冶金含铁尘泥制备的Mn–Ce掺杂Fe基催化剂及特性  

Preparation and characteristics of Mn–Ce-doped Fe-based catalysts using metallurgical dust and mud containing iron

作　　者：高志芳 龙红明 高翔鹏[1] 李明阳 张浩 周海成 GAO Zhifang;LONG Hongming;GAO Xiangpeng;LI Mingyang;ZHANG Hao;ZHOU Haicheng(School of Metallurgical Engineering,Anhui University of Technology,Maanshan 243002,China;Key Laboratory of Metallurgical Emission Reduction&Resources Recycling(Ministry of Education),Anhui University of Technology,Maanshan 243002,China)

机构地区：[1]安徽工业大学冶金工程学院,马鞍山243002 [2]安徽工业大学冶金减排与资源综合利用教育部重点实验室,马鞍山243002

出　　处：《工程科学学报》2024年第3期407-419,共13页Chinese Journal of Engineering

基　　金：安徽省高等学校科学研究重大资助项目(2023AH040147);安徽省高校优秀青年科研资助项目(2022AH030044);安徽省高等学校科学研究重点资助项目(2022AH050305)。

摘　　要：针对冶金工业固废–含铁冶金尘泥组分复杂的特性,结合当前冶金烧结过程NO_x排放也是钢铁行业污染治理的重中之重的现状,提出对冶金含铁尘泥进行改性制备掺杂低温催化剂的思路,并制备了Mn–Ce掺杂的含铁尘泥基催化剂(Mn_(0.05)Ce_(0.1)/ADM,ADM分别代表acidolysis,dust和mud),研究结果表明在170~430℃宽温度区间内,Mn_(0.05)Ce_(0.1)/ADM催化剂NO_x脱除率达到90%以上,并表现出优异的SO_(2)和H_(2)O抗性,抗水抗硫性测试表明Mn_(0.05)Ce_(0.1)/ADM催化剂得益于Fe、Ce优异的抗水抗硫性,其活性组分具有较好的分散性和优异的介孔结构,并降低了表面结晶度. Mn掺杂使催化剂在牺牲一定Ce^(3+)浓度和高价态Mnx+离子的同时提高了Fe^(3+)的浓度,结果使其具有最均衡脱硝活性.此外,Fe–Ce–Mn间的协同作用改善了催化剂的表面酸性从而增加了Lewis酸性位点,进而促进静电极化激活NO_(2)和硝酸盐物种生成.研究结果可为冶金固废的高附加值利用及以废治污的思路提供一定理论参考.Metallurgical solid wastes,such as metallurgical dust and mud containing iron,are formed during metallurgical sintering.They are composed of complex components and are harmful to the environment.Alongwith the current metallurgical sintering process,NOx emission control is the top priority of pollution control in the steel industry.This paper proposes a new idea of preparing doped low-temperature catalysts using metallurgical dust and mud containing iron.Herein,the metallurgical iron-containing mud was modified by acid leaching,and the products were doped with Ce and Mn by the precipitation method to prepare a new type of catalyst.The prepared Mn–Ce-doped mud-based catalyst(Mn_(0.05)Ce_(0.1)/ADM,the ADM represents the dust and mud from acidolysis)was characterized via X-ray diffraction,nitrogen adsorption/desorption isotherm method,scanning electron microscopy,X-ray photoelectron spectroscopy,temperature-programmed desorption of ammonia,and temperature-programmed reduction of hydrogen.The results showed that Mn_(0.05)Ce_(0.1)/ADM achieveda NOx removal rate of>90%within a wide temperature range from 170℃to 430℃.Moreover,itshowed excellent SO_(2) and H2O resistance.A microstructural analysis revealed that the strong interaction between Fe–Ce–Mn could improve the surface acidity of the catalyst,thus increasing Lewis acid sites.Further,the active components of Mn_(0.05)Ce_(0.1)/ADM prepared by Ce and Mn exhibited good dispersion and an excellent mesoporous structure.In particular,Mn doping could inhibit the crystallization degree on the catalyst surface,improve the dispersed state of the active components in Mn_(0.05)Ce_(0.1)/ADM,and help improve the catalyst SCR(Selective Catalytic Reduction)activity.Combined with theanalysis of the factors influencing the catalyst,the results showed that the Ce–Mn doped catalyst increased the Fe^(3+)concentration while sacrificing a certain amount of Ce^(3+)and high-valent Mn^(+),achieving the most balanced denitration activity.Mn_(0.05)Ce_(0.1)/ADM formed more NO active

关 键 词：冶金固废 含铁尘泥 掺杂 铁基 催化剂 

分 类 号：X756[环境科学与工程—环境工程]