In the height of production, Diffwys was quoted as being the largest in the region, but i think it had a head start as it was the first to begin work (?). However, as Merddinemrys points out it depends on the factors that have been used. Output, employment, land mass e.t.c.
Oakeleys shear size (land mass) is due to several smaller workings being swallowed up to create one big working.