Tailoring Lewis Acidic Metals and SO42-Functionalities on Bimetallic Mn-Fe Oxo-Spinels to Exploit Supported SO42-in Aqueous Pollutant Fragmentation
- Tailoring Lewis Acidic Metals and SO42-Functionalities on Bimetallic Mn-Fe Oxo-Spinels to Exploit Supported SO42-in Aqueous Pollutant Fragmentation
- 김상훈; 김종식; 최윤정
- Issue Date
- Chemical engineering journal
- VOL 413, 127550
- MnX) served as reservoirs to accommodate the Lewis acidic Fe/Mn and SO42-, whose properties were tailored by altering the metal compositions (X). The production of supported SO4radical dot- via the radical dotOH → SO4radical dot- was of high tangibility, as confirmed by their electron paramagnetic resonance spectra coupled with those simulated. A concave trend was observed in the plot of the Lewis acidic strength of Fe/Mn versus X of MnX with the minimum at X ~ 1.5. Hence, Mn1.5 could expedite radical dotOH liberation from the surface most proficiently and therefore exhibited the greatest initial H2O2 scission rate, as corroborated by its lowest energy barrier needed for activating the radical dotOH → SO4radical dot-. Meanwhile, a volcano-shaped trend was found in the plot of SO42- concentration versus X of MnX (other than Mn3). This could tentatively increase the collision frequency between radical dotOH and SO42- on the surface of Mn1.5, as partially substantiated by its second largest pre-factor among the catalysts. Therefore, Mn1.5 exhibited the highest phenol consumption rate (-rPHENOL, 0) among the catalysts, which was ~ 20-fold larger than those for SO42--modified Fe2O3 and NiO, w; Generation of SO4radical dot- anchored on metal oxides via radical transfer from radical dotOH to surface SO42- functionality (radical dotOH → SO4radical dot-) is singular, unraveled recently, and promising to decompose aqueous refractory contaminants. The core in furthering supported SO4radical dot- production is to reduce the energy required to accelerate the rate-determining step of the radical dotOH → SO4radical dot- (radical dotOH desorption), while increasing the collision frequency between the radical dotOH precursors (H2O2) and H2O2 activators (Lewis acidic metals) or between SO42--attacking radicals (radical dotOH) and supported SO4radical dot- precursors (SO42-). Herein, Mn-substituted Fe3O4 oxo-spinels (MnXFe3-XO4
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