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镁掺杂对用于NH-SCR的VO-MoO /TiO催化剂活性和磷耐受性的影响研究。

Investigation of Mg-doping effect on the activity and P tolerance of VO-MoO /TiO catalysts for NH-SCR.

作者信息

Qi Liqiang, Li Silan, Wang Wen, Li Jingxin

机构信息

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding, 071003, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2023 May;30(22):62880-62891. doi: 10.1007/s11356-023-26548-7. Epub 2023 Mar 23.

DOI:10.1007/s11356-023-26548-7
PMID:36952161
Abstract

VO-MoO/TiO catalyst modified by Mg was studied to obtain higher NOx SCR activity and higher P, SO, and HO resistance than the VO-MoO/TiO. The results show that Mg modification can promote the denitration activity of VO-MoO/TiO catalyst, and the maximum NOx removal efficiency of Mg-SCR catalyst was 97.5%; the optimum reaction temperature and flow rate were 350℃ and 1200 mL/min, respectively. Mg doping can broaden the reaction temperature window of the catalyst, and the denitration efficiency can reach more than 87% at 300℃. PO solution was prepared as poisoning precursor and mixed with catalyst to simulate the process of catalyst P-poisoning. The step-wise study showed that Mg-SCR and Mg-SCR catalyst displays higher durable resistance to P, SO, and HO than original catalyst. The degree of denitrification efficiency reduction of Mg-SCR is 4% smaller than that of Mg-SCR after passing SO. Mg-SCR catalyst achieves 88% denitrification efficiency at 350 °C after simulating phosphorus poisoning. The catalysts have been characterized by X-ray diffraction, Brunner - Emmet - Teller, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscop, programmed temperature desorption, and programmed temperature reduction. The obtained results suggested that the Mg doping made the active components more dispersed on the surface of the supports, improved the thermal stability of the catalyst, promoted the transition of VOx from monomeric state to polymerized state, inhibited the interaction between P and V, and protected the acid site.

摘要

研究了用镁改性的VO-MoO/TiO催化剂,以获得比VO-MoO/TiO更高的氮氧化物选择性催化还原(SCR)活性以及更高的抗磷、抗硫和抗水性能。结果表明,镁改性可促进VO-MoO/TiO催化剂的脱硝活性,镁-SCR催化剂的最大氮氧化物去除效率为97.5%;最佳反应温度和流速分别为350℃和1200 mL/min。镁掺杂可拓宽催化剂的反应温度窗口,在300℃时脱硝效率可达87%以上。制备了磷酸溶液作为中毒前驱体并与催化剂混合,以模拟催化剂磷中毒过程。逐步研究表明,镁-SCR和镁-SCR催化剂比原始催化剂对磷、硫和水具有更高的耐久性抗性。经过二氧化硫后,镁-SCR的脱硝效率降低程度比镁-SCR小4%。模拟磷中毒后,镁-SCR催化剂在350℃时脱硝效率达到88%。通过X射线衍射、布鲁诺尔-埃米特-泰勒法、扫描电子显微镜、透射电子显微镜、X射线光电子能谱、程序升温脱附和程序升温还原对催化剂进行了表征。所得结果表明,镁掺杂使活性组分更分散在载体表面,提高了催化剂的热稳定性,促进了VOx从单体态向聚合态的转变,抑制了磷与钒之间的相互作用,并保护了酸性位点。

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