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Cr-based MOF carbon material catalyst co-doped with loaded nano-palladium particles, preparation of Cr-based MOF carbon material catalyst and application of catalyst in hydrogen production from formic acid

A nano-palladium and co-doping technology, applied in the direction of physical/chemical process catalysts, organic compounds/hydrides/coordination complex catalysts, hydrogen, etc., can solve the problems of poisoned catalysts and achieve the effect of solving the aggregation of metal particles

Active Publication Date: 2021-12-03
SOUTH CHINA UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the released CO will poison the catalyst, which is not desirable

Method used

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  • Cr-based MOF carbon material catalyst co-doped with loaded nano-palladium particles, preparation of Cr-based MOF carbon material catalyst and application of catalyst in hydrogen production from formic acid
  • Cr-based MOF carbon material catalyst co-doped with loaded nano-palladium particles, preparation of Cr-based MOF carbon material catalyst and application of catalyst in hydrogen production from formic acid
  • Cr-based MOF carbon material catalyst co-doped with loaded nano-palladium particles, preparation of Cr-based MOF carbon material catalyst and application of catalyst in hydrogen production from formic acid

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0043] (1) During the preparation process, in order to improve the solubility of the organic ligands in the solvent, NaOH was used as the MOF synthesis regulator. First, add 3.2000g Cr(NO 3 ) 3 9H 2 O and 60 mL of ultrapure water, magnetically stirred until the solids were completely dissolved; subsequently, 1.4400 g of 2-aminoterephthalic acid (NH 2 -HBDC), into which a chromium salt solution is injected. Next, add 0.6400g NaOH regulator under strong stirring, and use ultrasonic-stirring technology to fully mix the materials in the solvent; the solution turns gray-green, and ultrasonically disperses it in water for 30 minutes; then, the mixed material liquid Transfer to the polytetrafluoroethylene liner of the hydrothermal kettle, and place the hydrothermal kettle in a muffle furnace (programmed temperature rise rate 1°C / min) at a constant temperature of 150°C for 12h. After the temperature of the muffle furnace was slowly lowered to room temperature, the hydrothermal ket...

Embodiment 2

[0048] Example 1 was treated by two activation methods (5mol / L, 150°C NaOH solution or potassium bromate solution activation) and loaded with Pd metal to obtain Pd@Cr 2 o 3 -NPCB-850, take 50mg and put them into different flasks, set at 60°C, and after the system is stable for 5 minutes, inject 5mL of reaction liquid into the flask (the molar ratio of formic acid to sodium formate=1:3, formic acid 1mol / L; Or for formic acid 1mol / L), start stirring and start the mass flow meter. When the flow meter gas velocity is less than 5SCCM, stop the reaction and record the gas production. The experimental results found that the catalytic effect after NaOH treatment is the best, see figure 1 .

Embodiment 3-7

[0050] Referring to Example 1, the theoretical load of synthetic palladium is 10wt% Cr 2 o 3 -NPCB-T, (T represents the calcination temperature, and the parallel test temperatures are 550, 650, 750, 850, 950°C respectively). Pour 100mg of catalyst into the flask, set at 60°C, and after the system stabilizes for 5 minutes, inject 5mL of reaction solution into the flask (the molar ratio of formic acid to sodium formate = 1:3, formic acid 1mol / L), start stirring and start the mass flow count. When the flow meter gas velocity is less than 5SCCM, stop the reaction and record the gas production. It is found that under the same conditions, 850°C calcination has the best catalytic effect. For details, see figure 2 .

[0051] Table 1 Effect of carrier calcination temperature on hydrogen production from formic acid

[0052] Example 3 4 5 6 7 Calcination temperature / ℃ 550 650 750 850 950 TOF / h -1

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Abstract

The invention discloses a Cr-based MOF carbon material catalyst co-doped with loaded nano-palladium particles, preparation of the Cr-based MOF carbon material catalyst and an application of the Cr-based MOF carbon material catalyst in hydrogen production from formic acid. On the basis of NH2-MIL-101 (Cr) which is high in specific surface area and can be modified, a nitrogen and chromium oxide co-doped metal organic framework derived carbon material is obtained in an in-situ pyrolysis mode at the temperature of 550-950 DEG C, then palladium metal is loaded, and the Cr-based MOF carbon material catalyst co-doped and loaded with nano palladium particles is obtained. The obtained catalyst shows excellent hydrogen production in a formic acid / sodium formate catalysis system.

Description

technical field [0001] The invention belongs to the field of formic acid hydrogen production, and in particular relates to a Cr-based MOF carbon material catalyst co-doped with nano palladium particles and its preparation and application in formic acid hydrogen production. Background technique [0002] As an efficient and clean energy carrier with promising application prospects, hydrogen is expected to meet the growing energy challenges. Formic acid is widely considered as a hydrogen storage material with great application potential, however, the release and storage of hydrogen face several challenges that hinder the development of hydrogen economy. Formic acid (FA), as an ideal liquid hydrogen carrier, has attracted much attention due to its good stability, wide range of sources, high volume capacity (53.4 g / L) and high H content (4.4 wt%), and is an important liquid hydrogen storage materials. Formic acid dehydrogenation (FAD) occurs in HCOOH→H 2 +CO 2 In the pathway,...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/22B01J35/10C01B3/22
CPCB01J31/1691B01J31/223C01B3/22B01J2531/48B01J35/61
Inventor 常杰段加超朱小凡付严
Owner SOUTH CHINA UNIV OF TECH
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