Catalytic oxidation of elemental mercury by Mn–Mo/CNT at low temperature

Catalytic oxidation of elemental mercury by Mn–Mo/CNT at low temperature
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Mn·Mo/CNT低温催化氧化单质汞

DOI:
10.1016/j.cej.2015.09.090
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发表时间:
2016-01
影响因子:
15.1
通讯作者:
Minghou Xu
Minghou Xu
中科院分区:
工程技术1区
文献类型:
--
作者:
Bo Zhao;Xiaowei Liu;Zijian Zhou;Haizhong Shao;Minghou Xu

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本文研究了一种新型碳纳米管催化剂对汞的氧化反应。结果表明,在没有HCl存在的情况下,在150~250℃的温度范围内,Mn/CNT能很好地催化O2氧化HgO的过程,即使只有10ppm的HCl存在,该催化剂也能达到很高的汞氧化效率。氧化汞的最佳温度和MnO2含量分别为250℃和5wt%。然而,在500ppm SO2存在下,Mn/CNT几乎失去了氧化汞的能力,因为SO2与催化剂中的MnO2反应生成了硫酸锰。对Mn-Mo/CNT氧化汞的实验表明,SO2对该催化剂的汞氧化有促进作用,其最佳氧化温度降至150℃,这主要是因为Mo能促进SO2转化为SO3,有利于汞的氧化,同时Mo还能保护MnO2在催化剂上的催化活性。长期的实验表明,Mn-Mo/CNT是一种有效的低温汞氧化催化剂,而HCl在Mn-Mo/CNT上氧化HgO遵循的是朗缪尔-辛谢尔伍德机理。
Mercury oxidized by a type of novel carbon nanotube catalyst was studied in this work. The results of this suggest that in the absence of HCl, Mn/CNT could perfectly catalytic the process of O2oxidizing Hg0at 150–250 °C, and even with only 10 ppm HCl present, this catalyst could attain a high mercury oxidation efficiency. The optimal temperature and MnO2content for mercury oxidation was 250 °C and 5 wt%. However, Mn/CNT almost lost the ability to oxidize mercury in the presence of 500 ppm SO2because SO2reacted with MnO2in the catalyst to form manganese sulfate. Tests of mercury oxidized by Mn–Mo/CNT indicated that SO2could enhance mercury oxidation by this catalyst and that the optimal temperature for mercury oxidized by Mn–Mo/CNT decreased to 150 °C mainly because Mo was able to promote the transformation of SO2to SO3,which is beneficial for mercury oxidation, and Mo was also able protect the catalytic activation of MnO2on the catalyst. Tests over a long period of time showed that Mn–Mo/CNT was an effective available low temperature catalyst for mercury oxidation and that Hg0oxidized by HCl over Mn–Mo/CNT follows the Langmuir–Hinshelwood mechanism.
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