How can I sync a previous library with a current one?

I got a new computer for Christmas and synched my Apple data with it. I have not synched any new music using my computer for several months now, because I either purchase it from iTunes on my phone or use another music service.
I recently downloaded an album from a third party site (bandcamp.com) and want to add my new Shakey Graves album to my phone. The issue is, for some reason my library is missing several gigs worth of music.
Music that I have on my phone from a previous library, but apparently don't have the files for on my new computer.
Am I able to just add this album onto my phone (or something along those lines) without disturbing my current content on my phone?
Thank you for your replies.

Libraries cannot be synced.
The correct way to handle a new computer is to copy the ENTIRE iTunes folder from the old comptuer to the new computer.  At this point, the same library exists on both comptuers and the user simply starts using the new computer and library.  The old computer can then be wiped or disposed of.
Syncing to the new computer at this point will remove all content from the device and replace it with content from the new computer/library.

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