A series
of mesoporous materials of SBA-16 were in situ incorporated
into ZSM-5 crystallites via a two-step self-assemble method, and hydrodesulfurization
(HDS) catalysts were prepared on the corresponding ZSM-5/SBA-16 (ZS)
composites. The characterization results indicated that ZSM-5 nanoseeds
were fabricated into the silica framework of the ZS composites, and
the three-dimensional Im3m cubic
structure of SBA-16 was retained simultaneously. In addition, the
ZS series materials possessed open pores and large surfaces, which
would facilitate the diffusion of reactants in the mesoporous channels.
Moreover, the introduction of ZSM-5 seeds into composites could enhance
the acidities of supports. As a result, the NiMo/ZS series catalysts
exhibited high activities for DBT HDS processes. The NiMo/ZS-160 catalyst
exhibited the highest catalytic efficiency (96.5%), which was apparently
attributed to the synergistic contributions of the physicochemical
properties of ZS supports and the dispersion states of active metals.
Correspondingly, DBT HDS reactions over the NiMo/ZS series catalysts
mainly proceeded via a hydrogenation desulfurization route that benefitted
from the enhanced acidities especially the total Brønsted acid.
Hydrogenation of naphthalene can effectively reduce the
content
of aromatics in oil and generate high-value products. A series of
Pt-based aluminum-modified core–shell-structured hierarchically
periodic mesoporous organosilica@mesoporous silica nanoparticles (Pt/Al-x-PMOs@MSNs) were successfully synthesized and tested for
the hydrogenation properties, with preferable mass transfer of macromolecular
reactants in the pores and increasing the total acidity of the catalysts.
Moreover, the physicochemical properties of the core–shell-structured
Pt-based catalysts were systematically analyzed using various characterization
techniques. At 300 °C, the naphthalene conversion on the Pt/Al-10-PMOs@MSNs
catalyst reached up to 100%, the selectivity of trans-decalin reached 83.9%, and the rate constants (k
1, k2) and TOF were 13.2 × 10–6 mol·g–1·s–1, 1.7 ×
10–7 mol·g–1·s–1, and 218.8 h–1, respectively. In the presence
of sulfur, the naphthalene hydrogenation over the Pt/Al-10-PMOs@MSN
catalyst first decreased to around 40% and then recovered to the original
level, which originated from the synergistic effect of the texture
and chemical properties over the Pt/Al-10-PMOs@MSNs with an excellent
performance.
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