Enhancing Desulfurization Performance by Regulating Ca(OH)2 Hygroscopicity: An Integrated Experimental and DFT Study

IF 5.3 3区 工程技术 Q2 ENERGY & FUELS Energy & Fuels Pub Date : 2025-04-02 DOI:10.1021/acs.energyfuels.5c00262
Shengwei Fan, Hongjian Tang*, Xiangqian Du, Weiyi Fan, Min Pan and Lunbo Duan*, 
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Abstract

Circulating fluidized-bed flue gas desulfurization (CFB-FGD) is a widely employed semidry flue gas desulfurization technology due to its cost-effectiveness and easy operation. However, CFB-FGD cannot satisfy the ultralow emission requirement, particularly under high SO2-containing flue gas conditions. This study aimed to enhance the CFB-FGD performance in a cost-effective way by regulating Ca(OH)2 hygroscopicity in the desulfurization reaction. MgSO4 was screened out from 7 hygroscopic additives. With a minor addition of 4.8 wt % MgSO4, the sulfur capacity of Ca(OH)2 increased significantly by over 15% compared to its pristine benchmark. By synthesizing structural characterization and DFT calculations, the pros and cons of the H2O effect on the Ca(OH)2 desulfurization reactivity were revealed and discussed from an atomic perspective. X-ray diffraction suggested that the introduction of water could activate the Ca(OH)2 interlayer by expanding the interplanar distance in the (001) orientation, thus enhancing SO2 adsorption. DFT calculations showed that the desulfurization reaction over Ca(OH)2(001) was kinetically promoted in the presence of H2O by facilitating proton transfer. By contrast, excessively high hygroscopicity was found to inhibit the desulfurization performance of Ca(OH)2 by blocking porosity and hindering SO2 diffusion by absorbing redundant moisture. This work demonstrated that tuning Ca(OH)2 hygroscopicity is a low-cost and efficient way to boost SO2 sorption, which advances Ca(OH)2-based solution technologies for wider applications in the flue gas decontamination field.

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通过调节Ca(OH)2吸湿性来提高脱硫性能:一项综合实验和DFT研究
循环流化床烟气脱硫(CFB-FGD)是一种应用广泛的半干法烟气脱硫技术,具有成本效益好、操作简便等优点。然而,CFB-FGD不能满足超低排放要求,特别是在高so2含量的烟气条件下。本研究旨在通过调节脱硫反应中的Ca(OH)2吸湿性,以经济有效的方式提高CFB-FGD的性能。从7种吸湿添加剂中筛选出MgSO4。在少量添加4.8 wt % MgSO4的情况下,Ca(OH)2的硫容量比其原始基准显著增加了15%以上。通过合成结构表征和DFT计算,揭示了H2O对Ca(OH)2脱硫反应性影响的利弊,并从原子的角度进行了讨论。x射线衍射表明,水的引入可以通过扩大(001)取向的面间距来激活Ca(OH)2中间层,从而增强对SO2的吸附。DFT计算表明,在H2O的存在下,Ca(OH)2(001)的脱硫反应通过质子转移得到了动力学的促进。而过高的吸湿性则会抑制Ca(OH)2的脱硫性能,因为过高的吸湿性会堵塞孔隙,并通过吸收多余水分阻碍SO2的扩散。本研究表明,调整Ca(OH)2吸湿性是一种低成本、高效的提高SO2吸附的方法,这将推动Ca(OH)2溶液技术在烟气净化领域的更广泛应用。
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来源期刊
Energy & Fuels
Energy & Fuels 工程技术-工程:化工
CiteScore
9.20
自引率
13.20%
发文量
1101
审稿时长
2.1 months
期刊介绍: Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.
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