Phospholipid concentration methods involve use of a dairy composition, such as buttermilk or butter serum, as a starting material. The dairy composition is subjected to a first ultrafiltration, yielding a first permeate and a first retentate. The first retentate is treated with carbon dioxide and subjected to microfiltration, yielding a second permeate and a second retentate. The second retentate is treated with carbon dioxide and subjected to a second ultrafiltration, yielding a third permeate and a third retentate. The third retentate includes at least 30 wt % phospholipids.