Abstract:【Objective】Dissolution reactions of clay minerals are one of the essential processes contributing to natural soil acidification and mineral weathering. However, the surface reaction mechanism of mineral dissolution remains unclear. 【Method】The strong electric field generated by the surface charges of minerals induces a new type of covalent bonding between the oxygen (O) atoms on the mineral surface and the hydrogen (H+) ions, a phenomenon known as polarization-induced covalent bonding (PICB). In this study, we selected montmorillonite (MMT), illite (ILI), and kaolinite (KLI) to explore the interfacial reaction mechanisms promoting the dissolution of clay minerals by PICB using mineral dissolution analysis and hydrothermal experiments. 【Result】The dissolution density of mineral elements increases with decreasing pH, and the initial stage of mineral dissolution aligns with three processes of chemical weathering: desalination, desilicification, and ferrallitization. The PICB significantly enhanced the H+ adsorption energy density (γH(0)), and the absolute value of γH(0) increased with the decrease of pH, indicating an interaction between H+ and the mineral. Also, the surface was stronger under low pH conditions, and a consistent critical pH of 3.0 was observed based on both the theoretical analyses of γH(0) and the dissolution density of mineral elements as a function of pH. At a pH < 3.0, the PICB was significantly enhanced, resulting in a notably weakened Si-O bonding energy and a substantial increase in the dissolution efficiency of silicate minerals. Although the dissolution behaviors of various minerals exhibited significant variations in response to pH, they can be described as a function of γH(0), indicating that γH(0) has an important influence on the structure of clay minerals. Moreover, the enhancement of γH(0) resulted in a higher content of SiO2 in the hydrothermal reaction products of MMT, accompanied by a subsequent reduction in the residual products represented by Al2O3. 【Conclusion】This study quantified the impact of H+-mineral bonding on the chemical weathering of minerals and revealed that the PICB between H+ and surface O atoms of minerals enhanced the γH(0) of H+ on the mineral surface and weakened the Si-O bond energy, thus significantly affecting the dissolution reactions of clay minerals. The results of this study provide theoretical insights for proposing targeted modulation techniques aimed at enhancing the structural stability of minerals.