Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, 030024, China.
Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan, 030024, China; Department of Chemistry and Chemical Engineering, Jining Normal University, Ulanqab, 012000, China.
Chemosphere. 2020 Jun;249:126164. doi: 10.1016/j.chemosphere.2020.126164. Epub 2020 Feb 10.
This study attempted to investigate the effect of impregnation sequence of the Pd/Ce/γ-AlO sorbents on Hg removal. To this end, five kinds of sorbents were prepared and tested in simulated coal derived fuel gas (N-H-CO-HS-Hg), including Pd/γ-AlO, Ce/γ-AlO and three kinds of Pd-based sorbents with Ce impregnation on γ-AlO substrate. The tests were conducted at 250 and 300 °C respectively. According to the results, bimetallic Ce-Pd/γ-AlO sorbent prepared by simultaneously impregnating Pd and Ce showed much higher and more stable removal efficiency of Hg than the other three kinds of sorbents. The Hg removal efficiency of Ce-Pd/γ-AlO sorbent reached above 98% within 480 min at 250 °C and 91% within 200 min at 300 °C. Characterization results indicated that the sorbent Ce-Pd/γ-AlO prepared by the co-impregnation method had bigger specific surface area (216.6 m/g) than the other three kinds of Pd-based sorbents. The content Pd and Ce on the sorbent Ce-Pd/γ-AlO surface is 0.21% and 0.61%, which proved higher than that of the other three kinds of Pd-based sorbents, and observation from STEM-XEDS maps showed it demonstrated the highest dispersion. It is found that Ce is likely to promote the dispersion of Pd on the support surface during the preparation of the sorbent under the co-impregnation method. Meanwhile, Ce enhanced the HS resistance of the sorbent. Thereby, Ce-Pd/γ-AlO sorbent is found to have the optimal performance of mercury removal. In this study, the Hg removal mechanism of the Pd/Ce/γ-AlO sorbents in the simulated coal derived fuel gas was also elaborated.
本研究旨在探讨浸渍顺序对 Pd/Ce/γ-AlO 吸附剂脱汞性能的影响。为此,采用浸渍法制备了 Pd/γ-AlO、Ce/γ-AlO 及三种负载型 Pd 基吸附剂,并在模拟煤衍生燃料气(N-H-CO-HS-Hg)中进行了性能评价,考察温度分别为 250 和 300°C。结果表明,同时浸渍制备的双金属 Ce-Pd/γ-AlO 吸附剂具有更高和更稳定的脱汞性能。在 250°C 时,Ce-Pd/γ-AlO 吸附剂在 480 min 内的汞去除率高于 98%,在 300°C 时在 200 min 内的汞去除率高于 91%。表征结果表明,共浸渍法制备的 Ce-Pd/γ-AlO 吸附剂比其他三种 Pd 基吸附剂具有更大的比表面积(216.6 m/g)。Ce-Pd/γ-AlO 表面的 Pd 和 Ce 含量分别为 0.21%和 0.61%,高于其他三种 Pd 基吸附剂,STEM-XEDS 图谱观察表明其分散度最高。研究发现,在共浸渍法制备吸附剂的过程中,Ce 可能促进了 Pd 在载体表面的分散。同时,Ce 增强了吸附剂的抗 HS 性能。因此,Ce-Pd/γ-AlO 吸附剂具有最佳的脱汞性能。本研究还阐述了 Pd/Ce/γ-AlO 吸附剂在模拟煤衍生燃料气中脱汞的机理。