title: An X-ray photoelectron spectroscopy study of surface changes on brominated and sulfur-treated activated carbon sorbents during mercury capture: performance of pellet versus fiber sorbents.
abstract: This work explores surface changes and the Hg capture performance of brominated activated carbon (AC) pellets, sulfur-treated AC pellets, and sulfur-treated AC fibers upon exposure to simulated Powder River Basin-fired flue gas. Hg breakthrough curves yielded specific Hg capture amounts by means of the breakthrough shapes and times for the three samples. The brominated AC pellets showed a sharp breakthrough after 170-180 h and a capacity of 585 μg of Hg/g, the sulfur-treated AC pellets exhibited a gradual breakthrough after 80-90 h and a capacity of 661 μg of Hg/g, and the sulfur-treated AC fibers showed no breakthrough even after 1400 h, exhibiting a capacity of >9700 μg of Hg/g. X-ray photoelectron spectroscopy was used to analyze sorbent surfaces before and after testing to show important changes in quantification and oxidation states of surface Br, N, and S after exposure to the simulated flue gas. For the brominated and sulfur-treated AC pellet samples, the amount of surface-bound Br and reduced sulfur groups decreased upon Hg capture testing, while the level of weaker Hg-binding surface S(VI) and N species (perhaps as NH4(+)) increased significantly. A high initial concentration of strong Hg-binding reduced sulfur groups on the surface of the sulfur-treated AC fiber is likely responsible for this sorbent's minimal accumulation of S(VI) species during exposure to the simulated flue gas and is linked to its superior Hg capture performance compared to that of the brominated and sulfur-treated AC pellet samples.
authors.affiliation: Department of Chemical Engineering, Stanford University , Stanford, California 94305, United States.
authors.forename: Arindom
authors.initials: A
authors.lastname: Saha
authors.forename: David N
authors.initials: DN
authors.lastname: Abram
authors.forename: Kendra P
authors.initials: KP
authors.lastname: Kuhl
authors.forename: Jennifer
authors.initials: J
authors.lastname: Paradis
authors.forename: Jenni L
authors.initials: JL
authors.lastname: Crawford
authors.forename: Erdem
authors.initials: E
authors.lastname: Sasmaz
authors.forename: Ramsay
authors.initials: R
authors.lastname: Chang
authors.forename: Thomas F
authors.initials: TF
authors.lastname: Jaramillo
authors.forename: Jennifer
authors.initials: J
authors.lastname: Wilcox
mesh_terms: D000327:Adsorption; D002244:Carbon / Q000737:chemistry*; D000077482:Carbon Fiber; D002606:Charcoal / Q000737:chemistry*; D005740:Gases / Q000032:analysis; D054879:Halogenation; D008628:Mercury / Q000032:analysis*; D010084:Oxidation-Reduction; D056951:Photoelectron Spectroscopy; D013455:Sulfur / Q000737:chemistry*; D013499:Surface Properties
chemical_list: D000077482:Carbon Fiber; D005740:Gases; D002606:Charcoal; D013455:Sulfur; D002244:Carbon; D008628:Mercury