Regulation on mesoporous structure of Ag doped SiO2 aerogel by microdroplet template method for adsorption desulfurization

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Journal of Solid State Chemistry Pub Date : 2025-07-01 Epub Date: 2025-03-13 DOI:10.1016/j.jssc.2025.125318
Bin Liu , Bo Zhang , Wanyi Tao , Kai Wang , Lanxia Hu , Jiawei Zuo , Wensheng Ning , Wanjin Yu
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Abstract

A series of Ag(I) doped silica (Ag/SiO2-tem-x/y) aerogel composites were prepared by microdroplet template method with different amount of template, whose physical and chemical properties were characterized by XRD, XPS, SEM-mapping, BET and XRF methods, and the sorption ability for thiophenics in model fuels was investigated, compared with Ag/SiO2 prepared by conventional sol-gel method. The results showed that compared with conventional sol-gel method, the use of microdroplet template method could obviously improve the regularity of pore structure, the specific surface area and the actual doped rate of Ag species, however, did not change the chemical state of Ag species in aerogel composites. Both Ag/SiO2-tem-x/y and Ag/SiO2 adsorbed thiophenics mainly through the π-complexion between thiophenics and Ag(I) species. However, compared with Ag/SiO2, the changes in physical and chemical properties of Ag/SiO2-tem-x/y generated more highly dispersed Ag(I) species on the surface and the quicker diffusion velocity of thiophenics in the pore channels, consequently, leading to a higher sorption uptake for thiophenics. Among Ag/SiO2-tem-x/y sorbents, Ag/SiO2-tem-20/1 had the maximal sorption uptake for thiophene, up to 10.7 mg-S/gads. Upon four regeneration cycles by solvent washing, the sorption uptake of Ag/SiO2-tem-20/1 could recover 74.11 % of fresh one, being better than that of Ag/SiO2-50 (59.67 %), owing to the lower loss rate of Ag(I) species in former. The sorption process of thiophene on Ag/SiO2-50 and Ag/SiO2-tem-20/1, which was spontaneous and exothermic with a decreased disorder, could be better described by the pseudo-second-order kinetics mode and Langmuir adsorption isotherm model, respectively.

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微滴模板法调控Ag掺杂SiO2气凝胶介孔结构的吸附脱硫
采用不同模板量的微滴模板法制备了一系列Ag(I)掺杂二氧化硅(Ag/SiO2-tem-x/y)气凝胶复合材料,采用XRD、XPS、SEM-mapping、BET和XRF等方法对其理化性质进行了表征,并与常规溶胶-凝胶法制备的Ag/SiO2相比,研究了其对模型燃料中噻吩类物质的吸附能力。结果表明,与传统的溶胶-凝胶法相比,微滴模板法可以明显改善气凝胶复合材料的孔隙结构的规整性、银的比表面积和实际掺杂率,但并未改变气凝胶复合材料中银的化学状态。Ag/SiO2-tem-x/y和Ag/SiO2主要通过噻吩与Ag(I)之间的π相关系吸附噻吩。然而,与Ag/SiO2相比,Ag/SiO2-tem-x/y的物理化学性质的变化使得Ag(I)在表面的分散程度更高,噻吩在孔道中的扩散速度更快,从而导致噻吩的吸附吸收率更高。Ag/SiO2-tem-x/y吸附剂中,Ag/SiO2-tem-20/1对噻吩的吸附量最大,可达10.7 mg-S/gads。经过4次溶剂洗涤再生循环后,Ag/SiO2-tem-20/1的吸附回收率为74.11%,优于Ag/SiO2-50的59.67%,这是由于前者的Ag(I)物种损失率较低。噻吩在Ag/SiO2-50和Ag/SiO2-tem-20/1上的吸附过程是自发的、放热的,无序程度较低,可以用拟二级动力学模型和Langmuir吸附等温线模型来描述。
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来源期刊
Journal of Solid State Chemistry
Journal of Solid State Chemistry 化学-无机化学与核化学
CiteScore
6.00
自引率
9.10%
发文量
848
审稿时长
25 days
期刊介绍: Covering major developments in the field of solid state chemistry and related areas such as ceramics and amorphous materials, the Journal of Solid State Chemistry features studies of chemical, structural, thermodynamic, electronic, magnetic, and optical properties and processes in solids.
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