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Review of H2S selective oxidation over carbon-based materials at low temperature from pollutant to energy storage materials

SUN Ming-hui WANG Xu-zhen ZHAO Zong-bin QIU Jie-shan

孙明慧, 王旭珍, 赵宗彬, 邱介山. 碳基材料在低温硫化氢选择性氧化中的研究进展:从污染物到储能材料. 新型炭材料, 2022, 37(4): 675-694. doi: 10.1016/S1872-5805(22)60622-X
引用本文: 孙明慧, 王旭珍, 赵宗彬, 邱介山. 碳基材料在低温硫化氢选择性氧化中的研究进展:从污染物到储能材料. 新型炭材料, 2022, 37(4): 675-694. doi: 10.1016/S1872-5805(22)60622-X
SUN Ming-hui, WANG Xu-zhen, ZHAO Zong-bin, QIU Jie-shan. Review of H2S selective oxidation over carbon-based materials at low temperature from pollutant to energy storage materials. New Carbon Mater., 2022, 37(4): 675-694. doi: 10.1016/S1872-5805(22)60622-X
Citation: SUN Ming-hui, WANG Xu-zhen, ZHAO Zong-bin, QIU Jie-shan. Review of H2S selective oxidation over carbon-based materials at low temperature from pollutant to energy storage materials. New Carbon Mater., 2022, 37(4): 675-694. doi: 10.1016/S1872-5805(22)60622-X

碳基材料在低温硫化氢选择性氧化中的研究进展:从污染物到储能材料

doi: 10.1016/S1872-5805(22)60622-X
基金项目: 国家自然科学基金项目(22179017,52172038,U1610105)
详细信息
    通讯作者:

    王旭珍,教授. E-mail:xzwang@dlut.edu.cn

  • 中图分类号: O643.32

Review of H2S selective oxidation over carbon-based materials at low temperature from pollutant to energy storage materials

Funds: The authors acknowledge the financial support from projects funded by National Natural Science Foundation of China (Grant Nos. 22179017, 52172038, U1610105)
More Information
  • 摘要: 在过去的几十年中,用碳基材料实现室温下硫化氢(H2S)选择性氧化技术受到越来越多的关注。本文综述了近年来碳基脱硫催化剂的研究进展,包括碱改性活性炭、杂原子掺杂或官能团改性的多孔炭以及碳/碱性金属氧化物复合材料。讨论了H2S在各种碳基催化剂上发生选择性氧化生成单质硫(S)的机理,指出了碳基材料的高比表面积、发达的孔隙结构和可调控的表面化学性质等优势在氧化脱硫中所起的重要作用。在此基础上,本文还总结了脱硫后得到的碳/硫复合材料的扩展应用——将其作为高性能锂硫电池(LSBs)的硫正极,进一步实现了含硫污染物的高附加值转化利用。最后,提出了目前碳基材料在低温H2S选择性氧化中面临的主要挑战和未来的应用前景,以期为该技术的进一步发展提供指导。
  • FIG. 1652.  FIG. 1652.

    FIG. 1652..  FIG. 1652.

    Figure  1.  Modulation strategies of carbon-based catalysts for H2S selective oxidation at room temperature.

    Figure  2.  (a) Relationships between saturation sulfur capacity (QS) and pore volume. (b) Relationships between the content of S (SOx) and the ratios V>0.7/Vt and V<0.7/Vt. (c) Schematic diagram of H2S oxidation and sulfur species deposition in the nanopores of ACFs[56]. (Reprinted with permission by American Chemical Society, Copyright 2010).

    Figure  3.  (a) Preparation schematic of AMCs. (b) SEM, TEM and elemental mapping images of pristine AMC-10%. (c) SEM, TEM and XRD pattern of the catalyst after H2S oxidation (AMC-10%-S)[38]. (Reprinted with permission by American Chemical Society, Copyright 2016) (d) H2S breakthrough curves of the catalysts with various alkalic impregnates. (e) Schematic diagram of H2S oxidation over MCSs with MgO and other soluble bases[63]. (Reprinted with permission by Elsevier, Copyright 2016).

    Figure  4.  (a) Schematic diagram of sulfur species disposition upon carbon aerogel with various microstructures[65]. (Copyright 2011, Elsevier) (b, c) FESEM images of typical N-PCNF-1/2-800 sample, the inset in (c) is the TEM image of sample. (d) N2 adsorption-desorption isotherms and pore-size distributions of samples prepared at different temperatures[26]. (Reprinted with permission by Elsevier, Copyright 2019).

    Figure  5.  (a) The configuration of N in NMC prepared at different temperatures. (b) Relationship between sulfur capacity and pyridinic-N content. (c) Schematic diagram of H2S oxidation and sulfur deposition on NMC[27]. (Reprinted with permission by American Chemical Society, Copyright 2013).

    Figure  6.  (a) Schematic diagram of H2S oxidation and sulfur deposition on MCNs-PEI-25. (b) EPR spectra of various catalysts under different conditions[46]. (Reprinted with permission by Elsevier, Copyright 2016) (c) Comparison of the desulfurization performance between NH2-PLCNFs and PLCNFs[25]. (Reprinted with permission by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim, Copyright 2022).

