Method of Development and Use of Catalyst-Functionalized Catalytic Particles to Increase the Mass Transfer Rate of Solvents Used in Acid Gas Cleanup

The present invention relates to methods for improving carbon capture using entrained catalytic-particles within an amine solvent. The particles are functionalized and appended with a CO2 hydration catalyst to enhance the kinetics of CO2 hydration and improve overall mass transfer of CO2 from an acid gas

Method and Apparatus for Increasing Mass Transfer in Aqueous Gas Adsorption Processes

A method of removing and capturing an acid gas from a fluid stream includes exposing the fluid stream to an aqueous scrubbing solution in the presence of a packing element including alternating hydrophobic and hydrophilic features or zones. A related apparatus is also disclosed

CO\u3csub\u3e2\u3c/sub\u3e Mass Transfer Enhancement of Aqueous Amine Solvents by Particle Additives

The present invention relates to methods for improving carbon capture by providing particles within an amine solvent. The particles provide for increased turbulence at the interface between the counter-flowing gas and solvent, which allows for increased amine and carbamate salt diffusion between the liquid film and bulk

Enhancements in Mass Transfer for Carbon Capture Solvents Part I: Homogeneous Catalyst

The novel small molecule carbonic anhydrase (CA) mimic [CoIII(Salphen-COO−)Cl]HNEt3 (1), was synthesized as an additive for increasing CO2 absorption rates in amine-based post-combustion carbon capture processes (CCS), and its efficacy was verified. 1 was designed for use in a kinetically slow but thermally stable blended solvent, containing the primary amines 1-amino-2-propanol (A2P) and 2-amino-2-methyl-1-propanol (AMP). Together, the A2P/AMP solvent and 1 reduce the overall energy penalty associated with CO2 capture from coal-derived flue gas, relative to the baseline solvent MEA. 1 is also effective at increasing absorption kinetics of kinetically fast solvents, such as MEA, which can reduce capital costs by requiring a smaller absorber tower. The transition from catalyst testing under idealized laboratory conditions, to process relevant lab- and bench-scale testing adds many additional variables that are not well understood and rarely discussed. The stepwise testing of both 1 and the novel A2P/AMP solvent blend is described through a transition process that identifies many of these process and evaluation challenges not often addressed when designing a chemical or catalytic additive for industrial CCS systems, where consideration of solvent chemistry is typically the primary goal

Selective Removal of Nitrosamines from a Model Amine Carbon-Capture Waterwash Using Low-Cost Activated-Carbon Sorbents

Nitrosamines generated in the amine solvent loop of postcombustion carbon capture systems are potent carcinogens, and their emission could pose a serious threat to the environment or human health. Nitrosamine emission control strategies are critical for the success of amine-based carbon capture as the technology approaches industrial-scale deployment. Waterwash systems have been used to control volatile and aerosol emissions, including nitrosamines, from carbon-capture plants, but it is still necessary to remove or destroy nitrosamines in the circulating waterwash to prevent their subsequent emission into the environment. In this study, a cost-effective method for selectively removing nitrosamines from the absorber waterwash effluent with activated-carbon sorbents was developed to reduce the environmental impact associated with amine-based carbon capture. The results show that the commercial activated-carbon sorbents tested have a high capacity and selectivity for nitrosamines over the parent solvent amines, with capacities up to 190 mg/g carbon, under simulated amine waterwash conditions. To further reduce costs, an aerobic thermal sorbent regeneration step was also examined due to the low thermal stability of nitrosamines. To model the effect of oxidation on the sorbent performance, thermal- and acid-oxidized sorbents were also prepared from the commercial sorbents and analyzed. The chemical and physical properties of nitrosamines, the parent amine, and the influence of the physical properties of the carbon sorbents on nitrosamine adsorption was examined. Key sorbent properties included the sorbent hydrophilicity and hydrophobicity, surface p<i>K</i>_a of the sorbent, and chemical structure of the parent amine and nitrosamine

Molecular Modeling of the Physical Properties for Aqueous Amine Solution Containing a CO₂ Hydration Catalyst

