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Vanadium-based catalysts have been extensively applied for the synergistic control of NO x and chlorinated organics. However, how the vanadia species affect the reaction activity and products distribution, and what are the dominant reaction sites of these vanadia species are still unknown. Herein, we investigated the reaction characteristics of monomeric and polymeric vanadate domains for the catalytically synergistic elimination of NO x and chlorobenzene (CB). Density functional theory (DFT) calculations and experimental investigations have been combined to clarify the effects of different vanadyl species on the synergistic reaction. It was noted that the main adsorption site of CB on the monomeric domain was V−OH bond, and that on the polymeric one was VO bond. The monomeric vanadyl was favorable for converting the Lewis VO into Brønsted V−OH, which provided sufficient H protons for HCl formation, whereas the polymeric species could effectively retain the V 4+ /V 5+ redox cycle, and yielded superior activity in CB catalytic oxidation (CBCO) reaction. However, the abundant oxygen vacancies and the inclined accumulation of Cl by forming the V−Cl bands led to significant polychlorinated byproducts on the polymeric vanadyl catalysts. Our work gives the first insight into different vanadate domain effects on the synergistic reaction, and is expected to provide theoretical basis for efficient design of the vanadium-based catalysts toward multipollutants elimination.

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