Isolated Single‐Atom Ruthenium Anchored on Beta Zeolite as an Efficient Heterogeneous Catalyst for Styrene Epoxidation,ChemNanoMat

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Isolated Single‐Atom Ruthenium Anchored on Beta Zeolite as an Efficient Heterogeneous Catalyst for Styrene Epoxidation
ChemNanoMat ( IF 2.6 ) Pub Date : 2020-08-29 , DOI: 10.1002/cnma.202000394
Hongling Yang ₁ , Qinggang Liu ₁ , Yang Li ₁ , Kaian Sun ₁ , Zhiqiang Chen ₁ , Qing Peng ₁ , Chen Chen ₁

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Exploring high‐performance styrene epoxidation catalysts is of great significance. However, it still remains a challenge to synthesize heterogeneous catalysts that simultaneously possess excellent styrene activity and styrene oxide selectivity. Herein, we report a heterogeneous isolated single‐atom Ru supported on microporous Beta zeolite (Ru₁/Beta) catalyst fabricated by a wet impregnation method. We reveal that the extraframework AlOH groups on Beta zeolite are responsible for anchoring Ru species, which is determined by ²⁷Al MAS NMR analyses. The abundant AlOH on microporous Beta zeolite can lead to single‐atom ruthenium dispersion, thereby resulting in marked enhanced catalytic performance in styrene epoxidation than Ru cluster on Beta zeolite. The turnover frequency (TOF) value of Ru₁/Beta reaches 353 h⁻¹, 3.8 times over Ru cluster. The unique styrene oxide selectivity is attributed to the isolated single‐atom Ru anchoring on the Lewis acid site (AlOH) of Beta zeolite, which hinders the further ring opening of styrene oxide to phenylacetaldehyde and cleavage of the double bond of styrene to benzaldehyde.

中文翻译：

固定在Beta沸石上的分离的单原子钌是一种高效的均相苯乙烯环氧化催化剂

探索高性能的苯乙烯环氧化催化剂具有重要意义。然而，合成同时具有优异的苯乙烯活性和苯乙烯氧化物选择性的非均相催化剂仍然是一个挑战。本文中，我们报道了通过湿法浸渍法制备的负载在微孔Beta沸石（Ru ₁ / Beta）催化剂上的非均相分离单原子Ru 。我们发现，β沸石上的骨架外AlOH基团负责锚定Ru物种，这由²⁷确定。Al MAS NMR分析。微孔Beta沸石上大量的AlOH可以导致单原子钌分散，因此与Ru簇在Beta沸石上相比，苯乙烯环氧化中的催化性能显着增强。Ru ₁ / Beta的周转频率（TOF）值达到353 h ^-1，是Ru簇的3.8倍。独特的苯乙烯氧化物选择性归因于在β沸石的路易斯酸位点（AlOH）上孤立的单原子Ru锚固，这阻碍了苯乙烯氧化物进一步开环成苯乙醛和阻止苯乙烯双键裂解成苯甲醛。

更新日期：2020-11-06

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