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Currently, the elimination of gaseous pollutants—particularly nitrogen oxides—has emerged as a significant concern. Among various deNO_x technologies, selective catalytic reduction (SCR) has gained prominence as the primary approach for NO_x abatement, owing to its superior performance. In this study, novel low-temperature SCR catalysts were developed by regulating the pH value and doping cobalt based on a V₂O₅-MoO₃/TiO₂ (VMT) catalyst. The results show an increased SCR performance with 82.8% and 91.1% for catalysts after pH (=10) modification (VMT-10) and (1 wt%) Co/pH (=10) modification (1CoVMT-10), respectively. H₂-TPR, NH₃-TPD, XPS and DRIFTS confirmed that the pH regulation transformed polymerization V species into isolated V⁵⁺=O, thus leading to an increase in the number of acid sites, which enhanced the NH₃ and NO₂ adsorption capacity. Furthermore, the DRIFTS study indicated that the NH₃-SCR reaction over 1CoVMT-10 followed the E–R and L–H mechanism.