期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 6, 期 9, 页码 11949-11958出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.8b02269
关键词
Aldol condensation; butadiene; ethanol; nonstoichiometric oxygen; perovskite
资金
- Taiwan's Deep Decarbonization Pathways toward a Sustainable Society [107-0210-02-19-01]
- Ministry of Science and Technology [105-2119-M-001-029-MY2, 106-2221-E-006-188-MY3, 106-2218-E-155-005]
- Ministry of Economic Affairs [H354DP2120]
This study reports that the C2-C2 aldolization in ethanol conversion to C4 products, particularly butadiene, can be catalyzed by silica-supported LaMnO3 catalysts. The concentration and strength of Mn-4(+) was discovered to be related to the particle size of supported LaMnO3: the smaller the particle size is, the higher the concentration and acidity of M4+ are. The presence of high concentration and acidity of Mn4+ of small LaMnO3 particles concurrently increases the amount of weak basic nonstoichiometric oxygen, with which the surface concentration of Lewis acid-base adducts can be elevated. The Mn4+/nonstoichiometric oxygen pair is intrinsically active in C2-C2 aldolization, and the concentration of the paired site is positively correlated to the selectivity of C4 products. By coreacting ethanol with its evolved intermediates, that is, acetaldehyde and crotonaldehyde, we discovered the aldol condensation of acetaldehyde molecules to be rate-limiting. Accordingly, a plausible mechanism of aldolization of acetaldehyde molecules into C4 products mediated by the Mn4+/nonstoichiometric oxygen adduct of LaMnO3 was established.
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