NO<sub>2</sub>对Cu/SAPO-34分子筛催化剂上NH<sub>3</sub>选择性催化还原NO性能的影响

引用本文: 郝腾, 王军, 于铁, 王建强, 沈美庆. NO₂对Cu/SAPO-34分子筛催化剂上NH₃选择性催化还原NO性能的影响[J]. 物理化学学报, 2014, 30(8): 1567-1574. doi: 10.3866/PKU.WHXB201405261 shu

Citation: HAO Teng, WANG Jun, YU Tie, WANG Jian-Qiang, SHEN Mei-Qing. Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst[J]. Acta Physico-Chimica Sinica, 2014, 30(8): 1567-1574. doi: 10.3866/PKU.WHXB201405261 shu

NO₂对Cu/SAPO-34分子筛催化剂上NH₃选择性催化还原NO性能的影响

郝腾 ^1, ,
王军 ^1, ,
于铁 ^1, ,
王建强 ^1, ,
沈美庆 ^1,2,

基金项目:
国家高技术研究发展计划项目（863）（2011AA03A405）资助

摘要:

主要考察了NO₂对Cu/SAPO-34 分子筛催化剂在整个温度范围内（100-500 ℃）NH₃选择性催化还原（SCR）NO性能的影响. 研究所使用样品为新鲜Cu/SAPO-34 催化剂在750 ℃下水热处理4 h 的稳定期样品.通过X射线衍射（XRD）和扫描电子显微镜（SEM）对样品的结构以及形貌进行表征，采用SCR活性评价、动力学实验以及原位漫反射傅里叶变换红外光谱（in situ-DRIFTS）表征催化剂的性能以及催化剂表面物种的变化. 活性评价实验结果表明，NO₂会抑制催化剂的低温（100-280 ℃）活性，但其存在会提高催化剂的高温（280 ℃以上）活性. 与此同时，随着反应物中NO/NO₂的摩尔比例减少，由于NH₄NO₃物种的分解，副产物（N₂2O）的浓度增大. 动力学结果表明，Cu/SAPO-34 催化剂上快速SCR反应的表观活化能（E_a=64.02 kJ·mol^-1）比标准SCR反应的表观活化能（E_a=48.00 kJ·mol^-1）更大. In situ-DRIFTS实验结果表明NO比NO₂更容易在催化剂表面形成硝酸盐，并且NO₂更容易与吸附在Brønsted 酸性位上的NH₃物种反应生成NH₄NO₃. 低温下，催化剂表面的NH₄NO₃物种会覆盖SCR反应的活性位，造成活性降低，但在高温时，形成的NH₄NO₃物种一部分会被NO还原为N2，而另一部分会直接热分解为N₂O，造成催化剂的选择性降低.

关键词:

English

Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst

1.
1. Key Laboratory for Green Chemical Technology, Ministry of Education of China, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, P. R. China;
2. State Key Laboratory of Engines, Tianjin University, Tianjin 300072, P. R. China
Received Date: 17 March 2014
Available Online: 18 July 2014
Fund Project:
国家高技术研究发展计划项目（863）（2011AA03A405）资助

Abstract:

This study investigated the effects of NO₂ on the selective catalytic reduction (SCR) of NO by NH₃ over Cu/SAPO-34 catalyst at temperatures ranging from 100 to 500 ℃. The Cu/SAPO- 34 sample was hydrothermally treated at 750 ℃ for 4 h to obtain a de-greened sample and X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to characterize the structure of the catalyst. SCR activity test, kinetic analysis, and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ-DRIFTS) were all applied to evaluate the changes in catalytic activity in the presence of various NO/NO₂ ratios. The SCR results for different NO/NO₂ molar ratios demonstrated that NO₂ inhibited the NO_x removal efficiency over the Cu/SAPO- 34 catalyst at low temperatures (100-280 ℃), but enhanced the efficiency at high temperatures (above 280 ℃). The amount of N₂O was observed to increase with decreasing NO/NO₂ ratios, owing to the decomposition of NH₄NO₃. The kinetic results showed that the fast SCR reaction exhibited a higher apparent activation energy (E_a=64.02 kJ·mol^-1) than that of the standard SCR reaction (E_a=48.00 kJ·mol^-1) over Cu/SAPO-34 catalyst. The results of in situ-DRIFTS showed that NO₂ did not efficiently generate nitrate species on Cu2+ sites compared with NO, and that some nitrate species combined with NH₄₊ on Brønsted acid sites to generate NH₄NO₃. The inhibitory effect of NO₂ at low temperatures is evidently caused by deposited NH₄NO₃ covering the active sites of Cu/SAPO-34 catalyst, while these NH₄NO₃ species can be reduced by NO or thermally decomposed as the temperature increases.

Key words:

Ammonia selective catalytic reduction
/ NO_x (NO and NO₂)
/ Cu/SAPO-34
/ Diffuse reflectance infrared Fourier transform spectrum
/ NH₄NO₃

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沈阳化工大学材料科学与工程学院沈阳 110142

NO₂对Cu/SAPO-34分子筛催化剂上NH₃选择性催化还原NO性能的影响

English

Effect of NO₂ on the Selective Catalytic Reduction of NO with NH₃ over Cu/SAPO-34 Molecular Sieve Catalyst

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中国化学会秘书处

NO2对Cu/SAPO-34分子筛催化剂上NH3选择性催化还原NO性能的影响

English

Effect of NO2 on the Selective Catalytic Reduction of NO with NH3 over Cu/SAPO-34 Molecular Sieve Catalyst

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

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