期刊
ACS CATALYSIS
卷 7, 期 7, 页码 4417-4422出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b00894
关键词
methanol-to-olefins; rare earth metal oxide; bifunctional catalysis; formaldehyde; deactivation; yttrium oxide
资金
- Dow Chemical Company
- National Science Foundation [CBET 1055846]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1055846] Funding Source: National Science Foundation
Bifunctional strategies exploiting the selective and catalytic decomposition of formaldehyde by Y2O3 improve 1 the lifetime of CHA zeotypes and zeolites for methanol-to olefins catalysis 4-fold, as quantified by total turnovers, without disrupting the inherently high selectivity to light olefins. The improvement in catalyst lifetime increases with increasing proximity between H+ sites of the zeotype/zeolite and the surface of the rare earth metal oxide. This proximity effect demonstrates crucial transport of formaldehyde between and within zeotypic/zeolitic domains on catalyst lifetime. These results provide mechanistic insights revealing formaldehyde as an accelerant for the initiation and termination of chain carriers and exemplify a strategy for designing improved methanol-to olefins catalysts by optimizing (bi)functionality and reaction-transport dynamical phenomena.
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