When you are trying to add a new Provider VDC to a newly deployed Cloud Director (VCD) you cannot select the vCenter instance as it is not displayed. Here attached is a screenshot of the issue:
VMware Cloud Director 10.5.1.1
The cause for this issue is because you enabled a tenant dedicated vCenter that will not be used as a provider VDC while registering the vCenter instance to VCD.
To resolve this issue we first need to unregister the previously registered vCenter instance from VCD following this document: Unregister a vCenter Instance From Your VMware Cloud Director
Now we need to re-add the vCenter instance again to VCD GUI following the same process, but only this time by turning off the Enable tenant access option following this document: Attach a vCenter Instance to VCD