Disparate reactivity from isomeric {Me2C(CH2N=CHPY)(2)} and {Me2C(CH=NCH2PY)(2)} chelates in iron complexation

Hulley Elliott B.; Williams Valerie A.; Morris Wesley D.; Wolczanski Peter T.; Hernandez-Burgos Kenneth; Lobkovsky Emil B.; Cundari Thomas R.

首页> 外文期刊>Polyhedron: The International Journal for Inorganic and Organometallic Chemistry >Disparate reactivity from isomeric {Me2C(CH2N=CHPY)(2)} and {Me2C(CH=NCH2PY)(2)} chelates in iron complexation

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Disparate reactivity from isomeric {Me2C(CH2N=CHPY)(2)} and {Me2C(CH=NCH2PY)(2)} chelates in iron complexation

机译：与{Me2C（CH2N = CHPY）（2）}和{Me2C（CH = NCH2PY）（2）}螯合物在铁络合物中的反应性不同

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Cyclizations of R2C(HCNCH2(2-py))(2) (R-2 = Me-2, dmp(PM)(2); R-2 = (CH2)(4), cpp(PM)(2)) to 4,4-dimethyl-2-(pyridin-2-yl)-N-(pyridin-2-ylmethylene)pyrrolidin-3-amine and 3-(pyridin-2-yl)-N-(pyridin-2-ylmethylene)-2-azaspiro-[4.4]-nonan-4-amine, respectively, were catalyzed by 10 mol% Fe{N(TMS)(2)}(2)(THF). A complex with the stoichiometry {Me2C(HCNCH2(2-py))(CHCNCH(2-py))}FeN(TMS)(2) (2-N(TMS)(2)) was shown to be catalytically competent. In contrast, the isomer Me2C(CH2NCH(2-py)H)(2) (dmp(PI)(2)) did not cyclize nor isomerize with Fe{N(TMS)(2)}(2)(THF), but generated {dmp(PI)(2)}FePMe3 (Fe-PMe3) when treated with (Me3P)(3)HFe(eta(2)-PMe2CH2). Calculations of Fe-L (L = PMe3, CO) support the electronics suggested by the metrics of its crystal structure, which revealed the chelate to be {dmp(PI)(2)}(2-) ligated to Fe(II). Electrochemical and brief reactivity studies were consistent with redox activity occurring at the chelate ligand, while the iron likely remains Fe(II). (C) 2014 Elsevier Ltd. All rights reserved.

机译：R2C（HCNCH2（2-py））（2）的环化（R-2 = Me-2，dmp（PM）（2）; R-2 =（CH2）（4），cpp（PM）（2））到4,4-二甲基-2-（吡啶-2-基）-N-（吡啶-2-基亚甲基）吡咯烷-3-胺和3-（吡啶-2-基）-N-（吡啶-2-基亚甲基））-2-氮杂螺-[4.4]-壬基-4-胺分别由10 mol％Fe {N（TMS）（2）}（2）（THF）催化。化学计量为{Me2C（HCNCH2（2-py））（CHCNCH（2-py））} FeN（TMS）（2）（2-N（TMS）（2））的配合物具有催化活性。相反，异构体Me2C（CH2NCH（2-py）H）（2）（dmp（PI）（2））没有环化或与Fe {N（TMS）（2）}（2）（THF）异构化，但在用（Me3P）（3）HFe（eta（2）-PMe2CH2）处理时生成{dmp（PI）（2）} FePMe3（Fe-PMe3）。 Fe-L（L = PMe3，CO）的计算支持了其晶体结构指标所建议的电子学，揭示了螯合物{dmp（PI）（2）}（2-）与Fe（II）连接。电化学和简短的反应性研究与螯合配体上发生的氧化还原活性一致，而铁可能仍为Fe（II）。（C）2014 Elsevier Ltd.保留所有权利。

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《Polyhedron: The International Journal for Inorganic and Organometallic Chemistry》 |2014年第null期|共10页
作者
Hulley Elliott B.; Williams Valerie A.; Morris Wesley D.; Wolczanski Peter T.; Hernandez-Burgos Kenneth; Lobkovsky Emil B.; Cundari Thomas R.;
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正文语种 eng
中图分类无机化学;
关键词
Iron; Redox non-innocence; Cyclization; Catalysis; Amide;

机译：铁氧化还原无毒环化催化酰胺;

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1. Disparate reactivity from isomeric {Me2C(CH2N=CHPY)(2)} and {Me2C(CH=NCH2PY)(2)} chelates in iron complexation [J] . Hulley Elliott B., Williams Valerie A., Morris Wesley D., Polyhedron: The International Journal for Inorganic and Organometallic Chemistry . 2014,第Null期

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Disparate reactivity from isomeric {Me2C(CH2N=CHPY)(2)} and {Me2C(CH=NCH2PY)(2)} chelates in iron complexation

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