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Preparation method and applications of MOF@MOF nanometer fiber composite catalyst

A composite catalyst and nanofiber technology, which is applied in the field of electrocatalysis and nanocomposite materials, can solve the problems of easy changes in the surrounding chemical environment, poor water stability of MOFs, and material loss of stability, and achieve good industrial prospects, low cost, and The effect of high yield

Inactive Publication Date: 2019-11-01
UNIV OF JINAN
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, MOFs still generally have defects such as poor water stability and poor chemical stability. The easy change of the surrounding chemical environment of the metal / metal coordination center in the MOFs framework structure is the direct cause of the loss of stability of the material.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0032] Example 1 Preparation method of MOF@MOF nanofiber composite catalyst

[0033] 0.8 mmol isophthalic acid H 3 The BTC ligand was dissolved in 4 mL of absolute ethanol and 4 mL of water, and ultrasonicated at 180 W for 1 min to obtain clear isophthalic acid H 3 BTC ligand solution;

[0034] 1.6 mmol Co(NO 3 ) 2 ·6H 2 O dissolved in 8 mL H 2 O, 180 W ultrasonic 1 min, to obtain a clear solution of cobalt nitrate;

[0035] 1.0 mmol of copper acetate, 1.0 mmol of terephthalic acid H 2 BDC ligand and 0.5 mmol of triethylenediamine dabco ligand were blended with 4 mL of N,N-dimethylformamide DMF to obtain a mixed solution of copper acetate-terephthalic acid-triethylenediamine;

[0036] Mix the isophthalic acid ligand solution and cobalt nitrate solution at room temperature, add 2.5 mL of 0.1 mol / L sodium carbonate solution, let stand at room temperature for 5 min, centrifuge, and wash with water and ethanol three times to obtain Co 3 (BTC) 2 12H 2 O nanofibrous materi...

Embodiment 2

[0040] Example 2 Preparation method of MOF@MOF nanofiber composite catalyst

[0041] 0.9 mmol isophthalic acid H 3 The BTC ligand was dissolved in 6 mL of absolute ethanol and 6 mL of water, and ultrasonicated at 180 W for 1 min to obtain clear isophthalic acid H 3 BTC ligand solution;

[0042] 1.8 mmol Co(NO 3 ) 2 ·6H 2 O dissolved in 12 mL H 2 O, 180 W ultrasonic 1 min, to obtain a clear solution of cobalt nitrate;

[0043] 1.1 mmol of copper acetate, 1.1 mmol of terephthalic acid H 2 BDC ligand and 0.55 mmol of triethylenediamine dabco ligand were blended with 6 mL of N,N-dimethylformamide DMF to obtain a mixed solution of copper acetate-terephthalic acid-triethylenediamine;

[0044] Mix the isophthalic acid ligand solution and cobalt nitrate solution at room temperature, add 5.0 mL of 0.1 mol / L sodium carbonate solution, let stand at room temperature for 7 min, centrifuge, and wash with water and ethanol three times to obtain Co 3 (BTC) 2 12H 2 O nanofibrous mate...

Embodiment 3

[0047] Example 3 Preparation method of a MOF@MOF nanofiber composite catalyst

[0048] 1.0 mmol isophthalic acid H 3 The BTC ligand was dissolved in 8 mL of absolute ethanol and 8 mL of water, and ultrasonicated at 180 W for 1 min to obtain clear isophthalic acid H 3 BTC ligand solution;

[0049] 2.0 mmol Co(NO 3 ) 2 ·6H 2 O dissolved in 16 mL H 2 O, 180 W ultrasonic 1 min, to obtain a clear solution of cobalt nitrate;

[0050] 1.2 mmol of copper acetate, 1.2 mmol of terephthalic acid H 2 BDC ligand and 0.6 mmol of triethylenediamine dabco ligand were blended with 7 mL of N,N-dimethylformamide DMF to obtain a mixed solution of copper acetate-terephthalic acid-triethylenediamine;

[0051] Mix the isophthalic acid ligand solution and cobalt nitrate solution at room temperature, add 7.5 mL of 0.1 mol / L sodium carbonate solution, let stand at room temperature for 10 min, centrifuge, and wash with water and ethanol three times to obtain Co 3 (BTC) 2 12H 2 O nanofibrous ma...

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PUM

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Abstract

The invention discloses a preparation method MOF@MOF nanometer fiber composite catalyst, and applications of the MOF@MOF nanometer fiber composite catalyst in catalysis of room temperature nitrogen gas into ammonia through reduction, and belongs to the technical field of electrocatalysis and nanometer composite material. The preparation method comprises following main steps: a 1,3,5-benzenetricarboxylic acid ligand solution, a cobalt nitrate solution, and a sodium carbonate solution are mixed to be uniform at room temperature so as to obtain a Co<3>(BTC)<2>*12H<2>O nanometer fiber material; the Co<3>(BTC)<2> nanometer fiber material and a copper acetate-terephthalic acid-triethylenediamine mixed solution are mixed so as to obtain a Co<3>(BTC)<2>*12H<2>O nanometer fiber epitaxial growth [Cu<2>(BDC)<2>(dabco)]DMF*3H<2>O composite material; and the composite material is placed in a microwave oven for 3min of activation at 250W so as to obtain the MOF@MOF nanometer fiber composite catalyst. The MOF@MOF nanometer fiber composite catalyst is used in catalysis of room temperature nitrogen gas into ammonia through reduction, the catalyst preparation cost is low, technology is simple, consumed time is short, and the industrial prospect is promising.

Description

technical field [0001] The invention discloses a preparation method of a MOF@MOF nanofiber composite catalyst and an application based on the catalyst for catalyzing the reduction of nitrogen at room temperature to ammonia, belonging to the fields of electrocatalysis technology, nanocomposite material technology and the like. Background technique [0002] Electrochemical nitrogen reduction to ammonia reaction is a method for producing ammonia from air and water via renewable electricity. Unlike the industrial Haber-Bosch process, where ammonia is synthesized from hydrogen and nitrogen at high temperature (400–500 °C) and pressure (200–300 atm), electrochemical nitrogen reduction to ammonia can be synthesized from nitrogen and electrons at ambient temperature. Despite tremendous current efforts, electrocatalysis for the selective and efficient reduction of nitrogen to ammonia remains unsatisfactory. Most of the catalysts are complex to prepare and show high overpotential, th...

Claims

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Application Information

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IPC IPC(8): B01J31/22B01J35/06C25B1/00C25B11/04B01J37/34
CPCB01J31/223C25B1/00B01J37/346B01J37/343B01J2531/16B01J2531/845C25B11/095B01J35/33B01J35/58B01J35/61
Inventor 侯莹匡轩
Owner UNIV OF JINAN
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