but with ACCESS_REJECTED. I'm guessing that is expected as it never asks for a password and I'm assuming it's just testing the actual radius connection?