Denitrification characteristics and reaction mechanism of Ce-doped Fe-based catalysts from modified metallurgical dust containing iron

Zhi-fang Gao, Hong-ming Long, Xiang-peng Gao, Hao Zhang
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Abstract

Metallurgical dust (MD) was used as raw material to prepare rare earth Ce-doped Fe-based catalysts. The results show that the Ce0.1/AMD-300 °C catalyst prepared from acid-modified diatomite (AMD) with mCe/mMD = 0.1 (mCe and mMD are the mass of Ce and MD, respectively) after being roasted at 300 °C can reach 99% NOx removal rate in the wide temperature range of 230–430 °C and exhibits excellent SO2 and H2O resistance. The MD effectively removes alkali metal elements by the modification process, increases the specific surface area and optimizes the pore structure of MD. The doping of Ce element makes Fe-based catalysts have more surface adsorbed oxygen Oα and a higher Ce3+/Ce4+ ratio. Through ammonia temperature-programmed desorption and hydrogen temperature-programmed reduction, it was found that the strong interaction between cerium and iron promotes the formation of more oxygen cavities in the catalyst, thereby generating more active and easily reducible oxygen species and promoting the transformation of Brønsted acid site to Lewis acid site. The research results provide a theoretical basis for the preparation of efficient and inexpensive Fe-based catalysts from MD.

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改性含铁冶金粉尘中掺杂 Ce 的铁基催化剂的脱氮特性和反应机理
以冶金粉尘(MD)为原料制备掺杂稀土铈的铁基催化剂。结果表明,以 mCe/mMD = 0.1(mCe 和 mMD 分别为 Ce 和 MD 的质量)的酸性改性硅藻土(AMD)为原料制备的 Ce0.1/AMD-300 ℃催化剂经 300 ℃焙烧后,在 230-430 ℃的宽温度范围内氮氧化物去除率可达 99%,并具有优异的抗 SO2 和 H2O 性能。MD 在改性过程中有效地去除了碱金属元素,增加了比表面积,优化了 MD 的孔隙结构。Ce 元素的掺杂使得铁基催化剂的表面吸附氧 Oα 更多,Ce3+/Ce4+ 比值更高。通过氨温编程解吸和氢温编程还原发现,铈与铁之间的强相互作用促进催化剂中形成更多的氧空穴,从而产生更多活泼易还原的氧物种,并促进布氏酸位点向路易斯酸位点转化。这些研究成果为利用 MD 制备高效、廉价的铁基催化剂提供了理论依据。
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来源期刊
自引率
16.00%
发文量
161
审稿时长
2.8 months
期刊介绍: Publishes critically reviewed original research of archival significance Covers hydrometallurgy, pyrometallurgy, electrometallurgy, transport phenomena, process control, physical chemistry, solidification, mechanical working, solid state reactions, materials processing, and more Includes welding & joining, surface treatment, mathematical modeling, corrosion, wear and abrasion Journal of Iron and Steel Research International publishes original papers and occasional invited reviews on aspects of research and technology in the process metallurgy and metallic materials. Coverage emphasizes the relationships among the processing, structure and properties of metals, including advanced steel materials, superalloy, intermetallics, metallic functional materials, powder metallurgy, structural titanium alloy, composite steel materials, high entropy alloy, amorphous alloys, metallic nanomaterials, etc..
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