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在低温下,烟气成分在 TiO2 负载的 MnOx-CeO2 混合氧化物上促进汞氧化的作用。

Role of flue gas components in mercury oxidation over TiO2 supported MnOx-CeO2 mixed-oxide at low temperature.

机构信息

School of Energy Science and Engineering, Central South University, Changsha, Hunan, 410083, China.

出版信息

J Hazard Mater. 2012 Dec;243:117-23. doi: 10.1016/j.jhazmat.2012.10.007. Epub 2012 Oct 13.

Abstract

MnO(x)-CeO(2) mixed-oxide supported on TiO(2) (Mn-Ce/Ti) was synthesized by an ultrasound-assisted impregnation method and employed to oxidize elemental mercury (Hg(0)) at 200°C in simulated coal combustion flue gas. Over 90% of Hg(0) oxidation was achieved on the Mn-Ce/Ti catalyst at 200°C under simulated flue gas representing those from burning low-rank coals with a high gas hourly space velocity of 60,000 h(-1). Gas-phase O(2) regenerated the lattice oxygen and replenished the chemisorbed oxygen, which facilitated Hg(0) oxidation. HCl was the most effective flue gas component responsible for Hg(0) oxidation. 10 ppm HCl plus 4% O(2) resulted in 100% Hg(0) oxidation under the experimental conditions. SO(2) competed with Hg(0) for active sites, thus deactivating the catalyst's capability in oxidizing Hg(0). NO covered the active sites and consumed surface oxygen active for Hg(0) oxidation, hence limiting Hg(0) oxidation. Water vapor showed prohibitive effect on Hg(0) oxidation due to its competition with HCl and Hg(0) for active adsorption sites. This study provides information about the promotional or inhibitory effects of individual flue gas components on Hg(0) oxidation over a highly effective Mn-Ce/Ti catalyst. Such knowledge is of fundamental importance for industrial applications of the Mn-Ce/Ti catalyst in coal-fired power plants.

摘要

MnO(x)-CeO(2) 负载在 TiO(2)上的混合氧化物(Mn-Ce/Ti)通过超声辅助浸渍法合成,并用于在模拟煤燃烧烟气中于 200°C 氧化元素汞(Hg(0))。在模拟烟气中,Mn-Ce/Ti 催化剂在 200°C 下,在高气体时空速度为 60000 h(-1)的情况下,燃烧低阶煤时,Hg(0)的氧化率超过 90%。气相 O(2)再生晶格氧并补充化学吸附氧,这有利于 Hg(0)氧化。HCl 是最有效的烟气成分,负责 Hg(0)氧化。在实验条件下,10 ppm HCl 加 4% O(2)导致 100% Hg(0)氧化。SO(2)与 Hg(0)竞争活性位,从而使催化剂氧化 Hg(0)的能力失活。NO 覆盖活性位并消耗表面氧,从而限制 Hg(0)氧化。水蒸气由于与 HCl 和 Hg(0)竞争活性吸附位,对 Hg(0)氧化表现出抑制作用。本研究提供了关于单个烟气成分对高效 Mn-Ce/Ti 催化剂上 Hg(0)氧化的促进或抑制作用的信息。这种知识对于 Mn-Ce/Ti 催化剂在燃煤电厂中的工业应用具有重要意义。

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