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a co 4 o 4 Preparation method and application of cobalt-based metal-organic framework compound with quasi-cubane structure

A technology of organic frameworks and compounds, applied in the preparation method and application field of cobalt-based metal-organic framework catalysts, can solve the problems of unfavorable mechanism research and practical application, poor stability, etc., and achieve easy large-scale promotion and application, easy operation, and good application foreground effect

Active Publication Date: 2022-06-03
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Abstract
  • Description
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Problems solved by technology

Moreover, the natural oxygen production center and Mn 4 Ca-clusters are less stable in water, which is not conducive to mechanistic studies and practical applications

Method used

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  • a co <sub>4</sub> o <sub>4</sub> Preparation method and application of cobalt-based metal-organic framework compound with quasi-cubane structure
  • a co <sub>4</sub> o <sub>4</sub> Preparation method and application of cobalt-based metal-organic framework compound with quasi-cubane structure
  • a co <sub>4</sub> o <sub>4</sub> Preparation method and application of cobalt-based metal-organic framework compound with quasi-cubane structure

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Experimental program
Comparison scheme
Effect test

Embodiment 1

[0045] (E)-4,4',4",4"'-(N,N,N',N'-tetraphenyl-p-diaminoazobenzene in azo-linked triphenylamine carboxylic acid derivatives ) formic acid C 40 H 28 N 4 O 8 (17.3 mg, 0.025 mmol), CoCl 2 ·6H 2 O (24.0 mg, 0.10 mmol) was dissolved in N,N'-dimethylformamide (4 mL) and deionized water (2 mL) and stirred well, then the solution was taken and placed in an oven, calcined at 130 °C for 72 h, Turn off the oven, cool to room temperature, reddish-brown transparent diamond-like crystals are produced, filter, and dry to obtain the target material Co-L with a yield of about 56%. Infrared spectral peak positions (IR): 3426(w), 2930(w), 1680(s), 1647(vs), 1592(vs), 1500(m), 1392(vs), 1315(vs), 1264( m), 1179(m), 1147(s), 1101(w), 843(m), 786(s), 701(w), 560(m), 521(w), 472(w)cm -1 . The obtained target material structure is as figure 1 , figure 2 , image 3 and Figure 4 shown. Figure 1-4 The specific structure of the target material is given, from figure 1 In a, it can be see...

Embodiment 2

[0047] (E)-4,4',4",4"'-(N,N,N',N'-tetraphenyl-p-diaminoazobenzene in azo-linked triphenylamine carboxylic acid derivatives ) formic acid C 40 H 28 N 4 O 8 (17.3mg, 0.025mmol), Co(NO 3 ) 2 ·6H 2 O (30.0 mg, 0.10 mmol) was dissolved in N,N'-dimethylformamide (4 mL) and deionized water (2 mL) and stirred well, then the solution was taken and placed in an oven, calcined at 130 °C for 72 h, Turn off the oven, cool down to room temperature, reddish-brown transparent diamond-like crystals are produced, filter, and dry to obtain the target material Co-L with a yield of about 49%.

Embodiment 3

[0049] (E)-4,4',4",4"'-(N,N,N',N'-tetraphenyl-p-diaminoazobenzene in azo-linked triphenylamine carboxylic acid derivatives ) formic acid C 40 H 28 N 4 O 8 (34.6 mg, 0.05 mmol), CoCl 2 ·6H 2 O (48.0 mg, 0.20 mmol) was dissolved in N,N'-dimethylformamide (80 mL) and deionized water (40 mL) and stirred well, and then the solution was placed in a 250 mL eggplant-shaped flask at 130° C. Heating under reflux for 24 h, stopping heating and cooling to room temperature, filtering and drying to obtain an orange powder, the target material Co-L with a micron size was obtained. The scanning electron microscope (SEM) image of the obtained micron-sized target material is as follows Figure 9 shown.

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Abstract

The invention discloses a Co-containing 4 o 4 The preparation method and application of the cobalt-based metal-organic framework catalyst of the quasi-cubane structure, the present invention uses the triphenylamine carboxylic acid derivative L containing the azo functional group as the bridging ligand, and the Co in the transition metal salt Tm 2+ As metal nodes, Co-containing 4 o 4 The three-dimensional metal-organic framework compound Tm-L with a quasi-cubane structure, the metal-organic framework Tm-L not only simulates the natural oxygen-generating active center in structure, but also realizes the heterogeneity of homogeneous catalysts; at the same time, azotriphenylamine-derived carboxylic acid The hydrophobicity of the ligand and its relationship with Co 4 o 4 The semi-open space composed of clusters can ensure the water stability of the catalyst while enhancing the entry of water molecules and the contact with the catalytic active sites. The experiments of heterogeneous photocatalytic water splitting for oxygen and hydrogen production show that the metal-organic framework material Tm-L involved in the present invention is a good bifunctional cocatalyst and has a good application prospect in the field of photocatalytic water splitting.

Description

technical field [0001] The present invention relates to a Co-containing 4 O 4 The invention discloses a preparation method and application of a cobalt-based metal-organic framework catalyst with a pseudocubicane structure, and belongs to the technical field of catalytic materials. Background technique [0002] With the rapid development of human society and the increasing degree of industrialization, the severe global climate problems and environmental pollution problems caused by the extensive use of fossil fuels have followed. Therefore, finding clean and efficient renewable energy to replace traditional fossil energy has become a research hotspot and difficulty in today's society. Artificial photosynthesis simulates the water splitting process of natural photosynthesis and converts solar energy into chemical energy. It is a very promising renewable energy utilization technology. A typical water splitting process requires the coupling of two half-reactions: (1) water ox...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J31/22B01J31/28C01B3/04C01B13/02C07C245/08
CPCB01J35/004B01J31/1691B01J31/2239B01J31/28C01B3/042C01B13/0207C07C245/08C07C253/30C01B2203/0277C01B2203/1052B01J2231/70B01J2231/62B01J2531/845C07C255/58Y02E60/36
Inventor 章福祥郭向阳刘利芳肖宇肖晔珺祁育
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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