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Ce-Mn Oxides for High-Temperature Gasifier Effluent Desulfurization

机译：高温气化炉废水脱硫用铈锰氧化物

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摘要

We examined Ce-Mn mixed oxides as high-temperature desulfurization materials, exploring various Mn/Ce ratios and the effects of admixing other rare earth oxides. The sulfur capacities at temperatures from 900 to 1025 K with simple air regeneration were measured for repeat cycles until a stable, reversible capacity was obtained. The measured sulfur capacities with a realistic model syngas containing H_2S, H_2, N_2, CO, H_2O, and CO_2 were compared to thermodynamically possible maximum sulfur capacities. The oxidized and sulfided (reduced) sorbents were characterized by X-ray diffraction (XRD), X-ray absorption near-edge spectroscopy (XANES), X-ray absorption fine structure (XAFS), temperature-programmed reduction (TPR), and Brunauer-Emmett-Teller (BET) surface area. Density functional theory calculations are used to aid in interpreting characterization data and in explaining the enhanced S adsorption capacities. There is a large synergistic effect on sulfur adsorption and reaction resulting from the intimate admixing of Mn with CeO_2 and CeO_2/La_2O_3 rare earth oxides. However, while these materials are stable at temperatures near 900 K, even using air regeneration, the observed stable sulfur capacities fall far short of predictions based on thermodynamic equilibrium. The differences are attributed to (a) inhibition by CO_2 and H_2O; (b) formation of some irreversible sulfates upon air regeneration; (c) inability of sulfur to diffuse into larger, sintered crystals of the mixed oxides; (d) gradual dissolution of Mn in an underlying support such as Al_2O_3 (when present).
机译：我们研究了作为高温脱硫材料的Ce-Mn混合氧化物，探索了各种Mn / Ce比以及混合其他稀土氧化物的效果。对900到1025 K的温度下具有简单的空气再生的硫容量进行重复循环测量，直到获得稳定的可逆容量。将包含H_2S，H_2，N_2，CO，H_2O和CO_2的实际模型合成气的测得硫容量与热力学上可能的最大硫容量进行了比较。氧化和硫化（还原）的吸附剂通过X射线衍射（XRD），X射线吸收近边缘光谱（XANES），X射线吸收精细结构（XAFS），程序升温还原（TPR）和Brunauer-Emmett-Teller（BET）表面积。密度泛函理论计算可用于解释特征数据和解释增强的S吸附能力。 Mn与CeO_2和CeO_2 / La_2O_3稀土氧化物的紧密混合，对硫的吸附和反应具有较大的协同作用。然而，尽管这些材料即使在使用空气再生的情况下也能在900 K左右的温度下保持稳定，但观察到的稳定硫容量远低于基于热力学平衡的预测值。差异归因于（a）被CO_2和H_2O抑制； （b）在空气再生时形成一些不可逆的硫酸盐； （c）硫不能扩散到混合氧化物的较大的烧结晶体中； （d）将Mn逐渐溶解在基础载体如Al_2O_3中（如果存在）。

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  • 来源
    《Energy & fuels》 |2012年第novaadeca期|6765-6776|共12页
  • 作者

    Rui Li; Matthew D. Krcha; Michael J. Janik; Amitava D. Roy; Kerry M. Dooley;

  • 作者单位

    Department of Chemical Engineering, Louisiana State University, Baton Rouge, Louisiana 70803, United States;

    Department of Chemical Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, United States;

    Department of Chemical Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, United States;

    Center for Advanced Microstructures & Devices, Louisiana State University, 6980 Jefferson Highway, Baton Rouge, Louisiana 70806, United States;

    Department of Chemical Engineering, Louisiana State University, Baton Rouge, Louisiana 70803, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
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