It seems you cannot remove unused licenses from your account. However, what you can do is to archive these licenses, so they won't be displayed any more. To do so, select the license, then click on the Archive link on the right side below the license key.
This will not really remove the license from your account but it won't show up any more in your list of licenses unless you specifically select to show archived licenses.
Thanks for signing up for Jira Ops! I’m Matt Ryall, leader for the Jira Ops product team at Atlassian. Since this is a brand new product, we’ll be delivering improvements quickly and sharing updates...
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