TY - JOUR

T1 - Versatile surface modification of aerogels by click chemistry as an approach to generate model systems for CO2 adsorption features in amine-containing organosilica

AU - Klinkenberg, Nele

AU - Klaiber, Alexander

AU - Müller, Magdalena

AU - Polarz, Sebastian

N1 - Funding information: We thank the SFB1214 and the IRTG for support. We thank the Electronmicroscopy Center and the Nanolab of the University of Konstanz for providing the measurement facilities. We thank Tobias Lemke for many fruitful scientific discussions and proof-reading of the manuscript. We thank Ilona Wimmer for the conduction of XPS measurements. We thank Julian Steinbrecher for his contribution to material synthesis.

PY - 2019/11/12

Y1 - 2019/11/12

N2 - The conversion of waste into valuable products is most appealing in the case of CO 2, a molecule which is produced in mass by our society and industries. Because its atmospheric concentration correlates to climate change and the green-house effect, major efforts are on the way to reduce the emission of CO 2. One promising strategy is the separation of CO 2 from the gas-phase (e.g. flue gases) by solid-adsorbents containing amine moieties. The synthesis of tailor-made adsorbents with changing surface properties remains a challenge. This work presents a click chemistry approach that enables the easy modification of organosilica materials with functional groups that can be used as model systems to study the influence of surface chemistry on CO 2 adsorption. As an example, the modification of the materials with primary amines is discussed in detail but furthermore the approach offers the possibility to tailor the surface properties using any desired functional group. The increased affinity of the used copper catalyst introduced some difficulties but we were able to remove all remains of copper. With this approach, we were able to synthesize materials with different degrees of functionalization up to 80%. This approach for the development of new carbon capture model systems offers high functionalization combined with the flexibility of a post-functionalization approach. Thus, surface chemistry can be tailored to study the influence of surface chemistry on CO 2 adsorption. As an example for the model character of our materials, we could show that the heat of adsorption can be tuned by systematically varying the degree of amine functionalization.

AB - The conversion of waste into valuable products is most appealing in the case of CO 2, a molecule which is produced in mass by our society and industries. Because its atmospheric concentration correlates to climate change and the green-house effect, major efforts are on the way to reduce the emission of CO 2. One promising strategy is the separation of CO 2 from the gas-phase (e.g. flue gases) by solid-adsorbents containing amine moieties. The synthesis of tailor-made adsorbents with changing surface properties remains a challenge. This work presents a click chemistry approach that enables the easy modification of organosilica materials with functional groups that can be used as model systems to study the influence of surface chemistry on CO 2 adsorption. As an example, the modification of the materials with primary amines is discussed in detail but furthermore the approach offers the possibility to tailor the surface properties using any desired functional group. The increased affinity of the used copper catalyst introduced some difficulties but we were able to remove all remains of copper. With this approach, we were able to synthesize materials with different degrees of functionalization up to 80%. This approach for the development of new carbon capture model systems offers high functionalization combined with the flexibility of a post-functionalization approach. Thus, surface chemistry can be tailored to study the influence of surface chemistry on CO 2 adsorption. As an example for the model character of our materials, we could show that the heat of adsorption can be tuned by systematically varying the degree of amine functionalization.

KW - Aerogels

KW - Amine-functionalized materials

KW - CO adsorption

KW - Carbon capture model systems

KW - Click chemistry

KW - Functional gradients

KW - Organosilica

UR - http://www.scopus.com/inward/record.url?scp=85076553937&partnerID=8YFLogxK

U2 - 10.1016/j.micromeso.2019.109879

DO - 10.1016/j.micromeso.2019.109879

M3 - Article

VL - 294

JO - Microporous and Mesoporous Materials

JF - Microporous and Mesoporous Materials

SN - 1387-1811

M1 - 109879

ER -