Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 11, Issue 4, Pages 1365-1374Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0cy01822h
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Funding
- National Natural Science Foundation of China [21671028, 21771027]
- Natural Science Foundation of Chongqing [cstc2019jcyj-msxmX0312, cstc2019jcyj-msxmX0330]
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The study synthesized Cr-substituted aluminoborate Cr-PKU-8 catalysts and successfully applied them in the oxidation of aliphatic and aromatic alcohols with high efficiency and selectivity in a H2O solvent medium. Analysis using isotopic tracer and cyclic voltammetry strategies revealed that chromium ions undergo a Cr3+-Cr2+-Cr3+ redox cycle, and proposed t-BuOO* as the key active species in the reaction process.
Catalytic oxidation reaction using green oxidants plays an important role in modern chemical engineering; however, the in situ generated active species and the related catalytic mechanism need to be understood in depth. For this purpose, Cr-substituted aluminoborate Cr-PKU-8 catalysts were synthesized and applied as recyclable heterogeneous catalysts for the oxidation of aliphatic and aromatic alcohols using tert-butylhydroperoxide (TBHP). Both high efficiency and selectivity (>99%) were achieved during the dehydrogenation of various sec-alcohols into acetone in H2O solvent medium. From the analyses using isotopic tracer, molecular probe and cyclic voltammetry strategies, the chromium ions were observed to undergo a Cr3+-Cr2+-Cr3+ redox cycle. DFT calculations suggest that t-BuOO* is more energetically favourable for hydrogen abstraction from sec-alcohol than t-BuO*, and probably acts as the key active species. Accordingly, the reaction scheme was proposed to interpret the catalytic process based on the observed results.
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