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Novel Effective Catalyst for Elemental Mercury Removal from Coal-Fired Flue Gas and the Mechanism Investigation

机译：新型有效去除燃煤烟气中汞的催化剂及其机理研究

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摘要

Mercury pollution from coal-fired power plants has drawn attention worldwide. To achieve efficient catalytic oxidation of Hg~0 at both high and low temperatures, we prepared and tested novel IrO_2 modified Ce-Zr solid solution catalysts under various conditions. It was found that the IrO_2/ Ce_(0.6)Zr_(0.4)O_2 catalyst, which was prepared using the poly-vinylpyrrolidone-assisted sol-gel method, displayed significantly higher catalytic activity for Hg~0 oxidation. The mechanism of Hg~0 removal over IrO_2/Ce_(0.6)Zr_(0.4)O_2 was studied using various methods, and the Hg~0 oxidation reaction was found to follow two possible pathways. For the new chemisorption-regeneration mechanism proposed in this study, the adsorbed Hg~0 was first oxidized with surface chemisorbed oxygen species to form HgO; the HgO could desorb from the surface of catalysts by itself or react with adsorbed HCl to be release in the form of gaseous HgCl_2. O_2 is indispensable for the chemisorption process, and the doping of IrO_2 could facilitate the chemisorption process. In addition, the Deacon reaction mechanism was also feasible for Hg~0 oxidation: this reaction would involve first oxidizing the adsorbed HCl to active Cl species, after which the Hg~0 could react with Cl to form HgCl_2. Additionally, doping IrO_2 could significantly improve the Cl yield process. In summary, the novel IrO_2 modified catalyst displayed excellent catalytic activity for elemental mercury oxidation, and the proposed reaction mechanisms were determined reasonably.
机译：燃煤电厂的汞污染引起了全世界的关注。为了在高温和低温下都能有效地催化Hg〜0的氧化，我们在各种条件下制备并测试了新型IrO_2改性的Ce-Zr固溶体催化剂。结果表明，采用聚乙烯吡咯烷酮辅助溶胶-凝胶法制备的IrO_2 / Ce_（0.6）Zr_（0.4）O_2催化剂对Hg〜0的催化活性显着提高。采用多种方法研究了IrO_2 / Ce_（0.6）Zr_（0.4）O_2上Hg〜0的去除机理，发现Hg〜0的氧化反应遵循两种可能的途径。对于这项研究提出的新的化学吸附-再生机理，首先将吸附的Hg〜0用表面化学吸附的氧物种氧化形成HgO。 HgO本身可从催化剂表面脱附或与吸附的HCl反应，以气态HgCl_2的形式释放。 O_2对于化学吸附过程是必不可少的，IrO_2的掺杂可以促进化学吸附过程。此外，Deacon反应机理对于Hg〜0的氧化也是可行的：该反应将首先将吸附的HCl氧化成活性Cl，然后Hg〜0可以与Cl反应形成HgCl_2。此外，掺杂IrO_2可以显着改善Cl的生成过程。综上所述，新型的IrO_2改性催化剂对元素汞氧化反应具有优异的催化活性，并合理确定了所提出的反应机理。

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  • 来源
    《Environmental Science & Technology》 |2016年第5期|2564-2572|共9页
  • 作者

    Wanmiao Chen; Yang Pei; Wenjun Huang; Zan Qu; Xiaofang Hu; Naiqiang Yan;

  • 作者单位

    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai, 200240 PR China;

    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai, 200240 PR China;

    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai, 200240 PR China;

    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai, 200240 PR China;

    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai, 200240 PR China;

    School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai, 200240 PR China;

  • 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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