Cobalt-containing catalysts exhibit good performance in the advancement of efficient catalytic oxidation reactions. However, achieving an optimal balance between reaction kinetics and adsorption, usually governed by variable spin states of Co ions, to enhance the performance remains a significant challenge. This study aims to develop a convenient compositional tuning strategy to achieve such balance in stable CoxZn1-xSn(OH)6 perovskite hydroxides. We systematically investigate the effect of varying spin state on a chosen representative catalytic oxidation reaction, namely peroxymonosulfate activation and tetracycline hydrochloride removal. The magnetic properties analysis reveal that the content of octahedral Co2+ ions with high-spin state increases with Co content (x) and reaches 59.5 % in Co0.5Zn0.5Sn(OH)6. Experimental results and DFT calculations reveal that the spin states transition of Co2+ ions enhance the interaction between Co and O atoms. This enhanced interaction not only improves the reactivity due to the formation of highly covalent Co-OH bonds that serve as catalytically activated charge transfer channels, but also optimizes the suitable adsorption energy of PMS molecules at −3.52 eV for Co0.5Zn0.5Sn(OH)6. Consequently, Co0.5Zn0.5Sn(OH)6 shows superior catalytic activity, achieving nearly 100 % antibiotic removal efficiency within just 10 min, surpassing previously reported catalysts. These findings underscore the potential of compositional tuning spin states of transition metal ions in advancing oxidation processes and designing innovative catalysts.
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