Novel reactions of homodinuclear Ni-2 complexes [Ni(RNPyS4)](2) with Fe-3(CO)(12) to give heterotrinuclear NiFe2 and mononuclear Fe complexes relevant to [NiFe]- and [Fe]-hydrogenases

Song Li-Cheng; Cao Meng; Wang Yong-Xiang

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Novel reactions of homodinuclear Ni-2 complexes [Ni(RNPyS4)](2) with Fe-3(CO)(12) to give heterotrinuclear NiFe2 and mononuclear Fe complexes relevant to [NiFe]- and [Fe]-hydrogenases

机译：同核Ni-2配合物[Ni（RNPyS4）]（2）与Fe-3（CO）（12）的新反应，得到与[NiFe]-和[Fe]-加氢酶有关的异三核NiFe2和单核Fe配合物

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The homodinuclear complexes [Ni(RNPyS4)](2) (1a-1e; RNPyS4 = 2,6-bis(2-mercaptophenylthiomethyl)-4-R-pyridine; R = H, MeO, Cl, Br, i-Pr) were found to be prepared by reactions of the in situ generated Li-2[Ni-(1,2-S2C6H4)(2)] with 2,6-bis[(tosyloxy)methyl]pyridine and its substituted derivatives 2,6-bis[(tosyloxy)-methyl]-4-R-pyridine. Further reactions of 1a-1e with Fe-3(CO)(12) gave both heterotrinuclear complexes NiFe2(RNPyS4)(CO)(5) (2a-2e) and mononuclear complexes Fe(RNPyS4)(CO) (3a-3e), unexpectedly. Interestingly, complexes 2a-2e and 3a-3e could be regarded as models for the active sites of [NiFe]- and [Fe]-hydrogenases, respectively. All the prepared complexes were characterized by elemental analysis, spectroscopy, and particularly for some of them, by X-ray crystallography. In addition, the electrochemical properties of 2a-2e and 3a-3e as well as the electrocatalytic H-2 production catalyzed by 2a-2e and 3a-3e were investigated by CV techniques.

机译：同核复合物[Ni（RNPyS4）]（2）（1a-1e; RNPyS4 = 2,6-双（2-巯基苯硫甲基）-4-R-吡啶; R = H，MeO，Cl，Br，i-Pr）被发现是通过原位生成的Li-2 [Ni-（1,2-S2C6H4）（2）]与2,6-双[（甲苯磺酰氧基）甲基]吡啶及其取代衍生物2,6-的反应制备的双[（甲苯磺酰氧基）-甲基] -4-R-吡啶。 1a-1e与Fe-3（CO）（12）的进一步反应生成异三核配合物NiFe2（RNPyS4）（CO）（5）（2a-2e）和单核配合物Fe（RNPyS4）（CO）（3a-3e），出乎意料。有趣的是，复合物2a-2e和3a-3e可以分别视为[NiFe]-和[Fe]-氢化酶活性位点的模型。所有制备的配合物均通过元素分析，光谱法进行表征，尤其是对其中某些配合物通过X射线晶体学进行表征。此外，通过CV技术研究了2a-2e和3a-3e的电化学性质以及2a-2e和3a-3e催化的H-2产生的电催化作用。

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《Dalton transactions: An international journal of inorganic chemistry》 |2015年第15期|共12页
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Song Li-Cheng; Cao Meng; Wang Yong-Xiang;
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1. Novel reactions of homodinuclear Ni-2 complexes [Ni(RNPyS4)](2) with Fe-3(CO)(12) to give heterotrinuclear NiFe2 and mononuclear Fe complexes relevant to [NiFe]- and [Fe]-hydrogenases [J] . Song Li-Cheng, Cao Meng, Wang Yong-Xiang Dalton transactions: An international journal of inorganic chemistry . 2015,第15期

机译：同核Ni-2配合物[Ni（RNPyS4）]（2）与Fe-3（CO）（12）的新反应，得到与[NiFe]-和[Fe]-加氢酶有关的异三核NiFe2和单核Fe配合物
2. Reactions of dinuclear Ni2 complexes [Ni(RNPyS4)]2 (RNPyS4 = 2,6-bis(2-mercaptophenylthiomethyl)-4-R-pyridine) with Fe(CO)3(BDA) (BDA = benzylidene acetone) leading to heterodinuclear NiFe and mononuclear Fe complexes related to the active sites of [NiFe]- and [Fe]-hydrogenases [J] . Li-Cheng Song, Yu Lu, Meng Cao, RSC Advances . 2016,第45期

机译：二核Ni2配合物的反应[Ni（RNPYS4）] 2（RNPYS4 = 2,6-双（2-巯基苯基甲基）-4-R-吡啶）用Fe（CO）3（BDA）（BDA =苄基丙酮）导致异核核与[NiFe] - 和[Fe] - 氢酶的活性位点相关的NiFe和单核Fe复合物相关
3. Synthesis, characterization and some properties of mononuclear Ni and trinuclear NiFe _2 complexes related to the active site of [NiFe]-hydrogenases [J] . Song L.-C., Sun X.-J., Zhao P.-H., Dalton transactions: An international journal of inorganic chemistry . 2012,第29期

机译：与[NiFe]-加氢酶活性位点有关的单核Ni和三核NiFe _2配合物的合成，表征和某些性质
4. Artificial hydrogenases: Utilization of peptide and redox non-innocent ligands in FeFe and NiFe complexes [C] . Souvik Roy, Lu Gan, Arnab Dutta National Meeting Exhibition . 2013

机译：人工氢酶：利用肽和氧化还原非无辜配体在Fefe和NiFe复合物中的用途
5. Synthesis and characterization of nickel-thiolate complexes as a model of the active site of (Ni-Fe) hydrogenase enzymes. [D] . Nguyen, Dao Hinh. 1997

机译：镍硫醇盐配合物的合成和表征，作为（Ni-Fe）氢化酶活性位点的模型。
6. Thiolate-bridged dinuclear iron(tris-carbonyl)–nickel complexes relevant to the active site of NiFe hydrogenase [O] . Yasuhiro Ohki, Kazunari Yasumura, Katsuaki Kuge, 2008

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7. Mononuclear Nickel(III) and Nickel(II) Thiolate Complexes with Intramolecular S-H Proton Interacting with Both Sulfur and Nickel: Relevance to the NiFe/NiFeSe Hydrogenases [O] . -1

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Novel reactions of homodinuclear Ni-2 complexes [Ni(RNPyS4)](2) with Fe-3(CO)(12) to give heterotrinuclear NiFe2 and mononuclear Fe complexes relevant to [NiFe]- and [Fe]-hydrogenases

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