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Title: Solvent-free and one-pot synthesis of ultramicroporous carbons with ultrahigh nitrogen contents for sulfur dioxide capture

Abstract

SO2 from industrial tail gas is of great significance to control the environmental issues potentially induced by SO2 emission. In the present work, porous carbons with rich ultramicropores and ultrahigh N contents (11.5–17.3 wt%) were synthesized by directly pyrolyzing the mixtures of glucose and urea at 700 °C, without the use of any solvents. Additionally, the synthesized porous carbons were characterized for porosity, morphology and elemental compositions, and also systematically investigated for SO2 capture performance. Furthermore, it is found that the adsorption of SO2 on synthesized porous carbons shows chemical behavior, owing to the strong acid-based interaction between SO2 and pyridinic N. As consequence, the SO2 capacities of synthesized porous carbons are very high, especially at low pressures (4.16 mmol/g at 296.2 K and 10 kPa). The synthesized porous carbons also display impressive adsorption selectivities for SO2/CO2/N2 mixed gas, and good reversibility for SO2 adsorption. Thus, it is believed that the synthesized porous carbons are promising candidates for selective and reversible SO2 capture.

Authors:
 [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Nanchang Univ. (China). Key Lab. of Poyang lake Environment and Research Utilization
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Science Foundation of Jiangxi Province
OSTI Identifier:
1651332
Alternate Identifier(s):
OSTI ID: 1780288
Grant/Contract Number:  
AC05-00OR22725; SC0012577; 20192ACB21016
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Engineering Journal
Additional Journal Information:
Journal Volume: 391; Journal Issue: 1; Journal ID: ISSN 1385-8947
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ultramicroporous carbon; facile synthesis; nitrogen content; SO2 capture; selective adsorption

Citation Formats

Zhang, Jia-Yin, Zhang, Jian-Bo, Li, Meijun, Wu, Zili, Dai, Sheng, and Huang, Kuan. Solvent-free and one-pot synthesis of ultramicroporous carbons with ultrahigh nitrogen contents for sulfur dioxide capture. United States: N. p., 2019. Web. https://doi.org/10.1016/j.cej.2019.123579.
Zhang, Jia-Yin, Zhang, Jian-Bo, Li, Meijun, Wu, Zili, Dai, Sheng, & Huang, Kuan. Solvent-free and one-pot synthesis of ultramicroporous carbons with ultrahigh nitrogen contents for sulfur dioxide capture. United States. https://doi.org/10.1016/j.cej.2019.123579
Zhang, Jia-Yin, Zhang, Jian-Bo, Li, Meijun, Wu, Zili, Dai, Sheng, and Huang, Kuan. Sat . "Solvent-free and one-pot synthesis of ultramicroporous carbons with ultrahigh nitrogen contents for sulfur dioxide capture". United States. https://doi.org/10.1016/j.cej.2019.123579. https://www.osti.gov/servlets/purl/1651332.
@article{osti_1651332,
title = {Solvent-free and one-pot synthesis of ultramicroporous carbons with ultrahigh nitrogen contents for sulfur dioxide capture},
author = {Zhang, Jia-Yin and Zhang, Jian-Bo and Li, Meijun and Wu, Zili and Dai, Sheng and Huang, Kuan},
abstractNote = {SO2 from industrial tail gas is of great significance to control the environmental issues potentially induced by SO2 emission. In the present work, porous carbons with rich ultramicropores and ultrahigh N contents (11.5–17.3 wt%) were synthesized by directly pyrolyzing the mixtures of glucose and urea at 700 °C, without the use of any solvents. Additionally, the synthesized porous carbons were characterized for porosity, morphology and elemental compositions, and also systematically investigated for SO2 capture performance. Furthermore, it is found that the adsorption of SO2 on synthesized porous carbons shows chemical behavior, owing to the strong acid-based interaction between SO2 and pyridinic N. As consequence, the SO2 capacities of synthesized porous carbons are very high, especially at low pressures (4.16 mmol/g at 296.2 K and 10 kPa). The synthesized porous carbons also display impressive adsorption selectivities for SO2/CO2/N2 mixed gas, and good reversibility for SO2 adsorption. Thus, it is believed that the synthesized porous carbons are promising candidates for selective and reversible SO2 capture.},
doi = {10.1016/j.cej.2019.123579},
journal = {Chemical Engineering Journal},
number = 1,
volume = 391,
place = {United States},
year = {2019},
month = {11}
}

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