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CeO2-TiO2 吸附剂用于从合成气中去除元素汞。

CeO2-TiO2 sorbents for the removal of elemental mercury from syngas.

机构信息

State Key Laboratory of Clean Energy Utilization, Zhejiang University , Hangzhou 310027, People's Republic of China.

出版信息

Environ Sci Technol. 2013 Sep 3;47(17):10056-62. doi: 10.1021/es401681y. Epub 2013 Aug 21.

Abstract

A series of CeO2-TiO2 (CeTi) sorbents with different CeO2/TiO2 mass ratios were prepared by an impregnation method and employed to remove elemental mercury (Hg(0)) in simulated syngas. The CeTi sorbents with a CeO2/TiO2 mass ratio of 0.2 exhibited superior Hg(0) removal efficiency from 80 to 150 °C, which could be ascribed to the greater amount of surface chemisorbed oxygen resulted from Ce(3+) on the sample surface. H2S was the most effective syngas component responsible for Hg(0) removal. The use of 400 ppm H2S resulted in 98% Hg(0) removal efficiency under the experimental conditions. H2 and CO had a negligible effect on the efficiency of Hg removal. In the presence of H2S, a prohibitive effect of HCl and NH3 on Hg(0) removal was observed because of the consumption of the surface oxygen. Water vapor also inhibited Hg(0) removal due to competitive adsorption with H2S. Hg(0) removal over CeTi sorbents was proposed to follow the Eley-Rideal mechanism, in which active surface sulfur reacts with gas-phase Hg(0). This large oxygen storage capacity of CeTi sorbents is quite favorable to H2S catalytic oxidation and Hg(0) emission control in an extremely reducing environment, such as when there is a deficiency of O2.

摘要

一系列不同 CeO2/TiO2 质量比的 CeO2-TiO2(CeTi)吸附剂通过浸渍法制备,并用于去除模拟合成气中的元素汞(Hg(0))。CeO2/TiO2 质量比为 0.2 的 CeTi 吸附剂在 80 至 150°C 之间表现出优异的 Hg(0)去除效率,这可归因于样品表面 Ce(3+) 导致的表面化学吸附氧的增加。H2S 是去除 Hg(0)最有效的合成气组分。在实验条件下,使用 400 ppm H2S 可实现 98%的 Hg(0)去除效率。H2 和 CO 对 Hg 去除效率的影响可以忽略不计。在 H2S 存在下,HCl 和 NH3 的消耗导致表面氧的减少,对 Hg(0)去除具有抑制作用。水蒸气也由于与 H2S 的竞争吸附而抑制 Hg(0)的去除。CeTi 吸附剂上的 Hg(0)去除被提出遵循 Eley-Rideal 机制,其中活性表面硫与气相 Hg(0)反应。CeTi 吸附剂的这种大的储氧能力对于在极度还原环境(例如当 O2 不足时)中进行 H2S 催化氧化和 Hg(0)排放控制非常有利。

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