You must create both a Communication Service and a Email Communication Service in Azure.
As at August 2024, the Azure Portal does not allow users to add MailFrom addresses unless they have applied for a quota increase. You must send a Quota increase for email domains request by raising a support request in Azure Portal. If you don't want to send a quota increase request, or you are waiting for it to be processed, then you must use the auto-generated "donotreply@your-domain.com" sender address.
Use the "Send Test" form at the bottom of the page to test your settings, then click "Save Changes".