As the initial process of preparing transparent conductive oxide materials from monobutyltin chloride (MBTC) to tin oxide, the hydrolysis and condensation of MBTC to form a dimer Sn2 play a critical role. However, the specific mechanism of this process is still unclear. Here we develop a step-by-step searching method based on density functional theory calculation and empirical chemical criteria to determine possible reaction pathways and reveal the most likely reaction mechanism. The wave function analyses of various intermediate species provide more insights into the changes of atomic charge population, chemical bond strength, and coordination situation of central tin in the reaction process. Further investigation on the ring-containing Sn2 reveals the existence of unique three-center four-electron (3c-4e) interactions to stabilize the four-membered Sn2O2 ring structure, which serves as the true driving force for dimerization reaction. These results provide a more detailed understanding of the hydrolysis and condensation process of MBTC and would be helpful for the future optimization of the preparation process of tin oxide films.
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