CaO对汞的选择性吸附及SO2毒化特性

doi:10.11949/j.issn.0438-1157.20170343

化工学报 ›› 2017, Vol. 68 ›› Issue (9): 3565-3572.DOI: 10.11949/j.issn.0438-1157.20170343

CaO对汞的选择性吸附及SO₂毒化特性

李春峰, 段钰锋, 汤红健, 朱纯, 郑逸武, 韦红旗

东南大学能源与环境学院, 能源热转换及其过程测控教育部重点实验室, 江苏南京 210096

收稿日期:2017-04-01 修回日期:2017-05-27 出版日期:2017-09-05 发布日期:2017-09-05
通讯作者: 段钰锋
基金资助:
国家重点研发计划项目（2016YFC0201105）；国家自然科学基金项目（51576044，51676041）。

Mercury selective adsorption characteristics and SO₂ poison performance on CaO

LI Chunfeng, DUAN Yufeng, TANG Hongjian, ZHU Chun, ZHENG Yiwu, WEI Hongqi

Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, Jiangsu, China

Received:2017-04-01 Revised:2017-05-27 Online:2017-09-05 Published:2017-09-05
Contact: 10.11949/j.issn.0438-1157.20170343
Supported by:
supported by the National Key R&D Program of China (2016YFC0201105) and the National Natural Science Foundation of China (51576044,51676041).

摘要/Abstract

摘要：

利用Ca（NO₃）₂作为前体，SiO₂为载体，制备了一种担载型CaO吸附剂，在固定床实验装置上分别研究了该吸附剂对元素汞（Hg⁰）和氯化汞（HgCl₂）等不同形态汞的选择性吸附性能，以及SO₂对CaO吸附剂汞形态吸附过程的影响，同时结合程序升温脱附和原位红外漫反射表征技术，深入探究了CaO的选择性吸附机理及SO₂毒化机制。汞形态吸附实验结果表明，在纯N₂气氛和掺杂SO₂气氛下，CaO对Hg⁰均保持了接近100%的穿透率，而对HgCl₂在两种气氛下则分别表现出66.0%和60.3%的吸附效率，说明SO₂与HgCl₂在CaO表面存在竞争吸附关系；吸附实验前后CaO的表征结果显示，与Hg⁰相比，HgCl₂更易与CaO表面各碱性位形成单配位、双配位等多种吸附构型，SO₂与HgCl₂在易形成单配位的活性位上形成竞争吸附关系，进而在一定程度上降低了CaO对HgCl₂的吸附效率。

关键词: CaO吸附剂, Hg, HgCl₂, 选择性吸附, SO₂毒化

Abstract:

Using Ca(NO₃)₂ as a precursor and SiO₂ as carrier, a supported CaO adsorbent was prepared. The selective adsorption performances of elemental mercury (Hg⁰) and mercuric chloride (HgCl₂) of the sorbent were conducted in a fixed bed, and the effects of SO₂ on CaO mercury adsorption process were also investigated. At the same time, combined with the program temperature desorption (TPD) and in situ diffuse reflectance infrared spectroscopy (in-situ DRIFT) characterization technology, the selective adsorption mechanism of CaO and the mechanism of SO₂ poisoning were deeply investigated. The mercury adsorption results showed that CaO maintained a breakthrough of nearly 100% for Hg⁰ in pure N₂ atmosphere and doped SO₂ atmosphere, while HgCl₂ manifested 66.0% and 60.3% adsorption efficiency in two atmospheres, respectively, indicating that there was a competitive adsorption relationship between SO₂ and HgCl₂ on CaO surface. The characterized results of CaO before and after adsorption suggested that as compared with Hg⁰, HgCl₂ was able to form monodentate, bidentate and other adsorption structure with the basic sites on the CaO surface. SO₂ and HgCl₂ formed a competitive adsorption relationship in the active sites where the bridged bidentate was easily formed, resulting in the reduction of adsorption efficiency of HgCl₂ on CaO.

Key words: CaO adsorbents, elemental mercury, mercuric chloride, selective adsorption, sulfur poisoning

中图分类号:

X511

李春峰, 段钰锋, 汤红健, 朱纯, 郑逸武, 韦红旗. CaO对汞的选择性吸附及SO₂毒化特性[J]. 化工学报, 2017, 68(9): 3565-3572.

LI Chunfeng, DUAN Yufeng, TANG Hongjian, ZHU Chun, ZHENG Yiwu, WEI Hongqi. Mercury selective adsorption characteristics and SO₂ poison performance on CaO[J]. CIESC Journal, 2017, 68(9): 3565-3572.

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CaO对汞的选择性吸附及SO₂毒化特性

Mercury selective adsorption characteristics and SO₂ poison performance on CaO

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