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Desulfurization of hot coal-derived fuel gases with manganese-based regenerable sorbents.

机译：锰基可再生吸附剂对热煤衍生燃料气进行脱硫。

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The focus of much current work being performed by the Morgantown Energy Technology Center (METC) of the Department of Energy on hot coal-derived fuel gas desulfurization is in the use of zinc-based sorbents. Extensive research, however, casts doubt that these sorbents can be utilized even for the mild conditions associated with fixed-bed operation. Accordingly, METC has shown interest in formulating and testing manganese-based pellets as alternative effective sulfur sorbents.; To substantiate the potential superiority of Mn-based pellets, a systematic approach toward the evaluation of the desulfurizing power of single-metal sorbents is developed based on thermodynamic considerations. Then, the feasibility of using Mn- based sorbents for the removal of H{dollar}sb2{dollar}S from hot coal-derived fuel gases, and the subsequent regeneration of loaded sorbents was established.; A novel process is developed for the manufacture of Mn-based spherical pellets which have the desired characteristics required during the long-term use in a high-temperature desulfurization operation. Screening sulfidation tests on a number of formulations were carried out using H{dollar}sb2{dollar}S-H{dollar}sb2{dollar} gas mixtures in a thermogravimetric apparatus (TGA) at temperatures ranging from 700 to 1000{dollar}spcirc{dollar}C. A formulation, designated FORM4-A, was found to possess the best combination of sulfur capacity, reactivity, and strength. Regeneration tests determined that for T {dollar}geq{dollar} 900{dollar}spcirc{dollar}C, loaded pellets can be fully regenerated with air in 10 to 15 minutes. Repeated cycling of FORM4-A pellets was then conducted. One important finding was that the pellet sulfur capacity and the kinetics of reduction, sulfidation, and regeneration reactions improved with recycling without compromising the strength.; Testing of FORM4-A pellet formulation was carried out in a 2-inch fixed-bed reactor using a Tampella-U fuel gas for sulfidation and air for regeneration. These tests also showed improvement in capacity and kinetics with the sulfur capacity being about 22% by weight of the original pellet, which corresponds to approximately 90% bed reactor using a Tampella-U fuel gas for sulfidation and air for regeneration. These tests also showed improvement in capacity and kinetics with the sulfur capacity being about 22% by weight of the original pellet, which corresponds to approximately 90% bed utilization.; Kinetic analysis of TGA experimental data, based on the shrinking unreacted-core model, determined that beyond approximately 35% reaction completion, sulfidation and regeneration reaction rates were controlled primarily by gaseous counter-diffusion through the porous product layer.
机译：能源部的Morgantown能源技术中心（METC）目前正在进行的许多工作的重点是热煤衍生的燃料气体脱硫，主要是使用锌基吸附剂。然而，广泛的研究使人们怀疑这些吸附剂是否可以用于与固定床操作有关的温和条件。因此，METC已显示出对配制和测试锰基颗粒作为替代有效硫吸附剂的兴趣。为了证实锰基颗粒的潜在优势，基于热力学考虑，开发了一种系统的方法来评估单金属吸附剂的脱硫能力。然后，确定了使用Mn基吸附剂从热煤衍生的燃料气体中去除H {sb2s {2} S和随后负载吸附剂的再生的可行性。开发了用于制造Mn基球形粒料的新方法，该Mn基球形粒料具有在高温脱硫操作中长期使用期间所需的所需特性。在热重分析仪（TGA）中使用H {dollar} sb2 {dollar} SH {dollar} sb2 {dollar}气体混合物对多种配方进行了硫化试验筛选，温度范围为700至1000 {dol} }C。发现指定为FORM4-A的配方具有最佳的硫容量，反应性和强度组合。再生测试确定，对于T {dolge} geq {dollar} 900 {dollar} spcirc {dollar} C，负载的颗粒可以在10至15分钟内用空气完全再生。然后进行FORM4-A粒料的重复循环。一个重要的发现是颗粒的硫容量以及还原，硫化和再生反应的动力学随着循环的进行而得到改善，而没有损害强度。 FORM4-A颗粒配方的测试是在2英寸固定床反应器中进行的，使用的是Tampella-U燃料气体进行硫化，而空气则进行再生。这些测试还显示出容量和动力学的改善，其中硫容量为原始粒料的约22％（重量），这相当于使用Tampella-U燃料气体进行硫化和使用空气进行再生的床反应器约为90％。这些试验还显示出容量和动力学的改善，其中硫容量为原始颗粒重量的约22％，相当于床利用率约为90％。 TGA实验数据的动力学分析基于收缩的未反应核模型，确定超过约35％的反应完成率，硫化和再生反应速率主要受通过多孔产物层的气态反扩散控制。

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