多壁碳纳米管负载FeS2的制备及脱汞性能分析

doi:10.16085/j.issn.1000-6613.2019-1904

摘要/Abstract

摘要：

采用硝酸铁与硫脲在溶剂热反应条件下制备FeS₂，利用物理浸渍法将FeS₂负载至多壁碳纳米管（MWCNTs）上，借助扫描电镜（SEM）、X射线衍射（XRD）、X光电子能谱（XPS）等分析测试手段对制备样品的结构特性进行探究，通过固定床反应器研究模拟烟气氛围下吸附剂对烟气中单质汞的吸附特性。实验考察了不同FeS₂负载量、烟气初始汞浓度、床层温度以及O₂、NO和SO₂对吸附剂脱汞效率的影响。结果表明，制备出的FeS₂分散性较好，呈球状晶体，表面均匀覆盖着MWCNTs，成团簇状。当负载量为10%、反应温度为70℃时，FeS₂/MWCNTs的吸附效果最好，最高脱除效率能达到100%，60min后脱除效率仍有80.3%。TPD脱附曲线和XPS分析结果进一步表明烟气中的Hg⁰被氧化成Hg²⁺以HgS的形式附着在吸附剂表面，证实吸附剂以化学吸附为主。此外，汞脱除效率随初始汞浓度的增加而降低，汞吸附容量却随之增加，60min最高能达到5.1μg/g。酸性气体NO和SO₂的存在，占据了吸附剂表面的活性点位，不利于Hg⁰的吸附，但低浓度NO对吸附剂的整体效果影响不大，抗NO性能较好。

关键词: 吸附剂, 表征, 汞, 固定床, 吸附

Abstract:

Ferric nitrate and thiourea were used to prepare FeS₂ under solvothermal reaction conditions which were loaded onto MWCNTs (multi-walled carbon nanotubes) by physical impregnation method. The structural characteristics of the prepared samples were investigated by means of analytical methods such as SEM, XRD and XPS. The adsorption characteristics of the adsorbent on the elemental mercury in the flue gas under simulated flue gas atmosphere were studied by a fixed bed reactor. The effects of different FeS₂ loading, initial mercury concentration, reaction temperature and O₂, NO and SO₂ on the mercury removal efficiency of the adsorbent were investigated. The results showed that the prepared FeS₂ had good dispersibility and was spherical crystal. The surface was evenly covered with MWCNTs and clustered. When the loading was 10% and the reaction temperature was 70℃, the adsorption effect of FeS₂/MWCNTs was the best, the highest removal efficiency could reach 100%, and the removal efficiency was 80.3% after 60min. The TPD desorption curve and XPS analysis results further indicated that Hg⁰ in the flue gas was oxidized to Hg²⁺ and was attached to the surface of the adsorbent in the form of HgS, confirming that the adsorbent was mainly chemisorbed. In addition, the mercury removal efficiency decreased with the increase of the initial mercury concentration, but the mercury adsorption capacity increased, and the highest could reach 5.1μg/g in 60min. The presence of NO and SO₂ occupied the active site on the surface of the adsorbent, which was not conducive to the adsorption of Hg⁰, but the low concentration of NO had little effect on the overall effect of the adsorbent, and the anti-NO performance of adsorbent was better.

Key words: adsorbents, characterization, mercury, fixed-bed, adsorption

中图分类号:

TQ424

吉睿, 吴昊, 周长松, 杨宏旻. 多壁碳纳米管负载FeS₂的制备及脱汞性能分析[J]. 化工进展, 2020, 39(9): 3502-3510.

Rui JI, Hao WU, Changsong ZHOU, Hongmin YANG. Preparation and demercuration analysis of multi-walled carbon nanotubes supported FeS₂[J]. Chemical Industry and Engineering Progress, 2020, 39(9): 3502-3510.

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多壁碳纳米管负载FeS₂的制备及脱汞性能分析

Preparation and demercuration analysis of multi-walled carbon nanotubes supported FeS₂

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