Mercury capture by a structured Au/C regenerable sorbent under oxycoal combustion representative and real conditions

• Published in: Fuel (Guildford) Vol. 207; pp. 821 - 829
• Main Authors: Gómez-Giménez, C., Izquierdo, M.T., de las Obras-Loscertales, M., de Diego, L.F., García-Labiano, F., Adánez, J.
• Format: Journal Article
• Language: English
• Published: Kidlington Elsevier Ltd 01.11.2017; Elsevier BV
• Subjects: Aluminum; Atmosphere; Bubbling; Carbon dioxide; Carbon sequestration; Chemical precipitation; Coal; Combustion; Emissions; Environmental impact; Flue gas; Fluidized bed combustion; Fluidized beds; Gold; Heat exchangers; Heavy metals; Lignite; Limestone; Mercury; Mercury (metal); Mercury retention; Mineralization; Nanoparticles; Oxidation; Oxycoal combustion; Oxygen; Precipitation; Regenerable sorbent; Regeneration; Solvents; Sulfur; Sulfur dioxide; Regenerable sorbent; Oxycoal combustion; Mercury retention
• ISSN: 0016-2361; 1873-7153
• DOI: 10.1016/j.fuel.2017.06.100

[Display omitted] •Au (0.1wt%)/C sorbent has Hg capture efficiency >90% under oxycombustion atmosphere.•Active sites for Hg chemisorption are created on the support under NO/HCl atmosphere.•Oxidized Hg monolayer on Au surface enhances Au-Hg amalgam formation.•High Hg capture capacity under >2500ppm SO2 if an oxidant (NO or HCl) is present.•Hg retention under real conditions makes the sorbent feasible for a waste-free process. The environmental implications of mercury do not correspond only to the emissions to the atmosphere; the quality of the captured CO2 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 CO2 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 O2, NO, SO2 and HCl in a gas containing Hg and CO2 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 3kWth oxycoal bubbling fluidized bed combustor. A lignite with high sulphur content was burned in presence of limestone. Despite high SO2 concentration that reached the Au/C sorbent, high capture efficiency was achieved and breakthrough occurred after 3.5h and 10% breakthrough is not reached during the experiments. Bearing in mind that regeneration time can be adjusted near 1h, two swing sorbent beds could be used to control mercury emissions under oxycoal combustion conditions.