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树脂基球状活性炭用于焦油加氢后油品脱色研究

武俊成 王建龙 管涛涛 张果丽 李开喜

武俊成, 王建龙, 管涛涛, 张果丽, 李开喜. 树脂基球状活性炭用于焦油加氢后油品脱色研究. 新型炭材料, 2021, 36(4): 843-850. doi: 10.1016/S1872-5805(21)60056-2
引用本文: 武俊成, 王建龙, 管涛涛, 张果丽, 李开喜. 树脂基球状活性炭用于焦油加氢后油品脱色研究. 新型炭材料, 2021, 36(4): 843-850. doi: 10.1016/S1872-5805(21)60056-2
WU Jun-cheng, WANG Jian-long, GUAN Tao-tao, ZHANG Guoli, LI Kai-xi. Adsorption and decolorization of hydrogenated coal tar on resin-based activated carbon spheres. New Carbon Mater., 2021, 36(4): 843-850. doi: 10.1016/S1872-5805(21)60056-2
Citation: WU Jun-cheng, WANG Jian-long, GUAN Tao-tao, ZHANG Guoli, LI Kai-xi. Adsorption and decolorization of hydrogenated coal tar on resin-based activated carbon spheres. New Carbon Mater., 2021, 36(4): 843-850. doi: 10.1016/S1872-5805(21)60056-2

树脂基球状活性炭用于焦油加氢后油品脱色研究

doi: 10.1016/S1872-5805(21)60056-2
基金项目: 国家自然科学基金(51902326,51672291,21276265);山西省重点研发计划(201803D121092);山西省优秀青年学者自然科学基金 (201901D211588)。
详细信息
    作者简介:

    武俊成,硕士生. E-mail:wujunch@hotmail.com

    通讯作者:

    李开喜,研究员. E-mail:likx@sxicc.ac.cn

  • 中图分类号: TQ127.1+1

Adsorption and decolorization of hydrogenated coal tar on resin-based activated carbon spheres

Funds: National Natural Science Foundation of China (51902326, 51672291, 21276265); Shanxi Province Key Research and Development Plan (201803D121092); Natural Science Foundation of Shanxi Province for Excellent Young Scholars, China (201901D211588).
More Information
  • 摘要: 采用悬浮聚合、水蒸气活化方法制备了树脂基球状活性炭(ACS),并进行硝酸氧化改性(NACS),用于焦油加氢后油品的脱色研究。通过SEM、N2吸附-脱附、FTIR、XPS、TG等技术对所制样品ACS和NACS进行结构性质表征。结果显示,经硝酸氧化改性后,NACS样品的表面形貌和孔结构并未受到显著影响,但球状活性炭表面的含氧官能团明显增加。选取两种典型的显色化合物对苯醌(PBQ)和N,N-二仲丁基对苯二胺(DBD)配置一定浓度的模型油进行吸附脱色,考察了吸附时间、吸附温度和吸附剂用量对吸附剂性能的影响。研究表明,NACS样品展现出良好的吸附性能,在一定的吸附条件下,对DBD和PBQ的脱色率分别达到94.5%和96.6%,除了球状活性炭表面微孔提供的活性位点之外,NACS表面官能团与有色物质形成的氢键可能对吸附性能的提升起着关键作用。重复使用6次后,吸附剂对两者的脱色率仍能达到90%以上,展现出良好的可再生性能。在对真实加氢油品脱色后,脱色效果显著,验证了所制备吸附剂在实际应用中的可行性。
  • FIG. 789.  FIG. 789.

    FIG. 789..  FIG. 789.

    图  1  树脂基球状活性炭的制备工艺路线示意图

    Figure  1.  Preparation process of resin-based spherical activated carbon.

    图  2  (a) PBQ外吸附光谱与(b) DBD紫外吸收光谱

    Figure  2.  (a) Ultraviolet absorption spectrum of p-benzoquinone and (b) DBD ultraviolet absorption spectrum.

