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Ensure you have enough space in the first place for the 2nd drive for whatever you're trying to download.
Click that and add the drive/folder you want to use.
So you CAN add an entire drive as your second or third or whatever library, but that drive must be totally empty.
So instead, it's best to create an empty folder ON that drive, and add that as the other library folder.
As others have said, you should have or be able to make a new, empty folder on your secondary hard drive, call it for example "My Second Steam Library", using Windows to just create an empty folder on the drive.
Then go to the settings menu mentioned here by others above, and once you get there, "My Second Steam Library" should now appear in the list of folders that you can add for downloads.
The folder must be totally empty to be able to add it to the list.
Now as far as why you can no longer but once were able to download to that drive, that might be an underlying issue that needs looking into first.
then you add new steam lib folder again then its the new patch location "?:\SteamLibrary" move old lib to athta place reboot steam, that worked for me , i dont recall need to even repair the steam lib, but that is same places at steam storage manager.
Thank you guys so much! I got the issue fixed!