AEI-type aluminosilicate zeolites with sheet-like morphology were successfully synthesized by the crystal growth inhibitors (CGI)-assisted method, where cetyltrimethylammonium bromide (CTAB) worked as a CGI. The obtained sheet-like AEI-type aluminosilicates showed...
The development of simple catalysts with high performance in the selective oxidation of methane to syngas at low temperature has attracted much attention. Here we report a nickel-based solid catalyst for the oxidation of methane, synthesised by a facile impregnation method. Highly dispersed ultra-small NiO particles of 1.6 nm in size are successfully formed on the MOR-type zeolite. The zeolite–supported nickel catalyst gives continuously 97–98% methane conversion, 91–92% of CO yield with a H2/CO ratio of 2.0, and high durability without serious carbon deposition onto the catalyst at 973 K. DFT calculations demonstrate the effect of NiO particle size on the C-H dissociation process of CH4. A decrease in the NiO particle size enhances the production of oxygen originating from the NiO nanoparticles, which contributes to the oxidation of methane under a reductive environment, effectively producing syngas.
A series
of MCM-68 zeolites with different Si/Al ratios were prepared
by treatment with nitric acid and compared with beta zeolites. Speciation
of aluminum and location of acid sites changed depending on the Si/Al
ratio. The location of Brønsted acid sites in MCM-68 samples
was able to be classified by FT-IR measurements with pyridine and
2,6-di-tert-butylpyridine as probe molecules, and
the number of Brønsted acid sites was quantified according to
the locations. For high-aluminum MCM-68, Brønsted acid sites
were broadly distributed in both the 12-ring channel and 10-ring windows
as well as inside the supercage. The Brønsted acid sites in the
12-ring channel were easily removed by the acid treatment, and consequently,
high-silica MCM-68 had Brønsted acid sites predominantly in the
10-ring windows and inside the supercage. 27Al MQMAS NMR
spectra of high-silica MCM-68 showed two specific peaks assignable
to T6 and T7 sites, which did not face the 12-ring channel, forming
the Brønsted acid sites highly tolerant to the acid treatment.
MCM-68 catalysts showed better catalytic performance in dehydration
of sorbitol than beta, mordenite, and ZSM-5. Large void spaces at
the intersection of 12- and 10-ring channels and inside the supercage
for MCM-68 made it easy to take bulky transition states in the dehydration
of sorbitol, resulting in its high catalytic performance.
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