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在VO/TiO催化剂上用NH3对NO进行选择性催化还原（SCR）过程中三氧化硫的形成。

Formation of sulfur trioxide during the SCR of NO with NH over a VO/TiO catalyst.

作者信息

Xiong Jin, Li Yuran, Lin Yuting, Zhu Tingyu

机构信息

Beijing Engineering Research Center of Process Pollution Control, National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process Engineering, Chinese Academy of Sciences Beijing 100190 China

University of Chinese Academy of Sciences Beijing 100049 China.

出版信息

RSC Adv. 2019 Nov 27;9(67):38952-38961. doi: 10.1039/c9ra08191g.

DOI:10.1039/c9ra08191g
PMID:35540665
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9076108/
Abstract

The oxidation of sulfur dioxide (SO) to sulfur trioxide (SO) is an undesirable reaction that occurs during the selective catalytic reduction (SCR) of nitrogen oxides (NO ) with ammonia (NH), which is a process applied to purify flue gas from coal-fired power plants. The objectives of this work were to establish the fundamental kinetics of SO formation over a VO/TiO catalyst and to illustrate the formation mechanism of SO in the presence of NO , HO and NH. A fixed-bed reactor was combined with a Fourier transform infrared (FTIR) spectrometer and a Pentol SO analyser to test the outlet concentrations of the multiple components. The results showed that the rate of SO oxidation was zero-order in O, 0.77-order in SO and -0.19-order in SO and that the apparent activation energy for SO oxidation was 74.3 kJ mol over the range of studied conditions. Based on diffuse reflectance infrared Fourier transform ( DRIFT) spectroscopy, X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPD) tests, the SO formation process is described here in detail. The adsorbed SO was oxidized by VO to produce adsorbed SO in the form of bridge tridentate sulfate, and the adsorbed SO was desorbed to the gas phase. NO promoted the oxidation of the adsorbed SO due to the promotion of the conversion of low-valent vanadium to high-valent vanadium. In addition, the desorption of the adsorbed SO was inhibited by HO or NH due to the conversion of tridentate sulfate to the more stable bidentate sulfate or ammonium bisulfate. Finally, the mechanism of the influence of NO , HO and NH on the formation of gaseous SO was proposed.

摘要

二氧化硫（SO₂）氧化为三氧化硫（SO₃）是一种不良反应，它发生在以氨（NH₃）选择性催化还原氮氧化物（NOₓ）的过程中，该过程用于净化燃煤电厂的烟气。本工作的目的是确定在VOₓ/TiO₂催化剂上SO₃形成的基本动力学，并阐明在NOₓ、H₂O和NH₃存在下SO₃的形成机理。将固定床反应器与傅里叶变换红外（FTIR）光谱仪和Pentol SO₃分析仪相结合，以测试多种组分的出口浓度。结果表明，在研究条件范围内，SO₂氧化速率对O₂为零级，对SO₂为0.77级，对SO₃为 -0.19级，SO₂氧化的表观活化能为74.3 kJ/mol。基于漫反射红外傅里叶变换（DRIFT）光谱、X射线光电子能谱（XPS）和程序升温脱附（TPD）测试，本文详细描述了SO₃的形成过程。吸附的SO₂被VOₓ氧化生成桥联三齿硫酸盐形式的吸附SO₃，吸附的SO₃解吸到气相中。由于促进了低价钒向高价钒的转化，NOₓ促进了吸附SO₂的氧化。此外，由于三齿硫酸盐转化为更稳定的双齿硫酸盐或硫酸氢铵，H₂O或NH₃抑制了吸附SO₃的解吸。最后，提出了NOₓ、H₂O和NH₃对气态SO₃形成影响的机理。

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