| 研究開始時の研究の概要 |
The collaborative process of different functional sites is called “relay” in catalysis, whose nature is tandem catalysis, which does not change the original reaction path. We proposed a reversal strategy for heterogenous catalysis by reconstruction of the reaction network for improving the catalytic activity.
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| 研究実績の概要 |
The design of heterogeneous catalysts traditionally centers on modifying their intrinsic physicochemical properties or adjusting electron states with additives at the sub-nanoscale level. However, constructing an entirely new reaction network, which entails a qualitative shift in reaction efficiency by disrupting the existing network, poses significant challenges.
In this research year, we utilized a reverse strategy: detaching one component (Cu) from its parent catalyst (MOR zeolite) on a centimeter scale to successfully reconstruct a completely new reaction network, achieving markedly improved catalytic performance of a record-breaking percentage gain of 266% in the space-time yield of methyl acetate product during the carbonylation of dimethyl ether.
In-situ high-pressure Synchrotron Vacuum Ultraviolet Photoionization Mass
Spectrometry, in-situ TEM, and in-situ DRIFTS were employed to make the brand-
new reaction mechanism clear. The previously unreported vital intermediate, acetic anhydride, was discovered for the first time when employing the detaching style of Cu/SiO2//H-MOR.
This noteworthy discovery not only underscores its profound implications but also emphasizes its extensive potential for deployment in designing various heterogeneous catalysts, applicable across a diverse array of chemical reactions.
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