Development of LnMnO_3+σ perovskite on low temperature Hg⁰ removal

LnMnO_3+σ (Ln = La, Pr, Nd, Sm, Eu, Gd or Dy) perovskites synthesized by sol-gel method were employed for gaseous elemental mercury (Hg⁰) removal from coal-fired flue gas. Characterization results revealed the structure of the perovskites presented a phase transition process from rhombohedral system to O- and O'-orthorhombic structure with the change of A-site rare earth elements. The perovskites showed satisfactory Hg⁰ removal capacity in a narrow temperature range of 100-150°C. NdMnO_3+σ with an O-O' orthorhombic structure presented the best Hg⁰ removal performance, which markedly depends on four factors: crystal structure, oxygen vacancy density, Mn⁴⁺/Mn³⁺ ratio and surface element segregation. The Hg⁰ removal mechanism was illustrated based on the mercury temperature programmed desorption experiment and X-ray photoelectron spectroscopy characterization. Both chemisorption and catalytic oxidation played a role in the Hg⁰ removal process. Chemisorption dominated the Hg⁰ removal, due to the slow catalytic oxidation rate at low temperature. This work preliminarily established the relation between the structure of rare earth manganese perovskite and Hg⁰ removal performance.