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Thirion, D.,Rozyyev, V.,Park, J.,Byun, J.,Jung, Y.,Atilhan, M.,Yavuz, C. T. The Royal Society of Chemistry 2016 Physical chemistry chemical physics Vol.18 No.21
<P>Liquid, solvated amine based carbon capture is the core of all commercial or planned CO2 capture operations. Despite the intense research, few have looked systematically into the nature of amine molecules and their CO2 interaction. Here, we report a systematic introduction of linear ethylene amines on the walls of highly porous Davankov type network structures through simple bromination intermediates. Surprisingly, isosteric heats of CO2 adsorption show a clear linear trend with the increase in the length of the tethered amine pendant groups, leading to a concerted cooperative binding with additional H-bonding contributions from the unassociated secondary amines. CO2 uptake capacities multiply with the nitrogen content, up to an unprecedented four to eight times of the starting porous network under flue gas conditions. The reported procedure can be generalized to all porous media with the robust hydrocarbon framework in order to convert them into effective CO2 capture adsorbents.</P>
Thirion, Damien,Kwon, Yonghyun,Rozyyev, Vepa,Byun, Jeehye,Yavuz, Cafer T. American Chemical Society 2016 Chemistry of materials Vol.28 No.16
<P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/cmatex/2016/cmatex.2016.28.issue-16/acs.chemmater.6b02152/production/images/medium/cm-2016-02152g_0006.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/cm6b02152'>ACS Electronic Supporting Info</A></P>
Song, Youngdong,Thirion, Damien,Subramanian, Saravanan,Lah, Myoung Soo,Yavuz, Cafer T. Elsevier 2017 Microporous and mesoporous materials Vol.243 No.-
<P><B>Abstract</B></P> <P>Carbon dioxide capture requires stable porous solids like zirconium based metal-organic frameworks (MOFs) in order to make sequestration efforts feasible. Because of the weak binding at low CO<SUB>2</SUB> partial pressures, oligomeric amines are commonly loaded on porous supports to maximize CO<SUB>2</SUB> capture while attempting to keep porosity for enhanced diffusion. Here we show the first temperature resolved stability study of linear-amine impregnated UiO-66 by in-situ monitoring of the PXRD pattern. Our findings show that the crystal structure shows a contraction at temperatures as low as 80 °C and deforms considerably above 120 °C, leading to significant doubts about their applicability in CO<SUB>2</SUB> capture from lean feeds. We confirm that all MOFs need to be thoroughly analyzed at least by means of PXRD at the process relevant temperatures, and reinforced before any plausible plans of application in CO<SUB>2</SUB> capture.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Temperature resolved in situ PXRD technique is a reliable technique in identifying feasibility of porous crystals in gas (e.g. CO<SUB>2</SUB>) capture. </LI> <LI> In depth data on amine loaded UiO-66 stability & performance in CO<SUB>2</SUB> capture conditions. </LI> <LI> Confirmation of negative thermal expansion (NTE) in bare and amine loaded UiO-66. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>
Mines, P.D.,Thirion, D.,Uthuppu, B.,Hwang, Y.,Jakobsen, M.H.,Andersen, H.R.,Yavuz, C.T. Elsevier 2017 Chemical engineering journal Vol.309 No.-
Nanoporous networks of covalent organic polymers (COPs) are successfully grafted on the surfaces of activated carbons, through a series of surface modification techniques, including acyl chloride formation by thionyl chloride. Hybrid composites of activated carbon functionalized with COPs exhibit a core-shell formation of COP material grafted to the outer layers of activated carbon. This general method brings features of both COPs and porous carbons together for target-specific environmental remediation applications, which was corroborated with successful adsorption tests for organic dyes and metals.