    图  3  吸附时间对脱色的影响: (a) ACS与(b) NACS

    Figure  3.  Influence of adsorption time on decolorization: (a) ACS and (b) NACS.

    图  4  吸附温度对脱色的影响: (a) ACS与(b) NACS

    Figure  4.  Influence of temperature on decolorization: (a) ACS and (b) NACS.

    图  5  吸附剂用量对脱色的影响: (a) ACS与(b) NACS

    Figure  5.  Influence of adsorbent dosage on decolorization: (a) ACS and (b) NACS.

    图  6  模型油和真实油品脱色效果图

    Figure  6.  Decolorization renderings of model oils and real oils.

    图  7  (a) ACS和 (b)NACS的扫描电镜照片

    Figure  7.  SEM images of (a) ACS and (b) NACS.

    图  8  (a) ACS和NACS的N2吸附等温线;(b) ACS和NACS的红外光谱;(c) ACS和NACS的XPS谱图;(d) ACS和NACS的TG/DTG曲线

    Figure  8.  (a) N2 adsorption isotherm of ACS and NACS, (b) FT-IR spectra of ACS and NACS, (c) XPS spectra of ACS and NACS,and (d) TG/DTG curves of ACS and NACS.

    图  9  O1s 分峰拟合图: (a) NACS与(b) ACS

    Figure  9.  O1s Peak-fitting: (a) NACS and (b) ACS.

    图  12  NACS 吸附脱色机理示意图

    Figure  12.  NACS adsorption decolorization mechanism.

    图  10  ACS吸附动力学拟合:(a)准一级动力学与(b)准二级动力学

    Figure  10.  ACS adsorption kinetics: (a) plots of pseudo-first-order and (b) pseudo-second-order.

    图  11  NACS吸附动力学拟合:(a)准一级动力学与(b)准二级动力学

    Figure  11.  ACS adsorption kinetics: (a) plots of pseudo-first-order and (b) pseudo-second-order.

    表  1  NACS吸附剂的再生性能

    Table  1.   Regeneration performance of NACS adsorbent.

    Cyclicity123456
    PBQ decolorization rate (%)96.696.294.893.192.590.8
    DBD decolorization rate (%)94.594.392.393.491.192.4
    下载: 导出CSV

    表  2  比表面积和孔结构参数。

    Table  2.   Specific surface area and pore structure parameters

    SampleSBET (m2 g−1)Smicro (m2 g−1)Smeso (m2 g−1)Vtotal (cm3 g−1)Vmicro (cm3 g−1)Vmeso (cm3 g−1)Pore size (nm)
    ACS10758871160.540.410.092.00
    NACS977829960.510.380.081.98
    下载: 导出CSV

    表  3  XPS表征参数

    Table  3.   XPS characterization parameters.

    SampleXPS analysis (at.%)
    CON
    ACS95.374.63-/-
    NACS83.4214.382.2
    下载: 导出CSV

    表  4  XPS O1s分峰拟合参数

    Table  4.   O1s Peak-fitting parameters of XPS.

    O1sPeak typePeak position(eV)ACS(%)NACS(%)
    Quinone531.318.0814.95
    C=O532.322.7823.68
    C―O533.330.7741.41
    C―OH534.228.3719.96
    下载: 导出CSV

    表  5  ACS和NACS吸附PBQ和DBD动力学参数

    Table  5.   The first-order and second-order kinetics fitting Parameters for adsorption of PBQ and DBD on the ACS and NACS.

    AdsorbentAdsorbatePseudo-first
    order kinetic
    Pseudo-second
    order kinetic
    K1qeR2K2qeR2
    ACSPBQ0.03712.390.99840.0053711.350.9790
    DBD0.0198.860.99810.007489.260.9811
    NACSPBQ0.00916.100.99720.0029714.700.9923
    DBD0.01313.400.99850.0041210.430.9890
    下载: 导出CSV
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出版历程
  • 收稿日期:  2020-09-16
  • 修回日期:  2021-02-05
  • 网络出版日期:  2021-04-28
  • 刊出日期:  2021-07-30

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