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Nickel-iron hydrogenase model substance, ionic nickel-iron hydrogenase model substance, preparation method and application thereof

A technology of nickel-iron hydrogenase and model substance, applied in organic compound/hydride/coordination complex catalysts, chemical instruments and methods, chemical/physical processes, etc., can solve structural instability, lack of catalytic activity, hindering Biomimetic enzyme hydrogen production development and other issues, to achieve the effect of stable crystal structure, easy implementation and mild reaction conditions

Active Publication Date: 2022-04-05
LUDONG UNIVERSITY
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0005] In view of this, the object of the present invention is to provide nickel-iron hydrogenase model substance, ionic nickel-iron hydrogenase model substance and preparation method and application, to solve the problem that most imitative enzyme model substances in the prior art do not possess catalytic activity, and a few have activity The complexes, whose structure is unstable, etc., hinder the technical problems of the development of biosimilar enzyme hydrogen production

Method used

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  • Nickel-iron hydrogenase model substance, ionic nickel-iron hydrogenase model substance, preparation method and application thereof
  • Nickel-iron hydrogenase model substance, ionic nickel-iron hydrogenase model substance, preparation method and application thereof
  • Nickel-iron hydrogenase model substance, ionic nickel-iron hydrogenase model substance, preparation method and application thereof

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preparation example Construction

[0053] For the nickel-iron hydrogenase model substance described above, the second aspect of the embodiment of the present invention provides a method for preparing the nickel-iron hydrogenase model substance, comprising the following steps:

[0054] S100, preparing the first intermediate product

[0055] NiCl 2 ·6H 2 O and NiCl 2 ·6H 2 The 2-(2-pyridine)-benzimidazole of the amount of substance such as O joins in the ethanol ethanol, after stirring at room temperature, decompression suction filtration obtains the first intermediate product; Wherein the molecular formula of the first intermediate product is Ni[N 2 ]Cl 2 , its chemical structure is:

[0056]

[0057] The reaction process of step S100 is as follows:

[0058]

[0059] In the reaction process of step S100, due to NiCl 2 ·6H 2 O coordination H 2 O is easy to leave, forming a vacant site, the reaction with the dinitrogen-containing conjugated ligand is spontaneous, and the first intermediate product p...

Embodiment 1

[0112] The first intermediate product is prepared by the following preparation method:

[0113] 1.19g or 5mmol of NiCl 2 ·6H 2 O and 0.98g, that is, 5mmol of 2-(2-pyridine)-benzimidazole were added to a 250mL round-bottomed flask containing magnetons, 100mL of ethanol was added, and after stirring at room temperature for 5h, after heating to 40°C, suction filtration under reduced pressure, The first intermediate product Ni[N] in the form of light green powder can be obtained 2 ] Cl 2 ; Wherein the first intermediate product Ni[N 2 ] Cl 2 The yield of is 1.5 g, the yield is 93%.

Embodiment 2

[0115] Model 1 was prepared by the following preparation steps:

[0116] in N 2 Under protection, the first intermediate product Ni[N 2 ] Cl 2 With 616mg or 1mmol of Fe(pdt)(CO) 2 (dppe) was dissolved in 50 mL of anhydrous acetone, stirred at room temperature for 10 min, and 120 mg (1.1 mmol) of NaBF was added 4 , after reacting for 2h, filter, vacuum dry to remove anhydrous acetone, obtain model 1, the molecular formula of model 1 is (dppe)(CO)Fe(μ-SCH 2 CH 2 CH 2 S)(μ-Cl)Ni[N 2 ](BF 4 );

[0117] Among them, model substance 1 is a reddish-brown powder, and its yield is 790 mg, and the yield rate is 80%.

[0118] combine Figure 2 to Figure 3 , the characterization data of model object 1 are as follows: FI-IR(acetone,ν CO ):1938cm -1 ; 31 P{ 1 H} NMR (202MHz, acetone): dd peak, 63, 48ppm.

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Abstract

The invention discloses a nickel-iron hydrogenase model substance. The chemical structural formula of the nickel-iron hydrogenase model substance is as follows: wherein, the nickel-iron hydrogenase model substance is composed of a mononuclear nickel structural unit and a mononuclear iron structure A bimetallic complex in which units are bridged by disulfide ligands, iron atoms and nickel atoms are connected by metal bonds, a diphosphine ligand and a carbonyl group are connected to the iron atom, and a dinitrogen-containing covalent compound is connected to the nickel atom Conjugated ligand; The bisphosphine ligand is 1,2-bisdiphenylphosphine ethane; The dinitrogen-containing conjugated ligand [N 2 ] is 2-(2-pyridine)-benzimidazole; the disulfide ligand is 1,3-propanedithiol; the nickel-iron hydrogenase model substance has catalytic activity and is a good imitation enzyme model catalyst , its crystal structure is stable, and the use of cheap metal nickel and metal iron can reduce costs and is economical.

Description

technical field [0001] The invention belongs to the technical field of new energy materials, and in particular relates to a nickel-iron hydrogenase model substance, an ionic nickel-iron hydrogenase model substance, a preparation method and an application. Background technique [0002] With the growth of population, the aggravation of environmental pollution and the reduction of mineral energy, the development of clean energy to replace traditional energy has become the general trend. Among these clean energy sources, hydrogen, with its high heat of combustion, is pollution-free after combustion and only releases H 2 O, renewable and other advantages, and has been widely concerned by everyone. [0003] At present, most of the hydrogen production methods in the industry are electrolysis of water and fossil energy gasification. The hydrogen production technology of electrolysis of water consumes a lot of energy and requires a high amount of electricity. level of demand. Hydr...

Claims

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Application Information

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IPC IPC(8): B01J31/24C07F19/00C25B1/02C25B11/085
CPCB01J31/2409C07F15/045C25B1/02C25B11/04B01J2531/842B01J2531/847B01J35/33
Inventor 初晓晓逄茂甫杨正龙马松梅李涛赵孟燊吴繁华
Owner LUDONG UNIVERSITY
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