Hi Corey,
UPDATE: Corey determined that Domain, SPF, DKIM, and DKIM2 needed to be showing as Verified for domain to be able to be selected. I added that check as #1 below.
1. Please make sure your email domain is showing Verified for Domain, SPF, DKIM, and DKIM2. You may do this by navigating to your Email Communication Service -- Settings -- Provision domains blade and making sure that all four columns show as Verified, similar to below:
2. The Data location for the Communication Service and the Email Communication Service must be the same in order to add the domain. For example, if Communication Service Data location is Europe then the Email Communication Service Data location must also be Europe.
You can see Data location on Overview blade of each service, shown below for ECS:
Please click Accept Answer and upvote if the above was helpful.
Thanks.
-TP