The effects of an amphiphilic CO₂ hydration catalyst (C3P) on the physical properties of aqueous monoethanolamine (MEA) solutions were studied using molecular simulations and verified experimentally. Adding 2.7–27.7 g/L of C3P in 30 wt % MEA aqueous solution did not significantly affect the solution viscosity, surface tension, or CO₂ diffusivity. These results confirm that the previously reported increase in CO₂ mass transfer by C3P is due to CO₂ hydration catalysis and not due to changes in the physical properties of the MEA solution. Additional simulations indicate that the catalyst molecules tend to aggregate in MEA solution and are preferentially adsorbed at the gas–liquid interface region. For the catalyst molecules remaining in the bulk solution, the local concentrations of CO₂ and MEA in the area immediately around the catalyst are increased while the local water concentration is decreased, relative to their concentrations in the rest of the bulk MEA solution

Synthesis and ligand non-innocence of thiolate-ligated (N4S) iron(II) and nickel(II) bis(imino)pyridine complexes

The known iron(II) complex [Fe(II)(LN(3)S)(OTf)] (1) was used as starting material to prepare the new biomimetic (N(4)S(thiolate)) iron(II) complexes [Fe(II)(LN(3)S)(py)](OTf) (2) and [Fe(II)(LN(3)S)(DMAP)](OTf) (3), where LN(3)S is a tetradentate bis(imino)pyridine (BIP) derivative with a covalently tethered phenylthiolate donor. These complexes were characterized by X-ray crystallography, UV-vis, (1)H NMR, and Mössbauer spectroscopy, as well as electrochemistry. A nickel(II) analogue, [Ni(II)(LN(3)S)](BF(4)) (5), was also synthesized and characterized by structural and spectroscopic methods. Cyclic voltammetric studies showed 1 – 3 and 5 undergo a single reduction process with E(1/2) between −0.9 to −1.2 V versus Fc(+)/Fc. Treatment of 3 with 0.5% Na/Hg amalgam gave the mono-reduced complex [Fe(LN(3)S)(DMAP)](0) (4), which was characterized by X-ray crystallography, UV-vis, EPR (g = [2.155, 2.057, 2.038]) and Mössbauer (δ = 0.33 mm s(−1); ΔE(Q) = 2.04 mm s(−1)) spectroscopies. Computational methods (DFT) were employed to model complexes 3 – 5. The combined experimental and computational studies show that 1 – 3 are 5-coordinate, high-spin (S = 2) Fe(II) complexes, whereas 4 is best described as a 5-coordinate, intermediate-spin (S = 1) Fe(II) complex antiferromagnetically coupled to a ligand radical. This unique electronic configuration leads to an overall doublet spin (S(total) = ½) ground state. Complexes 2 and 3 are shown to react with O(2) to give S-oxygenated products, as previously reported for 1. In contrast, the mono-reduced 4 appears to react with O(2) to give a mixture of S- and Fe-oxygenates. The nickel(II) complex 5 does not react with O(2), and even when the mono-reduced nickel complex is produced, it appears to undergo only outer-sphere oxidation with O(2)

Thioether-ligated iron(ii) and iron(iii)-hydroperoxo/alkylperoxo complexes with an H-bond donor in the second coordination sphere

The non-heme iron complexes, [Fe(II)(N3PySR)(CH(3)CN)](BF(4))(2) (1) and [Fe(II)(N3Py(amide)SR)](BF(4))(2) (2), afford rare examples of metastable Fe(iii)-OOH and Fe(iii)-OOtBu complexes containing equatorial thioether ligands and a single H-bond donor in the second coordination sphere. These peroxo complexes were characterized by a range of spectroscopic methods and density functional theory studies. The influence of a thioether ligand and of one H-bond donor on the stability and spectroscopic properties of these complexes was investigated

CCDC 955342: Experimental Crystal Structure Determination

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures

CCDC 955340: Experimental Crystal Structure Determination

An entry from the Cambridge Structural Database, the world’s repository for small molecule crystal structures. The entry contains experimental data from a crystal diffraction study. The deposited dataset for this entry is freely available from the CCDC and typically includes 3D coordinates, cell parameters, space group, experimental conditions and quality measures