Mechanism of NO removal by CO + NH3 coupling in iron–manganese/activated carbon catalysts at medium and low temperatures

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Research on Chemical Intermediates Pub Date : 2024-08-06 DOI:10.1007/s11164-024-05367-6
Fu Yuan, Bangfu Huang, Zhe Shi, Liubin Luo, Gaoyong Zi, Keying Zhu, Xinchao Fan, Linjing Yang
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Abstract

In this study, Fe–Mn/activated carbon (AC) catalysts were prepared to investigate the CO + NH3 coupling for deducing the NO removal mechanism by iron and manganese supported on AC catalysts under moderate to low-moderate aerobic conditions. Through the catalyst surface morphology, phase analysis, and other test results, we propose a mechanism for the CO + NH3 coupling that results in NO removal at medium to low temperatures. The results indicate that NO conversion initially decreases and then increases in the range of 150–300 °C with 9% oxygen content. The NO conversion of the 3.5Fe–7.0Mn/AC catalyst reached 95%, surpassing other catalysts, with an inflection point near 230 °C. Characterization of the 3.5Fe–7.0Mn/AC catalyst revealed a smooth surface, uniform pore development, a high number of micro and medium pores, and elevated surface oxygen species (Oα) content. Mn2O3 and Fe3O4 are uniformly distributed on the surface, enhancing the reaction gas contact area and thereby improving NO conversion. Fe2+ is identified as the primary active site for NO removal. Increased Mn loading raises the Fe2+ and Mn3+ levels, with Mn3+ improving the NO conversion rate.

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铁锰/活性碳催化剂在中低温条件下通过 CO + NH3 偶联去除 NO 的机理
本研究制备了铁锰/活性炭(AC)催化剂,研究了 AC 催化剂上支持的铁和锰在中低度有氧条件下的 CO + NH3 耦合,以推断 NO 的去除机理。通过催化剂表面形貌、相分析和其他测试结果,我们提出了中低温条件下 CO + NH3 耦合去除 NO 的机理。结果表明,在含氧量为 9% 的 150-300 °C 范围内,NO 转化率最初会降低,然后会升高。3.5Fe-7.0Mn/AC 催化剂的氮氧化物转化率达到 95%,超过了其他催化剂,在 230 °C 附近出现拐点。3.5Fe-7.0Mn/AC 催化剂的表征显示,催化剂表面光滑,孔隙发育均匀,微孔和中孔数量较多,表面氧物种 (Oα) 含量较高。Mn2O3 和 Fe3O4 在表面均匀分布,增加了反应气体的接触面积,从而提高了 NO 的转化率。Fe2+ 被确定为去除 NO 的主要活性位点。增加锰的含量可提高 Fe2+ 和 Mn3+ 的水平,其中 Mn3+ 可提高 NO 的转化率。
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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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