The objective of this work is to evaluate a novel regenerable sorbent for mercury capture based on gold nanoparticles supported on a honeycomb structured carbon monolith. A new methodology for gold nanoparticles deposition onto carbon monolith support has been developed to obtain an Au sorbent based on the direct reduction of a gold salt onto the carbon material. For comparison purposes, colloidal gold method was also used to obtain Au/C sorbents. Both types of sorbents were characterized by different techniques in order to obtain the bulk gold content, the particle size distribution and the chemical states of gold after deposition. The mercury capture capacity and mercury capture efficiency of sorbents were tested in a bench scale facility at different experimental conditions. The regenerability of the sorbents was tested along several cycles of Hg capture-regeneration. High retention efficiencies are found for both types of sorbents comparing their gold content. Moreover, the high retention efficiency is maintained along several cycles of Hg capture-regeneration. The study of the fresh sorbent, the sorbent after Hg exposition and after regeneration by XPS and XRD gives insight to explain those results.
The environmental implications of mercury do not correspond only to the emissions to the atmosphere; the quality of the captured CO 2 to be transported and sequestered has been subject of research, concerning trace quantities of heavy metals participating in mineralization and precipitation reactions in sequestration conditions. For oxycoal combustion, mercury is not an environmental issue alone but also an operational issue, particularly about where mercury could accumulate within the CO 2 processing unit. Therefore, Hg removal is necessary to prevent its attack on the aluminium heat exchangers. In this work, a regenerable sorbent based on carbon supported Au nanoparticles (0.1%wt) has been used for Hg capture under oxycoal combustion atmosphere. The influence of the presence of O 2 , NO, SO 2 and HCl in a gas containing Hg and CO 2 on the sorbent as well as on the Hg oxidation (Au can act as an oxidation catalyst) has been evaluated under a simulated flue gas. The presence of either NO or HCl in the simulated flue gas led to mercury oxidation, with oxidized mercury not evolving in the gas, indicating that it is retained on the sorbent; the oxidized mercury is well stabilized on Au surfaces of the sorbent and favours the Hg-Au amalgam formation. This sorbent has been also evaluated in 3 kWth oxycoal bubling fluidized bed combustor. A lignite with high sulphur content was burned in presence of limestone. Despite high SO 2 concentration that reached the Au/C sorbent, high capture efficiency was achieved and breakthrough occurred after 3.5 h and 10% breakthrough is not reached during the experiments. Bearing in mind that regeneration time can be adjusted near 1 h, two swing sorbent beds could be used to control mercury emissions under oxycoal combustion conditions.
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