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An Integrated Cobalt-Polyoxoniobate for Catalytic Aldehyde Oxidation
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DOI：10.1021/acs.inorgchem.6c00540.png)
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Abstract
En 中文
The efficient aerobic oxidation of aldehydes under mild conditions is a persistent challenge in heterogeneous catalysis, constrained by mass transfer in gas–liquid–solid triphasic systems. Herein, we report a cobalt-containing polyoxoniobate (PONb) heterogeneous integrated catalyst, Co0.6@Li2K3.8[Sb(H2O)][GeNb12O40(VVO)2]·8H2O (Co/FZU-3), that efficiently drives the additive-free aerobic oxidation of diverse aldehydes to carboxylic acids at room temperature, without external heating or cocatalysts. Co/FZU-3 delivers a record-high turnover frequency (TOF) of 333 h–1 among reported catalysts, alongside excellent recyclability and gram-scale applicability. The excellent catalytic performance originates from an efficient proton transfer process, synergistically enabled by the stable anchoring of active cobalt centers and the outstanding proton-conducting capability of the PONb framework. This work not only addresses key efficiency bottlenecks in triphasic aerobic oxidation but also demonstrates a design strategy for multifunctional, green catalytic systems.
Keywords:
Cobalt-polyoxoniobate
Aerobic oxidation
Aldehyde
Carboxylic acid
Proton transfer