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

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

Chongqing Key Laboratory of Catalysis and New Environmental Materials, College of Environment and Resources, Chongqing Technology and Business University, Chongqing 400067, China

Received Date: 22 December 2017
Revised Date: 19 January 2018

Fund Project: This work was supported by the National Key R&D Plan (2016YFC02047), the National Natural Science Foundation of China (51478070, 21501016, 21777011), the Innovative Research Team of Chongqing (CXTDG201602014), and the Natural Science Foundation of Chongqing (cstc2017jcyjBX0052).

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.
- MnO_x,
- g-C₃N₄,
- Synergistic catalysis,
- Photo-thermal,
- In situ DRIFTS,
- NO oxidation
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通讯作者: 陈斌, bchen63@163.com

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

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通讯作者: 陈斌, bchen63@163.com

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