2026-03-19 ワシントン州立大学（WSU）
＜関連情報＞
- https://news.wsu.edu/press-release/2026/03/19/carefully-controlled-atoms-make-renewables-more-viable-for-plastics-and-fuels-production/
- https://www.cell.com/chem-catalysis/fulltext/S2667-1093(25)00367-7
脱アルミニウム化ベータゼオライト中に原子分散したセリウムを閉じ込めて選択的なC–C結合と脱酸素化を行う Confinement of atomically dispersed Ce in dealuminated beta zeolite for selective C–C coupling and deoxygenation
Vannessa Caballero, ∙ Wenda Hu, ∙ Hao Xu ∙ … ∙ Mingwu Tan ∙ Konstantin Khivantsev ∙ Yong Wang
Chem Catalysis Published:February 24, 2026
DOI:https://doi.org/10.1016/j.checat.2025.101628
Graphical abstract
The bigger picture
Modern chemical manufacturing relies heavily on fossil fuels, and finding cleaner ways to make essential chemicals is a major challenge. One promising route is to convert ethanol—an abundant renewable fuel—into more valuable molecules used in plastics, fuels, and everyday products. A key step in this conversion is transforming acetone into isobutene. However, conventional catalysts often trigger competing reactions, wasting carbon and lowering efficiency.
Our work shows that atomic-scale catalyst control can dramatically improve the behavior of this reaction. By precisely positioning individual cerium (Ce) atoms inside the tiny pores of a zeolite—a crystalline material full of uniform nanoscale channels—we create highly selective reaction sites that steer acetone along the most efficient pathway. When Ce is dispersed as isolated atoms, it promotes a clean sequence of C–C bond formation and oxygen removal, maximizing the production of isobutene. But when Ce clusters into larger oxide nanoparticles, the reaction veers off course and generates unwanted byproducts. This discovery demonstrates a powerful principle: the size and placement of atoms inside a catalyst can determine the fate of every reaction step. The zeolite’s confined structure stabilizes the right intermediates and suppresses pathways that lead to waste and catalyst deactivation. More broadly, this work provides a blueprint for designing next-generation catalysts that convert renewable feedstocks into valuable chemicals with far greater efficiency. By harnessing atomic-level control to guide complex reactions, we can advance cleaner manufacturing routes, reduce energy inputs, and support emerging circular-carbon strategies.
Highlights
- Atomically dispersed Ce in zeolite beta (BEA framework) promotes selective acetone into isobutene
- CeO2 nanoparticles favor mesityl oxide formation via diacetone alcohol dehydration
- Structural confinement within the BEA framework suppresses undesired side reactions
- Kinetic experiments reveal that diacetone alcohol decomposition is the rate-limiting step
Summary
The acetone-to-isobutene reaction is a key step in the ethanol cascade process toward high-value chemicals. However, the effects of spatial confinement and the role of cerium (Ce) species remain poorly understood. Here, we reveal that Ce-incorporated dealuminated beta zeolite (CedeAlBEA) exhibits exceptional isobutene selectivity when Ce species are atomically dispersed within the BEA framework. Spectroscopy analyses show that isolated Ce atoms provide optimal Lewis acidity for facilitating selective isobutene formation. In contrast, increasing Ce loading leads to the formation of CeO2 nanoparticles, promoting mesityl oxide (MSO) as a byproduct. The Ce species in CedeAlBEA enhance C–C coupling and deoxygenation selectivity, whereas mesoporous and non-porous supports favor MSO formation because of the weaker confinement effects. Kinetic experiments reveal that oxygen elimination is the rate-limiting step. This study highlights the critical role of confined, atomically dispersed Ce cations in the BEA framework in directing acetone throughout diacetone alcohol decomposition to isobutene.
