This is caused by the account sending more than the limit set for free hosting per hour; if I'm not mistaken that limit is currently 100 emails/hr, although that was from a post in late 2011 so it may have changed since then. That said, in the last hour, I can see the account has attempted approximately 310 emails; to get more emails/hr, you would need to upgrade to premium, so it may not be a bad idea to see if it's possible to reduce the number of emails you're sending to below 100/hr to try and fix the greylisting for the moment.