How are you sending mail? PHP or SMTP? Are you sending mail in batches-delayed or immediate?
If you are using php, have you experimented with the -f option? Does your host allow php mail?
If it's SMTP, is the user name correct and the password correct? Do you have to have a user name or full email address there? Is "SMTP Secure Connection" checked and shouldn't be?
It's a good idea to use the same email address is all three places you can set an email address in vB IMO.
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