Energy & Fuels, Vol.26, No.6, 3393-3398, 2012
Interaction among Metal Components of Zn-Mn-Cu-Based Sorbents Prepared by High-Pressure Impregnation Method and Its Effect on the Removal of H2S from Hot Coal Gas
A series of metal oxide sorbents for the deep removal of H2S from hot coal gas were synthesized using a high-pressure impregnation method. Semicoke was selected as support and the solutions of one or more combination among zinc nitrate, manganese nitrate, and copper nitrate were selected as the active component precursors in the preparation process of sorbents. SEM results show that these metal oxides can be evenly dispersed onto semicoke support with nanometer particle sizes by a high-pressure impregnation method. Simultaneously, the pore structures of the sorbents are significantly improved through the hydrothermal process of high-pressure impregnation. The desulfurization activities of the Zn-Mn-Cu-based sorbents in a fixed-bed reactor under feeding gas of CO (33 vol %), H-2 (39 vol %), H2S (500 ppmv), and N-2 (balance) are much better than those of single Zn-, Mn-, and Cu-based as well as double Zn-Mn-based sorbents prepared under the same operating conditions. The Z20M4C6SC sorbent can remove H2S from 500 to 0.1 ppmv at 300-550 degrees C and hold for 56 h. The sulfur capacity is 13.84 g S/100 g sorbent at 500 degrees C, which is higher than the simple summation of three single metal oxide sorbents. On the basis of the X-ray diffraction (XRD) results, ZnO, MnO2, CuO, and ZnMnO3 served as the active components of Zn-Mn-Cu-based sorbents. ZnMnO3 played a main role in the removal of H2S from hot coal gas. The addition of CuO in the Zn Mn-based sorbent can improve the dispersion degree of active components on support and promote the formation of ZnMnO3, thereby improving the desulfurization capacity of sorbent.