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When OmniFocus attempts to sync, it'll check the Keychain for any entries that match your server. If it finds one, it'll use that; otherwise, it asks for the login info at that point.

Once a sync completes successfully, OmniFocus saves the info it to the keychain if the "save to keychain" box was checked in the login panel. There isn't a separate place to enter that info in OmniFocus, in other words.

I'm not a sysadmin, but guessing on the basis of the error message you're getting, I'd double-check the URL/path you're trying to connect to. Hope this helps at least a little.