If you previously synced to your VPO document library, you can stop syncing these folders at any time. When you stop syncing a folder, you disconnect the folder on your computer from the library on the server. You can always sync the library to your computer again.
You can also pause syncing. This allows you to temporarily stop syncing a folder without disconnecting it from the library on the server.
Instructions Update 4/2/2020:
Click on the blue cloud icon from your task manager toolbar (bottom right of screen). Select 'More' and then 'Settings'. Choose the 'Account' tab. This will bring up a dialog box with a list of all the synced folders.