潘磊, 卢平, 徐贵玲, 陈丹丹, 黄震, 宋涛. Mn/Fe改性碳基催化剂低温脱硝特性[J]. 中国电机工程学报, 2021, 41(24): 8510-8519. DOI: 10.13334/j.0258-8013.pcsee.202530
引用本文: 潘磊, 卢平, 徐贵玲, 陈丹丹, 黄震, 宋涛. Mn/Fe改性碳基催化剂低温脱硝特性[J]. 中国电机工程学报, 2021, 41(24): 8510-8519. DOI: 10.13334/j.0258-8013.pcsee.202530
PAN Lei, LU Ping, XU Guiling, CHEN Dandan, HUANG Zhen, SONG Tao. Low Temperature NO Reduction of Carbon-based Catalysts Modified by Mn/Fe Oxides[J]. Proceedings of the CSEE, 2021, 41(24): 8510-8519. DOI: 10.13334/j.0258-8013.pcsee.202530
Citation: PAN Lei, LU Ping, XU Guiling, CHEN Dandan, HUANG Zhen, SONG Tao. Low Temperature NO Reduction of Carbon-based Catalysts Modified by Mn/Fe Oxides[J]. Proceedings of the CSEE, 2021, 41(24): 8510-8519. DOI: 10.13334/j.0258-8013.pcsee.202530

Mn/Fe改性碳基催化剂低温脱硝特性

Low Temperature NO Reduction of Carbon-based Catalysts Modified by Mn/Fe Oxides

  • 摘要: 以椰壳活性炭为载体,以硝酸锰和硝酸铁为活性添加组分,采用硝酸氧化、等体积浸渍、中低温煅烧等相结合的方法,制备了Mn-Fe/HAC碳基催化剂。利用固定床脱硝实验台对碳基催化剂脱硝性能进行了评价,并结合傅里叶转换红外光谱(Fourier transform infrared spectroscopy,FT- IR)、N2吸附-脱附、扫描电镜(scanning electron microscopy,SEM)- mapping和X-射线光电子能谱(X-ray photoelectron spectrometry,XPS)等表征结果,探讨了碳基催化剂脱硝及其抗硫抗水机理。结果表明,Mn改性可以显著提升碳基催化剂的脱硝效率,Mn和Fe共同改性在有效提高碳基催化剂脱硝效率的基础上,使得其脱硝窗口温度下移至120℃。Mn-Fe改性催化剂的最佳负载量为7% Mn和0.5% Fe,最佳煅烧为中温400℃氮气煅烧与低温200℃空气煅烧组合煅烧法。Fe添加有效促进了Mn在碳基催化剂表面的均匀分布,并显著提高了Mn4+和表面吸附氧(Oα)的含量。在6% O2以及无水和SO2条件下,7Mn0.5Fe/HAC催化剂在温度为120℃下的脱硝效率可达82.0%,而在140-240℃脱硝效率则基本稳定在95%。Mn和Fe复合改性碳基催化剂具有良好的抗硫抗水性能,在温度为180℃、含有100 μL/L SO2和6% H2O的模拟烟气下,7Mn0.5Fe/HAC催化剂的脱硝效率可达85%以上。

     

    Abstract: Based on the carrier of coconut shell activated carbon and active components of manganese nitrate and ferric nitrate, carbon-based catalyst modified by Mn-Fe oxides was prepared by using a combined methods of nitric acid oxidation, constant volume impregnation, and medium-low temperature calcination. NO reduction of as-prepared carbon-based catalysts was carried out in a fixed-bed reactor. The mechanism of NO reduction and its resistance to SO2 and water by carbon- based catalyst was discussed on the basis of measurements of Fourier transform infrared spectroscopy (FT-IR), N2 adsorption-desorption, SEM-mapping and XPS. The obtained results indicate that Mn modification can effectively enhance NO reduction efficiency of carbon-based catalyst. And the addition of Fe and Mn not only improves NO reduction of carbon-based catalyst, but also makes window temperature downward to 120℃. The optimum loading capacity of Mn-Fe carbon-based catalyst is 7%Mn and 0.5%Fe, and the combined calcination with nitrogen calcination at 400℃ and air calcination at 200℃ is an optimal calcination method. The addition of Fe can effectively promote the uniform distribution of Mn on the surface of the carbon-based catalyst, and significantly increase the contents of Mn4+ and surface adsorbed oxygen (Oα). Under the conditions of 6% O2 and without water and SO2, NO reduction efficiency of 7Mn0.5Fe/HAC catalyst reaches 82.0% at 120℃, and can be stable at 95% at 140-240℃. Mn-Fe carbon-based catalyst has a good resistance performance to SO2 and moisture. NO reduction efficiency of 7Mn0.5Fe/HAC catalyst can reach more than 85% under the conditions of temperature of 180℃, 100μL/L SO2 and 6% moisture in the simulated flue gas.

     

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