In order to the improvement of steel quality and dephosphorization capacity, it is vital to realize the microscopic essence of dephosphorization reaction of the slags. In this work, the temperature dependence of phosphorus distribution ratio and phosphate capacity is discussed with respect to the structure characterized by Raman and MAS-NMR. As the temperature increases from 1550°C to 1600°C, the reduction of Q0(Si) and Q0(P) weakens the formation of the Si–O–Ca–O–P linkages that can stabilize the...