Experimental study on adsorption of arsenic and selenium in coal fired flue gas by Mn-Fe binary oxide
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摘要: 采用共沉淀法制备了一系列Mn-Fe复合氧化物,研究了物质的量比和温度对气相砷、硒吸附的影响,考察了As2O3和SeO2双组分气体的同时吸附特性,对吸附产物中砷、硒的稳定性进行测定。结果表明,As2O3和SeO2在Mn-Fe复合氧化物表面的吸附量随Mn含量增加呈先增大后减小的趋势,当Mn/Fe物质的量比为1∶1时吸附量达到最大;两者的最佳吸附温度分别为750和600 ℃;双组分气体同时吸附时,两者存在竞争作用,Mn-Fe复合氧化物会优先吸附As2O3,SeO2的吸附受到抑制;此外,预吸附的SeO2会增强临近原子吸附活性,促进As2O3的吸附;吸附后的Mn-Fe复合氧化物浸出液中砷和硒的质量浓度均低于控制限值,在随粉煤灰进行资源化利用(如作为混凝土成分、水泥原料等)过程中不会产生二次污染。
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关键词:
- Mn-Fe复合氧化物 /
- 吸附剂 /
- 砷 /
- 硒 /
- 同时吸附
Abstract: A series of Mn-Fe binary oxides with different molar ratios were synthesized by coprecipitation method, and their adsorption behaviors of gaseous arsenic and selenium in flue gas at different temperature were investigated. The simultaneous adsorption characteristics of As2O3 and SeO2 on Mn-Fe binary oxide were studied. To avoid secondary pollution for adsorbent utilization, As/Se leaching properties in Mn-Fe binary oxides were evaluated. Results show that the adsorption capacity of As2O3 and SeO2 on the Mn-Fe binary oxides increases firstly and then decreases with the increasing Mn content. The adsorption capacity reaches the maximum when the molar ratio is 1∶1. The optimum adsorption temperatures of As2O3 and SeO2 are 750 and 600 ℃, respectively. During the process for As2O3 and SeO2 adsorption on Mn-Fe binary oxide simultaneously, Mn-Fe binary oxides preferentially adsorb As2O3, while SeO2 is inhibited. In addition, the pre-adsorption SeO2 can enhance the adsorption activities of adjacent atoms, which is beneficial for As2O3 adsorption. The concentration of arsenic and selenium in the leaching solution of spent Mn-Fe binary oxide is far lower than the control limit, which will be no secondary pollution in the process of utilization with fly ash.-
Key words:
- Mn-Fe binary oxide /
- adsorbent /
- arsenic /
- selenium /
- simultaneous adsorption
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表 1 吸附剂的元素含量、比表面积和孔结构参数
Table 1 Contents of Mn and Fe elements, specific surface area and pore structure parameters of adsorbents
Mn/Fe
(mole
ratio)Mn/% Fe/% Surface
area/
(m2·g−1)Pore
volume/
(cm3·g−1)Pore
diameter/
nmFe2O3 0.00 100.00 16.37 0.11 22.10 0.25∶1 20.54 79.46 201.31 0.37 5.94 0.5∶1 35.39 64.61 160.06 0.32 6.28 1∶1 51.52 48.48 117.13 0.30 9.37 2∶1 69.41 30.59 76.48 0.25 11.68 Mn3O4 100.00 0.00 19.02 0.13 20.71 表 2 Mn-Fe复合氧化物中砷和硒的浸出特性
Table 2 Leaching characteristics of As and Se on spent Mn-Fe binary oxide
Leached As/Se Separate Simultaneous As Se As Se Amount /(mg·L−1) 0.0216 0.1078 0.0126 0.0525 Proportion /% 0.271 2.372 0.114 1.733 -
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