Comparative Study of Molecular Basket Sorbents Consisting of Polyallylamine and Polyethylenimine Functionalized SBA-15 for CO2 Capture from Flue Gas

Dongxiang Wang, Xiaoxing Wang, Chunshan Song

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

Polyallylamine (PAA)-based molecular basket sorbents (MBS) have been studied for CO2 capture in comparison with polyethylenimine (PEI)-based MBS. The characterizations including N2 physisorption, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermogravimetric analysis (TGA) showed that PAA (Mn=15 000) is more rigid and has more steric hindrance inside SBA-15 pores than PEI owing mainly to its different polymer structure. The effects of temperature and PAA loading on the CO2 sorption capacity of PAA-based MBS have been examined by TGA by using 100 % CO2 gas stream and compared with PEI/SBA-15. It was found that the capacity of the PAA/SBA-15 sorbent increased with increasing temperature. The optimum capacity of 88 mgCO2 gsorb −1 was obtained at 140 °C for PAA(50)/SBA-15 whereas the optimum sorption temperature was 75 and 90 °C for PEI-I(50)/SBA-15 (PEI-I, Mn=423) and PEI-II(50)/SBA-15 (PEI-II, Mn=25 000), respectively. The capacity initially increased with the increase of PAA loading and then dropped at high amine contents, owing to the increased diffusion barrier. The highest CO2 capacity of 109 mgCO2 gsorb −1 was obtained at a PAA loading of 65 wt %, whereas the PAA(50)/SBA-15 sorbent gave the best amine efficiency of 0.23 molCO2 molN −1. The effect of moisture was examined in a fixed-bed flow system with simulated flue gas containing 15 % CO2 and 4.5 % O2 in N2. It was found that the presence of moisture significantly enhanced CO2 sorption over PAA(50)/SBA-15 and greatly improved its cyclic stability and regenerability. Compared with PEI/SBA-15, PAA/SBA-15 possesses a better thermal stability and higher resistance to oxidative degradation. However, the CO2 sorption rate over the PAA(50)/SBA-15 sorbent was much slower.

Original languageEnglish (US)
Pages (from-to)3163-3173
Number of pages11
JournalChemPhysChem
Volume18
Issue number22
DOIs
StatePublished - Nov 17 2017

Fingerprint

baskets
Polyethyleneimine
flue gases
sorbents
Sorbents
Flue gases
sorption
moisture
Sorption
amines
gas streams
high resistance
Amines
temperature
Thermogravimetric analysis
SBA-15
polyallylamine
beds
thermal stability
Moisture

All Science Journal Classification (ASJC) codes

  • Atomic and Molecular Physics, and Optics
  • Physical and Theoretical Chemistry

Cite this

@article{fcf13ee5cefd4f4aa6b8f5c4e323fa5f,
title = "Comparative Study of Molecular Basket Sorbents Consisting of Polyallylamine and Polyethylenimine Functionalized SBA-15 for CO2 Capture from Flue Gas",
abstract = "Polyallylamine (PAA)-based molecular basket sorbents (MBS) have been studied for CO2 capture in comparison with polyethylenimine (PEI)-based MBS. The characterizations including N2 physisorption, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermogravimetric analysis (TGA) showed that PAA (Mn=15 000) is more rigid and has more steric hindrance inside SBA-15 pores than PEI owing mainly to its different polymer structure. The effects of temperature and PAA loading on the CO2 sorption capacity of PAA-based MBS have been examined by TGA by using 100 {\%} CO2 gas stream and compared with PEI/SBA-15. It was found that the capacity of the PAA/SBA-15 sorbent increased with increasing temperature. The optimum capacity of 88 mgCO2 gsorb −1 was obtained at 140 °C for PAA(50)/SBA-15 whereas the optimum sorption temperature was 75 and 90 °C for PEI-I(50)/SBA-15 (PEI-I, Mn=423) and PEI-II(50)/SBA-15 (PEI-II, Mn=25 000), respectively. The capacity initially increased with the increase of PAA loading and then dropped at high amine contents, owing to the increased diffusion barrier. The highest CO2 capacity of 109 mgCO2 gsorb −1 was obtained at a PAA loading of 65 wt {\%}, whereas the PAA(50)/SBA-15 sorbent gave the best amine efficiency of 0.23 molCO2 molN −1. The effect of moisture was examined in a fixed-bed flow system with simulated flue gas containing 15 {\%} CO2 and 4.5 {\%} O2 in N2. It was found that the presence of moisture significantly enhanced CO2 sorption over PAA(50)/SBA-15 and greatly improved its cyclic stability and regenerability. Compared with PEI/SBA-15, PAA/SBA-15 possesses a better thermal stability and higher resistance to oxidative degradation. However, the CO2 sorption rate over the PAA(50)/SBA-15 sorbent was much slower.",
author = "Dongxiang Wang and Xiaoxing Wang and Chunshan Song",
year = "2017",
month = "11",
day = "17",
doi = "10.1002/cphc.201700828",
language = "English (US)",
volume = "18",
pages = "3163--3173",
journal = "ChemPhysChem",
issn = "1439-4235",
publisher = "Wiley-VCH Verlag",
number = "22",

