Effect of chlorobenzene on the performance of NH3-SCR over Mn6Co4Ox catalyst

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-10-16 DOI:10.1016/j.seppur.2024.129901
Dongrui Kang, Peng Zhao, Qiqi Shi, Mingtao Yang, Ao Huang, Honghong Lyu, Boxiong Shen
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Abstract

The simultaneous removal of nitrogen oxides (NOx) and volatile organic compounds (VOCs) in NH3-SCR units can simplify the flue gas treatment process and has great potential for economic and environmental benefits. Mn-based catalysts have shown excellent performance in NOx/chlorobenzene (CB) synergistic removal, however, the mechanism of CB influence on NH3-SCR is not clear till now. In this paper, the impact of CB on the performance of NH3-SCR over Mn6Co4Ox catalysts is investigated in detail. The findings demonstrate that while the presence of CB clearly inhibits the adsorption of NH3 and NO, the Cl-produced during CB breakdown can actually promote the adsorption of them. In addition, the emission of N2O and NO2 in the NH3-SCR reaction with CB participation was significantly reduced, and the N2 selectivity was significantly improved at the same time. The impact of CB on the NH3-SCR reaction pathway under 250 ℃ was explored using in situ DRIFT further. It showed that the NH3-SCR reaction on the Mn6Co4Ox catalyst was found to follow both the Eley − Rideal (E-R) and Langmuir − Hinshelwood (L-H) mechanisms. The presence of CB in the reaction accelerated the rate of the nitrate reaction, hindered the synthesis of M−NO2 nitro compounds, and enhanced the generation of the intermediate product-NH2 for the improvement of the NH3-SCR reaction. Conversely, the slow deactivation of the Mn6Co4Ox catalysts could be attributed to the by-products of CB decomposition and the unfavorable accumulation of MnClx or CoClx on the catalyst surface, which inhibited the NH3-SCR reaction.

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氯苯对 Mn6Co4Ox 催化剂上 NH3-SCR 性能的影响
在 NH3-SCR 装置中同时去除氮氧化物(NOx)和挥发性有机化合物(VOCs)可简化烟气处理工艺,具有巨大的经济和环境效益潜力。锰基催化剂在氮氧化物/氯苯(CB)协同脱除方面表现出色,但迄今为止,氯苯对 NH3-SCR 的影响机理尚不清楚。本文详细研究了 CB 对 Mn6Co4Ox 催化剂上 NH3-SCR 性能的影响。研究结果表明,虽然 CB 的存在会明显抑制 NH3 和 NO 的吸附,但 CB 分解过程中产生的 Cl 实际上会促进 NH3 和 NO 的吸附。此外,在有 CB 参与的 NH3-SCR 反应中,N2O 和 NO2 的排放明显减少,同时 N2 的选择性也明显提高。利用原位 DRIFT 技术进一步探讨了 CB 在 250 ℃ 下对 NH3-SCR 反应途径的影响。结果表明,Mn6Co4Ox 催化剂上的 NH3-SCR 反应遵循 Eley - Rideal (E-R) 和 Langmuir - Hinshelwood (L-H) 两种机理。反应中 CB 的存在加快了硝酸反应的速率,阻碍了 M-NO2 硝基化合物的合成,并促进了中间产物-NH2 的生成,从而改善了 NH3-SCR 反应。相反,Mn6Co4Ox 催化剂失活缓慢的原因可能是 CB 分解的副产物和 MnClx 或 CoClx 在催化剂表面的不利积累,从而抑制了 NH3-SCR 反应。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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