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Formation of Fe2(SO4)3-Fe2O3 interface induced by OCFGs electrostatic anchoring on AC surface: High efficiency NH3-SCR performance at low temperatures
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2024-05-31 , DOI: 10.1016/j.seppur.2024.128210
Pan Li , Yan Huang , Simi Li , Mouli Liu

Low-temperature activity and SO2 poisoning were the key factors limiting the application of NH3-SCR catalysts. In this study, Fe2(SO4)3/AC and Fe2(SO4)3/OAC catalysts were prepared by oxidation function modification and incipient wetness impregnation. In the temperature range of 100–250 ℃, the catalytic performance and SO2 resistance of Fe2(SO4)3/AC and Fe2(SO4)3/OAC catalysts were investigated, the denitrification efficiency increased from 28 % (Fe2(SO4)3/AC) to 80 % at 100 °C and reached 100 % at 170 °C, and 100 ppm SO2 was introduced at 250 ℃ for 24 h, the denitrification efficiency remains 100 % unchanged. The mechanism of activity enhancement was further explored by BET, XRD, ICP, TG, XPS, FT-IR, H2-TPR and NH3-TPD. The results showed that (NH4)2S2O8 modification enhanced the surface acidity, and the increase of surface oxygen-containing functional groups improved the redox performance. At the same time, due to electrostatic anchoring effects of oxygen-containing functional groups, Fe3+ and SO42- were adsorbed at different sites and promoted the binding of S to the carbon skeleton to form −C-S-C-. Thus, the interaction between OAC and Fe2(SO4)3 caused part of Fe2(SO4)3 to decompose into Fe2O3, and the formation of Fe2(SO4)3-Fe2O3 interface further enhanced the acidity and redox properties. More importantly, the decomposition temperature of NH4HSO4 was lower and the decomposition was more thorough on the Fe2(SO4)3/OAC than that of Fe2(SO4)3/AC. Finally, the possible mechanism of (NH4)2S2O8-modified Fe2(SO4)3/OAC catalyst to improve NH3-SCR performance was proposed, which is of great significance for the development of NH3-SCR catalyst with sulfur resistance at low temperatures.

中文翻译:


OCFG 静电锚定在 AC 表面诱导 Fe2(SO4)3-Fe2O3 界面的形成:低温下高效 NH3-SCR 性能



低温活性和SO2中毒是限制NH3-SCR催化剂应用的关键因素。本研究通过氧化功能改性和初湿浸渍制备了Fe2(SO4)3/AC和Fe2(SO4)3/OAC催化剂。在100~250 ℃温度范围内,考察了Fe2(SO4)3/AC和Fe2(SO4)3/OAC催化剂的催化性能和抗SO2性能,脱硝效率从28%提高(Fe2(SO4)3/ AC)在100℃时达到80%,在170℃时达到100%,并在250℃下通入100 ppm SO2 24 h,反硝化效率保持100%不变。通过BET、XRD、ICP、TG、XPS、FT-IR、H2-TPR和NH3-TPD进一步探讨了活性增强的机制。结果表明,(NH4)2S2O8改性增强了表面酸性,表面含氧官能团的增加提高了氧化还原性能。同时,由于含氧官能团的静电锚定效应,Fe3+和SO42-被吸附在不同位点,促进S与碳骨架结合形成-CSC-。因此,OAC与Fe2(SO4)3之间的相互作用导致部分Fe2(SO4)3分解为Fe2O3,并且Fe2(SO4)3-Fe2O3界面的形成进一步增强了酸性和氧化还原性能。更重要的是,与Fe2(SO4)3/AC相比,NH4HSO4在Fe2(SO4)3/OAC上的分解温度更低,分解更彻底。最后提出了(NH4)2S2O8改性Fe2(SO4)3/OAC催化剂改善NH3-SCR性能的可能机制,这对于开发低温抗硫NH3-SCR催化剂具有重要意义。
更新日期:2024-05-31
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