Development of High-Capacity and Water-Lean CO2 Absorbents by a Concise Molecular Design Strategy through Viscosity Control.

The exponentially increasing viscosity of water-lean CO2 absorbents during carbon capture processes is a critical problem for practical application, owing to its strong correlation with systems' mass transfer properties, as well as convenience of transportation. In this work, a concise strategy based on structure-viscosity relationships is proposed and applied to construct a series of functionalized ethylenediamines as single-component absorbents for post-combustion CO2 capture. These nonaqueous absorbents have outstanding viscosities (50-200 cP, 25 °C) at their maximal CO2 capacities (up to 22 wt % or 4.92 mol kg-1 , 1 bar), and are readily regenerated at low temperatures (50-80 °C) under ambient pressure. Additional capture of CO2 through physisorption could also be achieved by operating at high pressures. The CO2 capture and release process is systematically investigated by means of 13 C NMR spectroscopy, differential scanning calorimetry (DSC), in situ FTIR analysis, and density functional theory (DFT) calculations, which could provide sufficient spectroscopic details to reveal the ease of reversibility and enable rational interpretation of the absorption mechanism.

Cu(II)-catalyzed esterification reaction via aerobic oxidative cleavage of C(CO)-C(alkyl) bonds.

A novel Cu(II)-catalyzed aerobic oxidative esterification of simple ketones for the synthesis of esters has been developed with wide functional group tolerance. This process is assumed to go through a tandem sequence consisting of α-oxygenation/esterification/nucleophilic addition/C-C bond cleavage and carbon dioxide is released as the only byproduct.

Highly efficient SO2 absorption/activation and subsequent utilization by polyethylene glycol-functionalized Lewis basic ionic liquids.

Up to now, flue-gas desulfurization (FGD) is one of the most effective techniques to control SO(2) emission from the combustion of fossil fuels. The conventional technology for FGD poses serious inherent drawbacks such as formation of byproducts and volatilization of solvents. In this work, polyethylene glycol (PEG)-functionalized Lewis basic ionic liquids (ILs) derived from DABCO were proved to be highly efficient absorbents for FGD due to its specific features such as high thermal stability, negligible vapor pressure, high loading capacity. Notably, PEG(150)MeDABCONTf(2) gave an extremely high SO(2) capacity (4.38 mol mol(-1) IL), even under 0.1 bar SO(2) partial pressure (1.01 mol mol(-1) IL), presumably owing to the strong SO(2)-philic characterization of the PEG chain. Furthermore, the absorbed SO(2) could be easy to release by just bubbling N(2) at room temperature, greatly reducing energy requirement for SO(2) desorption. In addition, SO(2)/CO(2) selectivity (110) of PEG(150)MeDABCONTf(2) is two times larger than the non-functionalized imidazolium IL (45). On the other hand, through activation of SO(2) with the tertiary nitrogen in the cation, Lewis basic ILs such as PEG(150)MeDABCOBr proved to be efficient catalysts for the conversion of SO(2) to some value-added chemicals such as cyclic sulfites without utilization of any organic solvent or additive. Thus, this protocol would pave the way for the development of technological innovation towards efficient and low energy demanded practical process for SO(2) absorption and subsequent transformation.

Equimolar CO2 capture by N-substituted amino acid salts and subsequent conversion.

Steric bulk controls CO(2) absorption: N-substituted amino acid salts in poly(ethylene glycol) reversibly absorb CO(2) in nearly 1:1 stoichiometry. Carbamic acid is thought to be the absorbed form of CO(2); this was supported by NMR and in situ IR spectroscopy, and DFT calculations. The captured CO(2) could be converted directly into oxazolidinones and thus CO(2) desorption could be sidestepped.

Quaternary ammonium bromide functionalized polyethylene glycol: a highly efficient and recyclable catalyst for selective synthesis of 5-aryl-2-oxazolidinones from carbon dioxide and aziridines under solvent-free conditions.

A quaternary ammonium bromide covalently bound to polyethylene glycol (PEG, MW = 6000), i.e., PEG(6000-)(NBu(3)Br)2, was found to be an efficient and recyclable catalyst for the cycloaddition reaction of aziridines to CO(2) under mild conditions without utilization of additional organic solvents or cocatalysts. As a result, 5-aryl-2-oxazolidinone was obtained in high yield with excellent regioselectivity. The catalyst worked well for a wide variety of 1-alkyl-2-arylaziridines. Besides, the catalyst could be recovered by centrifugation and reused without significant loss of catalytic activity and selectivity.

Controlled fabrication of cross-linked nanoparticles/polymer composite thin films through the combined use of surface-initiated atom transfer radical polymerization and gas/solid reaction.

A promising strategy for the controlled synthesis of inorganic/polymeric nanocomposites may be sustained by fabricating cross-linked PbS nanoparticles/polymer composite thin films through combining surface-initiated atom transfer radical polymerization (ATRP) and gas/solid reaction. The introduction of Pb ions through the extension of surface-initiated ATRP to the monomers containing metal ions provides an opportunity for generating nanoparticles on the substrate.