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Title: Design of Calix-Based Cages for CO2 Capture

Abstract

Cage compounds offer a unique opportunity to capture CO2, but a perfect design has been elusive. Herein, we computationally designed cage compounds by using linkers to connect two calix[4]pyrrole units together into a cage for capturing CO2. Quantum mechanical calculations based on dispersion-corrected density functional theory show that the -(CH2)n– linker has an optimal length at n = 5 where the N–H groups from the pyrrole molecules form four H···O interactions with the two terminal O atoms of CO2. The cationic and zwitterionic cages can also achieve high CO2 affinity and CO2/N2 selectivity in the cage cavity compared with previously synthesized cages. Based on the computed potential energy curves of gas entering the cage, we conclude that all the cages are easily accessible by CO2. This work shows that the calix-based cages have great potential for selective CO2 capture.

Authors:
 [1];  [2];  [2];  [3];  [3]; ORCiD logo [4]; ORCiD logo [2]
  1. Univ. of California, Riverside, CA (United States); East China Normal Univ. (ECNU), Shanghai (China)
  2. Univ. of California, Riverside, CA (United States)
  3. East China Normal Univ. (ECNU), Shanghai (China)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1480086
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 56; Journal Issue: 15; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; gas separation; CO2 capture; calix-based cages; binding energy; dispersioncorrected DFT

Citation Formats

Wu, Weihong, Tian, Ziqi, Wang, Song, Peng, Changjun, Liu, Honglai, Dai, Sheng, and Jiang, De-en. Design of Calix-Based Cages for CO2 Capture. United States: N. p., 2017. Web. doi:10.1021/acs.iecr.7b00189.
Wu, Weihong, Tian, Ziqi, Wang, Song, Peng, Changjun, Liu, Honglai, Dai, Sheng, & Jiang, De-en. Design of Calix-Based Cages for CO2 Capture. United States. https://doi.org/10.1021/acs.iecr.7b00189
Wu, Weihong, Tian, Ziqi, Wang, Song, Peng, Changjun, Liu, Honglai, Dai, Sheng, and Jiang, De-en. Tue . "Design of Calix-Based Cages for CO2 Capture". United States. https://doi.org/10.1021/acs.iecr.7b00189. https://www.osti.gov/servlets/purl/1480086.
@article{osti_1480086,
title = {Design of Calix-Based Cages for CO2 Capture},
author = {Wu, Weihong and Tian, Ziqi and Wang, Song and Peng, Changjun and Liu, Honglai and Dai, Sheng and Jiang, De-en},
abstractNote = {Cage compounds offer a unique opportunity to capture CO2, but a perfect design has been elusive. Herein, we computationally designed cage compounds by using linkers to connect two calix[4]pyrrole units together into a cage for capturing CO2. Quantum mechanical calculations based on dispersion-corrected density functional theory show that the -(CH2)n– linker has an optimal length at n = 5 where the N–H groups from the pyrrole molecules form four H···O interactions with the two terminal O atoms of CO2. The cationic and zwitterionic cages can also achieve high CO2 affinity and CO2/N2 selectivity in the cage cavity compared with previously synthesized cages. Based on the computed potential energy curves of gas entering the cage, we conclude that all the cages are easily accessible by CO2. This work shows that the calix-based cages have great potential for selective CO2 capture.},
doi = {10.1021/acs.iecr.7b00189},
journal = {Industrial and Engineering Chemistry Research},
number = 15,
volume = 56,
place = {United States},
year = {Tue Mar 28 00:00:00 EDT 2017},
month = {Tue Mar 28 00:00:00 EDT 2017}
}

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