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CO_2 Capture from Simulated Fuel Gas Mixtures Using Semiclathrate nHydrates Formed by Quaternary Ammonium Salts

机译:使用季铵盐形成的半水合物n-水合物从模拟的燃气混合物中捕获CO_2

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摘要

In order to investigate the feasibility of semiclathrate hydrate-based precombustion CO_2 capture, thermodynamic, kinetic, and spectroscopic studies were undertaken on the semiclathrate hydrates formed from a fuel gas mixture of H_2 (60%) + CO_2 (40%) in the presence of quaternary ammonium salts (QASs) such as tetra-n-butylammonium bromide (TBAB) and fluoride (TBAF). The inclusion of QASs demonstrated significantly stabilized hydrate dissociation conditions. This effect was greater for TBAF than TBAB. However, due to the presence of dodecahedral cages that are partially filled with water molecules, TBAF showed a relatively lower gas uptake than TBAB. From the stability condition measurements and compositional analyses, it was found that with only one step of semiclathrate hydrate formation with the fuel gas mixture from the IGCC plants, 95% CO_2 can be enriched in the semiclathrate hydrate phase at room temperature. The enclathration of both CO_2 and H_2 in the cages of the QAS semiclathrate hydrates and the structural transition that results from the inclusion of QASs were confirmed through Raman and ~1H NMR measurements. The experimental results obtained in this study provide the physicochemical background required for understanding selective partitioning and distributions of guest gases in the QAS semiclathrate hydrates and for investigating the feasibility of a semiclathrate hydrate-based precombustion CO_2 capture process.
机译:为了研究基于半水合物水合物的预燃烧CO_2捕集的可行性,在存在H2(60%)+ CO_2(40%)的混合气体的情况下,对由H_2(60%)+ CO_2(40%)的混合气体形成的半水合物水合物进行了热力学,动力学和光谱学研究。季铵盐(QAS),例如四正丁基溴化铵(TBAB)和氟化物(TBAF)。包括QASs证明水合物解离条件稳定。 TBAF的效果比TBAB大。但是,由于存在部分充满水分子的十二面体笼,TBAF的气体吸收量比TBAB相对低。通过稳定性条件测量和组成分析,发现仅一步就可以与IGCC工厂的燃料气体混合物一起形成半包合物水合物,在室温下半包合物水合物相中可以富集95%的CO_2。通过拉曼和〜1H NMR测量证实了QAS半包合物水合物笼中CO_2和H_2的包封以及由QAS的包埋引起的结构转变。这项研究中获得的实验结果为理解客气在QAS半水合物水合物中的选择性分配和分布以及研究基于半水合物水合物的预燃烧CO_2捕集过程的可行性提供了理化背景。

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  • 来源
    《Environmental Science & Technology》 |2013年第13期|7571-7577|共7页
  • 作者单位

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology, Ulsan 689-798, Republic of Korea;

    Offshore Plant Resources R&D Center, Korea Institute of Industrial Technology, Busan 618-230, Republic of Korea;

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology, Ulsan 689-798, Republic of Korea;

    School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology, Ulsan 689-798, Republic of Korea;

  • 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);
  • 原文格式 PDF
  • 正文语种 eng
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