When you reinstall OneCare and you already have a subscription active, you activate with the same LiveID that you originally subscribed with. You cannot use the key again.
If you don't recall the LiveID you used for your subscription, you will need to contact support who can provide that information to you using your Key and/or contact information.
How to reach support (FAQ) - http://forums.microsoft.com/WindowsOneCare/ShowPost.aspx?PostID=2421771&SiteID=2
Alternatively, sign in at http://billing.microsoft.com with email addresses that you have set up as LiveIDs and one will show your subscription listed - that would the LiveID to use to activate the reinstall.
-steve