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NO 3  • can compete with omnipotent • OH/SO 4  •- in decomposing aqueous pollutants because of its lengthy lifespan and significant tolerance to background scavengers present in H 2 O matrices, albeit with moderate oxidizing power. The generation of NO 3  • , however, is of grand demand due to the need of NO 2  • /O 3 , radioactive element, or NaNO 3 /HNO 3 in the presence of highly energized electron/light. This study has pioneered a singular pathway used to radicalize surface NO 3  - functionalities anchored on polymorphic α-/γ-MnO 2 surfaces (α-/γ-MnO 2 -N), in which Lewis acidic Mn 2+/3+ and NO 3  - served to form • OH via H 2 O 2 dissection and NO 3  • via radical transfer from • OH to NO 3  - ( • OH → NO 3  • ), respectively. The elementary steps proposed for the • OH → NO 3  • route could be energetically favorable and marginal except for two stages such as endothermic • OH desorption and exothermic • OH-mediated NO 3  - radicalization, as verified by EPR spectroscopy experiments and DFT calculations. The Lewis acidic strength of the Mn 2+/3+ species innate to α-MnO 2 -N was the smallest among those inherent to α-/β-/γ-MnO 2 and α-/γ-MnO 2 -N. Hence, α-MnO 2 -N prompted the rate-determining stage of the • OH → NO 3  • route ( • OH desorption) in the most efficient manner, as also evidenced by the analysis on the energy barrier required to proceed with the • OH → NO 3  • route. Meanwhile, XANES and in situ DRIFT spectroscopy experiments corroborated that α-MnO 2 -N provided a larger concentration of surface NO 3  - species with bi -dentate binding arrays than γ-MnO 2 -N. Hence, α-MnO 2 -N could outperform γ-MnO 2 -N in improving the collision frequency between • OH and NO 3  - species and in facilitating the exothermic transition of NO 3  - functionalities to surface NO 3  • analogues per unit time. These were corroborated by a greater efficiency of α-MnO 2 -N in decomposing phenol, in addition to scavenging/filtration control runs and DFT calculations. Importantly, supported NO 3  • species provided 5-7-fold greater efficiency in degrading textile wastewater than conventional • OH and supported SO 4  •- analogues we discovered previously.

jacs au

Deciphering Evolution Pathway of Supported NO3• Enabled via Radical Transfer from •OH to Surface NO3– Functionality for Oxidative Degradation of Aqueous Contaminants