Abstract
Copper sulfate (CuSO4) is a ubiquitous component in natural minerals and industrial dusts. However, CuSO4 has been believed usually that it has adverse effect on elemental mercury (Hg0) removal from flue gas. Here, we offered a new insight into the effect of crystal water in copper sulfate on Hg0 catalytic oxidation. The structure evolution of copper sulfate by density functional theory (DFT) calculation revealed anhydrous CuSO4 crystal contributing to a better HCl adsorption which provided a precondition for Hg0 oxidation. Experimental results about the catalytic activity sequence of CuSO4 > CuSO4·H2O > CuSO4·5H2O with HCl confirmed the negative effect of crystal water on Hg0 catalytic oxidation. To realize industrial application, supported catalysts CuSO4/α-Al2O3 synthesized by wet impregnation method was employed for elemental mercury (Hg0) oxidation and the results exhibited excellent performance in Hg0 oxidation under 250 °C–400 °C. The Hg0 conversion efficiency was above 97% in the presence of 2 ppm HCl + 6% O2 at 300 °C. Combining computational and X-ray photoelectron spectroscopy (XPS) analyses together, Cu atoms exposure on the surface of anhydrous CuSO4 were the critical active sites for Hg0 oxidation and the reaction obeyed the Eley–Rideal mechanism.
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