2023 Fiscal Year Annual Research Report
Project/Area Number |
22KJ1456
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Allocation Type | Multi-year Fund |
Research Institution | University of Toyama |
Principal Investigator |
姚 杰 富山大学, 工学部, 特別研究員(PD)
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Project Period (FY) |
2023-03-08 – 2024-03-31
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Keywords | Zeolite / Dimethyl ether / Carbonylation |
Outline of Annual Research Achievements |
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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