CO2 capture and conversion; polymeric membranes; porous organic polymers; Metal organic frameworks; heterogeneous catalysis
Ashirov Timur, Song Kyung Seob, Coskun Ali (2022), Salt-Templated Solvothermal Synthesis of Dioxane-Linked Three-Dimensional Nanoporous Organic Polymers for Carbon Dioxide and Iodine Capture, in
ACS Applied Nano Materials, 10.1021/ac.
Ashirov Timur, Yazaydin A. Ozgur, Coskun Ali (2022), Tuning the Transport Properties of Gases in Porous Graphene Membranes with Controlled Pore Size and Thickness, in
Advanced Materials, 2106785-2106785.
Ashirov Timur, Coskun Ali (2021), Ultrahigh permeance metal coated porous graphene membranes with tunable gas selectivities, in
Chem, 7(9), 2385-2394.
Kalkus Trevor J., Guha Anirvan, Scholten Philip B.V., Nagornii Dmitrii, Coskun Ali, Ianiro Alessandro, Mayer Michael (2021), The Green Lean Amine Machine: Harvesting Electric Power While Capturing Carbon Dioxide from Breath, in
Advanced Science, 8(15), 2100995-2100995.
Ashirov Timur, Alrayyani Maymounah, Song Kyung Seob, Miljanic Ognjen, Coskun Ali (2021), Cyclotetrabenzil-Based Porous Organic Polymers with High Carbon Dioxide Affinity, in
Organic Materials, 346.
Song Kyung Seob, Talapaneni Siddulu Naidu, Ashirov Timur, Coskun Ali (2021), Molten Salt Templated Synthesis of Covalent Isocyanurate Frameworks with Tunable Morphology and High CO2 Uptake Capacity, in
ACS Applied Materials and Interfaces, 13(22), 26102-26108.
Huang Hsin-Hua, Song Kyung Seob, Prescimone Alessandro, Aster Alexander, Cohen Gabriel, Mannancherry Rajesh, Vauthey Eric, Coskun Ali, Šolomek Tomáš (2021), Porous shape-persistent rylene imine cages with tunable optoelectronic properties and delayed fluorescence, in
Chemical Science, 5275.
Fritz Patrick W., Coskun Ali (2021), The Prospect of Dimensionality in Porous Semiconductors, in
Chemistry A European Journal, 7489.
Coskun Ali (2020), Tailor-made Functional Polymers for Energy Storage and Environmental Applications, in
CHIMIA, 74(9), 667-667.
Byun Yearin, Xie Lilia S., Fritz Patrick, Ashirov Timur, Dinca Mircea, Coskun Ali (2020), A Three‐Dimensional Porous Organic Semiconductor Based on Fully sp 2 ‐Hybridized Graphitic Polymer, in
Angewandte Chemie International Edition, 59(35), 15166-15170.
Song Kyung Seob, Kim Daeok, Coskun Ali (2020), Hierarchically Porous Reduced Graphene Oxide Coated with Metal–Organic Framework HKUST-1 for Enhanced Hydrogen Gas Affinity, in
ACS Applied Nano Materials, 3(2), 985-991.
Kaiser Selina K., Song Kyung Seob, Mitchell Sharon, Coskun Ali, Pérez-Ramírez Javier (2020), Nitrogen‐Doped Carbons with Hierarchical Porosity via Chemical Blowing Towards Long‐Lived Metal‐Free Catalysts for Acetylene Hydrochlorination, in
ChemCatChem, 1922.
Kim Daeok, Song Kyung Seob, Buyukcakir Onur, Yildirim Taner, Coskun Ali (2018), Bimetallic metal organic frameworks with precisely positioned metal centers for efficient H2 storage, in
Chemical Communications, 54, 12218.
Carbon dioxide emissions into the atmosphere accounts for the majority of environmental challenges and its global impact in the form of climate change, ocean acidification is well-documented. In this direction, absorption with amine solutions, adsorption with porous solids and cryogenic separation methods have been investigated conventionally, however, they possess major drawbacks such as high-energy penalty, environmental issues and complex operation procedures. Because of their fundamental engineering and economic advantages over competing separation technologies, membrane operations are now being explored for CO2 capture from power plants. However, the low CO2 selectivity of membrane systems is a major challenge yet to be tackled. Metal-organic frameworks (MOFs) and porous organic polymers (POPs) are emerging solid-sorbents for CO2 capture and their pore characteristics can be easily tailored by the combinational choice of building blocks. Accordingly, the incorporation of MOFs and POPs as fillers into the polymeric membranes could lead to the development of highly selective membrane systems with high gas selectivity over Knudsen diffusion. One of the great challenges for these membrane systems is, however, to realize simultaneous capture and conversion to not only use CO2 as a sustainable C1 building block, but also create an incentive for the further development of costly capture technologies. The research on these so-called “membrane reactors”, however, have been mostly limited to inorganic membranes, which are rather costly. Our main motivation in this proposal is to develop new catalytically active metal impregnated MOFs, MOF-derived core-shell porous carbons and metal impregnated POPs for the conversion of CO2 into value added products such as methanol from various emission sources at relatively low CO2 partial pressures and temperatures, which is highly important in the context of steam economy. The benchmark catalyst for the direct hydrogenation of CO2 is the Cu/ZnO/Al2O3 system. This catalyst operates at high pressures and temperatures through a widely accepted bifunctional mechanism, that is the hydrogen spillover on Cu nanoparticles and CO2 activation on ZnO to form CH3OH. However, the sintering of Cu nanoparticles and high pressures of CO2 and H2 were found to rapidly decrease the activity of the catalyst. We propose that highly CO2-philic porous materials in the form of MOFs and POPs can pre-concentrate CO2 even at very low pressures. The functionalization of pores with carbenes and amines, which can act as anchors for the chemical activation of the CO2 along with the presence of metal nanoparticles (MNPs) such as Cu, Pd for hydrogen spillover could transform these porous sorbents into efficient heterogeneous catalysts for the conversion of CO2 into MeOH. Importantly, by tuning (1) textural properties, (2) CO2-philicity and (3) catalyst loading of these porous sorbents, we will be able to obtain valuable fundamental insights for the conversion mechanism. Subsequent incorporation of these heterogeneous catalysts as fillers into the polymeric membranes will enable the realization of catalytic composite membranes for the continuous capture and conversion of CO2 at low temperature and pressures. More significantly, the ability of membranes to remove products from equilibrium reactions will further contribute the catalytic performance of these systems. Successful realization of this project will not only create economical value to the captured CO2, thus decreasing the cost of capture process, but it will also help to curb ever-increasing CO2 emissions.