In the production of vermicular graphite cast iron, the allowable range of residual magnesium content in molten iron after treatment is very narrow, amounting to only 0.008%. Therefore, thermal analysis technology was used to quickly evaluate the vermiculation and inoculation level of molten iron at the furnace itself, thus allowing the molten iron to be adjusted in time. The additives in the sample cups play a crucial role in obtaining cooling curves with remarkable characteristics. In this study, either FeS2 or FeSi75 additives were added to one chamber of a double-chamber sample cup made of resin sand, in which the cavities of the double chambers were spherical with diameters of 30 mm. The thermal analysis curves of molten iron in the double-chamber sample cup were acquired using a double channel temperature recorder, and the solidified spherical samples were analyzed quantitatively. The influence of FeS2 or FeSi75 additives on both the cooling curves of molten iron and the graphite morphology were investigated. The experiment’s results indicated that when 0.05% FeS2 is added to one chamber of the sample cup, the cooling curve changes to the solidification pattern of gray cast iron. The continuous increase in the FeS2 additive has little influence on the shape of cooling curves, and the graphite changes form from vermicular to flaked. When the amount of FeS2 is increased from 0.05% to 0.10%, the resulting graphite changes from D-type and E-type to A-type and B-type. When the amount of FeS2 reaches 0.20%, the morphology of graphite is short and thick. With the increase in the amount of FeSi75 additive, the amount of spherical graphite in the sample cup increases gradually, and the vermicularity decreases gradually from 89% to 46%. With the increase in FeSi75 additive from 0 to 0.45%, we observed that the average diameter of graphite decreases from 23 μm to 19 μm and then increases to 22 μm. The eutectic recalescence temperature shows a decreasing trend, and the cooling curve gradually changes from a hypoeutectic to a eutectic pattern. The addition of 0.05% FeS2 or 0.45% FeSi75 to one chamber is more appropriate for a double-chamber sample cup with two spherical cavities with diameters of 30 mm. This lays a foundation for the optimization of additives when using the double-chamber sample cup for thermal analysis of vermicular graphite cast iron.
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