1. National Engineering Laboratory for Reducing Emissions from Coal Combustion, Shandong University, Jinan 250061, China 2. Bingtuan Energy Development Institute, Shihezi University, Shihezi 832000, China
A nitrogen-doped carbon microsphere sorbent with a hierarchical porous structure was synthesized via aggregation-hydrothermal carbonization. The Hg0 adsorption performance of the nitrogen-doped carbon microsphere sorbent was tested and compared with that of the coconut shell activated carbon prepared in the laboratory. The effect of H2S on Hg0 adsorption was also investigated. The nitrogen-doped carbon microsphere sorbent exhibited superior mercury removal performance compared with that of coconut shell activated carbon. In the absence of H2S at a low temperature (≤ 100 °C), the Hg0 removal efficiency of the nitrogen-doped carbon microsphere sorbent exceeded 90%. This value is significantly higher than that of coconut shell activated carbon, which is approximately 45%. H2S significantly enhanced the Hg0 removal performance of the nitrogen-doped carbon microsphere sorbent at higher temperatures (100–180 °C). The hierarchical porous structure facilitated the diffusion and adsorption of H2S and Hg0, while the nitrogen-containing active sites significantly improved the adsorption and dissociation capabilities of H2S, contributing to the generation of more active sulfur species on the surface of the nitrogen-doped carbon microsphere sorbent. The formation of active sulfur species and HgS on the sorbent surface was further confirmed using X-ray photoelectron spectroscopy and Hg0 temperature-programmed desorption tests. Density functional theory was employed to elucidate the adsorption and transformation of Hg0 on the sorbent surface. H2S adsorbed and dissociated on the sorbent surface, generating active sulfur species that reacted with gaseous Hg0 to form HgS.
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