17616-04-5Relevant articles and documents
Strategically designed azolyl-carboxylate MOFs for potential humid CO2 capture
Nandi, Shyamapada,Haldar, Sattwick,Chakraborty, Debanjan,Vaidhyanathan, Ramanathan
, p. 535 - 543 (2017)
Development of solid sorbents with optimal CO2 capture characteristics is key to improving the efficiency of PSA based CO2 separation. Of the several potential sorbents, metal organic frameworks (MOFs) hold a key niche. This is owing to their modular tunable structures and manipulatable adsorption sites. Yet, developing a MOF that meets the multiple demands of a gas-separation sorbent remains a challenge. Particularly, tuning them to adsorb CO2 over the more polar water is quite difficult. The presence of highly polarizing metal centers and oxygen-rich sites in MOFs makes it difficult to retain their CO2 adsorption capacities under humid gas streams. However, tailoring the organic framework to incorporate humid CO2 capture properties should be feasible. Along these lines, here we have developed a family of iso-structural MOFs built from bi-functional ligands that carry basic azolyl and chelating carboxylate groups together. Importantly, the framework is built by employing acetate moieties as ‘modulators’; they provide a hydrophobic lining to the pore-walls. This not only enables selective adsorption of CO2, but also helps retain about 80% of the capture capacity even upon exposure to 75% RH. Along with its other advantageous features: high CO2 uptake and selectivity (3 mmol g?1 and s(CO2-N2) = ～500 for 85N2?:?15CO2@303 K); surface area: ～700 m2 g?1, working capacity: 2.6 mmol g?1; optimal HOA (22-30 kJ mol?1) and CO2 kinetics (Dc = 1.02 × 10?8 m2 s?1), these MOFs can qualify as efficient candidates for humid CO2 capture. Furthermore, we identify the most-favorable CO2 adsorption sites via simulated annealing methods, from which the presence of polarized CO2 molecules located adjacent to the π-electron rich pore walls can be seen. Importantly, these polarized molecules form T-shaped configurations among themselves via C(δ+ve)?O(δ?ve) interactions resembling those found in solid CO2, a cooperative feature that is not observed in the other CO2 molecules in the structure, which are not proximal to the polarizing walls.
Fragment-Based Discovery of a Qualified Hit Targeting the Latency-Associated Nuclear Antigen of the Oncogenic Kaposi's Sarcoma-Associated Herpesvirus/Human Herpesvirus 8
Kirsch, Philine,Jakob, Valentin,Oberhausen, Kevin,Stein, Saskia C.,Cucarro, Ivano,Schulz, Thomas F.,Empting, Martin
supporting information, (2019/05/01)
The latency-associated nuclear antigen (LANA) is required for latent replication and persistence of Kaposi's sarcoma-associated herpesvirus/human herpesvirus 8. It acts via replicating and tethering the virus episome to the host chromatin and exerts other functions. We conceived a new approach for the discovery of antiviral drugs to inhibit the interaction between LANA and the viral genome. We applied a biophysical screening cascade and identified the first LANA binders from small, structurally diverse compound libraries. Starting from a fragment-sized scaffold, we generated optimized hits via fragment growing using a dedicated fluorescence-polarization-based assay as the structure-activity-relationship driver. We improved compound potency to the double-digit micromolar range. Importantly, we qualified the resulting hit through orthogonal methods employing EMSA, STD-NMR, and MST methodologies. This optimized hit provides an ideal starting point for subsequent hit-to-lead campaigns providing evident target-binding, suitable ligand efficiencies, and favorable physicochemical properties.
3D printing of a heterogeneous copper-based catalyst
Tubío, Carmen R.,Azuaje, Jhonny,Escalante, Luz,Coelho, Alberto,Guitián, Francisco,Sotelo, Eddy,Gil, Alvaro
, p. 110 - 115 (2016/01/09)
One of the most important environmental challenges of modern society is to develop new catalysts that make possible chemical processes with reduced environmental impact. Catalyst immobilization is an appealing strategy that, in addition to facilitating catalyst recovery, has proved to give higher catalytic performance, since the solid support usually provides chemical, thermal, and mechanical stabilization to the catalytic species. In this work Cu/Al2O3 catalytic system with a woodpile porous structure is synthesized by 3D printing and then sintered at high temperature to generate a copper-supported rigid structure with high mechanical strength, a high surface-to-volume ratio, and controlled porosity. The catalytic species (Cu) are immobilized in the Al2O3 matrix to avoid the leaching of the metal into the reaction medium. Al2O3 was selected because it is a good material to obtain a structure with high mechanical stability after high-temperature treatment. The resulting device shows high catalytic efficacy and good recyclability and did not produce leaching of copper to the reaction medium in different Ullmann reactions. Ease of preparation, excellent reactivity, recyclability, and negligible metal contamination all make the 3D printing technique a good strategy for fabricating other types of metal/oxide heterogeneous catalytic systems.
