Modified cold-rolled sludge as catalyst for selective catalytic reduction of NOx with NH3 at low temperatures

Author links open overlay panelJian Gao a b, Lei Jiang b, Zhenhua Gu a, Wei Su d, Zhiqiang Li b, Danyang Li b c, Jiangyong Yuan b c, Kongzhai Li b c

https://doi.org/10.1016/j.fuel.2023.128569Get rights and content

Abstract

Iron-based mixed oxides are considered commercially promising environmentally friendly catalysts for selective catalytic reduction with NH3 (NH3-SCR) for removing nitrogen oxides (NOx) because of their high catalytic activity. In this work, cold-rolled sludge with high content of iron species was used as the iron precursor for preparing catalysts by supported MnOx and/or sulfuric acid modifications. The prepared catalyst showed 100 % of NOx conversion in the temperature range of 60–180 ℃ and exhibited good resistance to SO2 and H2O. This is mainly attributed to the synergy between MnOx and iron sulfate, which improved the denitration performance at super low-temperature by improving the textural properties, redox capacity, surface acidity, and surface chemical states of the catalyst. Furthermore, the presence of Fe3+ and SO42- protected the active ingredient from the poisoning of SO2 and improved its sulfur resistance. The super low-temperature reaction mechanism of the catalyst was unraveled by transient reaction experiments and In situ DRIFTS. The results show that both Brønsted and Lewis acid sites are present in 10 %Mn/CRS-S-400, and that the reaction is dominated by the Langmuir–Hinshelwood (L–H) mechanism. This study provides an innovative and cost-effective strategy for the design of NH3-SCR catalysts by sulfation iron-based mixed oxides.

顾振华

冶金能源工程专业，副教授，硕士生导师

学术任职及兼职

云南省力学教学指导委员会委员

云南省力学学会会员

主要招生专业：

农业工程、能源动力工程、材料学

主要研究方向：

太阳能热利用及储能相变材料

学历及研究简历：

2001年9月-2005年6月，河北科技大学，本科生，材料成型及控制工程专业；

2005年9月-2008年6月，昆明理工大学，硕士研究生，材料学专业

2014年9月-2020年6月，昆明理工大学，博士研究生，冶金能源工程专业

近三年代表论文和著作：

1. Yannan Zhao, Zhenhua Gu*, Danyang Li, Jiangyong Yuan, Lei Jiang,Haiwen Xu, Chunqiang Lu, Guixian Deng, Ming Li, Wei Xiao, Kongzhai Li. Catalytic combustion of lean methane over MnCo2O4/SiC catalysts:Enhanced activity and sulfur resistance[J]. Fuel, 2022,323：124399.

2. Zhiqiang Li, Xiangbo Feng, Zhenhua Gu*, Chunqiang Lu, Danyang Li, Xing Zhu, Lei Jiang, Guixian Deng, Kongzhai Li. Enhanced performance of the CeO2–MgO oxygen carrier by NiO for chemical looping CO2 splitting[J].Fuel Processing Technology, 2022, 225(12): 107045.

3. Cheng Xianming, Gu Zhenhua*,Li Fashe, Zhu Xing, Wei Yonggang, Zheng Min, Tian Dong, Wang Hua,Li Kongzhai. Enhanced resistance to carbon deposition in chemical-looping combustion of methane: Synergistic effect of different oxygen carriers via sequence filling[J]. Chemical Engineering Journal, 2021, 421: 129776.

4. Gu Zhenhua, Zhang Ling, Lu Chunqiang, Qing Shan, Li Kongzhai. Enhanced performance of copper ore oxygen carrier by red mud modification for chemical looping combustion[J]. Applied Energy, 2020, 277: 115590.

5. Shen Lin, Zhenhua Gu *, Xing Zhu , Yonggang Wei , Yanhui Long , Kun Yang ,Fang He , Hua Wang, Kongzhai Li. Synergy of red mud oxygen carrier with MgO and NiO for enhanced chemical-looping combustion[J]. Energy,2020, 197 :117202.

6.顾振华，卿山，张玉辉，赵毅然，杜万基. 赤泥特性及资源化应用现状，应用化工，2020,49(8):2087-2090.

7. Yike Liu, Yanhui Long, Yaqin Tang, Zhenhua Gu*, Kongzhai Li. Effect of preparation method on the structural characteristics of NiO-ZrO2 oxygen carriers for chemical-looping combustion, Chemical Research In Chinese Universities, 2019, 35(6), 1024-1031.

8. Zhenhua Gu, Kongzhai Li, Hua Wang, Shan Qing, Xing Zhu, Yonggang Wei, Xianming Cheng, He Yu, Yan Cao. Bulk monolithic Ce–Zr–Fe–O/Al2O3 oxygen carriers for a fixed bed scheme of the chemical looping combustion: Reactivity of oxygen carrier[J]. Applied Energy, 2016, 163: 19-31.

近五年获奖成果和荣誉称号：

1.全国徐芝纶力学优秀教师奖

2.第二届伍达天教育基金教师奖

近三年主持的国家级或百万以上其他项目：

1.国家自然科学基金—高铁赤泥储放氧功能调控及其化学链燃烧服役行为研究（项目编号：51604137）

2.入选“兴滇英才支持计划”青年人才专项，主持国家地区基金：太阳能化学链重整中蓄热型氧载体的构建与性能调控，编号：52266008

近三年主持的教学教改及省级以上教学质量工程：

1. 云南省教育厅教学改革基金，JG2018262，基于“混合学习”模式的基础力学课程体系应用型教学研究。

2. 云南省一流课程重点培育项目-《材料力学》。

近三年主讲课程（研究生、本科生）：

1.研究生课程：“工程燃烧学及煤的清洁利用技术”

2.本科生课程：“工程力学”、“理论力学”、“材料力学”、“太阳能热利用技术”和“概

率论与数理统计”