KCl Supported by γ-Al2O3 for Selective Adsorption of Gaseous Oxidized Mercury: Flue Gas Influence and Application

IF 1.6 4区 工程技术 Q3 ENGINEERING, CHEMICAL
Jiangyi Tong, Haiyang Li, Rui Jin, Xiaoshuo Liu, Haitao Hu, Yufeng Duan, Xiuyuan Ma, Li Zhong, Lipeng Han
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Abstract

The KCl supported by γ-Al2O3 for selective adsorption of gaseous HgCl2 has demonstrated high selectivity and adsorption capacity, which is crucial for mercury speciation partitioning from flue gas. However, its influence and stability in complex flue gas remains uncertain. Therefore, this paper explores the impact of common flue gas components (HCl, SO2, H2O, CO2, NO, O2) on the adsorption process and elucidates the underlying mechanisms from experiment and DFT view. The experimental results demonstrate that the HgCl2 breakthrough rate increases significantly from 2.119% to 17.921% as the concentration of HCl rises from 0 to 200 ppm. Comparatively, the HgCl2 breakthrough rate affected by SO2 and H2O is less than 8%, weakly reducing the adsorption efficiency of HgCl2, and that by CO2, NO, and O2 is less than 5%, showing negligible effects on the HgCl2 adsorption efficiency. The DFT indicates that HCl competes with HgCl2 at the Top-Cl site in KCl, thereby reducing the adsorption efficiency of HgCl2, with the adsorption energy decreasing from −87.11 to −43.39 kJ/mol. In contrast, SO2 and H2O exhibit relatively weak interactions with Top-Cl site of KCl, which exerts little influence on HgCl2 adsorption. The 100-h running in low-concentration simulated flue gas test in laboratory and on-site test in coal-fired flue gas demonstrate that the KCl/γ-Al2O3 achieves a very low HgCl2 breakthrough rate of less than 10%, highlighting its superior interference immunity for the complex flue gas components and strong suitability and stability for industrial applications. This study provides solid evidence to support the industrial application of KCl/γ-Al2O3 for highly selective adsorption of gaseous HgCl2 in coal-fired power plant.

γ-Al2O3负载KCl选择性吸附气态氧化汞:烟气影响及应用
γ-Al2O3负载的KCl对气态HgCl2的选择性吸附表现出较高的选择性和吸附能力,这对烟气中汞的形态分配至关重要。然而,其在复杂烟气中的影响和稳定性仍不确定。因此,本文探讨了常见烟气组分(HCl, SO2, H2O, CO2, NO, O2)对吸附过程的影响,并从实验和DFT角度阐明了其潜在机制。实验结果表明,当HCl浓度从0增加到200 ppm时,HgCl2的突破率从2.119%显著增加到17.921%。相比之下,SO2和H2O对HgCl2的突破率影响小于8%,对HgCl2的吸附效率降低较弱;CO2、NO和O2对HgCl2的突破率影响小于5%,对HgCl2的吸附效率影响可以忽略不计。DFT表明,HCl与HgCl2在KCl的Top-Cl位发生竞争,从而降低了HgCl2的吸附效率,吸附能从−87.11 kJ/mol下降到−43.39 kJ/mol。SO2和H2O与KCl的Top-Cl位点的相互作用相对较弱,对HgCl2的吸附影响较小。实验室低浓度模拟烟气100 h运行试验和燃煤烟气现场试验表明,KCl/γ-Al2O3对HgCl2的突破率非常低,小于10%,突出了其对复杂烟气组分的良好抗干扰能力和工业应用的强适用性和稳定性。本研究为KCl/γ-Al2O3在燃煤电厂高选择性吸附气态HgCl2的工业应用提供了坚实的依据。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
自引率
11.10%
发文量
111
期刊介绍: Asia-Pacific Journal of Chemical Engineering is aimed at capturing current developments and initiatives in chemical engineering related and specialised areas. Publishing six issues each year, the journal showcases innovative technological developments, providing an opportunity for technology transfer and collaboration. Asia-Pacific Journal of Chemical Engineering will focus particular attention on the key areas of: Process Application (separation, polymer, catalysis, nanotechnology, electrochemistry, nuclear technology); Energy and Environmental Technology (materials for energy storage and conversion, coal gasification, gas liquefaction, air pollution control, water treatment, waste utilization and management, nuclear waste remediation); and Biochemical Engineering (including targeted drug delivery applications).
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