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
制备方法对FeMnCeOx催化剂(超)低温NH3-SCR性能的影响
PDF下载 ()
孙敬方1,蔡彦迪2,余雅昕3,安冬琦3,田笑丛4,邹伟欣2*,董林1,2,3*
(1 南京大学 现代分析中心,江苏省机动车尾气污染控制重点实验室,江苏 南京 210093;2 南京大学 环境学院,江苏 南京 210093;3 南京大学 化学化工学院,教育部介观化学重点实验室,江苏 南京210093;4 南京大学 化学国家级实验教学示范中心,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:zouweixin2011@163.com;董林,男,教授,博士生导师,研究方向为环境催化。E-mail:donglin@nju.edu.cn
摘要:
锰基催化剂在(超)低温氨选择性催化还原(NH3-SCR)反应中具有优异的催化性能,但抗硫性差等问题限制了其进一步工业化应用。通过改变活性组分比例及调控制备方法等手段对FeMnCeOx催化剂的理化性质和NH3-SCR催化性能进行了优化研究,结果表明:采用溶胶-凝胶法制备的FeMnCeOx(S)催化剂比采用共沉淀法制备的FeMnCeOx(C)催化剂的催化性能更优,能够在80~150 ℃温度范围内获得超过90%的NO转化率;与此同时,FeMnCeOx(S)催化剂在120 ℃、体积分数为0.01%的SO2气氛中能够保持活性稳定,具有优异的耐硫性。结合催化剂的织构性质、表面酸性、氧化还原性能及表面物种化学态的表征结果,发现利用溶胶-凝胶法制备的催化剂样品具有更优异的氧化还原性、更强的表面酸性及更多利于低温SCR反应的表面物种,同时其NH3-SCR反应遵循Eley-Rideal反应机理,上述因素综合作用使FeMnCeOx(S)表现出更好的脱硝性能。
关键词:
溶胶-凝胶法;脱硝性能;(超)低温;FeMnCeOx催化剂
收稿日期:
2021-10-20
中图分类号:
TQ426;TQ241.21
文献标识码:
A
文章编号:
1672-4291(2022)02-0077-09
基金项目:
国家自然科学基金(21972063,21976081)
Doi:
10.15983/j.cnki.jsnu.2022010
Influence of preparation method on the performance of FeMnCeOx catalyst in NH3-SCR at (ultra) low temperature
SUN Jingfang1, CAI Yandi2, YU Yaxin3, AN Dongqi3,TIAN Xiaocong4, ZOU Weixin2*, DONG Lin1, 2, 3*
(1 Jiangsu Key Laboratory of Vehicle Emissions Control, Center of Modern Analysis, Nanjing University, Nanjing 210093, Jiangsu, China;2 School of Environment, Nanjing University, Nanjing 210093, Jiangsu, China;3 Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, Jiangsu, China;4 National Demonstration Center for Experimental Chemistry Education, Nanjing University, Nanjing 210093, Jiangsu, China)
Abstract:
Mn-based catalysts possess excellent catalytic performance in NH3 selective catalytic reduction (NH3-SCR) at (ultra) low temperature, but the poor sulfur resistance limits their further industrial application. In this study, FeMnCeOx catalysts were modified by optimizing the ratios of active components and adjusting the preparation method. The results indicated that FeMnCeOx(S) catalyst prepared by the sol-gel method had better catalytic performance than FeMnCeOx(C) catalyst prepared by the co-precipitation method, and could obtain NO conversion rate of more than 90% between 80 ℃ and 150 ℃. At the same time, the activity of FeMnCeOx(S) catalyst can be stably maintained in the atmosphere of 0.01% (volume fraction) SO2 at 120 ℃, showing excellent sulfur resistance. Combined with the characterization results of textural properties, surface acidity, redox performance and the chemical states of surface species, it was found that the samples prepared by the sol-gel method exhibited better redox property, stronger surface acidity and more surface species conducive to low temperature SCR.Furthermore, the NH3-SCR reaction on FeMnCex(S) followed the Eley-Rideal reaction mechanism. The combined effects of the above factors produced a better deNOx performance for FeMnCeOx(S) catalyst.
KeyWords:
sol-gel method; deNOx performance; (ultra) low temperature; FeMnCeOx catalysts