skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · ChemSusChem
 [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)

Abstract Meso–macroporous polymers possessing nitrogen functionality were innovatively synthesized through an aqueous and template‐free route herein. Specifically, 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). Furthermore, after complexed with metal ions, the synthesized polymers show excellent activity for catalyzing the cycloaddition of propylene oxide with CO 2 (yield>98.5 %, turnover frequency: 612.9–761.1 h −1 ).

Research Organization:
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 Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
SC0012577
OSTI ID:
1469891
Alternate ID(s):
OSTI ID: 1399273
Journal Information:
ChemSusChem, Vol. 10, 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; ISSN 1864-5631
Publisher:
ChemPubSoc EuropeCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 29 works
Citation information provided by
Web of Science

References (72)

Effect of pore size on carbon dioxide sorption by carbide derived carbon journal January 2011
Efficient CO2 capture by a task-specific porous organic polymer bifunctionalized with carbazole and triazine groups journal January 2014
Design and Preparation of Porous Polymers journal April 2012
Thermodynamics of mixed-gas adsorption journal January 1965
Importance of Micropore-Mesopore Interfaces in Carbon Dioxide Capture by Carbon-Based Materials journal June 2016
Nitrogen-Rich Covalent Triazine Frameworks as High-Performance Platforms for Selective Carbon Capture and Storage journal November 2015
Hypercrosslinked Aromatic Heterocyclic Microporous Polymers: A New Class of Highly Selective CO 2 Capturing Materials journal September 2012
Fabrication of mesoporous polymer monolith: a template-free approach journal January 2011
Expanding Radical SAM Chemistry by Using Radical Addition Reactions and SAM Analogues journal August 2016
Supramolecular Aggregates as Templates: Ordered Mesoporous Polymers and Carbons journal February 2008
Highly Stable Porous Polymer Networks with Exceptionally High Gas-Uptake Capacities journal July 2011
Novel hollow and yolk–shell structured periodic mesoporous polymer nanoparticles journal January 2016
Carbon dioxide capture in amorphous porous organic polymers journal January 2017
Triptycene based 1,2,3-triazole linked network polymers (TNPs): small gas storage and selective CO 2 capture journal January 2015
A facile soft-template synthesis of mesoporous polymeric and carbonaceous nanospheres journal December 2013
Mesoporous Poly(Melamine-Formaldehyde) Solid Sorbent for Carbon Dioxide Capture journal June 2013
Nitrogen-rich conjugated microporous polymers: impact of building blocks on porosity and gas adsorption journal January 2015
High CO 2 uptake and selectivity by triptycene-derived benzimidazole-linked polymers journal January 2012
Conjugated porous polymers for energy applications journal January 2012
Phosphonium salt incorporated hypercrosslinked porous polymers for CO 2 capture and conversion journal January 2015
Systematic Tuning and Multifunctionalization of Covalent Organic Polymers for Enhanced Carbon Capture journal October 2015
Ordered Mesoporous Polymers and Homologous Carbon Frameworks: Amphiphilic Surfactant Templating and Direct Transformation journal November 2005
Porous polymer catalysts with hierarchical structures journal January 2015
Imidazolium salt-modified porous hypercrosslinked polymers for synergistic CO 2 capture and conversion journal January 2015
High and selective CO 2 adsorption by a phthalocyanine nanoporous polymer journal January 2015
Is N-Doping in Porous Carbons Beneficial for CO 2 Storage? Experimental Demonstration of the Relative Effects of Pore Size and N-Doping journal January 2016
Hydroxyl-functionalized ionic liquid: a novel efficient catalyst for chemical fixation of CO2 to cyclic carbonate journal May 2008
Microporous organic polymers for gas storage and separation applications journal January 2013
A sustainable protocol for the facile synthesis of zinc-glutamate MOF: an efficient catalyst for room temperature CO 2 fixation reactions under wet conditions journal January 2016
A Facile Aqueous Route to Synthesize Highly Ordered Mesoporous Polymers and Carbon Frameworks with Iad Bicontinuous Cubic Structure journal October 2005
Conjugated Microporous Polymers with Dimensionality-Controlled Heterostructures for Green Energy Devices journal May 2015
Imine-Linked Porous Polymer Frameworks with High Small Gas (H 2 , CO 2 , CH 4 , C 2 H 2 ) Uptake and CO 2 /N 2 Selectivity journal April 2013
