a.College of Materials and Energy, South China Agricultural University, Guangzhou 510642, China
b.School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
boping@scau.edu.cn
收稿:2019-03-30,
修回:2019-5-13,
录用:2019-5-16,
网络首发:2019-07-02,
纸质出版:2019-10
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Citation: Jin, Y. L.; Liu, L.; Wang, Y. J.; Liu, Z.; Liu, B. P. Mechanistic study on the dominant promotion effect of Al-/Ti-/Zr-modifications over the VO
Yu-Long Jin, Lin Liu, Yu-Jie Wang, et al. Mechanistic Study on the Dominant Promotion Effect of Al-/Ti-/Zr-modifications over the VO
Citation: Jin, Y. L.; Liu, L.; Wang, Y. J.; Liu, Z.; Liu, B. P. Mechanistic study on the dominant promotion effect of Al-/Ti-/Zr-modifications over the VO
Yu-Long Jin, Lin Liu, Yu-Jie Wang, et al. Mechanistic Study on the Dominant Promotion Effect of Al-/Ti-/Zr-modifications over the VO
Recently
we reported the first VO
x
/SiO
2
ethylene polymerization catalyst for making Cl-free UHMWPE
and found the dominant promotion effects of Al-/Ti-/Zr-modifications over this catalyst system (Macromol. Chem. Phys. 2017
218
1600443). In this work
density functional theory is applied to investigate the underlying mechanism of this remarkable promotion effect of Al-/Ti-/Zr-modifications on a molecular and atomic level. The cluster model with V(III) is found to be the most possible active site due to its lowest overall energy barrier for monomer insertion
though the process of C
2
H
4
coordination and the subsequent formation of transition state are most energy favored for V(II) species. By modifying one of or both V―O―Si in the active model with V―O―M (M = Al
Ti
or Zr)
the energy barrier for the binding of the upcoming C
2
H
4
gets lower (particularly for Al- and Zr-modified catalysts)
and the transition state also becomes more stable. Generally
the insertion process of C
2
H
4
gets easier after support Al-/Ti-/Zr-modifications. This dominant promotion effect is partially ascribed to the more enriched positive charge distribution on or nearby the V center
and the narrower energy gap between the LUMO of model catalysts and the HOMO of C
2
H
4
for these modified catalysts also contributes much. In addition
the decreased steric hindrance around the V center should be taken into account for the modified models as well. Furthermore
the Brønsted acidity of the catalysts is investigated by introducing a pendent hydroxyl group to the model catalysts
which has a close contact with the V center. Similar promotion effect of support modification by Al
Ti
and Zr could still be observed.
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