Details
| Original language | English |
|---|---|
| Article number | 2007734 |
| Number of pages | 6 |
| Journal | Advanced Materials |
| Volume | 33 |
| Issue number | 8 |
| Early online date | 20 Jan 2021 |
| Publication status | Published - 24 Feb 2021 |
Abstract
Improved carbon capture materials are crucial for managing the CO2 level in the atmosphere. The past focus was on increasing adsorption capacities. It is widely known that controlling the heat of adsorption (ΔHads) is equally important. If it is too low, CO2 uptake takes place at unfavorable conditions and with insufficient selectivity. If it is too high, chemisorption occurs, and the materials can hardly be regenerated. The conventional approach for influencing ΔHads is the modification of the adsorbing center. This paper proposes an alternative strategy. The hypothesis is that fine-tuning of the molecular environment around the adsorbing center is a powerful tool for the adjustment of CO2-binding properties. Via click chemistry, any desired neighboring group (NG) can be incorporated on the surfaces of the nanoporous organosilica model materials. Passive NGs induce a change in the polarity of the surface, whereas active NGs are capable of direct interaction with the active center/CO2 pair. The effects on ΔHads and on the selectivity are studied. A situation can be realized which resembles frustrated Lewis acid–base pairs, and the investigation of the binding-species by solid-state NMR indicates that the push–pull effects could play an essential role not only in CO2 adsorption but also in its activation.
Keywords
- carbon capture, carbon dioxide activation, organic–inorganic hybrids, porous materials, surface design
ASJC Scopus subject areas
- Materials Science(all)
- Engineering(all)
- Mechanics of Materials
- Engineering(all)
- Mechanical Engineering
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In: Advanced Materials, Vol. 33, No. 8, 2007734, 24.02.2021.
Research output: Contribution to journal › Short/Brief/Rapid Communication › Research › peer review
}
TY - JOUR
T1 - Great Location
T2 - About Effects of Surface Bound Neighboring Groups for Passive and Active Fine-Tuning of CO2 Adsorption Properties in Model Carbon Capture Materials
AU - Klinkenberg, Nele
AU - Kraft, Sophia
AU - Polarz, Sebastian
N1 - Funding Information: The authors thank the German Research Foundation (DFG PO 780/23-1). The authors thank the PANDOTA scholarship program of the University of Konstanz. The authors thank Magdalena Müller and Enes Ünver for their contribution to material synthesis. The authors thank Ulrich Haunz and the NMR Core Facility for the help with 13C-CP-MAS-NMR spectroscopy. The authors thank Hannah Bronner for conducting additional CO2 measurements in the revision process. Open access funding enabled and organized by Projekt DEAL.
PY - 2021/2/24
Y1 - 2021/2/24
N2 - Improved carbon capture materials are crucial for managing the CO2 level in the atmosphere. The past focus was on increasing adsorption capacities. It is widely known that controlling the heat of adsorption (ΔHads) is equally important. If it is too low, CO2 uptake takes place at unfavorable conditions and with insufficient selectivity. If it is too high, chemisorption occurs, and the materials can hardly be regenerated. The conventional approach for influencing ΔHads is the modification of the adsorbing center. This paper proposes an alternative strategy. The hypothesis is that fine-tuning of the molecular environment around the adsorbing center is a powerful tool for the adjustment of CO2-binding properties. Via click chemistry, any desired neighboring group (NG) can be incorporated on the surfaces of the nanoporous organosilica model materials. Passive NGs induce a change in the polarity of the surface, whereas active NGs are capable of direct interaction with the active center/CO2 pair. The effects on ΔHads and on the selectivity are studied. A situation can be realized which resembles frustrated Lewis acid–base pairs, and the investigation of the binding-species by solid-state NMR indicates that the push–pull effects could play an essential role not only in CO2 adsorption but also in its activation.
AB - Improved carbon capture materials are crucial for managing the CO2 level in the atmosphere. The past focus was on increasing adsorption capacities. It is widely known that controlling the heat of adsorption (ΔHads) is equally important. If it is too low, CO2 uptake takes place at unfavorable conditions and with insufficient selectivity. If it is too high, chemisorption occurs, and the materials can hardly be regenerated. The conventional approach for influencing ΔHads is the modification of the adsorbing center. This paper proposes an alternative strategy. The hypothesis is that fine-tuning of the molecular environment around the adsorbing center is a powerful tool for the adjustment of CO2-binding properties. Via click chemistry, any desired neighboring group (NG) can be incorporated on the surfaces of the nanoporous organosilica model materials. Passive NGs induce a change in the polarity of the surface, whereas active NGs are capable of direct interaction with the active center/CO2 pair. The effects on ΔHads and on the selectivity are studied. A situation can be realized which resembles frustrated Lewis acid–base pairs, and the investigation of the binding-species by solid-state NMR indicates that the push–pull effects could play an essential role not only in CO2 adsorption but also in its activation.
KW - carbon capture
KW - carbon dioxide activation
KW - organic–inorganic hybrids
KW - porous materials
KW - surface design
UR - http://www.scopus.com/inward/record.url?scp=85100085289&partnerID=8YFLogxK
U2 - 10.1002/adma.202007734
DO - 10.1002/adma.202007734
M3 - Short/Brief/Rapid Communication
C2 - 33470469
AN - SCOPUS:85100085289
VL - 33
JO - Advanced Materials
JF - Advanced Materials
SN - 0935-9648
IS - 8
M1 - 2007734
ER -