Citation: ZOU Jing, FAN Zhi-Lin, JIANG Li-Sha, ZHOU Dan-Hong. Theoretical Study of the Solvent Adsorption on Ti-Peroxo Active Center in Ti-MWW Zeolite[J]. Acta Physico-Chimica Sinica, ;2016, 32(4): 935-942. doi: 10.3866/PKU.WHXB201601201 shu

Theoretical Study of the Solvent Adsorption on Ti-Peroxo Active Center in Ti-MWW Zeolite

1.
College of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian 116029, Liaoning Province, P. R. China

Corresponding author: ZHOU Dan-Hong,
Received Date: 24 November 2015
Available Online: 18 January 2016
Fund Project: 国家自然科学基金(21343010)资助项目 (21343010)

Density functional theory is used to study the structures of the Ti-peroxide species in a Ti-MWW/H₂O₂ system and the influence of the coordination with solvent molecules on the geometries and electronic features. The result indicated that the framework Ti can interact with H₂O₂ to form two kinds of Ti-peroxide species, the five-membered ring Ti-η¹-OOH and the three-membered ring Ti-η²-OOH. The framework Ti center can further interact with solvent molecules of H₂O, CH₃OH, and CH₃CN to form 6-coordinated complexes. The adsorption energies decreased as H₂O > CH₃OH > CH₃CN. Both Ti-peroxide species display different adsorption capacity as Ti-η¹-OOH > Ti-η²-OOH. The location of Ti also has a distinct effect on the adsorption. The central Ti at T1 prefers to adsorb solvent molecule over the Ti at T3. In addition, solvent adsorption also influences the electrophilicity of the active oxygen atom. The calculated results indicate that on the Ti-η²-OOH active center with adsorbed CH₃CN, the activation energy of the epoxidation of chloropropene has been reduced.
- Ti-MWW zeolite,
- Aqueous H₂O₂,
- Ti-peroxide intermediate,
- Solvent effect,
- Density functional theory
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