Details
| Original language | English |
|---|---|
| Pages (from-to) | 11332-11343 |
| Number of pages | 12 |
| Journal | Journal of Materials Chemistry A |
| Volume | 12 |
| Issue number | 19 |
| Early online date | 4 Apr 2024 |
| Publication status | Published - 21 May 2024 |
Abstract
Functional gradient materials can process more complex tasks than a mixture of their homogeneous analogs. Generating such materials is difficult as it necessitates spatial control over chemical and/or structural properties. A gradient is a unique degree of freedom in hierarchical material architectures, and as such, biology has managed exploiting the full potential of graded structures. For instance, despite being present at a comparably low concentration (approaching 420 ppm in 2023), plants are capable of capturing carbon dioxide from the air. Binding occurs in the carboxysome, a complex entity characterized by pores with engineered surfaces composed of shell proteins that create a concentration gradient of CO2 towards an enzyme responsible for the first conversion step. The current paper hypothesizes that porous organosilica materials can mimic some of the features of the mentioned biological paragon. Primary amines as sites for interacting with CO2 are surrounded by spectator groups on bifunctional surfaces. It is found that the proper choice of the spectator group almost doubles the adsorption enthalpy. Above a critical density, the hydrophobic moieties create a quasi-solvent layer on the surfaces in which CO2 molecules dissolve. When the density of the spectator groups gradually changes inside a graded organosilica monolith, one obtains zones varying systematically in adsorption enthalpy. Directionality in affinity towards CO2 and controlled transport properties are realized.
ASJC Scopus subject areas
Sustainable Development Goals
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In: Journal of Materials Chemistry A, Vol. 12, No. 19, 21.05.2024, p. 11332-11343.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Spatial tuning of adsorption enthalpies by exploiting spectator group effects in organosilica carbon capture materials
AU - Evers, Mario
AU - Hauser, Karin
AU - Hinze, Wolfgang G.
AU - Klinkenberg, Nele
AU - Krysiak, Yasar
AU - Mombers, Daniel
AU - Polarz, Sebastian
N1 - Publisher Copyright: © 2024 The Royal Society of Chemistry.
PY - 2024/5/21
Y1 - 2024/5/21
N2 - Functional gradient materials can process more complex tasks than a mixture of their homogeneous analogs. Generating such materials is difficult as it necessitates spatial control over chemical and/or structural properties. A gradient is a unique degree of freedom in hierarchical material architectures, and as such, biology has managed exploiting the full potential of graded structures. For instance, despite being present at a comparably low concentration (approaching 420 ppm in 2023), plants are capable of capturing carbon dioxide from the air. Binding occurs in the carboxysome, a complex entity characterized by pores with engineered surfaces composed of shell proteins that create a concentration gradient of CO2 towards an enzyme responsible for the first conversion step. The current paper hypothesizes that porous organosilica materials can mimic some of the features of the mentioned biological paragon. Primary amines as sites for interacting with CO2 are surrounded by spectator groups on bifunctional surfaces. It is found that the proper choice of the spectator group almost doubles the adsorption enthalpy. Above a critical density, the hydrophobic moieties create a quasi-solvent layer on the surfaces in which CO2 molecules dissolve. When the density of the spectator groups gradually changes inside a graded organosilica monolith, one obtains zones varying systematically in adsorption enthalpy. Directionality in affinity towards CO2 and controlled transport properties are realized.
AB - Functional gradient materials can process more complex tasks than a mixture of their homogeneous analogs. Generating such materials is difficult as it necessitates spatial control over chemical and/or structural properties. A gradient is a unique degree of freedom in hierarchical material architectures, and as such, biology has managed exploiting the full potential of graded structures. For instance, despite being present at a comparably low concentration (approaching 420 ppm in 2023), plants are capable of capturing carbon dioxide from the air. Binding occurs in the carboxysome, a complex entity characterized by pores with engineered surfaces composed of shell proteins that create a concentration gradient of CO2 towards an enzyme responsible for the first conversion step. The current paper hypothesizes that porous organosilica materials can mimic some of the features of the mentioned biological paragon. Primary amines as sites for interacting with CO2 are surrounded by spectator groups on bifunctional surfaces. It is found that the proper choice of the spectator group almost doubles the adsorption enthalpy. Above a critical density, the hydrophobic moieties create a quasi-solvent layer on the surfaces in which CO2 molecules dissolve. When the density of the spectator groups gradually changes inside a graded organosilica monolith, one obtains zones varying systematically in adsorption enthalpy. Directionality in affinity towards CO2 and controlled transport properties are realized.
UR - http://www.scopus.com/inward/record.url?scp=85190729208&partnerID=8YFLogxK
U2 - 10.1039/d4ta01381f
DO - 10.1039/d4ta01381f
M3 - Article
AN - SCOPUS:85190729208
VL - 12
SP - 11332
EP - 11343
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 19
ER -