Hi @Tyler Miller ,
Welcome to our forum!
Does this issue occur recently? If so, have you done any specific operation?
And what's the version of your Outlook? (File > Office Account > About Outlook). Please make sure you have upgraded your Outlook to the latest version.
If you are using Microsoft account, it's suggested that you could try to use the Microsoft Support and Recovery Assistant, which works by running tests to figure out what's wrong and offers the best solution for the identified problem.
If it doesn't work, please try the following troubleshooting steps:
1.Considering that it may be caused by the damage of the profile/data file in the Outlook client, it is suggested that you could try to create a new profile (Control Panel>Mail>Show Profiles>add) and add the account for testing to check if there are some differences.
2.If the issue persists, based on my research on the error "The set of folders cannot be opened. The information store could not be opened", i found a thread mentioned that it may be related to iCloud. If you have enabled iCloud, it's suggested that you could try the solution as Steve P_1960 mentioned:
Hope to help you!
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