Cameron A. Lippert

Improving carbon capture from power plant emissions with zinc- and cobalt-based catalysts

We report homogeneous catalysts that are soluble and stable in primary amine-based CO2 capture solvents. The zinc(II) and cobalt(III) complexes, which contain electron-donating multi-dentate anionic ligands, perform catalytic CO2 hydration at unparalleled observed rates under conditions conducive to industrial post-combustion carbon capture processes.

Carbonic anhydrase mimics for enhanced CO2 absorption in an amine-based capture solvent

Two new small-molecule enzyme mimics of carbonic anhydrase were prepared and characterized. These complexes contain the salen-like ligand bis(hydroxyphenyl)phenanthroline. This ligand is similar to the salen-type ligands previously incorporated into carbonic anhydrase mimics but contains no hydrolyzable imine groups and therefore serves as a promising ligand scaffold for the synthesis of a more robust CO2 hydration catalyst. These homogeneous catalysts were investigated for CO2 hydration in concentrated primary amine solutions through which a dilute CO2 (14%) fluid stream was flowed and showed exceptional activity for increased CO2 absorption rates.

Spray-Coated Multiwalled Carbon Nanotube Composite Electrodes for Thermal Energy Scavenging Electrochemical Cells

Spray-coated multiwalled carbon nanotube/poly(vinylidene fluoride) (MWCNT/PVDF) composite electrodes, scCNTs, with varying CNT compositions (2 to 70 wt %) are presented for use in a simple thermal energy-scavenging cell (thermocell) based on the ferro/ferricyanide redox couple. Their utility for direct thermal-to-electrical energy conversion is explored at various temperature differentials and cell orientations. Performance is compared to that of buckypaper, a 100% CNT sheet material used as a benchmark electrode in thermocell research. The 30 to 70 wt % scCNT composites give the highest power output by electrode area-seven times greater than buckypaper at ΔT = 50 °C. CNT utilization is drastically enhanced in our electrodes, reaching 1 W gCNT(-1) compared to 0.036 W gCNT(-1) for buckypaper. Superior performance of our spray-coated electrodes is attributed to both wettability with better use of a large portion of electrochemically active CNTs and minimization of ohmic and thermal contact resistances. Even composites with as low as 2 wt % CNTs are still competitive with prior art. The MWCNT/PVDF composites developed herein are inexpensive, scalable, and serve a general need for CNT electrode optimization in next-generation devices.

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 pKa of the sorbent, and chemical structure of the parent amine and nitrosamine.