}

TY - JOUR

T1 - Comparative Study of Molecular Basket Sorbents Consisting of Polyallylamine and Polyethylenimine Functionalized SBA-15 for CO2 Capture from Flue Gas

AU - Wang, Dongxiang

AU - Wang, Xiaoxing

AU - Song, Chunshan

PY - 2017/11/17

Y1 - 2017/11/17

N2 - Polyallylamine (PAA)-based molecular basket sorbents (MBS) have been studied for CO2 capture in comparison with polyethylenimine (PEI)-based MBS. The characterizations including N2 physisorption, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermogravimetric analysis (TGA) showed that PAA (Mn=15 000) is more rigid and has more steric hindrance inside SBA-15 pores than PEI owing mainly to its different polymer structure. The effects of temperature and PAA loading on the CO2 sorption capacity of PAA-based MBS have been examined by TGA by using 100 % CO2 gas stream and compared with PEI/SBA-15. It was found that the capacity of the PAA/SBA-15 sorbent increased with increasing temperature. The optimum capacity of 88 mgCO2 gsorb −1 was obtained at 140 °C for PAA(50)/SBA-15 whereas the optimum sorption temperature was 75 and 90 °C for PEI-I(50)/SBA-15 (PEI-I, Mn=423) and PEI-II(50)/SBA-15 (PEI-II, Mn=25 000), respectively. The capacity initially increased with the increase of PAA loading and then dropped at high amine contents, owing to the increased diffusion barrier. The highest CO2 capacity of 109 mgCO2 gsorb −1 was obtained at a PAA loading of 65 wt %, whereas the PAA(50)/SBA-15 sorbent gave the best amine efficiency of 0.23 molCO2 molN −1. The effect of moisture was examined in a fixed-bed flow system with simulated flue gas containing 15 % CO2 and 4.5 % O2 in N2. It was found that the presence of moisture significantly enhanced CO2 sorption over PAA(50)/SBA-15 and greatly improved its cyclic stability and regenerability. Compared with PEI/SBA-15, PAA/SBA-15 possesses a better thermal stability and higher resistance to oxidative degradation. However, the CO2 sorption rate over the PAA(50)/SBA-15 sorbent was much slower.

AB - Polyallylamine (PAA)-based molecular basket sorbents (MBS) have been studied for CO2 capture in comparison with polyethylenimine (PEI)-based MBS. The characterizations including N2 physisorption, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and thermogravimetric analysis (TGA) showed that PAA (Mn=15 000) is more rigid and has more steric hindrance inside SBA-15 pores than PEI owing mainly to its different polymer structure. The effects of temperature and PAA loading on the CO2 sorption capacity of PAA-based MBS have been examined by TGA by using 100 % CO2 gas stream and compared with PEI/SBA-15. It was found that the capacity of the PAA/SBA-15 sorbent increased with increasing temperature. The optimum capacity of 88 mgCO2 gsorb −1 was obtained at 140 °C for PAA(50)/SBA-15 whereas the optimum sorption temperature was 75 and 90 °C for PEI-I(50)/SBA-15 (PEI-I, Mn=423) and PEI-II(50)/SBA-15 (PEI-II, Mn=25 000), respectively. The capacity initially increased with the increase of PAA loading and then dropped at high amine contents, owing to the increased diffusion barrier. The highest CO2 capacity of 109 mgCO2 gsorb −1 was obtained at a PAA loading of 65 wt %, whereas the PAA(50)/SBA-15 sorbent gave the best amine efficiency of 0.23 molCO2 molN −1. The effect of moisture was examined in a fixed-bed flow system with simulated flue gas containing 15 % CO2 and 4.5 % O2 in N2. It was found that the presence of moisture significantly enhanced CO2 sorption over PAA(50)/SBA-15 and greatly improved its cyclic stability and regenerability. Compared with PEI/SBA-15, PAA/SBA-15 possesses a better thermal stability and higher resistance to oxidative degradation. However, the CO2 sorption rate over the PAA(50)/SBA-15 sorbent was much slower.

UR - http://www.scopus.com/inward/record.url?scp=85031670730&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85031670730&partnerID=8YFLogxK

U2 - 10.1002/cphc.201700828

DO - 10.1002/cphc.201700828

M3 - Article

C2 - 28940634

AN - SCOPUS:85031670730

VL - 18

SP - 3163

EP - 3173

JO - ChemPhysChem

JF - ChemPhysChem

SN - 1439-4235

IS - 22

ER -