Adsorptive separation of CO2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation

Saha, Dipendu; Orkoulas, Gerassimos; Chen, Jihua; Hensley, Dale K.

doi:10.1016/j.micromeso.2016.12.015

Title: Adsorptive separation of CO₂ in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation

Journal Article · Wed Mar 01 00:00:00 EST 2017 · Microporous and Mesoporous Materials

DOI:https://doi.org/10.1016/j.micromeso.2016.12.015· OSTI ID:1394439

Saha, Dipendu ^[1]; Orkoulas, Gerassimos ^[1]; Chen, Jihua ^[2]; Hensley, Dale K. ^[2]

Widener Univ., Chester, PA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

In this research, we have synthesized two sulfur functionalized nanoporous carbons by post-synthesis modifications with sulfur bearing activating agents that simultaneously enhanced the surface area and introduced sulfur functionalities on the carbon surface. The Brunauer–Emmett–Teller (BET) surface areas of these materials were 2865 and 837 m²/g with total sulfur contents of 8.2 and 12.9 %, respectively. The sulfur-functionalized carbons were characterized with pore textural properties, X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA) and electron microscopy (SEM and TEM). In both the carbons, CO₂ adsorption isotherms and kinetics were measured in three different temperatures of 298, 288 and 278 K and pressures up to 760 torr. The gravimetric CO₂ uptake followed the trend with BET surface area but the surface area-based uptake was reversed and it followed the trend of sulfur content. The heat of adsorption of CO₂ in low uptake was 60-65 kJ/mol, which is the highest for CO₂ adsorption in porous carbons. In order to investigate the adsorptive separation of CO₂, N₂ and CH₄ adsorption isotherms were also measured at 298 K and 760 torr. The selectivity of separation for CO₂/N₂ and CO₂/CH₄ was calculated based on the Ideal Adsorbed Solution Theory (IAST) and all the results demonstrated the high CO₂ selectivity for the carbon with higher sulfur content. The adsorption isotherms were combined with mass balances to calculate the breakthrough behavior of the binary mixtures of CO₂/N₂ and CO₂/CH₄. The simulation results demonstrated that the dimensionless breakthrough time is a decreasing function of the mole fraction of CO₂ in the feed stream. The overall results suggest that the sulfurfunctionalized carbons can be employed as potential adsorbents for CO₂ separation.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1394439

Journal Information:: Microporous and Mesoporous Materials, Vol. 241, Issue C; ISSN 1387-1811

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 44 works

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