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Supported Polytertiary Amines: Highly Efficient and Selective SO_2 Adsorbents

机译：支持的多胺：高效且选择性的SO_2吸附剂

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Tertiary amine containing poly(propyleneimine) second (G2) and third (G3) generation dendrimers as well as polyethyleneimine (PEI) were developed for the selective removal of SO_2. N-Alkylation of primary and secondary amines into tertiary amines was confirmed by FTIR and NMR analysis. Such modified polyamines were impregnated on two nanoporous supports, namely, SBA-15PL silica with platelet morphology and ethanol-extracted pore-expanded MCM-41 (PME) composite. In the presence of 0.1% SO_2/N_2 at 23 ℃, the uptake of modified PEI, G2, and G3 supported on SBA-15PL was 2.07, 2.35, and 1.71 mmol/g, respectively; corresponding to SO_2/N ratios of 0.22, 0.4, and 0.3. Under the same conditions, the SO_2 adsorption capacity of PME-supported modified PEI and G3 was significantly higher, reaching 4.68 and 4.34 mmol/g, corresponding to SO_2/N ratios of 0.41 and 0.82, respectively. The working SO_2 adsorption capacity decreased with increasing temperature, reflecting the exothermic nature of the process. The adsorption capacity of these materials was enhanced dramatically in the presence of humidity in the gas mixture. FTIR data before SO_2 adsorption and after adsorption and regeneration did not indicate any change in the materials. Nonetheless, the SO_2 working capacity decreased in consecutive adsorption/regeneration cycles due to evaporation of impregnated polyamines, rather than actual deactivation. FTIR and ~(13)C and ~(15)N CP-MAS NMR of fresh and SO_2 adsorbed modified G3 on PME confirmed the formation of a complexation adduct.
机译：开发了含叔胺的聚（丙烯亚胺）第二（G2）和第三（G3）树状大分子以及聚乙烯亚胺（PEI），用于选择性去除SO_2。通过FTIR和NMR分析证实伯胺和仲胺的N-烷基化为叔胺。将这种改性的多胺浸渍在两个纳米多孔载体上，即具有血小板形态的SBA-15PL二氧化硅和乙醇提取的扩孔MCM-41（PME）复合材料。在23℃下，在0.1％SO_2 / N_2存在下，负载在SBA-15PL上的改性PEI，G2和G3的吸收分别为2.07、2.35和1.71 mmol / g。对应于SO_2 / N比为0.22、0.4和0.3。在相同条件下，PME负载的改性PEI和G3的SO_2吸附能力显着提高，分别达到4.68和4.34 mmol / g，分别对应于SO_2 / N比为0.41和0.82。随着温度的升高，工作SO_2的吸附能力降低，反映了该过程的放热性质。在混合气体中存在湿气的情况下，这些材料的吸附能力显着提高。 SO_2吸附之前以及吸附和再生之后的FTIR数据未表明材料的任何变化。然而，由于浸渍的多胺的蒸发而不是实际的失活，在连续的吸附/再生循环中SO_2的工作能力降低了。在PME上新鲜和SO_2吸附的改性G3的FTIR和〜（13）C和〜（15）N CP-MAS NMR证实了络合物加合物的形成。

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  • 来源
    《Environmental Science & Technology》 |2014年第3期|2025-2034|共10页
  • 作者

    Ritesh Tailor; Mohamed Abboud; Abdelhamid Sayari;

  • 作者单位

    Department of Chemistry, Centre for Catalysis Research and Innovation (CCRI), University of Ottawa, Ottawa, Ontario, Canada K1N 6N5;

    Department of Chemistry, Centre for Catalysis Research and Innovation (CCRI), University of Ottawa, Ottawa, Ontario, Canada K1N 6N5;

    Department of Chemistry, Centre for Catalysis Research and Innovation (CCRI), University of Ottawa, Ottawa, Ontario, Canada K1N 6N5;

  • 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);美国《化学文摘》(CA);
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