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铈掺杂 Mn/SAPO-34 催化剂上汞的催化转化:抗硫性和 SO/SO 转化。

Catalytic conversion of mercury over Ce doped Mn/SAPO-34 catalyst: Sulphur tolerance and SO/SO conversion.

机构信息

Key Laboratory of Condition Monitoring and Control for Power Plant Equipment, Ministry of Education, North China Electric Power University, Beijing 102206, China.

Key Laboratory of Condition Monitoring and Control for Power Plant Equipment, Ministry of Education, North China Electric Power University, Beijing 102206, China.

出版信息

J Hazard Mater. 2020 Jan 5;381:120986. doi: 10.1016/j.jhazmat.2019.120986. Epub 2019 Aug 10.

Abstract

A series of Mn-Ce/SAPO-34 catalysts were prepared to study the catalytic oxidisation of elemental mercury (Hg). Sulphur tolerance and SO formation over the catalyst were studied further. Hg was transported by compressed air from PSA Cavkit. NO, SO, and NH are standard gases, and HO is produced by gas carrying. Mn could incorporate into the cerium oxide lattice to form capping oxygen and well-dispersed high valance manganese ions after the addition of Ce, which was conducive to NO removal and Hg oxidisation. 9 Mn-9Ce showed the best performance regarding Hg conversion, achieving more than 92% Hg conversion efficiency at 50-300 °C. The sulphur resistance of the Mn-based catalyst was significantly improved after the addition of cerium due to the high affinity of Ce for SO, and the relative content of HgSO was exceeded 72% on the 9 Mn-9Ce catalyst with SO; SO formation over the 9 Mn-9Ce decreased by 17% compared with the 9 Mn. HO not only reduced the available active site, but also decreased the oxidation rate of SO. The active sites were preferentially occupied by NH rather than Hg and SO, generated NH occupied cation vacancies. Therefore, both HO and NH have inhibitory effects on Hg conversion and SO formation.

摘要

一系列 Mn-Ce/SAPO-34 催化剂被制备用于研究元素汞 (Hg) 的催化氧化。进一步研究了催化剂上的耐硫性和 SO 生成。Hg 由压缩空气从 PSA Cavkit 输送。NO、SO 和 NH 是标准气体,HO 通过气体携带生成。添加 Ce 后,Mn 可以掺入氧化铈晶格中,形成盖帽氧和高度分散的高价锰离子,这有利于 NO 去除和 Hg 氧化。9Mn-9Ce 在 Hg 转化率方面表现出最佳性能,在 50-300°C 下实现了超过 92%的 Hg 转化率效率。由于 Ce 对 SO 的高亲和力,Mn 基催化剂的硫抗性在添加 Ce 后得到显著提高,在含有 SO 的 9Mn-9Ce 催化剂上,HgSO 的相对含量超过 72%;与 9Mn 相比,9Mn-9Ce 上的 SO 生成减少了 17%。HO 不仅减少了可用的活性位,还降低了 SO 的氧化速率。活性位优先被 NH 而不是 Hg 和 SO 占据,生成的 NH 占据阳离子空位。因此,HO 和 NH 都对 Hg 转化率和 SO 生成有抑制作用。

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