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关于氨在硫酸化铁基催化剂上选择性催化还原NO的研究。

A study on the selective catalytic reduction of NO by ammonia on sulphated iron-based catalysts.

作者信息

Liu Caixia, Wang Huijun, Bi Yalian, Zhang Ziyin

机构信息

School of Environmental Science and Engineering, Tianjin University Tianjin 300072 China

Langfang City Beichen Entrepreneurship Resin Materials Incorporated Company Langfang 065000 China

出版信息

RSC Adv. 2020 Nov 10;10(67):40948-40959. doi: 10.1039/d0ra06697d. eCollection 2020 Nov 9.

Abstract

A series of sulphated iron-based catalysts was prepared an impregnation method by changing the loading content of Fe and SO on ZrO, and their performance in the selective catalytic reduction (SCR) of NO by ammonia was investigated. The NO conversion exhibited large differences among the sulphated iron-based catalysts. To explore the synergistic mechanism of iron and sulphates, XRD, BET, H-TPR, XPS, TPD and DRIFTS were used to characterize the catalysts, and it was found that among all the catalysts, the NO conversion by FeSZr was greater than 90% at 350-450 °C. The results indicated that the interaction between Fe and SO can have an effect on the redox ability, acid sites, and adsorption of NO and NH. With an increase in the content of Fe, the redox activity of the catalyst and the adsorption of ammonia improved at medium and low temperatures. However, at higher temperatures, an increase in Fe led to a decrease in the conversion of NO due to the enhanced oxidation of NH. At medium and low temperatures, an increase in the content of SO decreased the concentration of Fe on the surface of the catalyst and inhibited the adsorption of NO and NH. The addition of SO reduced the redox activity of the catalyst and inhibited the oxidation reaction of NH, which follows the Eley-Rideal mechanism at high temperatures, further enhancing the SCR activity of the Fe S Zr catalyst.

摘要

通过浸渍法,改变ZrO₂上Fe和SO₄的负载量,制备了一系列硫酸化铁基催化剂,并研究了它们在氨选择性催化还原(SCR)NO反应中的性能。硫酸化铁基催化剂之间的NO转化率表现出很大差异。为了探究铁和硫酸盐的协同作用机制,采用XRD、BET、H-TPR、XPS、TPD和DRIFTS对催化剂进行表征,发现在所有催化剂中,FeSZr在350 - 450℃时的NO转化率大于90%。结果表明,Fe和SO₄之间的相互作用会影响氧化还原能力、酸性位点以及NO和NH₃的吸附。随着Fe含量的增加,催化剂的氧化还原活性和氨的吸附在中低温下得到改善。然而,在较高温度下,Fe含量的增加导致NO转化率下降,这是由于NH₃的氧化增强所致。在中低温下,SO₄含量的增加降低了催化剂表面Fe的浓度,抑制了NO和NH₃的吸附。SO₄的添加降低了催化剂的氧化还原活性,抑制了NH₃的氧化反应,该反应在高温下遵循Eley-Rideal机理,进一步提高了Fe₂(SO₄)₃/Zr催化剂的SCR活性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4370/9057717/b3f7124fb4e9/d0ra06697d-f1.jpg

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