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通过胶体硅籽晶诱导合成调控小粒径TS-1沸石及其在氧化脱硫中的应用

Regulation of TS-1 Zeolite with Small Particle Size by Colloidal Silicon Seed-Induced Synthesis and Application in Oxidative Desulfurization.

作者信息

Ren Tieqiang, Sun Yue, Wang Yujia, Wang Lulu, Yu Qian, Liang Lisheng, Kong Xianming, Wang Haiyan

机构信息

College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao 266555, China.

School of Petrochemical Engineering, Liaoning Petrochemical University, Fushun 113001, China.

出版信息

Materials (Basel). 2024 Nov 22;17(23):5722. doi: 10.3390/ma17235722.

Abstract

The dosages of colloidal silicon seeds in the seed-induced synthesis of TS-1 zeolites were investigated in detail. The characterization results revealed that the colloidal silicon seeds not only reduced the particle sizes but also promoted the incorporation of titanium atoms into the framework of TS-1 zeolites as prepared. SEM images and particle size distribution (PSD) confirmed that the particle sizes of TS-1 zeolite could be effectively reduced to about 150 nm. The lattice plane [2 1 0] and [0 2 0] of 7.0-Seed-TS-1 zeolite were well exposed, as observed by the HRTEM images. It is worth noting that the ratio of non-framework Ti atoms incorporated onto the surface of TS-1 zeolites increased slightly to 0.11% by XPS. By regulating the dosage of colloidal Si seeds and promoting rapid nucleation, the size of the crystals could be easily tuned, and then the resulting high external specific surface area and pore volume ensured the reactant accessibility to the active site. The TS-1 zeolites regulated by the 5.0~7.0% dosages of colloidal silicon seeds possessed high external specific surface areas (148.1 m/g and 130.9 m/g) and small particle sizes (about 150 nm). The oxidative desulfurization of 500 ppm DBT by 7.0-Seed-TS-1 zeolite could reach to 100%.

摘要

详细研究了在种子诱导合成TS-1沸石过程中胶体硅源的用量。表征结果表明,胶体硅源不仅减小了粒径,还促进了钛原子进入所制备的TS-1沸石骨架中。扫描电子显微镜(SEM)图像和粒度分布(PSD)证实,TS-1沸石的粒径可有效减小至约150 nm。高分辨透射电子显微镜(HRTEM)图像显示,7.0-种子-TS-1沸石的(2 1 0)和(0 2 0)晶格面充分暴露。值得注意的是,X射线光电子能谱(XPS)表明,结合在TS-1沸石表面的非骨架钛原子比例略有增加,达到0.11%。通过调节胶体硅源的用量并促进快速成核,可以轻松调节晶体尺寸,进而获得的高外表面积和孔体积确保了反应物能够接触到活性位点。由5.0%~7.0%用量的胶体硅源调节的TS-1沸石具有较高的外表面积(分别为148.1 m²/g和130.9 m²/g)和较小的粒径(约150 nm)。7.0-种子-TS-1沸石对500 ppm二苯并噻吩(DBT)的氧化脱硫率可达100%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d95/11642129/b3a0ab164410/materials-17-05722-g001.jpg

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