Abstract
Selective catalytic reduction of NO with methane (NO-CH4-SCR) in the presence of excess oxygen was investigated over the synthesized MnH-ZZs-n zeolite composite catalysts with FAU (as core) and BEA (as shell) topologies. XRD, SEM, and NH3-TPD technologies were employed to characterize the catalysts. It is found that the topological structure of the zeolite affected the catalytic properties and H2O/SO2 tolerances considerably. MnH-ZZs-n catalysts exhibited much higher NO-CH4-SCR activity than the physical mixture catalysts with comparable relative mass content of Y and Beta zeolites, particularly the ratio of Y and Beta at the range of 0.2–0.5 than the MnH-Beta catalysts with single topology. NH3-TPD results showed that one new type of strong acidic sites formed in H-ZZs-n and remained in MnH-ZZs-n resulted from the interaction between the Lewis and Brönsted acid sites under a particular environment. The special zeolite-zeolite structure with ion-exchanged Mn ions in the core-shell zeolite composite catalysts contributed to the novel NO-CH4-SCR properties.
Highlights
The combustion of coal, gasoline, and natural gas meets mankind’s demands for energy
Compared to each individual-zeolite catalyst, the catalytic performance of the zeolite composite was significantly improved because of the synergic effects of the zeolites
MnNa-ZZs-n and MnH-ZZs-n exhibited similar activity at a temperature lower than 673 K, indicating the ion-exchange Mn in the zeolite composites play a key role in NO-CH4 -SCR
Summary
The combustion of coal, gasoline, and natural gas meets mankind’s demands for energy. Armor’s group reported that NO can be selectively reduced by CH4 over Co ion-exchange ZSM-5 and ferrierite in the presence of excess oxygen [4] This is of considerable interest because there are plenty of CH4 and natural gas vehicles increasing worldwide, and CH4 itself is a greenhouse gas with a stronger greenhouse effect than carbon dioxide. Zeolite-based catalysts containing different metals have been reported as active materials for the selective catalytic reduction of NOx with methane (CH4 -SCR) [4]. Mn/TNT showed an impressive deNOx potential compared to other active components in titania nanotubes [22] In this contribution, NO-CH4 -SCR over MnH-ZZs-n is investigated. Effects of H2 O and SO2 on the catalytic performance of MnH-ZZs-n are reported
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