Deactivation behaviors of MoS2/Si-ZrO2 catalyst during sulfur-resistant CO methanation

被引:0
|
作者
Gu J. [1 ]
Xin Z. [1 ,2 ]
Gao W. [1 ]
He L. [1 ]
Zhao R. [1 ]
机构
[1] Materials Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai
[2] State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai
来源
Huagong Xuebao/CIESC Journal | 2019年 / 70卷 / 10期
关键词
Bridging S_2^(2-) species; Catalyst; Deactivation; Natural gas; Stability; Sulfur loss; Sulfur-resistant methanation;
D O I
10.11949/0438-1157.20190565
中图分类号
学科分类号
摘要
The MoS2/Si-ZrO2 catalyst was prepared by an equal volume impregnation method, and the catalytic activity stability of CO for sulfur-tolerant methanation was evaluated. The CO conversion of the MoS2/Si-ZrO2 catalyst decreased by 11% under the following condition: molar ratio of feed gas composition was 2H2:2CO:1N2; concentration of H2S was 0.01%; weight hourly space velocity was 6000 ml/(g•h); reaction temperature was 450℃ and reaction pressure was 2.5 MPa. The catalysts were further characterized by hydrogen temperature programmed reduction (H2-TPR), X-rays photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM), Raman spectra (RS), inductively coupled plasma emission spectra (ICP-OES), thermogravimetric analysis (TGA) and elemental analysis. The results demonstrated that little carbon deposited on the surface of spent catalyst, which did not cause catalyst deactivation. The minor cause was that MoS2 slabs grew longer and stacked more layers after long-term reaction and then covered the active sites. The root deactivation cause was attributed to parts of catalytic active bridging S22- species converting to less active S2- species and H2S, which resulted in the loss of active sites and sulfur element. © All Right Reserved.
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页码:3941 / 3948
页数:7
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  • [1] Ronsch S., Schneider J., Matthischke S., Et al., Review on methanation-from fundamentals to current projects, Fuel, 166, 2, pp. 276-296, (2016)
  • [2] Cao H.X., Zhang J., Guo C.L., Et al., Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation: effect of promoter species on catalytic performance, Chinese Journal of Catalysis, 38, 7, pp. 1127-1137, (2017)
  • [3] Zhang X., Rui N., Jia X., Et al., Effect of decomposition of catalyst precursor on Ni/CeO<sub>2</sub> activity for CO methanation, Chinese Journal of Catalysis, 40, 4, pp. 495-503, (2019)
  • [4] Tao M., Xin Z., Meng X., Et al., Highly dispersed nickel within mesochannels of SBA-15 for CO methanation with enhanced activity and excellent thermostability, Fuel, 188, 1, pp. 267-276, (2017)
  • [5] Gao J.J., Liu Q., Gu F.N., Et al., Recent advances in methanation catalysts for the production of synthetic natural gas, RSC Advances, 5, 29, pp. 22759-22776, (2015)
  • [6] Andersson R., Boutonnet M., Jaras S., Higher alcohols from syngas using a K/Ni/MoS<sub>2</sub> catalyst: trace sulfur in the product and effect of H<sub>2</sub>S-containing feed, Fuel, 115, 1, pp. 544-550, (2014)
  • [7] Shi G., Han W., Yuan P., Et al., Sulfided Mo/Al<sub>2</sub>O<sub>3</sub> hydrodesulfurization catalyst prepared by ethanol-assisted chemical deposition method, Chinese Journal of Catalysis, 34, 4, pp. 659-666, (2013)
  • [8] Hao L., Xiong G., Liu L., Et al., Preparation of highly dispersed desulfurization catalysts and their catalytic performance in hydrodesulfurization of dibenzothiophene, Chinese Journal of Catalysis, 37, 3, pp. 412-419, (2016)
  • [9] Li M., Wang D., Li J., Et al., Surfactant-assisted hydrothermally synthesized MoS<sub>2</sub> samples with controllable morphologies and structures for anthracene hydrogenation, Chinese Journal of Catalysis, 38, 3, pp. 597-606, (2017)
  • [10] Wang B., Yu W., Wang W., Et al., Effect of boron addition on the MoO<sub>3</sub>/CeO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub> catalyst in the sulfur-resistant methanation, Chinese Journal of Chemical Engineering, 26, 3, pp. 509-513, (2018)