Abstract Due to the water-insoluble nature of Hg0, its oxidization to Hg2+, which is water-soluble, is a viable approach for its effective removal at coal-fired plants using existing flue gas desulfurization (FGD) unit. In this study, the adsorption and oxidation of elemental mercury on an Mn-doped g-C3N4 material were investigated. The spin-polarized density functional theory method was adapted to optimize the geometry structures and then to determine the corresponding electronic structures, while the CI-NEB method was adopted to search for the stable intermediates during the reaction(s). The analysis of energy and project density of states shows that the Mn-g-C3N4 exhibits an excellent affinity to Hg atoms. It is found that it is feasible for Hg atoms to oxidize on the Mn-g-C3N4 surface via two possible E-R paths, but with relatively high energy barriers. This research provides insights into a viable way for mercury removal using O2 as the oxidizing agent.

中文翻译：

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O2 在 Mn 掺杂的屈曲 g-C3N4 催化剂上对 Hg0 氧化的 DFT 研究

摘要 由于 Hg0 的不溶于水的性质，将其氧化为水溶性的 Hg2+ 是使用现有烟气脱硫 (FGD) 装置的燃煤电厂有效去除 Hg2+ 的可行方法。在这项研究中，研究了元素汞在 Mn 掺杂的 g-C3N4 材料上的吸附和氧化。自旋极化密度泛函理论方法用于优化几何结构，然后确定相应的电子结构，而 CI-NEB 方法用于寻找反应过程中的稳定中间体。能量和状态密度的分析表明，Mn-g-C3N4 对 Hg 原子表现出极好的亲和力。发现 Hg 原子通过两种可能的 ER 路径在 Mn-g-C3N4 表面氧化是可行的，但能量壁垒相对较高。这项研究提供了对使用 O2 作为氧化剂去除汞的可行方法的见解。