New nanostructured sorbents for desulfurization of natural gas

doi:10.1007/s11705-014-1411-4

Front. Chem. Sci. Eng.

2014, Vol. 8

Issue (1) : 8-19 https://doi.org/10.1007/s11705-014-1411-4

REVIEW ARTICLE

New nanostructured sorbents for desulfurization of natural gas

Lifeng WANG, Ralph T. YANG(

)

Department of Chemical Engineering, University of Michigan, Ann Arbor, MI 48109, USA

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Abstract

Desulfurization of natural gas is achieved commercially by absorption with liquid amine solutions. Adsorption technology could potentially replace the solvent extraction process, particularly for the emerging shale gas wells with production rates that are generally lower than that from the large conventional reservoirs, if a superior adsorbent (sorbent) is developed. In this review, we focus our discussion on three types of sorbents: metal-oxide based sorbents, Cu/Ag-based and other commercial sorbents, and amine-grafted silicas. The advantages and disadvantages of each type are analyzed. Possible approaches for future developments to further improve these sorbents are suggested, particularly for the most promising amine-grafted silicas.

Keywords desulfurization natural gas desulfurization hydrogen sulfide sorbent amine-silica sorbent

Corresponding Author(s): Ralph T. YANG

Issue Date: 05 March 2014

Cite this article:

Lifeng WANG,Ralph T. YANG. New nanostructured sorbents for desulfurization of natural gas[J]. Front. Chem. Sci. Eng., 2014, 8(1): 8-19.

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https://academic.hep.com.cn/fcse/EN/10.1007/s11705-014-1411-4
https://academic.hep.com.cn/fcse/EN/Y2014/V8/I1/8

Fig.1 Adsorption isotherms of H₂S on zeolite 5A in the presence of different H₂O concentrations (T = 298.15?K, P = 1.3 bar). The addition of H₂O led to a marked capacity loss of H₂S over zeolite. Reprinted with permission of Ref. [16]

Fig.2 H₂S breakthrough curves in a mixture of H₂S/CH₄ for (a) MSU-1 copper samples and (b) MSU-1 zinc samples. Reprinted with permission of [34]

Fig.3 Schematic representation of the reaction process. (left) low metal oxide content and (right) high metal oxide content. Reprinted with permission of [34]

Fig.4 Breakthrough curves of various transition metals doped ZnO sorbents tested with 2?vol-% H₂S-H₂ at room temperature. Test condition: room temperature; flow rate: 125?mL/min; face velocity: 3?cm/s; sample weight: 1?g; bed size: 1?cm (dia.) × 2?cm. Reprinted with permission of [39]

Fig.5 Breakthrough curves for fresh and regenerated commercial ZnO sorbent particles (top) and breakthrough curves for regenerated ZnO/SiO₂ at various regeneration temperatures (bottom). Sorbents (0.5?g) were tested at room temperature (20°C) with 8000?ppmv H₂S at a face (i.e., superficial) velocity of 2.3?cm/s. Reprinted with permission of [39]

Fig.6 Adsorption isotherms for H₂S adsorption on commercial and new sorbents at 25°C (H₂S in He, at 1 atm).; Langmuir-Freundlich isotherm fitting data (line). Reprinted with permission of [44]

Fig.7 Isotherms of CH₄ on Cu(I)Y zeolite at different temperatures. Reprinted with permission of [44]

Tab.1 Energies of adsorption in kcal/mol for sulfur adsorbates: (a) experimental vs. (b) ab initio molecular orbital theory

Fig.8 Grafting of silanes (using 3-aminopropyltriethoxy-silane as an example) on silica surface, showing two silanols are needed for each silane. Reprinted with permission of [9]

Fig.9 FTIR spectra of (a) MCM-48 mesoporous silica and (b) amine-grafted MCM-48 at room temperature. Reprinted with permission of [10]

Fig.10 FTIR spectra of aminosilane-grafted MCM-48 heated at different temperatures in He atmosphere, from top down: (a) 25°C, (b) 100°C, (c) 200°C, (d) 250°C and (e) 350°C. Reprinted with permission of [10]

Fig.11 Adsorption isotherms for H₂S on amine-grafted silicas (MCM-48 and xerogel SiO₂) at 25°C. Reprinted with permission of [10]

Fig.12 Isotherms for CH₄ on the same sorbents at 25°C. Note: P_H2S (of H₂S in He) is in the range 0-1000 ppm (of 1 atm), while the pressure of CH₄ is 0–1 atm. Reprinted with permission of [10]

Fig.13 Cyclic H₂S adsorption-desorption on amine-MCM-48. Adsorption was by flowing in 1000?ppm H₂S carried in helium at 25°C whereas desorption was in helium at 60°C. Total desorption occurred by inert (He) purge at 60°C. Reprinted with permission of [10]

Fig.14 TPD profiles of H₂S from amine-MCM-48 after exposure to 1% H₂S (in He) with and without 2% H₂O. Heating rate= 5°C/min. Reprinted with permission of [10]

Fig.15 Adsorption isotherms for pure CO₂, H₂S, and CH₄ on triamine-grafted pore-expanded mesoporous silica “TRI-PE-MCM-41” at 25°C. Reprinted with permission of [12]

Fig.16 Three types of silanol (hydroxyl) groups on silicas. Reprinted with permission of [9]

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