用于催化氢氧化的均配型铑吡啶配合物
Homoleptic Rhodium Pyridine Complexes for Catalytic Hydrogen Oxidation.
作者信息
Zhang Yu, Woods Toby J, Rauchfuss Thomas B
机构信息
School of Chemical Sciences, University of Illinois at Urbana-Champaign, 600 South Goodwin Avenue, Urbana, Illinois 61801, United States.
出版信息
J Am Chem Soc. 2021 Jul 14;143(27):10065-10069. doi: 10.1021/jacs.1c05060. Epub 2021 Jun 28.
The homoleptic rhodium pyridine complex [Rh(py)] ([]) is prepared from simple precursors. Lacking good π-acceptor ligands but being sterically protected, [] reversibly oxidizes to colorless [Rh(py)(thf)]. This monomeric = 1/2 Rh(II) complex activates H to give [HRh(py)L], which can also be generated by protonation of []. The Rh(III)-H bond is weak, being susceptible to H atom abstraction as well as deprotonation. These results underpin a novel catalytic system for the oxidation of H by ferrocenium.
同配体铑吡啶配合物[Rh(py)]（[]）由简单的前体合成。由于缺乏良好的π受体配体但具有空间保护作用，[]可逆地氧化为无色的[Rh(py)(thf)]。这种单核的 = 1/2 Rh(II)配合物活化H生成[HRh(py)L]，它也可以通过[]的质子化产生。Rh(III) - H键较弱，容易受到氢原子夺取以及去质子化的影响。这些结果为二茂铁氧化H的新型催化体系奠定了基础。
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