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A large number of Xinjiang Zhundong coal was found in China. Its high content of alkali metals can cause serious fouling/slagging problems which may lead to economic losses. It is significant to control the release of alkali metals from Zhundong coal during the combustion. Si-Al additives are used to capture Na released from the Zhundong coal. In this work, a combination of experimental research and quantum chemical calculation was used to study the effect of coal ash on the capture of alkali metal in Zhundong high alkali Coal and the related mineral evolution mechanism during melting processes. The experiments were done with Zhundong coal/coal ash mixtures at 900–1200°C. The behavior mechanism of coal ash capturing alkali metals was analyzed from the perspective of mineral microstructure features by using XRD, ICP and quantum chemical calculation methods. The results show that during the process of combustions, complex chemical reactions occur among minerals after sodium is released from the coal and captured by the coal ash. The coal ash’s ability to capture sodium in Zhundong high alkali coal rises firstly, and then gradually decreases with the rise of temperature. It shows the best capture performance for sodium at 1000∼1100°C. The maximum efficiency of sodium absorption can reach to 50.6%. The coal ash shows a rather high efficiency compared with other additives. Furthermore, metals in Zhundong coal have opposite directions of migration. The Na, K, Al, Ca, and Mg migrated to the coal ash far away from the reaction interface, and the Fe and Mn were moved to the coal from the reaction interface. The original minerals of Zhundong coal mainly include calcium sulfate hydrate, quartz and kaolinite. Investigating the capture mechanism, it indicates that O (26) and O (22) in kaolinite have electrophilic reaction with Na+ and K+ easily, which would promote the rupture of aluminum-oxygen bonds. The O2- of alkali metal or alkaline earth metal oxide would easily have nucleophilic reaction with Si (6) and Si (8) and prompt the rupture of bridging oxygen bonds (Si-O-Si). Kaolinite would be transformed into some other minerals that contains Na+ or K+ which have trend to form eutectics or evaporate into the flue gas easily, the degree of fouling and slagging on heating surface can be reduced based on these two most easily reaction paths.