段晓谞, 窦金孝, 魏傲然, 赵永奇, 余江龙. 粉煤灰负载锰基催化剂低温脱硝活性及水硫抗性的实验研究[J]. 中国电机工程学报, 2022, 42(11): 4102-4111. DOI: 10.13334/j.0258-8013.pcsee.210977
引用本文: 段晓谞, 窦金孝, 魏傲然, 赵永奇, 余江龙. 粉煤灰负载锰基催化剂低温脱硝活性及水硫抗性的实验研究[J]. 中国电机工程学报, 2022, 42(11): 4102-4111. DOI: 10.13334/j.0258-8013.pcsee.210977
DUAN Xiaoxu, DOU Jinxiao, WEI Aoran, ZHAO Yongqi, YU Jianglong. Experimental Study of Mn-based Catalysts Supported on Coal Fly Ash for Selective Catalytic Reduction of NOx and Their Resistance to SO2/H2O at Low-temperatures[J]. Proceedings of the CSEE, 2022, 42(11): 4102-4111. DOI: 10.13334/j.0258-8013.pcsee.210977
Citation: DUAN Xiaoxu, DOU Jinxiao, WEI Aoran, ZHAO Yongqi, YU Jianglong. Experimental Study of Mn-based Catalysts Supported on Coal Fly Ash for Selective Catalytic Reduction of NOx and Their Resistance to SO2/H2O at Low-temperatures[J]. Proceedings of the CSEE, 2022, 42(11): 4102-4111. DOI: 10.13334/j.0258-8013.pcsee.210977

粉煤灰负载锰基催化剂低温脱硝活性及水硫抗性的实验研究

Experimental Study of Mn-based Catalysts Supported on Coal Fly Ash for Selective Catalytic Reduction of NOx and Their Resistance to SO2/H2O at Low-temperatures

  • 摘要: 采用超声波辅助浸渍法,以燃煤电厂粉煤灰为载体,硝酸铁为铁源,硝酸锰和高锰酸钾为不同锰源,分别制备Mn-Fe/FA(N)和Mn-Fe/FA粉煤灰负载锰基脱硝催化剂。利用自制固定床装置评价催化剂的脱硝活性,结合X射线光电子能谱(X-ray photoelectron spectroscopy,XPS),NH3-程序升温脱附(temperature programmed desorption TPD)和H2-程序升温还原(H2- temperature programmed reduction,TPR)等技术表征催化剂的化学特性,明晰催化剂的脱硝活性和水硫抗性机制。结果表明,Mn-Fe/FA催化剂的低温脱硝活性显著高于Mn-Fe/FA(N)催化剂;Mn-Fe/FA催化剂的脱硝活性温度窗较宽(70~200℃);在200℃,模拟烟气中水蒸气(体积分数5%或10%)对催化剂的脱硝活性没有影响;在含有5% H2O和52mg/m3 SO2的模拟烟气中运行4h后,NOx的转化率仍保持在75%。以KMnO4作为锰源可以提高催化剂的表面氧化还原特性、提高活性金属离子(Mn4+,Fe3+)以及化学吸附氧的含量、抑制硫酸盐在催化剂表面的沉积。

     

    Abstract: Mn-Fe/FA(N) and Mn-Fe/FA catalysts were synthesized by using the ultrasonic-assisted precipitation method. These catalysts consisted of fly ash (as the carrier), Fe (ferric nitrate as the precursor) and Mn (manganese nitrate or potassium permanganate as the precursor). The NH3-SCR reactions were conducted in a specially designed fixed-bed reactor. The de-NOx and the resistance (SO2 and H2O) mechanism of catalysts were analyzed by X-ray photoelectron spectroscopy (XPS), NH3-temperature programmed desorption (NH3-TPD) and H2-temperature programmed reduction (H2-TPR). The results showed that the NOx conversion of Mn-Fe/FA was significantly higher than that of Mn-Fe/FA(N). The Mn-Fe/FA catalyst exhibited a wider operating temperature range (70~200℃). Moreover, Mn-Fe/FA catalyst maintained the initial NOx conversion (99%) for 4h in the H2O (5 or 10%) at 200℃. In the presence of SO2 and H2O at 200℃, Mn-Fe/FA was able to maintain over 75% NOx conversion after 4h. KMnO4, as a source of Mn in Mn-Fe/FA, promoted the redox properties of the corresponding catalyst and increased the concentrations of active metal ions (Mn4+, Fe3+) and chemically adsorbed oxygen. It was found that using KMnO4 as a source of Mn can inhibit the formation of metal sulfates.

     

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