自然科学版
陕西师范大学学报(自然科学版)
双碳背景下的稀土催化专刊
Nb对FeCeOx催化剂NH3选择性催化还原NO的促进机制
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安冬琦1,杨钰垚1,蔡彦迪2,邹伟欣2*,孙敬方3*,董林1,2,3
(1 介观化学教育部重点实验室,南京大学 化学化工学院,江苏 南京 210093;2 南京大学 环境学院,江苏 南京 210093;3 江苏省机动车尾气污染控制重点实验室,南京大学 现代分析中心,江苏 南京 210093)
邹伟欣,女,副教授,硕士生导师,研究方向为环境催化。E-mail:wxzou2016@nju.edu.cn;孙敬方,女,工程师,研究方向为环境催化。E-mail:sunjf@nju.edu.cn
摘要:
以NH3为还原剂的选择性催化还原(NH3-SCR)是消除大气重要污染物氮氧化物(NOx)的关键技术之一。采用共沉淀法制备了一系列Nb促进的NbaFe1-aCeOx(a=0、0.1、0.2、0.4)催化剂用于NH3选择性催化还原NO反应,并利用BET、XRD、XRF、NH3-TPD、H2-TPR、in situ DRIFTS等技术对催化剂的物理化学性质进行表征。结果表明:Nb的引入能显著提升FeCeOx催化剂的中低温脱硝性能,其中,Nb0.1Fe0.9CeOx催化剂在175~350 ℃温度区间内获得超过80%的NOx转化率,显示出优异的中低温NH3-SCR催化活性。进一步分析发现,Nb0.1Fe0.9CeOx催化剂上的SCR反应主要遵从Eley-Rideal反应机理,适量Nb的引入使得Nb、Fe、Ce之间产生了强相互作用,不仅可以降低催化剂的结晶度,增加催化剂的比表面积,还有利于氧化还原能力和表面酸量的提升,进而有助于NH3的吸附、活化以及NH3-SCR反应活性的增强。
关键词:
NH3-SCR;低温脱硝;Nb物种改性;FeCeOx催化剂
收稿日期:
2021-09-26
中图分类号:
X511; TQ426.99
文献标识码:
A
文章编号:
1672-4291(2022)02-0044-07
基金项目:
国家自然科学基金(21976111,21976081)
Doi:
10.15983/j.cnki.jsnu.2022006
Mechanism for Nb promoting NO selective catalytic reduction with NH3 over FeCeOx catalysts
AN Dongqi1, YANG Yuyao1, CAI Yandi2, ZOU Weixin2*, SUN Jingfang3*, DONG Lin1, 2, 3
(1 Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China;2 School of the Environment, Nanjing University,Nanjing 210093, Jiangsu, China;3 Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Nanjing University,Nanjing 210093, Jiangsu, China)
Abstract:
The selective catalytic reduction with NH3(NH3-SCR) is one of the most prominent technologies to eliminate the important pollutants of nitrogen oxides (NOx) in the atmosphere. A series of Nb promoted NbaFe1-aCeOx(a=0, 0.1, 0.2, 0.4) catalysts were prepared by co-precipitation method for NH3-SCR of NO. The physical and chemical properties of the catalysts were characterized by BET, XRD, XRF, NH3-TPD, H2-TPR and in situ DRIFTS. Results showed that the introduction of Nb significantly improved the low- and mid-temperature denitration performance of the FeCeOxcatalysts. The Nb0.1Fe0.9CeOxcatalyst achieved more than 80% of NOxconversion rate between 175 ℃ and 350 ℃, exhibiting the best NH3-SCR activity among the prepared NbaFe1-aCeOxcatalysts. The SCR reaction on the Nb0.1Fe0.9CeOxcatalyst followed the Eley-Rideal reaction mechanism,and its excellent SCR performance could be ascribed to the strong interaction between Nb, Fe and Ce due to the introduction of appropriate amount of Nb, which decreased the crystallinity, increased the specific surface area and gave rise to the redox property of the catalyst.The adsorption and activation of NH3were also encouraged by the enhanced surface acidity.
KeyWords:
NH3-SCR; low-temperature denitration; Nb species modification; FeCeOxcatalysts