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The interactions between Fe 2 SiO 4 and ZnO play an essential role in the recovery of zinc from copper slag. The dissolution and substitution mechanism of ZnO in fayalite were investigated by using TG-DSC, XRD, PPMS DynaCool, XPS, Mossbauer and SEM-EDS analyses and compared with MS calculation results. The results indicate that the dissolution and substitution are actually processes of the penetrating dissolution of Zn(II) ions that can be divided into three steps: 1) ZnO dissociates into Zn 1-y O and Zn(II) ions; 2) Zn(II) penetrates the gap of the octahedron outer layer to substitute Fe(II) sites in the internal structure of SiOFe(II) (M2) to form (Fe 2-x , Zn x )SiO 4 ; 3) Fe(II) is forced to migrate to the surface of (Fe 2-x , Zn x )SiO 4 to form (Zn 1-y , Fe(II) y )O. These findings can be derived the occurrence state and distribution of zinc in copper slag theoretically., (Copyright © 2018 Elsevier B.V. All rights reserved.)