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Title: Adsorptive separation of CO 2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation

Abstract

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 m 2/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, CO 2 adsorption isotherms and kinetics were measured in three different temperatures of 298, 288 and 278 K and pressures up to 760 torr. The gravimetric CO 2 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 CO 2 in low uptake was 60-65 kJ/mol, which is the highest for CO 2 adsorption in porous carbons. In order to investigate the adsorptive separation of CO 2, N 2 and CH 4 adsorption isotherms were also measured at 298 K and 760 torr. The selectivity of separation for CO 2/N 2 and CO 2/CH 4 was calculated based onmore » the Ideal Adsorbed Solution Theory (IAST) and all the results demonstrated the high CO 2 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 CO 2/N 2 and CO 2/CH 4. The simulation results demonstrated that the dimensionless breakthrough time is a decreasing function of the mole fraction of CO 2 in the feed stream. The overall results suggest that the sulfurfunctionalized carbons can be employed as potential adsorbents for CO 2 separation.« less

Authors:
 [1];  [1];  [2];  [2]
  1. Widener Univ., Chester, PA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1394439
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Microporous and Mesoporous Materials
Additional Journal Information:
Journal Volume: 241; Journal Issue: C; Journal ID: ISSN 1387-1811
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Saha, Dipendu, Orkoulas, Gerassimos, Chen, Jihua, and Hensley, Dale K. Adsorptive separation of CO2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation. United States: N. p., 2017. Web. doi:10.1016/j.micromeso.2016.12.015.
Saha, Dipendu, Orkoulas, Gerassimos, Chen, Jihua, & Hensley, Dale K. Adsorptive separation of CO2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation. United States. doi:10.1016/j.micromeso.2016.12.015.
Saha, Dipendu, Orkoulas, Gerassimos, Chen, Jihua, and Hensley, Dale K. Wed . "Adsorptive separation of CO2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation". United States. doi:10.1016/j.micromeso.2016.12.015. https://www.osti.gov/servlets/purl/1394439.
@article{osti_1394439,
title = {Adsorptive separation of CO2 in sulfur-doped nanoporous carbons: Selectivity and breakthrough simulation},
author = {Saha, Dipendu and Orkoulas, Gerassimos and Chen, Jihua and Hensley, Dale K.},
abstractNote = {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.},
doi = {10.1016/j.micromeso.2016.12.015},
journal = {Microporous and Mesoporous Materials},
number = C,
volume = 241,
place = {United States},
year = {Wed Mar 01 00:00:00 EST 2017},
month = {Wed Mar 01 00:00:00 EST 2017}
}

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