Towards a novel approach to capture CO2 in hierarchically organized chemically functionalized materials
Final Report Abstract
Over the course of the project the synthesis of hierarchically porous spheres was improved by tailoring the components of the precursor solution and the synthesis parameters. Especially varying the interior structure by employing a slurry based synthesis had a major impact on the resulting materials. Describing the surface chemistry of the amine species as function of their functionality and loading, as well as the absence and presence of H2O, improved the understanding of the parameters critical for the development of CO2 sorbents based on solid supported amines. The dynamics of CO2 adsorption from flue gases were found to be mostly affected by amine loading. While the hierarchically porous spheres showed a distinct reduction of CO2 adsorption capacities, capping of silanol groups showed that structural effects can be remedied by surface functionalization. For high pressure CO2 sorption the macro- and mesoporous spheres showed lower heats of adsorption and performed better than zeolite 13X in conditions typical for pressure or temperature swing adsorption. However, elimination of small mesopores is necessary to match or even surpass the performance of SBA-15 under the investigated conditions. The reactive regeneration of amine functionalized CO2 adsorbents was demonstrated to be highly feasible, as the hydrogenation of CO2 to products such as methanol is viable at low pressures and temperatures using carbamates as intermediates to activate the CO2. The outcome of the project significantly improved the understanding essential for the further rational development of a new generation of solid amine functionalized hierarchically porous sorbents for CO2 removal from dilutes gas streams. A novel concept for the regeneration, the conversion of surface bound CO2 with H2 was introduced and its feasibility was demonstrated in preliminary experiments.
Publications
- A Mechanistic study of amine impregnated sorbents for post-combustion applications, 26th Deutsche Zeolithtagung, 2014, Paderborn, Germany
M.W. Hahn, M. Steib, A. Jentys, J.A. Lercher
- J Mater Chem A, 2014, 2, 13624-13634
M. W. Hahn, M. Steib, A. Jentys, J. A. Lercher
(See online at https://doi.org/10.1039/c4ta02145b) - Mechanism and interactions of amines impregnated on SBA-15 during CO2 separation, 47th Jahrestreffen deutscher Katalytiker, 2014, Weimar, Germany
M.W. Hahn, M. Steib, A. Jentys, J.A. Lercher
- One-step synthesized mesoscale organized silica spheres for CO2 adsorption, COPS-X, 2014, Granada, Spain
M.W. Hahn, E. Ball, M. Steib, A. Jentys, J.A. Lercher
- Impact of water on CO2 adsorption of amino-functionalized hierarchical silica spheres, MSE Kolloquium, 2015, Garching
E. Berger, A. Jentys, J.A. Lercher
- J Phys Chem C, 2015, 119 (8), 4126-4135
M. W. Hahn, M. Steib, A. Jentys, J. A. Lercher
(See online at https://doi.org/10.1021/jp512001t) - Novel Solid Sorbents for CO2 Capture and Evaluation to Applied Systems, Technische Universität München, 2015
M. W. Hahn
- The role of amine functionality to the CO2 capture mechanism of anhydrous solid sorbents, 48th Jahrestreffen Deutscher Katalytiker, 2015, Weimar, Germany
M.W. Hahn, J. Jelic, E. Ball, K. Reuter, A. Jentys, J.A. Lercher
- Functional and structural influences on CO2 adsorption capacities of silica-based sorbents in the presence of H2O, 28th Deutsche Zeolithtagung, 2016, Gießen
E. Berger, A. Jentys, J.A. Lercher
- J Phys Chem B, 2016, 120 (8), 1988-1995
M.W. Hahn, J. Jelic, E. Berger, K. Reuter, A. Jentys, J. A. Lercher
(See online at https://doi.org/10.1021/acs.jpcb.5b10012) - Journal of Energy Chemistry, 2016, 25 (2), 327-335
E. Berger, M. W. Hahn, T. Przybilla, B. Winter, E. Spiecker, A. Jentys, J. A. Lercher
(See online at https://doi.org/10.1016/j.jechem.2016.02.005) - Influence of amine type and presence of H2O on adsorbed species during CO2 adsorption on silica-based materials, 29th Deutsche Zeolithtagung, 2017, Frankfurt
E. Berger, A. Jentys, J.A. Lercher
- Effects of additional hydrophobic functionalization of silicabased amino-functionalized sorbents, 30th Deutsche Zeolithtagung, 2018, Kiel
E. Berger, A. Jentys, J.A. Lercher
