Liu Shou-Heng, Yan Nai-Qiang, Liu Zhao-Rong, Qu Zan, Wang H Paul, Chang Shih-Ger, Miller Charles
Environmental Energy Technology Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, California 94720, USA.
Environ Sci Technol. 2007 Feb 15;41(4):1405-12. doi: 10.1021/es061705p.
Bromine gas was evaluated for converting elemental mercury (Hg0) to oxidized mercury, a form that can readily be captured by the existing air pollution control device. The gas-phase oxidation rates of Hg0 by Br2 decreased with increasing temperatures. SO2, CO, HCl, and H2O had insignificant effect, while NO exhibited a reverse course of effect on the Hg0 oxidation: promotion at low NO concentrations and inhibition at high NO concentrations. A reaction mechanism involving the formation of van der Waals clusters is proposed to accountfor NO's reverse effect. The apparent gas-phase oxidation rate constant, obtained under conditions simulating a flue gas without flyash, was 3.61 x 10(-17) cm3 x molecule(-1) x s(-1) at 410 K corresponding to a 50% Hg0 oxidation using 52 ppm Br2 in a reaction time of 15 s. Flyash in flue gas significantly promoted the oxidation of Hg0 by Br2, and the unburned carbon component played a major role in the promotion primarily through the rapid adsorption of Br2 which effectively removed Hg0 from the gas phase. At a typical flue gas temperature, SO2 slightly inhibited the flyash-induced Hg0 removal. Conversely, NO slightly promoted the flyash induced Hg0 removal by Br2. Norit Darco-Hg-LH and Darco-Hg powder activated carbons, which have been demonstrated in field tests, were inferred for estimating the flyash induced Hg0 oxidation by Br2. Approximately 60% of Hg0 is estimated to be oxidized with the addition of 0.4 ppm of gaseous Br2 into full scale power plant flue gas.
对溴气进行了评估,以将元素汞(Hg0)转化为氧化汞,氧化汞这种形式能够很容易地被现有的空气污染控制装置捕获。Hg0被Br2的气相氧化速率随温度升高而降低。SO2、CO、HCl和H2O的影响不显著,而NO对Hg0氧化呈现相反的影响过程:在低NO浓度下促进氧化,在高NO浓度下抑制氧化。提出了一种涉及范德华簇形成的反应机理来解释NO的这种相反影响。在模拟无飞灰烟气的条件下获得的表观气相氧化速率常数,在410K时为3.61×10(-17) cm3×分子(-1)×s(-1),这对应于在15秒的反应时间内使用52ppm Br2时50%的Hg0氧化。烟气中的飞灰显著促进了Br2对Hg0的氧化,未燃碳成分在这种促进作用中起主要作用,主要是通过对Br2的快速吸附,从而有效地从气相中去除Hg0。在典型的烟气温度下,SO2对飞灰诱导的Hg0去除略有抑制作用。相反,NO对飞灰诱导的Br2去除Hg0略有促进作用。推断在现场测试中已得到验证的Norit Darco-Hg-LH和Darco-Hg粉末活性炭可用于估算飞灰诱导的Br2对Hg0的氧化。估计在向全尺寸电厂烟气中添加0.4ppm气态Br2的情况下,约60%的Hg0会被氧化。