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Title: Amidine-Functionalized Poly(2-vinyl-4,4-dimethylazlactone) for Selective and Efficient CO2 Fixing

Development of novel polymeric materials capable of efficient CO2 capture and separation under ambient conditions is crucial for cost-effective and practical industrial applications. Here we report the facile synthesis of a new CO2-responsive polymer through post-polymerization modification of poly(2 vinyl-4,4-dimethylazlactone) (PVDMA). The reactive pendant azlactone groups of PVDMA are easily modified with 4-(N-methyltetrahydropyrimidine) benzyl alcohol (PBA) without any by-product formation. FTIR and TGA experiments show the new PBA functionalized polymer powder can reversibly capture CO2 at room temperature and under atmospheric pressure. CO2 capture was selective, showing a high fixing efficiency even with a mixed gas system (20% CO2, 80% N2) similar to flue gas. CO2 release occurred at room temperature and release profiles were investigated as a function of temperature. Density Functional Theory (DFT) calculations coupled with modeling and simulation reveal the presence of two CO2 binding sites in the PBA functionalized polymer resulting in a two-step CO2 release at room temperature. Finally, we find that the ease of material preparation, high fixing efficiency, and robust release characteristics suggest that post-polymerization modification may be a useful route to designing new materials for CO2 capture.
 [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [1] ;  [1] ;  [1] ;  [1] ;  [4] ;  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  3. Comenius Univ., Bratislava (Slovakia). Dept. of Nuclear Physics and Biophysics
  4. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Publication Date:
OSTI Identifier:
Grant/Contract Number:
AC05-00OR22725; 1133320
Accepted Manuscript
Journal Name:
Additional Journal Information:
Journal Volume: 49; Journal Issue: 5; Journal ID: ISSN 0024-9297
American Chemical Society
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 Capture; Polymer; Solid-state; First Principle; Binding Energy; Kinetic Rate Laws