Method for catalyzing formic acid dehydrogenation by using PdAu nanosheet catalyst under visible light

A technology for catalyzing formic acid and nanosheets, applied in chemical instruments and methods, physical/chemical process catalysts, metal/metal oxide/metal hydroxide catalysts, etc., can solve problems such as difficult to separate and recycle and limit large-scale application, To achieve the effect of improved catalytic activity

Inactive Publication Date: 2019-12-13
ANHUI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although homogeneous catalysts exhibit excellent catalytic performance, their difficulty in separation and recycling greatly limits their large-scale applications.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0025] Catalyst preparation process

[0026] Grind and mix 3g of melamine and 12g of lithium chloride uniformly, roast at 520°C for 7h under nitrogen atmosphere, wash the roasted mixture with water at 20°C for 50h, and dry to obtain g-C3 N 4 Nanosheet; Weigh 1gTi 2 AlC was placed in 30wt% HF solution for 6.0h, filtered, washed and dried to obtain Ti 2 C; 0.1mmolTi 2 C and 2mmol g-C 3 N 4 Nanosheets were placed in 40mL deionized water, and NaHSO was added 3 , adjusted to NaHSO 3 The concentration is 0.03mol / L, the hydrothermal synthesis temperature is 120°C, and the hydrothermal synthesis time is 12h, to obtain (Mxene-TiO 2 ) 1 / 20 @g-C 3 N 4 Nanosheets, weighed 20mmol (Mxene-TiO 2 ) 1 / 20 @g-C 3 N 4 Nanosheets were placed in a solution containing 1mmol palladium chloride and 0.1mmol chloroauric acid, and reduced with 0.05mol / L formaldehyde solution at 10°C for 8h to obtain a catalyst, which was denoted as PdAu 0.1 / (Mxene-TiO 2 ) 1 / 20 @g-C 3 N 4 Nanosheet catal...

Embodiment 2

[0030] Catalyst preparation process

[0031] Grind and mix 3g of melamine and 24g of lithium chloride uniformly, roast at 550°C for 4h under a nitrogen atmosphere, wash the roasted mixture with water at 20°C for 50h, and dry to obtain g-C 3 N 4 Nanosheet; Weigh 1gTi 2 AlC is placed in 50wt% HF solution for 4.0h, filtered, washed and dried to obtain Ti 2 C; 0.1mmolTi 2 C and 3.5 mmol g-C 3 N 4 Nanosheets were placed in 40mL deionized water, and NaHSO was added 3 , adjusted to NaHSO 3 The concentration is 0.05mol / L, the hydrothermal synthesis temperature is 150°C, and the hydrothermal synthesis time is 8h, to obtain (Mxene-TiO 2 ) 1 / 35 @g-C 3 N 4 Nanosheets, weighed 25mmol (Mxene-TiO 2 ) 1 / 35 @g-C 3 N 4 Nanosheets were placed in a solution containing 1mmol palladium chloride and 0.3mmol chloroauric acid, and reduced with 0.09mol / L formaldehyde solution at 10°C for 5h to obtain a catalyst, which was denoted as PdAu 0.3 / (Mxene-TiO 2 ) 1 / 35 @g-C 3 N 4 Nanosheet ...

Embodiment 3

[0035] Catalyst preparation process

[0036] Grind and mix 3g of melamine and 21g of lithium chloride uniformly, roast at 540°C for 6h under a nitrogen atmosphere, wash the roasted mixture with water at 30°C for 43h, and dry to obtain g-C 3 N 4 Nanosheet; Weigh 1gTi 2 AlC was placed in 45wt% HF solution for 4.5h, filtered, washed and dried to obtain Ti 2 C; 0.1mmolTi 2 C and 2.5 mmol g-C 3 N 4 Nanosheets were placed in 40mL deionized water, and NaHSO was added 3 , adjusted to NaHSO 3 The concentration is 0.04mol / L, the hydrothermal synthesis temperature is 140°C, and the hydrothermal synthesis time is 10h, (Mxene-TiO 2 ) 1 / 25 @g-C 3 N 4 Nanosheets, weighed 23mmol (Mxene-TiO 2 ) 1 / 25 @g-C 3 N 4 Nanosheets were placed in a solution containing 1mmol palladium chloride and 0.2mmol chloroauric acid, and reduced with 0.05mol / L formaldehyde solution at 25°C for 6h to obtain a catalyst, which was denoted as PdAu 0.2 / (Mxene-TiO 2 ) 1 / 25 @g-C 3 N 4 Nanosheet catalyst...

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Abstract

The invention discloses a method for catalyzing formic acid dehydrogenation by using a PdAu nanosheet catalyst under visible light, and belongs to the technical field of chemistry and chemical engineering. The method comprises the following steps: putting the prepared PdAu nanosheet catalyst into a jacketed reactor, controlling the reaction to be carried out at a certain temperature through a constant-temperature circulating tank, irradiating a reaction solution from the upper part of the jacketed reactor with the visible light, then adding a mixed solution of formic acid and sodium formate into the reactor, carrying out a reaction, and collecting generated hydrogen by adopting a drainage method. Different from the traditional supported catalyst, the high-activity and high-selectivity supported PdAu nanosheet catalyst for hydrogen production by photocatalytic formic acid dehydrogenation can be prepared by adjusting the contents of metal palladium and gold in the catalyst and the content of Mxene-TiO2. When the catalyst is used for visible light formic acid dehydrogenation reaction, the dehydrogenation conversion rate and selectivity are both 100%, the TOF value of the reaction is greater than 850h <-1 >, and after the catalyst is recycled for 8h, the TOF value of the reaction is still greater than 834h <-1 >.

Description

technical field [0001] The invention belongs to the technical field of chemistry and chemical engineering, in particular to the use of PdAu / TiO 2 @g-C 3 N 4 Nanosheet catalyst visible light catalyzed method for formic acid dehydrogenation. Background technique [0002] Hydrogen is an efficient, clean, and green energy, but hydrogen has very low volumetric energy density and mass energy density. Efficient and safe storage and transportation of hydrogen has become a major challenge for hydrogen energy utilization. In order to solve this problem, researchers have developed and explored a variety of different types of hydrogen storage materials, among which formic acid has attracted extensive attention from researchers because of its non-toxic, high mass energy density, and safe storage and transportation. [0003] The key to the current application of formic acid as a hydrogen storage material lies in the development of efficient dehydrogenation catalysts. At present, the ca...

Claims

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Application Information

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IPC IPC(8): C01B3/22B01J27/24B01J23/52
CPCC01B3/22B01J27/24B01J23/52C01B2203/107B01J35/399B01J35/39Y02P20/584
Inventor 万超周柳王嘉佩吴胜华许立信张代林
Owner ANHUI UNIVERSITY OF TECHNOLOGY
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