Steven Reynolds Hai Du

Savannah River Site has used the metal hydride LaNi_4.25Al_0.75 (LANA.75) in the Tritium Facilities for over two decades. LANA.75 beds store significant quantities of tritium but have a limited service life due to the radiolytic decay of tritium to ³He within the metal matrix. It has been shown that the isotherm performance of a tritium-aged LANA.75 sample can be restored by heating under vacuum. Additional investigation is needed to ensure there are no unexpected changes to the hydride before this technique is employed in full-scale beds in the Tritium Facilities. In addition, it is necessary to verify the regenerable behavior and thermal stability of LANA.75 on a small scale prior to it being implemented on a large scale. A non-tritiated bench-scale LANA.75 sample was held at 750°C under vacuum for 200 h to simulate exposure to multiple restoration evolutions. Hydride isotherm performance, chemical composition, crystallinity, and morphology are compared between the pre-restorative and post-restorative testing samples. No significant changes were observed in composition or crystallinity. Comparison of pre-anneal and post-anneal isotherms showed that performance improved rather than deteriorated during the evolution. Scanning electron microscopy analysis showed small growths on the particle surface after exposure to regeneration conditions. Additional testing will be required to determine the cause of these growths.

The objective of this three-year project was to study new pressure swing adsorption (PSA) cycles for CO{sub 2} capture and concentration at high temperature. The heavy reflux (HR) PSA concept and the use of a hydrotalcite like (HTlc) adsorbent that captures CO{sub 2} reversibly at high temperatures simply by changing the pressure were two key features of these new PSA cycles. Through the completion or initiation of nine tasks, a bench-scale experimental and theoretical program has been carried out to complement and extend the process simulation study that was carried out during Phase I (DE-FG26-03NT41799). This final report covers the entire project from August 1, 2005 to July 31, 2008. This program included the study of PSA cycles for CO{sub 2} capture by both rigorous numerical simulation and equilibrium theory analysis. The insight gained from these studies was invaluable toward the applicability of PSA for CO{sub 2} capture, whether done at ambient or high temperature. The rigorous numerical simulation studies showed that it is indeed possible to capture and concentrate CO{sub 2} by PSA. Over a wide range of conditions it was possible to achieve greater than 90% CO{sub 2} purity and/or greater than 90% CO{sub 2} recovery, depending onmore » the particular heavy reflux (HR) PSA cycle under consideration. Three HR PSA cycles were identified as viable candidates for further study experimentally. The equilibrium theory analysis, which represents the upper thermodynamic limit of the performance of PSA process, further validated the use of certain HR PSA cycles for CO{sub 2} capture and concentration. A new graphical approach for complex PSA cycle scheduling was also developed during the course of this program. This new methodology involves a priori specifying the cycle steps, their sequence, and the number of beds, and then following a systematic procedure that requires filling in a 2-D grid based on a few simple rules, some heuristics and some experience. It has been tested successfully against several cycle schedules taken from the literature, including a 2-bed 4-step Skarstrom cycle, a 4-bed 9-step process with 2 equalization steps, a 9-bed 11-step process with 3 equalization steps, and a 6-bed 13-step process with 4 equalization steps and 4 idle steps. With respect to CO{sub 2} capture and concentration by PSA, this new approach is now providing a very straightforward way to determine all the viable 3-bed, 4-bed, 5-bed, n-bed, etc. HR PSA cycle schedules to explore using both simulation and experimentation. This program also touted the use of K-promoted HTlc as a high temperature, reversible adsorbent for CO{sub 2} capture by PSA. This program not only showed how to use this material in HR PSA cycles, but it also proposed a new CO{sub 2} interaction mechanism in conjunction with a non-equilibrium kinetic model that adequately describes the uptake and release of CO{sub 2} in this material, and some preliminary fixed bed adsorption breakthrough and desorption elution experiments were carried out to demonstrate complete reversibility on a larger scale. This information was essentially missing from the literature and deemed invaluable toward promoting the use of K-promoted HTlc as a high temperature, reversible adsorbent for CO{sub 2} capture by PSA. Overall, the objectives of this project were met. It showed the feasibility of using K-promoted hydrotalcite (HTlc) as a high temperature, reversible adsorbent for CO{sub 2} capture by PSA. It discovered some novel HR PSA cycles that might be useful for this purpose. Finally, it revealed a mechanistic understanding of the interaction of CO{sub 2} with K-promoted HTlc. « less

A cyclic adsorption process simulator was used to determine preliminary bed size and characteristics for a sorbent-based atmosphere revitalization (SBAR) system being designed by NASA for the Crew Exploration Vehicle. An initial study of a 2-bed 3-step 3-layer, vacuum swing adsorption cycle, utilizing 50% silica gel, 17% 13X zeolite, and 33% 5A zeolite revealed that a 10 L bed could easily meet the CO2 and H2 O removal criteria for a 3 person crew. A parametric study showed that the cycle time, layering percentage of silica gel, and H2 O-silica gel mass transfer coefficient were important parameters in the SBAR design. Increasing the cycle time diminished the CO2 and H2 O removal performances but resulted in less O2 lost to space. The CO2 and H2 O removal performances increased considerably when a silica gel layer was added to the bed, with the above layering percentages being close to optimum. As more silica gel was added to the bed slightly more O2 was lost. Larger values of the H2 O-silica gel mass transfer coefficient improved the CO2 and H2 O removal performances but at the expense of slightly more O2 lost.