烟气
焚化
催化作用
化学
氯
化学工程
脱氢
Mercury(编程语言)
无机化学
氧化物
环境化学
氧气
离解(化学)
烟道
汞元素
废物管理
活化能
多相催化
密度泛函理论
卤化物
催化氧化
城市固体废物
合成气
作者
Hongyuan Qi,Yurui Fan,Yongpeng Ma,Mingze Jiao,Wuwen Luo,Liang Shan,Zhisong Liu,Qinyuan Hong,Wenjun Huang,Zan Qu,Naiqiang Yan,Haomiao Xu
标识
DOI:10.1021/acs.est.6c04609
摘要
Municipal solid waste incineration (MSWI) is an important anthropogenic source of elemental mercury (Hg 0 ) emissions. In MSWI flue gas treatment, achieving efficient Hg 0 oxidation relies on the active participation of HCl under typical downstream operating conditions (<200 °C). However, the activation of HCl remains a formidable challenge at low temperatures. Herein, we rationally design a perovskite oxide catalyst featuring Ru–O–Mn coordinated active sites to promote HCl activation via a low-temperature Deacon-like pathway, enabling efficient in situ Cl* generation for Hg 0 oxidation. The optimized catalyst achieves over 99% conversion of Hg 0 to Hg 2+ at 150 °C. Combined experimental characterization with density functional theory (DFT) calculations demonstrates that Ru incorporation markedly enhances O 2 dissociation at the Ru–O–Mn interfacial sites and substantially lowers the energy barrier for HCl dehydrogenation by 0.52 eV, thereby promoting Cl* formation. The generated Cl* species further interact with surface oxygen (O*) to form highly reactive ClO x intermediates, which facilitate HgCl 2 formation and significantly improve Hg 0 oxidation efficiency. This work provides fundamental insights into low-temperature HCl activation and offers a promising strategy for mercury abatement in incineration flue gas.
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