Construction of Sole Benzene Ring Porous Aromatic Frameworks and Their High Adsorption Properties journal December 2014
Direct Capture of CO2 from Ambient Air journal August 2016
Polymer sensors for nitroaromatic explosives detection journal January 2006
Functional porous organic polymers for heterogeneous catalysis journal January 2012
Expanding Radical SAM Chemistry by Using Radical Addition Reactions and SAM Analogues journal August 2016
Ordered Mesoporous Polymers and Homologous Carbon Frameworks: Amphiphilic Surfactant Templating and Direct Transformation journal November 2005
Synthesis, Properties, and Gas Separation Studies of a Robust Diimide-Based Microporous Organic Polymer journal July 2009
Triazine functionalized ordered mesoporous polymer: a novel solid support for Pd-mediated C–C cross-coupling reactions in water journal January 2011
Porous Ionic Polymers as a Robust and Efficient Platform for Capture and Chemical Fixation of Atmospheric CO 2 journal December 2016
Porous polymer particles—A comprehensive guide to synthesis, characterization, functionalization and applications journal March 2012
Enhanced Carbon Dioxide Capture from Landfill Gas Using Bifunctionalized Benzimidazole-Linked Polymers journal June 2016
A Family of Highly Ordered Mesoporous Polymer Resin and Carbon Structures from Organic−Organic Self-Assembly journal September 2006
Funktionale poröse Koordinationspolymere journal April 2004
Targeted Synthesis of a Porous Aromatic Framework with High Stability and Exceptionally High Surface Area journal November 2009
Porous Organic Polymers in Catalysis Opportunities and Challenges journal May 2011
Supercapacitive Energy Storage and Electric Power Supply Using an Aza-Fused π-Conjugated Microporous Framework journal August 2011
Adsorbent Materials for Carbon Dioxide Capture from Large Anthropogenic Point Sources journal September 2009
Capture and conversion of CO2 at ambient conditions by a conjugated microporous polymer journal June 2013
Importance of Micropore–Mesopore Interfaces in Carbon Dioxide Capture by Carbon‐Based Materials journal March 2016
One-step synthesis of nitrogen-doped graphene-like meso-macroporous carbons as highly efficient and selective adsorbents for CO 2 capture journal January 2016
Microporous Polycarbazole with High Specific Surface Area for Gas Storage and Separation journal March 2012
Sulfonate-Grafted Porous Polymer Networks for Preferential CO2 Adsorption at Low Pressure journal November 2011
Hierarchically porous organic polymers: highly enhanced gas uptake and transport through templated synthesis journal January 2015
Azo-functionalized microporous organic polymers: synthesis and applications in CO 2 capture and conversion journal January 2015
Supercapacitive Energy Storage and Electric Power Supply Using an Aza-Fused π-Conjugated Microporous Framework journal August 2011
Efficient Fixation of CO 2 by a Zinc-Coordinated Conjugated Microporous Polymer journal May 2014
Zn( ii ) assisted synthesis of porous salen as an efficient heterogeneous scaffold for capture and conversion of CO 2 journal January 2015
Targeted Synthesis of a Porous Aromatic Framework with High Stability and Exceptionally High Surface Area journal November 2009
Porous Polymer Networks: Synthesis, Porosity, and Applications in Gas Storage/Separation journal November 2010
Covalent Organic Frameworks for CO 2 Capture journal February 2016
Functional Porous Coordination Polymers journal April 2004
Porous Phosphorescent Coordination Polymers for Oxygen Sensing journal January 2010
Ionic liquid thermal stabilities: decomposition mechanisms and analysis tools journal January 2013
Combined CO 2 -philicity and Ordered Mesoporosity for Highly Selective CO 2 Capture at High Temperatures journal June 2015
Solvothermal synthesis of hierarchically nanoporous organic polymers with tunable nitrogen functionality for highly selective capture of CO 2 journal January 2016
Nanoscale covalent organic frameworks as smart carriers for drug delivery journal January 2016
3D Porous Crystalline Polyimide Covalent Organic Frameworks for Drug Delivery journal June 2015
Facile fabrication of cost-effective porous polymer networks for highly selective CO 2 capture journal January 2015
Nitrogen-Containing Microporous Conjugated Polymers via Carbazole-Based Oxidative Coupling Polymerization: Preparation, Porosity, and Gas Uptake journal August 2013
CO2 capture by solid adsorbents and their applications: current status and new trends journal January 2011

Cited By (3)