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凹凸棒石(PG)负载MnOx催化剂脱除气态Hg0的研究

王钧伟 徐灿 秦伟 张建利 张先龙 董彦杰 崔晓峰

王钧伟, 徐灿, 秦伟, 张建利, 张先龙, 董彦杰, 崔晓峰. 凹凸棒石(PG)负载MnOx催化剂脱除气态Hg0的研究[J]. 燃料化学学报(中英文), 2020, 48(12): 1442-1451.
引用本文: 王钧伟, 徐灿, 秦伟, 张建利, 张先龙, 董彦杰, 崔晓峰. 凹凸棒石(PG)负载MnOx催化剂脱除气态Hg0的研究[J]. 燃料化学学报(中英文), 2020, 48(12): 1442-1451.
WANG Jun-wei, XU Can, QIN Wei, ZHANG Jian-li, ZHANG Xian-long, DONG Yan-jie, CUI Xiao-feng. Hg0 removal by palygorskite (PG) supported MnOx catalyst[J]. Journal of Fuel Chemistry and Technology, 2020, 48(12): 1442-1451.
Citation: WANG Jun-wei, XU Can, QIN Wei, ZHANG Jian-li, ZHANG Xian-long, DONG Yan-jie, CUI Xiao-feng. Hg0 removal by palygorskite (PG) supported MnOx catalyst[J]. Journal of Fuel Chemistry and Technology, 2020, 48(12): 1442-1451.

凹凸棒石(PG)负载MnOx催化剂脱除气态Hg0的研究

基金项目: 

国家自然科学基金 21203003

国家自然科学基金 51404014

安徽省自然科学基金面上项目 1708085MB49

安徽省高校优秀青年人才支持计划重点项目 gxyqZD2017062

省部共建煤炭高效利用与绿色化工国家重点实验室开放课题 2020-KF-28

详细信息
  • 本文的英文电子版由Elsevier出版社在ScienceDirect上出版(http://www.sciencedirect.com/science/journal/18725813).
  • 中图分类号: 0643.3

Hg0 removal by palygorskite (PG) supported MnOx catalyst

Funds: 

the National Natural Science Foundation of China 21203003

the National Natural Science Foundation of China 51404014

the Anhui Provincial Natural Science Foundation 1708085MB49

Key Project of Anhui Provincial Outstanding Young Scholars in Colleges and Universities gxyqZD2017062

Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering 2020-KF-28

More Information
  • 摘要: 利用凹凸棒石(PG)负载Mn氧化物制备MnOx/PG催化剂并用于脱除模拟烟气中的Hg0,并采用比表面积分析(BET)、X射线衍射(XRD)、X射线光电子能谱(XPS)等技术对催化剂进行了分析表征。结果表明,MnOx和凹凸棒石的共同作用明显增强了对Hg0脱除性能,MnOx负载量为8%的MnOx/PG催化剂脱除Hg0的活性最高,在400 min内反应温度为210 ℃、空速为6000 h-1、汞质量浓度为80 μg/m3的条件下Hg0的脱除效率可达95%以上。O2对MnOx/PG催化剂脱除Hg0具有促进作用,而SO2和H2O具有抑制作用,但气氛中有O2存在时可明显减弱SO2的抑制作用。X射线衍射(XRD)、X射线光电子能谱分析(XPS)和程序升温脱附实验(TPD)等结果表明,活性组分MnOx在载体PG上分散良好,Hg0在MnOx/PG催化剂上的脱除过程包含了吸附、氧化、反应等步骤,生成了HgO和HgSO4并吸附在催化剂上。
    1)  本文的英文电子版由Elsevier出版社在ScienceDirect上出版(http://www.sciencedirect.com/science/journal/18725813).
  • 图  1  固定床脱汞实验装置示意图

    Figure  1  Fixed bed system of mercury adsorption test

    图  2  MnOx负载量对MnOx/PG脱除Hg0的影响

    Figure  2  Effect of MnOx loading on Hg0 removal by MnOx/PG

    图  3  PG和MnOx/PG催化剂的XRD谱图

    Figure  3  XRD of PG and MnOx/PG catalysts a: PG; b: Mn3/PG; c: Mn5/PG; d: Mn8/PG; e: Mn10/PG

    图  4  温度对MnOx/PG催化剂脱除Hg0的影响

    Figure  4  Effect of temperature on Hg0 removal by MnOx/PG

    图  5  烟气成分对MnOx/PG催化剂脱除Hg0的影响

    Figure  5  Effect of flue gas components on Hg0 removal by MnOx/PG

    图  6  O2体积分数对MnOx/PG脱除Hg0的影响

    Figure  6  Effect of O2 on Hg0 removal by MnOx/PG

    图  7  O2暂态响应实验

    Figure  7  O2 transient response experiment for Hg0 removal over MnOx/PG

    图  8  SO2体积分数对MnOx/PG脱除Hg0的影响

    Figure  8  Effect of SO2 on Hg0 removal by MnOx/PG

    图  9  SO2暂态响应实验

    Figure  9  SO2 transient response experiment for Hg0 removal over MnOx/PG

    图  10  脱除Hg0前(a)后(b)MnOx/PG催化剂O 1s的XPS谱图

    Figure  10  O 1s XPS profiles of the fresh MnOx/PG (a) and used MnOx/PG (b)

    图  11  脱除Hg0前(a)后(b)MnOx/PG催化剂Mn 2p的XPS谱图

    Figure  11  Mn 2p XPS profiles of the fresh MnOx/PG(a)and used MnOx/PG(b)

    图  12  新鲜MnOx/PG和吸附Hg0后MnOx/PG的TPD谱图

    Figure  12  TPD profiles of the fresh MnOx/PG and used MnOx/PG

    图  13  Hg0在MnOx/PG催化剂上的脱除过程

    Figure  13  Hg0 removal process on MnOx/PG

    表  1  PG和MnOx/PG的比表面积和孔结构

    Table  1  Properties of PG and MnOx/PG

    Sample ABET /(m2·g-1) vt/(cm3·g-1) dave/nm
    PG 135.85 0.553 16.93
    1%MnOx/PG 137.79 0.526 16.92
    3%MnOx/PG 133.82 0.519 16.91
    5%MnOx/PG 130.04 0.512 16.90
    8%MnOx/PG 133.21 0.499 17.10
    10%MnOx/PG 127.73 0.492 17.10
    下载: 导出CSV

    表  2  MnOx/PG催化剂表面的原子浓度

    Table  2  Surface atomic salinity of MnOx/PG

    MnOx/PG Oα/% Oβ/% Oγ/% Mn2+/% Mn3+/% Mn4+/%
    Fresh 18.8 53.4 27.8 - 46.2 53.8
    Used 8.8 44.7 46.5 20.9 36.2 42.9
    下载: 导出CSV
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  • 收稿日期:  2020-09-10
  • 修回日期:  2020-09-27
  • 网络出版日期:  2021-01-23
  • 刊出日期:  2020-12-10

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