Synergistic photo-thermal catalytic NO purification of MnOx/g-C3N4: Enhanced performance and reaction mechanism

doi:10.1016/S1872-2067(18)63029-3

Abstract

Abstract:

Both MnO_x and g-C₃N₄ have been proved to be active in the catalytic oxidation of NO, and their individual mechanisms for catalytic NO conversion have also been investigated. However, the mechanism of photo-thermal catalysis of the MnO_x/g-C₃N₄composite remains unresolved. In this paper, MnO_x/g-C₃N₄ catalysts with different molar ratios were synthesized by the precipitation approach at room temperature. The as-prepared catalysts exhibit excellent synergistic photo-thermal catalytic performance towards the purification of NO in air. The MnO_x/g-C₃N₄ catalysts contain MnO_x with different valence states on the surface of g-C₃N₄. The thermal catalytic reaction for NO oxidation on MnO_x and the photo-thermal catalytic reaction on 1:5 MnO_x/g-C₃N₄ were investigated by in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). The results show that light exerted a weak effect on NO oxidation over MnO_x,and it exerted a positive synergistic effect on NO conversion over 1:5 MnO_x/g-C₃N₄. A synergistic photo-thermal catalytic cycle of NO oxidation on MnO_x/g-C₃N₄ is proposed. Specifically, photo-generated electrons (e^-) are transferred to MnO_x and participate in the synergistic photo-thermal reduction cycle (Mn⁴⁺→Mn³⁺→Mn²⁺). The reverse cycle (Mn²⁺→Mn³⁺→Mn⁴⁺) can regenerate the active oxygen vacancy sites and inject electrons into the g-C₃N₄ hole (h⁺). The active oxygen (O^-) was generated in the redox cycles among manganese species (Mn⁴⁺/Mn³⁺/Mn²⁺) and could oxidize the intermediates (NOH and N₂O₂^-) to final products (NO₂^- and NO₃^-). This paper can provide insightful guidance for the development of better catalysts for NO_x purification.

Key words: MnO_x, g-C₃N₄, Synergistic catalysis, Photo-thermal, In situ DRIFTS, NO oxidation

Peng Chen, Fan Dong, Maoxi Ran, Jiarui Li. Synergistic photo-thermal catalytic NO purification of MnO_x/g-C₃N₄: Enhanced performance and reaction mechanism[J]. Chinese Journal of Catalysis, 2018, 39(4): 619-629.

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Synergistic photo-thermal catalytic NO purification of MnO_x/g-C₃N₄: Enhanced performance and reaction mechanism

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