Qi Hao, Xu Wenqing, Wang Jian, Tong Li, Zhu Tingyu
Beijing Engineering Research Center of Process Pollution Control, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China; University of Chinese Academy of Sciences, Beijing 100049, China.
Beijing Engineering Research Center of Process Pollution Control, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
J Environ Sci (China). 2015 Feb 1;28:110-7. doi: 10.1016/j.jes.2014.05.050. Epub 2014 Dec 10.
The elemental mercury removal abilities of three different zeolites (NaA, NaX, HZSM-5) impregnated with iron(III) chloride were studied on a lab-scale fixed-bed reactor. X-ray diffraction, nitrogen adsorption porosimetry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and temperature programmed desorption (TPD) analyses were used to investigate the physicochemical properties. Results indicated that the pore structure and active chloride species on the surface of the samples are the key factors for physisorption and oxidation of Hg0, respectively. Relatively high surface area and micropore volume are beneficial to efficient mercury adsorption. The active Cl species generated on the surface of the samples were effective oxidants able to convert elemental mercury (Hg0) into oxidized mercury (Hg2+). The crystallization of NaCl due to the ion exchange effect during the impregnation of NaA and NaX reduced the number of active Cl species on the surface, and restricted the physisorption of Hg0. Therefore, the Hg0 removal efficiencies of the samples were inhibited. The TPD analysis revealed that the species of mercury on the surface of FeCl3-HZSM-5 was mainly in the form of mercuric chloride (HgCl2), while on FeCl3-NaX and FeCl3-NaA it was mainly mercuric oxide (HgO).
在实验室规模的固定床反应器上研究了三种负载氯化铁(III)的不同沸石(NaA、NaX、HZSM-5)对元素汞的去除能力。采用X射线衍射、氮气吸附孔隙率测定、傅里叶变换红外光谱、X射线光电子能谱和程序升温脱附(TPD)分析来研究其物理化学性质。结果表明,样品表面的孔结构和活性氯物种分别是Hg0物理吸附和氧化的关键因素。相对较高的比表面积和微孔体积有利于高效汞吸附。样品表面生成的活性Cl物种是能够将元素汞(Hg0)转化为氧化汞(Hg2+)的有效氧化剂。在NaA和NaX浸渍过程中由于离子交换效应导致的NaCl结晶减少了表面活性Cl物种的数量,并限制了Hg0的物理吸附。因此,样品的Hg0去除效率受到抑制。TPD分析表明,FeCl3-HZSM-5表面汞的物种主要以氯化汞(HgCl2)的形式存在,而在FeCl3-NaX和FeCl3-NaA上主要是氧化汞(HgO)。