In Nd2Fe14B-based permanent materials, the intergranular phase has a strong influence on magnetic properties. Here, we study the effect of partial substitution of Fe by Co on the microstructure to gain insight into the mechanism of enhancing magnetic properties of (Nd0.8Pr0.2)2.2Fe14−xCoxB (x = 0, 1.75, 2, 2.25) alloys. Our results show that the substitution Co for Fe changes the magnetic properties obviously by tuning the chemistry and distribution of the intergranular phase between hard magnetic grains. In particular, for (Nd0.8Pr0.2)2.2Fe12Co2B (x = 2) alloy, no obvious intergranular phase is observed. And the through-thickness homogeneity and ultrafine microstructure with an average size of ~25 nm is obtained, which produces maximum product ((BH)max) of 141 kJ/m3, 29% higher than that of quaternary alloy. Our findings provide a new idea to design prospective permanent alloys with increased magnetic properties by tuning the distribution and chemical composition of the intergranular phase.
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