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Low temperature selective catalytic reduction of NO X with NH 3 by activated coke loaded with Fe x Co y Ce z O m : The enhanced activity, mechanism and kinetics
Fuel ( IF 7.4 ) Pub Date : 2018-12-01 , DOI: 10.1016/j.fuel.2018.05.076
Pei Lu , Rui Li , Yi Xing , Yuran Li , Tingyu Zhu , Huifang Yue , Wanrong Wu

Abstract The existing catalysts based on activated coke had generally poor denitration performance at low temperature, which could not meet the urgent needs of power plants and steel enterprises. In this study, activated coke loaded with FexCoyCezOm was prepared by incipient wetness impregnation method and employed to remove NOx at 100–350 °C in simulated flue gas. 3%Fe0.6Co0.2Ce0.2O1.57/AC catalyst exhibited highest NOx removal efficiency as it had more than 70%NOx conversion rate at 100 °C and achieved more than 90%denitrition efficiency at 250–350 °C. The catalyst also showed stable catalytic performance and good resistance to H2O or/and SO2 at 250 °C. Based on the results of Brunauer–Emmett–Teller (BET), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), temperature programmed desorption (TPD), temperature programmed reduction (TPR) and Fourier transform infrared spectroscopy (FTIR), the enhanced performance could be attributed to the co-participation of Fe, Co and Ce species with different valence states, the high concentration of chemisorbed oxygen, highly dispersed active components, the increase of weak acid sites, good redox properties of metallic oxides and abundant founctional groups on the catalyts surface. Finally, the possible mechanism and kinetics of NOx removal over FexCoyCezOm/AC catalyst were discussed in detail, which revealed that the enhanced performance was resulted from the increased active sites and the redox cycle among Fe, Co and Ce.

中文翻译:

负载Fe x Co y Ce z O m 的活性焦低温选择性催化还原NO x 与NH 3 :增强的活性、机理和动力学

摘要 现有的活性焦催化剂低温脱硝性能普遍较差,不能满足电厂和钢铁企业的迫切需求。在本研究中,负载 FexCoyCezOm 的活性焦采用初湿浸渍法制备,用于在 100-350 °C 下去除模拟烟气中的 NOx。3%Fe0.6Co0.2Ce0.2O1.57/AC 催化剂表现出最高的 NOx 去除效率,因为它在 100 °C 时具有超过 70% 的 NOx 转化率,并在 250-350 °C 下达到超过 90% 的脱硝效率。该催化剂还表现出稳定的催化性能,并在 250 °C 下具有良好的耐 H2O 或/和 SO2 性能。基于 Brunauer-Emmett-Teller (BET)、X 射线光电子能谱 (XPS)、X 射线衍射 (XRD)、程序升温脱附 (TPD) 的结果,程序升温还原 (TPR) 和傅里叶变换红外光谱 (FTIR),增强的性能可归因于具有不同价态的 Fe、Co 和 Ce 物种的共同参与、高浓度的化学吸附氧、高度分散的活性成分,弱酸性位点的增加,金属氧化物良好的氧化还原性能和催化剂表面丰富的官能团。最后,详细讨论了 FexCoyCezOm/AC 催化剂去除 NOx 的可能机制和动力学,结果表明性能增强是由于活性位点增加和 Fe、Co 和 Ce 之间的氧化还原循环所致。高浓度的化学吸附氧、高度分散的活性组分、弱酸位点的增加、金属氧化物良好的氧化还原性能和催化剂表面丰富的官能团。最后,详细讨论了 FexCoyCezOm/AC 催化剂去除 NOx 的可能机制和动力学,结果表明性能增强是由于活性位点增加和 Fe、Co 和 Ce 之间的氧化还原循环所致。高浓度的化学吸附氧、高度分散的活性组分、弱酸位点的增加、金属氧化物良好的氧化还原性能和催化剂表面丰富的官能团。最后,详细讨论了 FexCoyCezOm/AC 催化剂去除 NOx 的可能机制和动力学,结果表明性能增强是由于活性位点增加和 Fe、Co 和 Ce 之间的氧化还原循环所致。
更新日期:2018-12-01
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