Role of Amine Structure on Carbon Dioxide Adsorption from Ultradilute Gas Streams such as Ambient Air

ChemSusChem ◽  
2012 ◽  
Vol 5 (10) ◽  
pp. 2058-2064 ◽  
Author(s):  
Stephanie A. Didas ◽  
Ambarish R. Kulkarni ◽  
David S. Sholl ◽  
Christopher W. Jones
2018 ◽  
Vol 32 (6) ◽  
pp. 6926-6933 ◽  
Author(s):  
Claudia N. Okonkwo ◽  
Chukwuemeka Okolie ◽  
Achintya Sujan ◽  
Guanghui Zhu ◽  
Christopher W. Jones

2021 ◽  
Author(s):  
Athanasios Koutsianos ◽  
Louise B. Hamdy ◽  
Chun-Jae Yoo ◽  
Jason J. Lee ◽  
Marco Taddei ◽  
...  

Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, especially at ambient temperature. High polymer contents curtail diffusion pathways, hindering CO2 from reaching and reacting with the numerous amine functions. Here, we overcome this issue using poly(allylamine) (PAA) grafted with short fluoroalkyl chains and then cross-linked with C60. As experimentally evidenced by positron annihilation lifetime spectroscopy, the incorporation of fluoroalkyl chains generates free volume elements that act as additional diffusion pathways within the material. The inclusion of void volume in fluoroalkyl-functionalized PAA sorbents results in radically increased CO2 uptakes and amine efficiencies in diluted gas streams at room temperature, including simulated air. We speculate that the hydrophobic fluorinated functions interfere with the strong amine hydrogen bonding network disrupting and consequently altering the packing and conformation of the polymer chains. The evidence presented here is a blueprint for the development of more efficient amine-based CO2 sorbents


2021 ◽  
Author(s):  
Athanasios Koutsianos ◽  
Louise B. Hamdy ◽  
Chun-Jae Yoo ◽  
Jason J. Lee ◽  
Marco Taddei ◽  
...  

Polyamine-based carbon dioxide sorbents suffer from a seesaw relationship between amine content and amine efficiency. High polyamine loadings equate to increased amine contents, but often at the expense of amine efficiency. Carbon dioxide mass transport in compact polymers is severely limited, especially at ambient temperature. High polymer contents curtail diffusion pathways, hindering CO2 from reaching and reacting with the numerous amine functions. Here, we overcome this issue using poly(allylamine) (PAA) grafted with short fluoroalkyl chains and then cross-linked with C60. As experimentally evidenced by positron annihilation lifetime spectroscopy, the incorporation of fluoroalkyl chains generates free volume elements that act as additional diffusion pathways within the material. The inclusion of void volume in fluoroalkyl-functionalized PAA sorbents results in radically increased CO2 uptakes and amine efficiencies in diluted gas streams at room temperature, including simulated air. We speculate that the hydrophobic fluorinated functions interfere with the strong amine hydrogen bonding network disrupting and consequently altering the packing and conformation of the polymer chains. The evidence presented here is a blueprint for the development of more efficient amine-based CO2 sorbents


2018 ◽  
Author(s):  
Jaya Prakash Madda ◽  
Pilli Govindaiah ◽  
Sushant Kumar Jena ◽  
Sabbhavat Krishna ◽  
Rupak Kishor

<p>Covalent organic Imine polymers with intrinsic meso-porosity were synthesized by condensation reaction between 4,4-diamino diphenyl methane and (para/meta/ortho)-phthaladehyde. Even though these polymers were synthesized from precursors of bis-bis covalent link mode, the bulk materials were micrometer size particles with intrinsic mesoporous enables nitrogen as well as carbon dioxide adsorption in the void spaces. These polymers were showed stability up to 260<sup>o</sup> centigrade. Nitrogen gas adsorption capacity up to 250 cc/g in the ambient pressure was observed with type III adsorption characteristic nature. Carbon dioxide adsorption experiments reveal the possible terminal amine functional group to carbamate with CO<sub>2</sub> gas molecule to the polymers. One of the imine polymers, COP-3 showed more carbon dioxide sorption capacity and isosteric heat of adsorption (Q<sub>st</sub>) than COP-1 and COP-2 at 273 K even though COP-3 had lower porosity for nitrogen gas than COP-1 and COP-2. We explained the trends in gas adsorption capacities and Qst values as a consequence of the intra molecular interactions confirmed by Density Functional Theory computational experiments on small molecular fragments.</p>


Author(s):  
A Pertiwiningrum ◽  
R N Besari ◽  
M A Wuri ◽  
A W Harto ◽  
N A Fitriyanto ◽  
...  

Sign in / Sign up

Export Citation Format

Share Document