废SCR脱硝催化剂中砷元素赋存形态与氧化碱浸脱除

doi:10.11896/cldb.20060294

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Abstract The valence state and speciation of As in spent SCR catalysts used in coal-fired power plants was studied by XPS and ICP. The results show that As in spent SCR catalysts exists in the form of As₂O₃ and As₂O₅. As₂O₃ is difficult to be leached directly in weak alkaline solution, so it is difficult to be removed completely. In order to solve this problem, the alkali method with oxidant added was proposed. The effects of oxidizer species, time, temperature, NaOH concentration, H₂O₂ concentration, solid to liquid ratio on the removal efficiency of As were studied. The results show that the removal efficiency of As could reach as high as 98.5% under the optimal leaching conditions of reaction temperature 30 ℃, reaction time 4 h, NaOH concentration 10wt%, H₂O₂ concentration 5wt%, the ratio of liquid to solid 2 mL/g, and the arsenic oxide content in the solid was reduced from 1 334×10^-6 to 50×10^-6. The content of As in detoxified SCR catalysts could reach the requirement of fresh SCR catalysts. The removal mechanism of As was studied by EPR and XPS methods, and a new advanced oxidation process was used to treat spent SCR catalysts. The V₂O₅ in spent SCR catalysts reacts with NaOH to form HV₂O₅^- and VO₄^3-. Under the influence of HV₂O₅^- and VO₄^3- in the leaching solution, H₂O₂ produces hydroxyl radicals (·OH) in alkali solution. Hydroxyl radicals have strong oxidizing properties and oxidize As³⁺, which is not easily soluble in weak alkali, to As⁵⁺.

Key words： spent SCR denitrification catalyst arsenic waste treatment advanced oxidation process leaching

Published: 12 March 2021

CLC number:

X705

Fund:National Key Research and Development Program of China (2019YFC1907502) and Youth Program of National Natural Science Foundation of China (51904287).

About author:: Chen Zhao received his bachelor’s degree in chemical engineering from Shandong Normal University in 2017. He is currently a graduate student in the Institute of Process Engineering (IPE) of the Chinese Academy of Sciences under the supervision of Researcher Huiquan Li. His research has focused on the recycling of spent SCR catalysts.
Huiquan Li, a researcher at the Institute of Process Engineering (IPE), Chinese Academy of Sciences, a professor at the University of Chinese Academy of Sciences. He received his Ph.D. degree in chemical engineering from the Dalian University of Technology in 1999. He is currently the director of the National Engineering Laboratory for Clean Production Technology of Hydrometallurgy and the leader of the expert group of the national key research and development program—“Resource Utilization of Solid Waste”. His research interests are the application basis and engineering research of resource recycling and clean technology. He has won the second prize of the National Technology Invention Award and the Beijing Science and Technology Progress Award, and was selected as a national high-level talent. In recent years, he has published more than 150 papers in J. Phys, Chem. B, Green Chemistry and other journals, and applied for more than 100 technical invention patents.

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	ZHAO Chen
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Cite this article:

ZHAO Chen,WU Wenfen,MENG Ziheng, et al. Chemical Speciation and Removal Mechanism of Arsenic from Spent SCR Catalysts[J]. Materials Reports, 2021, 35(5): 5001-5010.

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http://www.mater-rep.com/EN/10.11896/cldb.20060294 OR http://www.mater-rep.com/EN/Y2021/V35/I5/5001

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