Can non-VxRail ESXi hosts be added as a new workload domain within a VxRail on VCF environment?
This is not supported.
The workload domain can consist of one or more VxRail clusters.
The VxRail cluster is the building block for the VI Workload Domain. See, VMware Cloud Foundation on VxRail Architecture Guide VCF 5.2 on VxRail
When adding a VI workload domain in VxRail on VCF, the VxRail VI configuration needs to be added. See, Create a VxRail VI Workload Domain in the SDDC Manager UI