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用于高温煤气脱硫的高稳定性和可再生 Mn 基/SBA-15 吸附剂。

Highly stable and regenerable Mn-based/SBA-15 sorbents for desulfurization of hot coal gas.

机构信息

Department of Chemistry, Tianjin University, Tianjin, PR China.

出版信息

J Hazard Mater. 2012 Sep 30;233-234:219-27. doi: 10.1016/j.jhazmat.2012.07.023. Epub 2012 Jul 14.

Abstract

A series of mesoporous xCuyMn/SBA-15 sorbents with different Cu/Mn atomic ratios were prepared by wet impregnation method and their desulfurization performance in hot coal gas was investigated in a fixed-bed quartz reactor in the range of 700-850°C. The successive nine desulfurization-regeneration cycles at 800°C revealed that 1Cu9Mn/SBA-15 presented high performance with durable regeneration ability due to the high dispersion of Mn(2)O(3) particles incorporated with a certain amount of copper oxides. The breakthrough sulfur capacity of 1Cu9Mn/SBA-15 observed 800°C is 13.8 g S/100g sorbents, which is remarkably higher than these of 40 wt%LaFeO(3)/SBA-15 (4.8 g S/100g sorbents) and 50 wt%LaFe(2)O(x)/MCM-41 (5.58 g S/100g sorbents) used only at 500-550°C. This suggested that the loading of Mn(2)O(3) active species with high thermal stability to SBA-15 support significantly increased sulfur capacity at relatively higher sulfidation temperature. The fresh and used xCuyMn/SBA-15 sorbents were characterized by means of BET, XRD, XPS, XAES, TG/DSC and HRTEM techniques, confirmed that the structure of the sorbents remained intact before and after hot coal gas desulfurization.

摘要

一系列具有不同 Cu/Mn 原子比的介孔 xCuyMn/SBA-15 吸附剂通过浸渍法制备,并在固定床石英反应器中于 700-850°C 范围内考察了它们在热煤气中的脱硫性能。在 800°C 下进行了连续九次脱硫-再生循环,结果表明 1Cu9Mn/SBA-15 由于 Mn(2)O(3)颗粒的高分散性以及与一定量的铜氧化物结合,表现出高脱硫性能和持久的再生能力。在 800°C 下观察到 1Cu9Mn/SBA-15 的穿透硫容量为 13.8 g S/100g 吸附剂,明显高于仅在 500-550°C 下使用的 40wt%LaFeO(3)/SBA-15(4.8 g S/100g 吸附剂)和 50wt%LaFe(2)O(x)/MCM-41(5.58 g S/100g 吸附剂)。这表明将具有高热稳定性的 Mn(2)O(3)活性物质负载到 SBA-15 载体上,显著提高了相对较高硫化温度下的硫容量。采用 BET、XRD、XPS、XAES、TG/DSC 和 HRTEM 技术对新鲜和使用过的 xCuyMn/SBA-15 吸附剂进行了表征,证实了吸附剂在热煤气脱硫前后的结构保持完整。

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