Abstract
A series of Cu-doped activated cokes (CuO/ACs) were synthesized via an impregnation method and applied for the removal of elemental mercury (Hg0). Structure-activity relationships between Hg0 removal and CuO/AC surface characteristics were identified. Hg0 removal over CuO/AC occurs through a combination of physisorption and chemisorption and is mainly dominated by chemisorption. It was found that 1 nm micropores facilitate Hg0 physisorption. Hg0 could weakly adsorb onto an O-terminated crystal layer, whereas strongly adsorb onto Cu-terminated single highly dispersed, clustered and bulk CuO (110) crystal planes via the Mars-Maessen mechanism. Product distributions and mechanisms of Hg0 adsorption and oxidation over the CuO/AC catalyst under multi-component flue gases are also discussed. O2 enhances both physisorption and chemisorption toward Hg0 by 38%. Inhibition of Hg0 removal by SO2 originates from the competitive adsorption and deactivation of CuO cation vacancies, whereas the impact is weakened by O2 through generating 20% of physically adsorbed mercury product species. NO and O2 promote Hg0 chemisorption efficiency by 93% to form Hg(NO3)2. HOCl and/or Cl2 produced by HCl can oxidize 100% of Hg0 to HgCl2, and the catalytic oxidation efficiency is approximately 29%, but O2 slightly lowers the Hg0 catalytic oxidation efficiency by 8%. The affinity ability between various flue gases and Hg0 follows the order O2 < NO < HCl.
Published Version
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