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Singlet versus Triplet Reactivity in an Mn(V)-Oxo Species: Testing Theoretical Predictions Against Experimental Evidence.锰(V)-氧物种中单重态与三重态反应性：理论预测与实验证据的检验。
J Am Chem Soc. 2016 Sep 28;138(38):12375-86. doi: 10.1021/jacs.6b05027. Epub 2016 Sep 14.
2
Intramolecular C-H and C-F Bond Oxygenation Mediated by a Putative Terminal Oxo Species in Tetranuclear Iron Complexes.四核铁配合物中假定的末端氧代物种介导的分子内C-H和C-F键氧化反应
J Am Chem Soc. 2016 Feb 10;138(5):1486-9. doi: 10.1021/jacs.5b12214. Epub 2016 Feb 1.
3
Nitric oxide activation by distal redox modulation in tetranuclear iron nitrosyl complexes.通过四核亚硝酰基铁配合物中的远程氧化还原调节实现一氧化氮的活化
J Am Chem Soc. 2015 Nov 11;137(44):14094-106. doi: 10.1021/jacs.5b07397. Epub 2015 Nov 2.
4
A Balancing Act: Stability versus Reactivity of Mn(O) Complexes.一种平衡行为：锰（氧）配合物的稳定性与反应活性
Acc Chem Res. 2015 Oct 20;48(10):2754-64. doi: 10.1021/acs.accounts.5b00273. Epub 2015 Sep 9.
5
A self-assembled octanuclear complex bearing the uncommon close-packed {Fe4Mn4(μ4-O)4(μ-O)4} molecular core.一种自组装的八核配合物，具有不常见的密堆积 {Fe4Mn4(μ4-O)4(μ-O)4} 分子核。
Dalton Trans. 2015 Sep 7;44(33):14918-24. doi: 10.1039/c5dt02076j.
6
Synthetic mononuclear nonheme iron-oxygen intermediates.合成单核非血红素铁-氧中间体。
Acc Chem Res. 2015 Aug 18;48(8):2415-23. doi: 10.1021/acs.accounts.5b00218. Epub 2015 Jul 23.
7
Molecular designs for controlling the local environments around metal ions.用于控制金属离子周围局部环境的分子设计。
Acc Chem Res. 2015 Aug 18;48(8):2407-14. doi: 10.1021/acs.accounts.5b00212. Epub 2015 Jul 16.
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Toward the synthesis of more reactive S = 2 non-heme oxoiron(IV) complexes.迈向更具反应性的 S = 2 非血红素氧代铁（IV）配合物的合成。
Acc Chem Res. 2015 Aug 18;48(8):2443-52. doi: 10.1021/acs.accounts.5b00244. Epub 2015 Jul 15.
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Exploring Mn-O bonding in the context of an electronically flexible secondary coordination sphere: synthesis of a Mn(III)-oxo.在电子柔性二级配位环境中探索锰-氧键：一种锰（III）-氧代物的合成。
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Ferryl protonation in oxoiron(IV) porphyrins and its role in oxygen transfer.氧代铁（IV）卟啉中的高铁质子化及其在氧转移中的作用。
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铁锰-碘代苯过氧配合物中远程氧化还原变化促进的氧原子转移和 C-H 键氧化。

Accelerated Oxygen Atom Transfer and C-H Bond Oxygenation by Remote Redox Changes in Fe Mn-Iodosobenzene Adducts.

机构信息

Department of Chemistry and Chemical Engineering, California Institute of Technology; MC 127-72, Pasadena, CA, 91125, USA.

Molecular Biophysics & Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.

出版信息

Angew Chem Int Ed Engl. 2017 Apr 18;56(17):4772-4776. doi: 10.1002/anie.201701319. Epub 2017 Mar 24.

DOI:10.1002/anie.201701319
PMID:28338266
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC5505263/
Abstract

We report the synthesis, characterization, and reactivity of [LFe (PhPz) OMn( PhIO)][OTf] (3: x=2; 4: x=3), where 4 is one of very few examples of iodosobenzene-metal adducts characterized by X-ray crystallography. Access to these rare heterometallic clusters enabled differentiation of the metal centers involved in oxygen atom transfer (Mn) or redox modulation (Fe). Specifically, Fe Mössbauer and X-ray absorption spectroscopy provided unique insights into how changes in oxidation state (Fe Fe Mn vs. Fe Mn ) influence oxygen atom transfer in tetranuclear Fe Mn clusters. In particular, a one-electron redox change at a distal metal site leads to a change in oxygen atom transfer reactivity by ca. two orders of magnitude.

摘要

我们报告了[LFe(PhPz)OMn(PhIO)][OTf]（3：x=2；4：x=3）的合成、表征和反应性，其中 4 是通过 X 射线晶体学表征的碘代苯醌-金属加合物的少数几个实例之一。获得这些罕见的杂金属簇使我们能够区分涉及氧原子转移（Mn）或氧化还原调节（Fe）的金属中心。具体来说，Fe Mössbauer 和 X 射线吸收光谱提供了独特的见解，了解氧化态变化（Fe Fe Mn 与 Fe Mn ）如何影响四核 Fe Mn 簇中的氧原子转移。特别是，在远端金属位点发生单电子氧化还原变化会导致氧原子转移反应性发生约两个数量级的变化。