    Figure  7.  (a) A proposed mechanism of Na2CO3 deposition on graphene nanosheets. (b) Schematic diagram of H2S oxidation and sulfur deposition on AGAs[47]. (Reprinted with permission by Elsevier, Copyright 2020).

    Figure  8.  (a) Binding energy of O2•− radical on the surface of various catalysts, the inset in (a) is the front view of the adsorption model. (b) Comparison of the binding energy of O2 and O2•− radical adsorbed on various surfaces. EPR spectra of (c) different systems and (d) various alkali-modified PC catalysts in an airflow. (e) Schematic diagram of H2S oxidation and sulfur deposition on PC/MgO catalysts[24]. (Reprinted with permission by American Chemical Society, Copyright 2021).

    Figure  9.  (a) Preparation schematic and (b) SEM image of HRGO/S composite. (c) XRD patterns, and (d) Raman spectra of different samples. (e) CV curves (scan rate: 0.1 mV s–1), and (f) discharge/charge profiles of HRGO/S cathode. (g) Rate performance of different S cathodes[78]. (Reprinted with permission by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim, Copyright 2013)

    Figure  10.  (a) Preparation schematic of WDS. (b) SEM and (c) TEM images of S-38/MWCNT, the inset in (b) is a photograph of the membrane. (d) Cycling performance (current density: 1.0 A g–1), and (e) rate performance of S/MWCNT cathode, the inset in (d) is the schematic of coin cell composition[85]. (Reprinted with permission by Elsevier Copyright 2017)

    Figure  11.  (a) Schematic diagram of the in-situ fabrication of LSB cathodes by H2S selective oxidation. (b) Cycling performance (current density: 1 C), and (c) rate performance of various S cathodes[25]. (Reprinted with permission by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim, Copyright 2022).

    Table  1.   Carbon-based catalysts for the selective oxidation of H2S to elemental sulfur at low temperature.

    CatalystsReaction conditions${{\boldsymbol{Q}}_{\bf{S}}({\bf{g}}_{{{\bf{H}}_{\bf{2}}}{\bf{S}}}/{\bf{g}}_{{\bf{catalyst}}} )}$Reference
    Na2CO3-impregnated activated carbon fibersH2S 1000×10−6; O2 1%; RH 80%; 30 °C;
    flow rate 150 mL min−1.
    0.2-0.8[56]
    Alkaline mesoporous carbonsH2S 1000×10−6; O2 1%; RH 80%; 25 °C;
    flow rate 150 mL min−1.
    4.49[38]
    Na2CO3-impregnated carbon aerogelsH2S 1000×10−6; O2 1%; RH 80%; 30 °C;
    flow rate 150 mL min−1.
    2.26[65]
    Millimeter-sized mesoporous carbon spheresH2S 1000×10−6; O2 1%; RH 80%; 30 °C;
    flow rate 150 mL min−1.
    2.46[63]
    N-rich mesoporous carbonH2S 1000×10−6; O2 1%; RH 80%; 30 °C;
    flow rate 150 mL min−1.
    2.77[27]
    N-doped porous carbon nanofibersH2S 1000×10−6; O2 2%; RH 70%; 25 °C;
    flow rate 100 mL min−1.
    3.57[26]
    N-doped mesoporous carbon nanosheetsH2S 1000×10−6; O2 2%; RH 70%; room temperature;
    flow rate 200 mL min−1.
    1.37[39]
    Graphene aerogelsH2S 1000×10−6; O2 1%; RH 80%; 30 °C;
    flow rate 150 mL min−1.
    3.19[47]
    N-functionalized mesoporous carbon nanosheetsH2S 1000×10−6; O2 1%; RH 80%; 25 °C;
    flow rate 150 mL min−1.
    0.47[46]
    Amino-functionalized lotus-root-like carbon nanofibersH2S 1000×10−6; O2 1%; RH 80%; 25 °C;
    flow rate 25 mL min−1.
    3.46[25]
    ZnO/N-modified ACH2S 600 mg/m3; pre-humidified for 1.5 h using the moist N2
    (ca. 3% moisture); 30 °C; flow rate 100 mL min−1.
    0.06[79]
    MgO-loaded porous carbonH2S 1000×10−6; O2 1%; RH 80%; 30 °C;
    flow rate 150 mL min−1.
    2.40[24]
    ZnO-MgO/activated carbonH2S 850 mg/m3; pre-humidified for 1.5 h using the moist N2
    (ca. 3% moisture); 30 °C; flow rate 100 mL min−1.
    0.11[83]
    CaO/carbon nanosheetsH2S 1000×10−6; O2 1%; RH, 80%; 30 °C;
    flow rate 150 mL min−1.
    9.10[71]
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出版历程
  • 收稿日期:  2022-04-18
  • 修回日期:  2022-06-11
  • 网络出版日期:  2022-06-17
  • 刊出日期:  2022-08-01

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