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:
-
- Univ. of California, Riverside, CA (United States); East China Normal Univ. (ECNU), Shanghai (China)
- Univ. of California, Riverside, CA (United States)
- East China Normal Univ. (ECNU), Shanghai (China)
- 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}
}
Web of Science
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