Abstract
Nitrogen oxides (NOX) and volatile organic compounds (VOCs) are generated during the coal-fired power plant’s combustion. They can be simultaneously removed in SCR (selective catalytic reduction) region. Herein, the performance of V-W/Ti and Fe-V-W/Ti synthesized by wet impregnation in removing NOX and VOCs was evaluated. XPS (X-ray photoelectron spectroscopy) result indicated that a redox cycle of Fe2+ + V5+ ⇌ Fe3+ + V4+ could form electron vacancy through electron transfer. Besides, the mechanisms of NH3-SCR and VOCs catalytic oxidation were explored with in situ DRIFTS experience and DFT calculation. On Fe-V-W/Ti, in situ DRIFTS study found more absorption sites of NH3, and different intermediates during simultaneously removal process. DFT calculation demonstrated that absorption energy of O2 was decreased and O = O bond was lengthened with Fe doped. Both V-W/Ti and Fe-V-W/Ti followed the L–H mechanism and shared a common NH3-SCR pathway: \({NO\left(g\right)+\frac{1}{2}O}_{2}\left(g\right)+{e}^{-}\to {{NO}_{2}}^{-}(ads)\stackrel{{\mathrm{NH}}_{4}^{+}(\mathrm{ads})}{\to }{NH}_{4}{NO}_{2}(\mathrm{ads})\to {N}_{2}\left(g\right)+{H}_{2}O\left(g\right)\). However, the bidentate nitrate and monodentate nitrate were also revealed on Fe-V-W/Ti, which combined with NH4+ and decomposed into N2 and H2O, or N2O and H2O, respectively. The detected NH2 species combined with NO on the Fe-V-W/Ti, following the E-R mechanism. As for VOCs, the intermediates of benzene and toluene were revealed by in situ DRIFTS study, and detailed Mars–van Krevelen mechanism was discovered.
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The datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.
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Acknowledgements
The financial supports of the National Key R&D Program of China (No. 2018YFB0605200) are greatly acknowledged by the authors, and Guangdong Key Laboratory of Efficient and Clean Energy Utilization, South China University of technology (No. 2013A061401005). We thank the State Key Laboratory of Coal Combustion, Huazhong University of Science and Technology for providing the copyright support of Materials Studio software for this paper.
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Zhuofan Chen wrote the first draft of this paper, carried out DFT calculation, and performed XPS & in situ DRIFT characterization; Yanfen Liao proposed the conceptualization and supervised the project, reviewed & edited the first draft of this paper, and acquired the sponsored funding; Yin Chen assisted data curation and investigated many previous studies of NOx and VOCs removal; Xiaoqian Ma reviewed & edited the first draft of this paper and gave comments.
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Chen, Z., Liao, Y., Chen, Y. et al. In situ DRIFTS FT-IR and DFT study on Fe-V-W/Ti removal of NOx and VOCs. Environ Sci Pollut Res 29, 81571–81582 (2022). https://doi.org/10.1007/s11356-022-21244-4
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DOI: https://doi.org/10.1007/s11356-022-21244-4