Catalytic oxygen production system containing duplex pyridine ruthenium (II) complex, preparation method of duplex pyridine ruthenium (II) complex and oxygen production method

A technology of ruthenium bipyridine and complexes is applied in the field of oxygen production in catalytic systems, and can solve the problems of poor catalyst stability, catalyst deactivation, and no Ca atoms obtained.

Active Publication Date: 2014-11-19
TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

In 2001, Witt, Saenger et al. first obtained the resolution of The three-dimensional crystal structure of OEC obtained the size, shape and distribution information of Mn clusters, but did not obtain the position of Ca atoms
In 2012, the Sun group reported the most efficient oxygen production system, namely [Ru(bda)(isoq) 2 ](H 2 bda=2,2’-bipyridine-6,6’-dicarboxylic acid;isoq=isoquinoline) (TOF=303s -1 ), but the lifetime of this WOC is only 5 minutes (see Nat.Chem.2012, 4, 418-423)
[0006] The above research results are of great significance for the development of thermocatalytic and photocatalytic oxygen production systems, but the common problems of these systems are poor catalyst stability and catalyst deactivation caused by the decomposition of organic ligands in the process of catalytic oxygen production.

Method used

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  • Catalytic oxygen production system containing duplex pyridine ruthenium (II) complex, preparation method of duplex pyridine ruthenium (II) complex and oxygen production method
  • Catalytic oxygen production system containing duplex pyridine ruthenium (II) complex, preparation method of duplex pyridine ruthenium (II) complex and oxygen production method
  • Catalytic oxygen production system containing duplex pyridine ruthenium (II) complex, preparation method of duplex pyridine ruthenium (II) complex and oxygen production method

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0058] A catalytic oxygen generation system containing bipyridyl ruthenium (Ⅱ) complex: the concentration of bipyridyl ruthenium (Ⅱ) complex is 2.0×10 -4 mol / L; the concentration of ammonium cerium nitrate is 0.6mol / L; the concentration of trifluoromethanesulfonic acid is 0.2mol / L; the solvent is water; the total sample volume is 4mL.

[0059]The method of preparing oxygen by using the above-mentioned thermal catalytic oxygen generation system is: stir the sample at room temperature, and monitor the amount of oxygen generated in the sample by the drainage method; after stirring for 4 hours, the calculated oxygen production of the sample is about 17.6mL (TON=979) ; Indicating that the system was stable during the first 4 hours of reaction.

[0060] The bipyridine ruthenium (II) complex is a compound with the following molecular formula (F2):

[0061]

Embodiment 2

[0063] A catalytic oxygen generation system containing bipyridyl ruthenium (Ⅱ) complex: the concentration of bipyridyl ruthenium (Ⅱ) complex is 2.0×10 -4 mol / L; the concentration of ceric ammonium nitrate is 0.6mol / L; the concentration of trifluoromethanesulfonic acid is 0.2mol / L; the solvent is water and acetonitrile; the volume ratio of water and acetonitrile is 9:1; the total sample volume is 4mL.

[0064] The method of preparing oxygen by using the above thermocatalytic oxygen generation system is: stir the sample at room temperature, and monitor the amount of oxygen generated in the sample by the drainage method; after stirring for 4 hours, the calculated oxygen production of the sample is about 15.6mL (TON=868) ; Indicating that the system was stable during the first 4 hours of reaction.

[0065] The bipyridyl ruthenium (II) complex and the bipyridyl ruthenium (II) complex in Example 1 are the same substance.

Embodiment 3

[0067] A catalytic oxygen generation system containing bipyridyl ruthenium (Ⅱ) complex: the concentration of bipyridyl ruthenium (Ⅱ) complex is 2.0×10 -4 mol / L; the concentration of ammonium cerium nitrate is 0.6mol / L; the concentration of trifluoromethanesulfonic acid is 0.2mol / L; the solvent is water and DMF; the volume ratio of water and DMF is 9:1; the total sample volume is 4mL.

[0068] The method of preparing oxygen by using the above thermocatalytic oxygen generation system is: stir the sample at room temperature, and monitor the amount of oxygen generated in the sample by the drainage method; after stirring for 5 hours, the calculated oxygen production of the sample is about 3.0mL (TON=166) ; Indicating that the system was stable during the first 5 hours of reaction.

[0069] The bipyridyl ruthenium (II) complex and the bipyridyl ruthenium (II) complex in Example 1 are the same substance.

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Abstract

The invention discloses a catalytic system containing a duplex pyridine ruthenium (II) complex, which includes a duplex pyridine ruthenium (II) complex, an oxidizing agent and a solvent. The invention further discloses a preparation method of the duplex pyridine ruthenium (II) complex, and an oxygen production method utilizing the catalytic system. The catalytic system can realize efficient catalytic oxygen production, and is simple to operate, good in repeatability and high in oxygen production efficiency; and the system is high in stability, the oxygen production amount is calculated to be up to 783mumol based on the total volume of the system, which is 4ml, the oxygen conversion number is calculated to be 979 based on a catalyst, and the system service life is as long as 8 hours.

Description

technical field [0001] The invention relates to a catalyst based on bipyridine ruthenium (II), a preparation method, and a method for producing oxygen in a catalytic system containing the catalyst. Background technique [0002] In order to solve the sharp contradiction between the ever-increasing energy demand and the increasingly serious environmental pollution, people are exploring a variety of renewable energy sources. Nature itself faces and solves energy problems through photosynthesis, that is, converting carbon dioxide into carbohydrates through light to store energy, while water serves as a continuous electron donor. So people were inspired and designed artificial water splitting system. A complete water splitting system consists of two half-reactions: 1) proton reduction and 2) water oxidation. Compared with the proton reduction reaction, the water oxidation reaction is more energy demanding, so the water oxidation reaction is generally considered to be a bottlene...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/22C07F15/00C01B13/02
Inventor 吴骊珠杨冰邢令宝简经鑫佟振合
Owner TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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