Preparation and Catalytic Activity of Morphologically Controlled MoO₃/SiO₂ for Hydrodesulfurization

결정상과 분산도의 조절이 가능한 MoO₃/SiO₂ 촉매의 제조 및 탈황반응특성 연구

Several series of morphologically controlled $MoO_3$/$SiO_2$ catalysts were prepared, characterized, and tested for hydrodesulfurization (HDS) of dibenzothiophene (DBT) activity. Molybdenum surface loaded with 4.0 atoms $Mo/nm^2$ was prepared as sintered hexagonal and sintered orthorhombic, as well as a novel "well dispersed hexagonal" phase. Characterization by XRD, Raman, and $O_2$ chemisorption results reveals that the dispersion of $MoO_3$ over silica depends on the final $MoO_3$ phase in the order of; sintered hexagonal < sintered orthorhombic < dispersed hexagonal phase. Temperature programmed reduction (TPR) results show that both bulk and dispersed microcrystalline of $MoO_3$ reduce to $MoO_2$ at $650^{\circ}C$ and to Mo metal at $1000^{\circ}C$. HDS of DBT was performed in a differential reactor at 30 atm over the temperature range $350{\sim}500^{\circ}C$. Activity of $MoO_3$/$SiO_2$ toward HDS of DBT is proportional to dispersion.

결정상과 분산도가 조절된 $MoO_3$/$SiO_2$ 담지촉매를 제조하여 촉매의 표면특성과 디벤조티오펜 탈황반응의 활성도를 고찰하였다. Mo의 표면담지량은 4 atoms $Mo/nm^2$이었으며, 실리카 표면 위에 형성된 $MoO_3$의 결정상은 sintered hexagonal, sintered orthorhombic, 및 dispersed hexagonal상이었다. XRD, Raman, 및 $O_2$ 흡착 결과 $MoO_3$의 표면분산도는 sintered hexagonal < sintered orthorhombic < dispersed hexagonal 순으로 증가하였다. TPR 결과 $MoO_3$ 결정은 $650^{\circ}C$에서 $MoO_2$로, $1000^{\circ}C$에서 Mo로 환원됨을 알 수 있었다. 디벤조티오펜 탈황반응을 30기압, $350{\sim}500^{\circ}C$ 온도범위에서 수행하였으며, 실험 결과 활성도는 $MoO_3$ 결정체의 $SiO_2$ 표면에서의 분산도에 비례하여 증가함을 알 수 있었다.