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A novel and efficient adsorbent (TM-MoSe2, TM = Fe, Co, Ni) for mercury removal was developed and studied. The adsorption of mercury species (Hg0, HgCl, and HgCl2) and the oxidation of Hg0 by HCl on TM-MoSe2 (001) surface were explored at molecular level by density functional theory (DFT). The results shown that the Hg0 adsorption capacity of MoSe2 was improved by the doping of Fe/Co/Ni, which was also confirmed by experiments. The initial Hg0 removal efficiency of MoSe2-based adsorbents reached 96.4-100.0%. In addition, HgCl was mainl