i'm sure those older sata 2 drives are ready to be retired. rather than an add-on card i'd get another 3 tb or so drive like you already have and replace one of the older sata 2 drives. that would give the best performance. especially if you are concerned abut speed, then those old drives are molasses slow compared to even a new sata spinning drive.
i use WD blue sata drives myself and have 3 of them installed (1 tb and 2 tb models). the new ones read and write a ton faster than any of the old spinning drives i've ever used. not as fast as ssd for sure, but well over 100 MB/s which is great for a spinning disk.
but if you do decide on an add-on card, then the sata option is the best choice. but for just static data drive, speed is...