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Title: Aqueous and Template-Free Synthesis of Meso-Macroporous Polymers for Highly Selective Capture and Conversion of Carbon Dioxide

Abstract

Meso–macroporous polymers possessing nitrogen functionality were innovatively synthesized through an aqueous and template-free route herein. In particular, the polymerization of 1-(4-vinylbenzyl)-1,3,5,7-tetraazaadamantan-1-ium chloride in aqueous solution under high temperatures induces the decomposition of the hexamethylenetetramine unit into ammonia and formaldehyde molecules, followed by the cross-linking of benzene rings through “resol chemistry”. During this process, extended meso–macroporous frameworks were constructed, and active nitrogen species were incorporated. Taking the advantage of the meso–macroporosity and nitrogen functionality, the synthesized polymers offer competitive CO 2 capacities (0.37–1.58 mmol g –1 at 0 °C and 0.15 bar) and outstanding CO 2/N 2 selectivities (155–324 at 0 °C). Moreover, after complexed with metal ions, the synthesized polymers show excellent activity for catalyzing the cycloaddition of propylene oxide with CO2 (yield>98.5 %, turnover frequency: 612.9–761.1 h –1).

Authors:
 [1]; ORCiD logo [2];  [2];  [3]
  1. Nanchang Univ. (China)
  2. Fuzhou Univ. (China)
  3. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Georgia Inst. of Technology, Atlanta, GA (United States). Energy Frontier Research Center (EFRC) Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1469891
Alternate Identifier(s):
OSTI ID: 1399273
Grant/Contract Number:  
SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 21; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; 36 MATERIALS SCIENCE; carbon dioxide capture; carbon dioxide conversion; meso-macropores; nitrogen functionality; porous organic polymers

Citation Formats

Huang, Kuan, Liu, Fujian, Jiang, Lilong, and Dai, Sheng. Aqueous and Template-Free Synthesis of Meso-Macroporous Polymers for Highly Selective Capture and Conversion of Carbon Dioxide. United States: N. p., 2017. Web. doi:10.1002/cssc.201701666.
Huang, Kuan, Liu, Fujian, Jiang, Lilong, & Dai, Sheng. Aqueous and Template-Free Synthesis of Meso-Macroporous Polymers for Highly Selective Capture and Conversion of Carbon Dioxide. United States. doi:10.1002/cssc.201701666.
Huang, Kuan, Liu, Fujian, Jiang, Lilong, and Dai, Sheng. Fri . "Aqueous and Template-Free Synthesis of Meso-Macroporous Polymers for Highly Selective Capture and Conversion of Carbon Dioxide". United States. doi:10.1002/cssc.201701666. https://www.osti.gov/servlets/purl/1469891.
@article{osti_1469891,
title = {Aqueous and Template-Free Synthesis of Meso-Macroporous Polymers for Highly Selective Capture and Conversion of Carbon Dioxide},
author = {Huang, Kuan and Liu, Fujian and Jiang, Lilong and Dai, Sheng},
abstractNote = {Meso–macroporous polymers possessing nitrogen functionality were innovatively synthesized through an aqueous and template-free route herein. In particular, the polymerization of 1-(4-vinylbenzyl)-1,3,5,7-tetraazaadamantan-1-ium chloride in aqueous solution under high temperatures induces the decomposition of the hexamethylenetetramine unit into ammonia and formaldehyde molecules, followed by the cross-linking of benzene rings through “resol chemistry”. During this process, extended meso–macroporous frameworks were constructed, and active nitrogen species were incorporated. Taking the advantage of the meso–macroporosity and nitrogen functionality, the synthesized polymers offer competitive CO2 capacities (0.37–1.58 mmol g–1 at 0 °C and 0.15 bar) and outstanding CO2/N2 selectivities (155–324 at 0 °C). Moreover, after complexed with metal ions, the synthesized polymers show excellent activity for catalyzing the cycloaddition of propylene oxide with CO2 (yield>98.5 %, turnover frequency: 612.9–761.1 h–1).},
doi = {10.1002/cssc.201701666},
journal = {ChemSusChem},
number = 21,
volume = 10,
place = {United States},
year = {2017},
month = {9}
}

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