Identification of key oxidative intermediates and the function of chromium dopants in PKU-8: catalytic dehydrogenation of sec-alcohols with tert-butylhydroperoxide

Wang Weilu; He Yang; He JunkaiDang YanliuKankanmkapuge TharinduGao WenliangCong RihongSuib Steven L.Yang Tao

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Identification of key oxidative intermediates and the function of chromium dopants in PKU-8: catalytic dehydrogenation of sec-alcohols with tert-butylhydroperoxide

机译：氧化中间体和识别的关键在PKU-8铬掺杂物的功能:催化脱氢的sec-alcoholstert-butylhydroperoxide

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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.

机译：使用绿色氧化剂催化氧化反应在现代化学中起着重要的作用工程;活跃的物种和相关的催化需要深入理解机制。这个目的,Cr-substituted aluminoborateCr-PKU-8催化剂合成和应用作为异构催化剂的回收利用氧化脂肪族和芳香族醇使用tert-butylhydroperoxide (TBHP)。效率和选择性(> 99%)在各种的脱氢sec-alcohols在水溶剂丙酮介质。从分析使用同位素示踪剂,分子探针和循环伏安法策略,铬离子被观察到三价铬cr2 + Cr3 +进行氧化还原循环。计算表明,t-BuOO *是更多积极有利于氢抽象从sec-alcohol t-BuO *,可能的行为的关键活性物种。反应计划提出了解释催化过程基于观察的结果。

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来源
《Catalysis science & technology》 |2021年第4期|1365-1374|共10页
作者
Wang Weilu; He Yang; He JunkaiDang YanliuKankanmkapuge TharinduGao WenliangCong RihongSuib Steven L.Yang Tao;
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作者单位

Univ Tennessee, Dept Chem & Chem Engn, Knoxville, TN 37996 USA;

Univ Connecticut, Dept Chem, Storrs, CT 06269 USA;

Chongqing Univ, Coll Chem & Chem Engn, Chongqing 401331, Peoples R China;

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正文语种英语
中图分类汉语教学;
关键词
Catalysis; tert-Butylhydroperoxide; DEHYDROGENATORSchromiumadulterated products;

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Identification of key oxidative intermediates and the function of chromium dopants in PKU-8: catalytic dehydrogenation of sec-alcohols with tert-butylhydroperoxide

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