失活钒基催化剂再生-改性用于低负荷烟气脱硝
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摘要
基于电厂失活催化剂,采用物相分析、化学组分测试、比表面积测量表征手段确定导致V_2O_5/TiO_2失活的原因为As_2O_3、碱金属中毒,而失活催化剂晶型结构没有发生改变且具有高的比表面积.采用0. 01 mol/L的H_2C_2O_4溶液和0. 015 mol/L的NH_3·H_2O溶液对催化剂进行洗涤再生处理可将催化剂表面SO_3,As_2O_3,K2_O和Na_2O质量分数分别降至0. 09%,0. 05%,0. 02%和0. 01%,重新负载1. 5%质量分数V_2O_5后催化剂活性得以恢复.负载3%质量分数CuO后催化剂表现出好的低温催化活性,220℃,250℃,280℃和310℃下V_2O_5-CuO/TiO_2的NO_x转化率分别为62. 4%,82. 2%,90. 8%和95. 5%.
The power plant based deactivated catalyst was characterized by XRD,XRF and BET and the cause of deactivation was determined as As_2O_3,alkali metal poisoning. However,the crystal structure of the deactivated catalyst did not change and had a high specific surface area.H_2C_2O_4( 0. 01 mol/L) and NH_3·H_2O( 0. 015 mol/L) was applied to regenerate the catalyst,and the content of SO_3,As_2O_3,K_2O and Na_2O on the surface of the catalyst could be reduced to 0. 09 wt. %,0. 05 wt. %,0. 02 wt. % and 0. 01 wt. %,respectively. The activity of the catalyst could be recovered after the reloading of 1. 5% V_2O_5. After loading 3 wt. % CuO,the catalyst showed good catalytic activity at low temperatures. The NO_x conversion rate of V_2O_5-CuO/TiO_2 at220,250,280 and 310 ℃ was 62. 4%,82. 2%,90. 8% and 95. 5%,respectively.
The power plant based deactivated catalyst was characterized by XRD,XRF and BET and the cause of deactivation was determined as As_2O_3,alkali metal poisoning. However,the crystal structure of the deactivated catalyst did not change and had a high specific surface area.H_2C_2O_4( 0. 01 mol/L) and NH_3·H_2O( 0. 015 mol/L) was applied to regenerate the catalyst,and the content of SO_3,As_2O_3,K_2O and Na_2O on the surface of the catalyst could be reduced to 0. 09 wt. %,0. 05 wt. %,0. 02 wt. % and 0. 01 wt. %,respectively. The activity of the catalyst could be recovered after the reloading of 1. 5% V_2O_5. After loading 3 wt. % CuO,the catalyst showed good catalytic activity at low temperatures. The NO_x conversion rate of V_2O_5-CuO/TiO_2 at220,250,280 and 310 ℃ was 62. 4%,82. 2%,90. 8% and 95. 5%,respectively.
引文
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[12]王丽霞,仲兆平,朱林,等.铁铈复合选择性催化还原脱硝催化剂的碱金属(钾)中毒机理[J].化工进展,2017,36(11):4064-4071.(Wang Li-xia,Zhong Zhao-ping,Zhu Lin,et al. Alkali metal(potassium)poisoning mechanism of CeFeOx catalysts for selective catalytic reduction of NOx[J]. Chemical Industry and Engineering Progress,2017,36(11):4064-4071.)
[13] Kong M,Liu Q C,Wang X Q,et al. Performance impact and poisoning mechanism of arsenic over commercial V2O5-WO3/TiO2 SCR catalyst[J]. Catalysis Communications,2015,72:121-126.
[2] Zhang M H,Huang B J, Jiang H X, et al. Research progress in the SO2 resistance of the catalysts for selective catalytic reduction of NOx[J]. Chinese Journal of Chemical Engineering, 2017,25(12):1695-1705.
[3] Zheng K Z,Yang G H,Shen W J,et al. Preparation and denitration performance of V-W/TiO2-SiO2 nanotube catalysts[J]. Water Air and Soil Pollution, 2018,229(4):1-11.
[4] Khodayari R,Odenbrand C U I. Regeneration of commercial TiO2-V2O5-WO3 SCR catalysts used in bio fuel plants[J].Applied Catalysis B—Environmental,2001, 30(1/2):87-99.
[5] Peng Y,Li J H,Si W Z,et al. Insight into deactivation of commercial SCR catalyst by arsenic:an experiment and DFT study[J]. Environmental Science&Technology,2014,48(23):13895-13900.
[6] Li X,Li X S,Li J H,et al. High calcium resistance of CeO2-WO3 SCR catalysts:structure investigation and deactivation analysis[J]. Chemical Engineering Journal,2017,317:70-79.
[7] Xu T F,Wu X D,Liu X S,et al. Effect of barium sulfate modification on the SO2 tolerance of V2O5/TiO2 catalyst for NH3-SCR reaction[J]. Journal of Environmental Sciences,2017, 57:110-117.
[8] Yu Y K,He C,Chen J S,et al. Regeneration of deactivated commercial SCR catalyst by alkali washing[J]. Catalysis Communications,2013,39:78-81.
[9] Panahi P N,Salari D,Niaei A,et al. Study of M-ZSM-5nanocatalysts(M:Cu,Mn,Fe,Co...)for selective catalytic reduction of NO with NH3:process optimization by Taguchi method[J]. Chinese Journal of Chemical Engineering,2015,23(10):1647-1654.
[10] Yao X J,Kong T T,Chen L,et al. Enhanced low-temperature NH3-SCR performance of MnOx/CeO2 catalysts by optimal solvent effect[J]. Applied Surface Science,2017,420:407-415.
[11]贾勇,周军,柏家串,等.砷、钾复合中毒选择性催化还原脱硝催化剂的再生[J].硅酸盐学报,2016,44(7):1025-1032.(Jia Yong,Zhou Jun,Bai Jia-chuan, et al. Hybrid regeneration of selective catalytic reduction denitration catalyst poisoned by arsenic and potassium[J]. Journal of the Chinese Ceramic Society,2016,44(7):1025-1032.)
[12]王丽霞,仲兆平,朱林,等.铁铈复合选择性催化还原脱硝催化剂的碱金属(钾)中毒机理[J].化工进展,2017,36(11):4064-4071.(Wang Li-xia,Zhong Zhao-ping,Zhu Lin,et al. Alkali metal(potassium)poisoning mechanism of CeFeOx catalysts for selective catalytic reduction of NOx[J]. Chemical Industry and Engineering Progress,2017,36(11):4064-4071.)
[13] Kong M,Liu Q C,Wang X Q,et al. Performance impact and poisoning mechanism of arsenic over commercial V2O5-WO3/TiO2 SCR catalyst[J]. Catalysis Communications,2015,72:121-126.
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