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Synthetic and Structural Studies on a New Type of [Fe]‐Hydrogenase Mimics Each Containing One Hantzsch Ester Moiety
European Journal of Inorganic Chemistry ( IF 2.2 ) Pub Date : 2020-07-12 , DOI: 10.1002/ejic.202000523
Li-Cheng Song 1, 2 , Bei-Bei Liu 1 , Kai-Kai Xu 1
Affiliation  

To develop the synthetic methodology for [Fe]‐H2ase models, a new type of the Hantzsch ester moiety‐containing [Fe]‐H2ase models (1–7 ) has been synthesized on the basis of preparing a series of new 2,6‐disubstituted pyridine precursors (L1–L10 ). Thus, the iodo models [2‐COCH2‐6‐(HEH)C5H3N]Fe(CO)2I (1 ), {2‐COCH2‐6‐[C6H4(HEH)]C5H3N}Fe(CO)2I (2 ), and {2‐COCH2‐6‐[Me(HEH)]C5H3N}Fe(CO)2I (3 ) could be prepared by reactions of precursors 2‐TsOCH2‐6‐(HEH)C5H3N (L2 ), 2‐TsOCH2‐6‐[C6H4(HEH)]C5H3N (L6 ), and 2‐TsOCH2‐6‐[Me(HEH)]C5H3N (L10 ) with Na2Fe(CO)4 followed by treatment of the resulting Fe(0) intermediates M1 , M2 and M3 with iodine, respectively. In addition, further treatment of model 1 with AgOTf followed by reaction of the resulting Fe(II) intermediate M4 with MeCN gave the MeCN‐coordinated model {[2‐COCH2‐6‐(HEH)C5H3N]Fe(CO)2(MeCN)}(OTf) (4 ), whereas reaction of precursor L2 with Na2Fe(CO)4 followed by treatment of intermediate M1 with dimers (RCO2)2 afforded benzoato models [2‐COCH2‐6‐(HEH)C5H3N]Fe(CO)2(O2CR) (5 , R = 4‐ClC6H4; 6 , 2,6‐F2C6H3; 7 , 2‐F3CC6H4). All the new precursors L1 L10 and models 1 7 were characterized by various spectroscopic methods and for some of them by X‐ray crystallography.

中文翻译:

一种新型[Fe]-氢加氢酶模拟物的合成和结构研究,每个模拟物均包含一个汉茨酯部分

为了开发用于[Fe] -H 2酶模型的合成方法,在准备一系列新的方法的基础上,合成了一种新型的含汉茨基酯部分的[Fe] -H 2酶模型(1-7)。 2,6-二取代吡啶前体(L 1–L10)。因此,碘模型[2-COCH 2 -6((HEH)C 5 H 3 N] Fe(CO)2 I(1),{2-COCH 2 -6-6 [C 6 H 4(HEH​​)] C 5 H 3 N} Fe(CO)2 I(2)和{2-COCH 2 -6 [Me(HEH)] C 5 H3 N}的Fe(CO)2 I(3)可通过2- TsOCH前体的反应制备2 -6-(HEH)C 5 H ^ 3 N(L2),2- TsOCH 2 -6- [C 6 H ^ 4(HEH​​)] c ^ 5 ħ 3 N(L6),和2- TsOCH 2 -6- [我(HEH​​)] c ^ 5 ħ 3 N(L10)用Na 2的Fe(CO)4,接着处理所得到的Fe的(0)中间体M1M2M3分别用碘。此外,模型的进一步处理1用的AgOTf接着将得到的Fe(II)中间体的反应M4用MeCN得到的MeCN协调模型{[2- COCH 2 -6-(HEH)C 5 H ^ 3 N]的Fe( CO)2(MeCN中)}(OTF)(4),而前体的反应L2用Na 2的Fe(CO)4,接着处理中间的M1与二聚体(RCO 22,得到benzoato模型[2- COCH 2 -6 ‐(HEH)C 5 H 3 N] Fe(CO)2(O2 CR)(5,R = 4-CLC 6 ħ 4 ; 6,2,6-F 2 C ^ 6 ħ 3 ; 7,2-F 3 CC 6 H ^ 4)。所有新的前体L1L1017型都通过各种光谱方法进行了表征,其中一些通过X射线晶体学表征。
更新日期:2020-08-10
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