Desulfurization and Regeneration Performance of Sorbent Prepared by Subcritical Water Impregnation

Abstract:

A series of metal oxides sorbents supported on γ-Al₂O₃ were directly prepared by subcritical water impregnation (SCWI) method using an autoclave reactor. The effects of active components, preparation pressure, temperature, and time on the desulfurization activity of sorbents in hot coal-based gases at mid-temperature were investigated. The samples were characterized by X-ray diffraction (XRD), nitrogen adsorption and atomic absorption spectrophotometer (AAS). The results showed that Mn-based sorbent loaded on γ-Al₂O₃ by SCWI presented a good desulfurization performance. The optimal preparation parameters of sorbent were the temperature of 350 °C, the pressure of 18.9 MPa, impregnation time of 30 min, the precursor solution concentration of 0.287 mol/L and the volume of 100 ml, respectively. The Mn/γ-Al₂O₃ sorbent prepared under the optimal conditions presented a good desulfurization precision and regeneration performance. After regeneration, the mechanical strengths of the sorbents were higher than that of raw support and the breakthrough time at the desulfurization efficiency of above 99% was not obviously decreased.

• Periodical: Materials Science Forum (Volumes 743-744)
• Pages: 443-448
• DOI: https://doi.org/10.4028/www.scientific.net/MSF.743-744.443
• Online since: January 2013
• Authors: Hao Chen Qin, Lian Wei Liu, Wei Ping Si, Li Ping Chang, Wei Ren Bao, Li Na Han
• Keywords: Coal-Based Gas, Desulfurization, MnO_x/γ-Al₂O₃, Sub-Critical Water Impregnation

References

[1] E. Reverchon, R. Adami, Nanomaterials and supercritical fluids, J. Supercrit. Fluid. 37 (2006) 1-22.

[2] J. Otsu, Y. Oshima, New approaches to the preparation of metal or metal oxide particles on the surface of porous materials using supercritical water: Development of supercritical water impregnation method, J. Supercrit. Fluid. 33 (2005) 61-67.

DOI: 10.1016/s0896-8446(04)00098-1

[3] C.B. Xu, A. S Teja, Supercritical water synthesis and deposition of iron oxide (alpha-Fe2O3) nanoparticles in activated carbon, J. Supercrit. Fluid. 39 (2006) 135-141.

DOI: 10.1016/j.supflu.2006.02.004

[4] R.B. Slimane, J. Abbasian, Regenerable mixed metal oxide sorbents for coal gas desulfurization at moderate temperatures, Adv. Environ. Res. 4 (2000) 147-162.

DOI: 10.1016/s1093-0191(00)00017-4

[5] P.R. Westmoreland, D.P. Harrison, Evaluation of candidate solids for high-temperature desulfurization of low-Btu gases, Environ. Sci. Technol. 10 (1976) 659-661.

DOI: 10.1021/es60118a010

[6] P.R. Westmoreland, J.B. Gibson, D.P. Harrison, Comparative kinetics of high-temperature reaction between hydrogen sulfide and selected metal oxides, Environ. Sci. Technol. 11 (1977) 488-491.

DOI: 10.1021/es60128a007

[7] J. Wang, B. Qiu, L. Han, G. Feng, Y. Hu, L. Chang, W. Bao, Effect of precursor and preparation method on manganese based activated carbon sorbents for removing H2S from hot coal gas, J. Hazard. Mater. 213–214 (2012) 184-192.

DOI: 10.1016/j.jhazmat.2012.01.080

[8] B.A. Qiu, L.N. Han, J.C. Wang, L.P. Chang, W.R. Bao, Preparation of sorbents loaded on activated carbon to remove H2S from hot coal gas by supercritical water Impregnation, Energ. Fuel. 25 (2011) 591-595.

DOI: 10.1021/ef101358x

[9] W. Si, J. Wang, L. Chang, W. Bao, Preparation of Desulfurizer by Super-critical Water Impregnation Method and Its Sulfidation Properties at Mid-temperature, J. Taiyuan U. Technol. 41 (2010) 733-736.

[10] A. Aimable, H. Muhr, C. Gentric, F. Bernard, F. L. e Cras, D. Aymes, Continuous hydrothermal synthesis of inorganic nanopowders in supercritical water: Towards a better control of the process, Powder Technol. 190 (2009) 99-106.

DOI: 10.1016/j.powtec.2008.04.064

[11] J. Zhang, Y. Wang, R. Ma, D. Wu, A study on regeneration of Mn-Fe-Zn-O supported upon [gamma]-Al2O3 sorbents for hot gas desulfurization, Fuel Process. Technol. 84 (2003) 217-227.

DOI: 10.1016/s0378-3820(03)00057-2