固体吸附剂脱除燃煤烟气汞的实验与机理分析-experimental and mechanism analysis of mercury removal from coal-fired flue gas by solid adsorbent.docx

ABSTRACTAs the largest source of anthropogenic mercury emissions, mercury emitted from coal-fired power plants has been identified as a hazardous pollutant to both human health and environment. Therefore, the control of mercury emission from coal-fired utilities is vital to mitigate global mercury pollution. In recent years, many studies have been conducted to evaluate the effectiveness of Hg0 adsorption by solid sorbents. However, little theoretical calculations have been carried out to gain an increased understanding of the details of interactions between Hg0 and solid sorbents. In this paper, Density Functional Theory (DFT) was employed to examine the binding mechanism of elemental mercury (Hg0) on the simulated CaO and activated carbon (AC) surface. Furthermore, modified calcium-based rice husk ash sorbents and novle silver nano-particles sorbnts were synthesized and evaluated their effectiveness of Hg0 adsorption. These investigations will provide useful information for developing mercury emission control technologies.Adsorption of mercury and mercury chloride on a CaO surface has been investigated by means of DFT cluster model calculations. The systematic comparison of different embedding clusters (shell models, point charges cluster and bare cluster) and calculation functions and basis used for mercury are presented. The results clearly indicate that the SM (shell model) cluster is better than PC embedding clusters and bare clusters in the aspects of computational accuracy in the gas-solid adsorption system. The computations also showthat the elemental mercury can only coordinate to the O2- anion and has a very weakbinding energy, which infers mercury is weakly physisorbed at the surface of the CaO. When the mercury chloride molecular axis is parallel to the surface, the Hg atom coordinate to the O2- anion and has a large binding energy, which means that mercury chloride adsorbed on surface of CaO is mainly chemisorption. The present calculations indicate th