Reversible water capture by a charged metal-free porous polymer
Byun, J.,Patel, H.A.,Thirion, D.,Yavuz, C.T. Elsevier 2017 Polymer Vol.126 No.-
<P><B>Abstract</B></P> <P>Climate change and industrial pollution threatens the availability of clean water. Although established protocols of water treatment exist, water capture by porous materials has emerged as a viable alternative to energy intensive processes. Here we introduce a new charged porous polymer that is capable of capturing and releasing water by simple humidity or temperature swings. The quaternary amines on the framework structure attract water molecules and further solvate by coordination. The porosity of the network structure also provides enough void where water can diffuse throughout the solid. Water uptake capacity of the porous polymer surpasses common desiccants like silica gel and molecular sieves, and has the potential to act as an organic desiccant in applications like electronics or food packaging.</P> <P><B>Highlights</B></P> <P> <UL> <LI> A new charged porous polymer that captures water from atmosphere reversibly. </LI> <LI> The maximum water uptake capacity reaches up to 72 wt% at RH 90%. </LI> <LI> The cyclic water uptake performance excels that of commercial desiccants. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>3D graphical illustration of water adsorbing porous polymer, COP-120.</P> <P>[DISPLAY OMISSION]</P>
Mines, Paul D.,Uthuppu, Basil,Thirion, Damien,Jakobsen, Mogens H.,Yavuz, Cafer T.,Andersen, Henrik R.,Hwang, Yuhoon Elsevier 2018 Chemical engineering journal Vol.339 No.-
<P><B>Abstract</B></P> <P>Granular activated carbon was customized with a chemical grafting procedure of a nanoporous polymeric network for the purpose of nanoscale zero-valent iron impregnation and subsequent water contaminant remediation. Characterization of the prepared composite material revealed that not only was the polymer attachment and iron impregnation successful, but also that the polymeric shell acted as a protective barrier against the effects of oxidation from the surrounding environment, nearly 99% of total iron content was in the form of zero-valent iron. When applied towards the remediation of two common water contaminants, nitrobenzene and nitrate, the composite material exploited the qualities of both the activated carbon and the polymeric network to work together in a synergistic manner. In that the increased protection from oxidation allowed for increased reactivity of the nanoscale zero-valent iron, and that the adsorption abilities of both the carbon and the polymer achieved a higher amount of total removal of the contaminants.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Nanoporous polymeric networks are chemically grafted to activated carbon granules. </LI> <LI> Hybrid polymer/carbon composites are impregnated with nanoscale zero-valent iron. </LI> <LI> Composite materials increase nZVI content and protect against oxidation. </LI> <LI> Materials provide effective simultaneous adsorption and degradation of pollutants. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>
Ullah, Ruh,Atilhan, Mert,Anaya, Baraa,Al-Muhtaseb, Shaheen,Aparicio, Santiago,Patel, Hasmukh,Thirion, Damien,Yavuz, Cafer T. American Chemical Society 2016 ACS APPLIED MATERIALS & INTERFACES Vol.8 No.32
<P>Organic compounds, such as covalent organic framework, metal organic frameworks, and covalent organic polymers have been under investigation to replace the well-known amine-based solvent sorption technology of CO2 and introduce the most efficient and economical material for CO2 capture and storage. Various organic polymers having different function groups have been under investigation both for low and high pressure CO2 capture. However, search for a promising material to overcome the issues of lower selectivity, less capturing capacity, lower mass transfer coefficient and instability in materials performance at high pressure and various temperatures is still ongoing process. Herein, we report synthesis of six covalent organic polymers (COPs) and their CO2, N-2, and CH4 adsorption performances at low and high pressures up to 200 bar. All the presented COPs materials were characterized by using elemental analysis method, Fourier transform infrared spectroscopy (FTIR) and solid state nuclear magnetic resonance (NMR) spectroscopy techniques. Physical properties of the materials such as surface areas, pore volume and pore size were determined through BET analysis at 77 K. All the materials were tested for CO2, CH4, and N-2 adsorption using state of the art equipment, magnetic suspension balance (MSB). Results indicated that, amide based material i.e. COP-33 has the largest pore volume of 0.2 cm(2)/g which can capture up to the maximum of 1.44 mmol/g CO2 at room temperature and at pressure of 10 bar. However, at higher pressure of 200 bar and 308 K ester-based compound, that is, COP-35 adsorb as large as 144 mmol/g, which is the largest gas capturing capacity of any COPs material obtained so far. Importantly, single gas measurement based selectivity of COP-33 was comparatively better than all other COPs materials at all condition. Nevertheless, overall performance of COP-35 rate of adsorption and heat of adsorption has indicated that this material can be considered for further exploration as efficient and cheaply available solid sorbent material for CO2 capture and separation.</P>