Defect‐Engineered Ruthenium MOFs as Versatile Heterogeneous Hydrogenation Catalysts,ChemCatChem

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Defect‐Engineered Ruthenium MOFs as Versatile Heterogeneous Hydrogenation Catalysts
ChemCatChem ( IF 3.8 ) Pub Date : 2020-02-19 , DOI: 10.1002/cctc.201902079
Konstantin Epp ₁ , Ignacio Luz _{2,

3} , Werner R. Heinz ₁ , Anastasia Rapeyko ₂ , Francesc X. Llabrés i Xamena ₂ , Roland A. Fischer ₁

Affiliation

Ruthenium MOF [Ru₃(BTC)₂Y_y] ⋅ G_g (BTC=benzene‐1,3,5‐tricarboxylate; Y=counter ions=Cl⁻, OH⁻, OAc⁻; G=guest molecules=HOAc, H₂O) is modified via a mixed‐linker approach, using mixtures of BTC and pyridine‐3,5‐dicarboxylate (PYDC) linkers, triggering structural defects at the distinct Ru₂ paddlewheel (PW) nodes. This defect‐engineering leads to enhanced catalytic properties due to the formation of partially reduced Ru₂‐nodes. Application of a hydrogen pre‐treatment protocol to the Ru−MOFs, leads to a further boost in catalytic activity. We study the benefits of (1) defect engineering and (2) hydrogen pre‐treatment on the catalytic activity of Ru−MOFs in the Meerwein‐Ponndorf‐Verley reaction and the isomerization of allylic alcohols to saturated ketones. Simple solvent washing could not avoid catalyst deactivation during recycling for the latter reaction, while hydrogen treatment prior to each catalytic run proved to facilitate materials recyclability with constant activity over five runs.

中文翻译：

缺陷工程钌MOF作为多功能多相加氢催化剂

钌MOF的[Ru ₃（BTC）₂ ÿ _ÿ ]⋅ģ_克（BTC =苯-1,3,5-三羧酸酯; Y =抗衡离子=氯^-，OH ^-，OAC ^- ; G =客体分子的HOAc =，H ₂ O）通过使用BTC和吡啶3,5-二羧酸酯（PYDC）接头的混合物的混合接头方法进行修饰，从而在不同的Ru ₂桨轮（PW）节点处引发结构缺陷。由于部分还原的Ru ₂的形成，这种缺陷工程可以提高催化性能。节点。将氢预处理方案应用于Ru-MOF，可进一步提高催化活性。我们研究了（1）缺陷工程和（2）氢预处理对Meerwein-Ponndorf-Verley反应中Ru-MOFs催化活性以及烯丙基醇异构化为饱和酮的好处。简单的溶剂洗涤不能避免在再循环用于后面的反应的过程中催化剂失活，而事实证明，在每次催化运行之前进行氢处理有助于在五个运行中以恒定的活性实现材料的可回收性。

更新日期：2020-02-19

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