化工进展

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类水滑石衍生锌基复合氧化物的硫化再生行为

李俏春1,郭恩惠1,李阳2,米杰2,武蒙蒙2   

  1. 1. 太原理工大学
    2. 太原理工大学煤科学与技术教育部和山西省重点实验室
  • 收稿日期:2020-12-01 修回日期:2021-01-16 发布日期:2021-03-02
  • 通讯作者: 武蒙蒙
  • 基金资助:
    国家自然科学基金青年科学基金

Desulfurization and regeneration behaviors of zinc-based composite oxides derived from hydrotalcite

  • Received:2020-12-01 Revised:2021-01-16 Published:2021-03-02

摘要: 通过共沉淀法合成了具有片状堆积结构的类水滑石衍生锌基(钴或镍掺杂)复合金属氧化物,并将其用于中高温煤气脱硫。采用X射线衍射(XRD)、扫描电子显微镜(SEM)分析了脱硫剂及其前驱体的物相组成与形貌织构,发现镍(或钴)掺杂后脱硫剂的主要晶相仍为具有六方纤锌矿结构的氧化锌,且镍(或钴)的引入并未明显改变锌铝复合氧化物及其类水滑石前驱体的形貌结构。在固定床评价装置上研究了脱硫剂的硫化与再生行为,研究表明,锌镍(或钴)摩尔比为20时对应的掺杂型脱硫剂穿透时间最长(324min)、硫容最高(25.4%)。与未掺杂脱硫剂相比,掺杂镍(或钴)的脱硫剂最佳再生温度降低60℃左右。引入镍(或钴)后,脱硫剂不仅在多次硫化再生循环过程中维持高硫容,而且仍具有片状结构,硫化再生循环稳定性显著增强。

关键词: 热煤气, 硫化氢, 类水滑石, 吸附, 氧化锌脱硫剂

Abstract: A zinc-based (cobalt or nickel doped) composite metal oxide derived from a hydrotalcite-like structure with a sheet-like stacked structure was synthesized by the co-precipitation method and used for medium and high temperature gas desulfurization. X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to analyze the phase composition and morphology of the sorbents and their precursors. It is found that the main crystal phase of the desulfurizer with nickel (or cobalt) doping is still zinc oxide with hexagonal wurtzite structure, and the introduction of nickel (or cobalt) does not significantly change morphology structure of the zinc-aluminum composite oxide and its precursor. The vulcanization and regeneration behavior of the desulfurizer was studied on the fixed bed evaluation device. The results shows that when the molar ratio of zinc to nickel (or cobalt) is 20, the corresponding doped desulfurizer has the longest breakthrough time (324min) and the highest sulfur capacity (25.4%). Compared with the undoped desulfurizer, the optimal regeneration temperature of the sorbent doped with nickel (or cobalt) is reduced by about 60℃. After the introduction of nickel (or cobalt), the desulfurizer not only maintains a high sulfur capacity during multiple desulfurization-regeneration cycles, but also has a sheet-like structure, indicating enhanced desulfurization-regeneration stability of sorbents.

Key words: hot coal gas, hydrogen sulfide, hydrotalcite-like compounds, adsorption, zinc oxide sorbent

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