Abstract
Both the performance and regenerability of SO2 adsorbents made of CuO supported on SBA-15 ordered mesoporous silica were studied for a cyclic DeSOx process under wet and dry conditions. H2O vapor decreases the performance of a 16 wt% loading CuO/SBA-15 (16CuO/SBA-15) adsorbent along the adsorption/regeneration cycles performed at 400 °C. Indeed, the SO2 breakthrough adsorption capacity of this adsorbent after ten adsorption- regeneration cycles under wet conditions (5 vol% of H2O) decreases of 61% compared to the SO2 performance obtained under dry conditions. The impact of the temperature as well as the CuO loading on the performance and regenerability of CuO/SBA-15 sorbents were also investigated under dry and wet conditions. XRD, TEM/EDX, N2 physisorption characterizations of the adsorbents were performed after the last cycle to correlate the structural and textural properties of the adsorbents and therefore the copper species, with the performance of the adsorbents. Increasing the temperature up to 450 °C with or without water increases the SO2 adsorption capacity of the 16CuO/SBA-15 adsorbent with higher SO2 adsorption capacity at 450 °C with water than without water. In the presence of water vapor, the 8CuO/SBA-15 adsorbent presents the highest average loss of SO2 adsorption capacity at the breakthrough of around 71% when expressed in mgSO2/gCuO, compared to the ones obtained with the 16CuO/SBA-15 and the 26CuO/SBA-15 adsorbents. The increase of the CuO loading up to 26 wt%, shows that the contribution of the surface copper active phase highlighted by the desorption curves, decreases significantly for the highest CuO loading under wet conditions. Moreover, with or without water, the highest total SO2 adsorption capacities obtained after the tenth cycle are observed for the lowest CuO loading (8 wt% of CuO: 547 and 495 mgSO2/gCuO without and with H2O, respectively). These higher total SO2 adsorption capacities could be explained by a better CuO phase dispersion on the SBA-15 support, which makes the copper active species more reactive especially with H2O.
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