Hi Linda,
Think of a Workspace like a bucket which includes the boards and the people you're collaborating with. We have more info on what a Workspace is here: https://support.atlassian.com/trello/docs/what-are-trello-workspaces/
Within a Workspace, you can have multiple boards and users.
Similarly, you can be part of multiple Workspace (e.g. if people invite you to their Workspaces).
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For the Workspace that exceeds the limit, and where you're having some difficulties removing collaborators - it's likely that some of these boards may have been created by other people.
We're working on rolling out some new features to make managing this a little bit more easily, particularly with the user limits change rolling out. For now, please see below for our suggested workaround.
For context, in a Free Workspace - Workspace admins aren't admins of all boards by default, only the boards they create.
Workaround
In the meantime, there's a handy workaround. Simply start a 14 day free trial of Premium via this link: https://trello.com/en/free-trial (no credit card required or obligation to stay). Once done, per our paid Workspace admin capabilities - you should automatically become admin of those individual board/s, and be able to remove the users.
Hope this helps! Let us know how things go, and if you have any further questions.
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