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了解铁锑二元金属氧化物催化剂在氨选择性催化还原一氧化氮中的高性能及其对水/二氧化硫的耐受性。

Understanding the high performance of an iron-antimony binary metal oxide catalyst in selective catalytic reduction of nitric oxide with ammonia and its tolerance of water/sulfur dioxide.

作者信息

Jia Xuanxuan, Liu Hao, Zhang Yu, Chen Wei, Tong Qing, Piao Guangxia, Sun Chuanzhi, Dong Lin

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals, Institute of Materials and Clean Energy, Shandong Normal University, Jinan 250014, PR China.

College of Chemistry, Chemical Engineering and Materials Science, Shandong Provincial Key Laboratory of Clean Production of Fine Chemicals, Institute of Materials and Clean Energy, Shandong Normal University, Jinan 250014, PR China; School of Energy Engineering, Kyungpook National University, Daegu 41566, Republic of Korea.

出版信息

J Colloid Interface Sci. 2021 Jan 1;581(Pt A):427-441. doi: 10.1016/j.jcis.2020.07.089. Epub 2020 Jul 21.

Abstract

In recent years, Fe-based catalysts for the selective catalytic reduction of NO with NH (NH-SCR) have been attracting more attention. In this work, a novel Fe-Sb binary metal oxide catalyst was synthesized using the ethylene glycol assisted co-precipitation method and was characterized using a series of techniques. It was found that the catalyst with a molar ratio of 7:3 (Fe:Sb) displayed the best NH-SCR activity with 100% conversion of NO (nitrogen oxides) over a wide temperature window and with good resistance to HO + SO at 250 °C. The X-ray photoelectron spectroscopy (XPS) and in situ diffused reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) of NO adsorption results suggested that strong electron interactions between Fe and Sb in Fe-O-Sb species existed and electrons of Sb could be transferred to Fe through the 2Fe + Sb ↔ 2Fe + Sb redox cycle. The introduction of Sb significantly improved the adsorption behaviour of NO species on the FeSbO surface, which benefitted the adsorption/transformation of NO, thereby facilitating the NH-SCR reaction. In addition, the FeSbO catalyst demonstrated a good tolerance of HO and SO, since the decomposition of NHHSO on the catalyst surface was promoted by the introduction of Sb.

摘要

近年来,用于氨选择性催化还原氮氧化物(NH-SCR)的铁基催化剂受到了更多关注。在本工作中,采用乙二醇辅助共沉淀法合成了一种新型的铁-锑二元金属氧化物催化剂,并通过一系列技术对其进行了表征。结果发现,摩尔比为7:3(铁:锑)的催化剂在较宽的温度窗口内表现出最佳的NH-SCR活性,氮氧化物转化率可达100%,且在250℃时对H₂O + SO₂具有良好的抗性。X射线光电子能谱(XPS)和NO吸附的原位漫反射红外傅里叶变换光谱(原位DRIFTS)结果表明,Fe-O-Sb物种中Fe和Sb之间存在强烈的电子相互作用,并且Sb的电子可以通过2Fe³⁺ + Sb³⁺ ↔ 2Fe²⁺ + Sb⁵⁺氧化还原循环转移到Fe上。Sb的引入显著改善了NO物种在FeSbO表面的吸附行为,这有利于NO的吸附/转化,从而促进了NH-SCR反应。此外,FeSbO催化剂对H₂O和SO₂表现出良好的耐受性,因为Sb的引入促进了催化剂表面硫酸氢铵的分解。

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