ITunes - "There were problems downloading some purchased items. The required file can not be found."

I'm having a few problems in iTunes.
I have had iTunes for years through many different devices. I work in music education, so I have music for work and music for home all in my same iTunes account.
In the past year, I have gotten another new computer (a laptop - so I keep my iTunes on an external drive) and also tried my hand at making a separate library for my work music.
Now on summer vacation, I was finally trying to sort out all of my music and get it to the correct iTunes library so that I could sync up my iPods. I hit a brick wall so to speak. In iTunes, I see albums I purchased on iTunes and I try to click the cloud symbol to download them from my cloud. Sometimes, it does NOTHING (no download starts) and sometimes I get an error message like "The iTunes Library can not be saved. An unknown error occurred (13010)." I have also noticed that some things I have purchased have NO cloud symbol and they are not available to be played either (can't click on them - they are greyed out). In addition, I have been getting an error that says it is unknown error 21 - a problem downloading.
It really seems like I have many separate issues but since I don't know what the problem really is, I'm having trouble searching for the answer. I tried searching the problems on the forum and even tried a few things like deleting the genius and extras files everyone was talking about, but it didn't help. Apple won't help me unless I pay them, so I'm trying you first. Thanks for any thoughts you might have.
I have a Windows 8 PC.
I have Home Sharing and Match.
I use iPod Nano, iPod Touch, iPad 2.

P.S the error message i got during the download is (err = - 5000)
Thanks in advance

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