Method for catalyzing dehydrogenation of formic acid through NiAgPd/porous CexCuyOz nano catalyst

A nano-catalyst and formic acid technology, applied in the direction of heterogeneous catalyst chemical elements, physical/chemical process catalysts, metal/metal oxide/metal hydroxide catalysts, etc., can solve environmental pollution and other problems, achieve high activity, and operate easy effect

Inactive Publication Date: 2019-03-12
ANHUI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

In particular, the large-scale utilization of traditional fossil energy has caused increasingly serious environmental pollution. The above problems force us to seek new renewable and clean energy

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0022] Catalyst preparation process

[0023] Dissolve 3mmol cerium nitrate, 8mmol copper nitrate and 31mmol 2-methylimidazole in 200mL methanol to form a homogeneous solution, stir at 26°C for 33h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to the tube Furnace, calcination time 6h at 490℃, calcination atmosphere is 18%O 2 / N 2 , roasted to produce porous CexCuyOz, the prepared porous CexCuyOz placed in a solution containing 1mmol nickel nitrate, 0.1mmol silver nitrate and 0.4mmol potassium chloropalladate solution, using 0.18mol / L ammonia borane solution at 3 ℃ for 2.5h , namely the prepared catalyst, denoted as NiAg 0.1 PD 0.4 / Porous Ce 3 Cu 8 Oz nano-catalyst, airtight storage.

[0024] Dehydrogenation process

[0025] Put 50 mg of the above catalyst into a tubular reactor, then place the tubular reactor in a water bath to control the reaction temperature to 35°C, add dropwise 1.5 g of a mixture of formic acid and sodium formate with a molar ratio of 1:1.3, ...

Embodiment 2

[0027] Catalyst preparation process

[0028] Dissolve 5mmol cerium nitrate, 6mmol copper nitrate and 42mmol 2-methylimidazole in 200mL methanol to form a homogeneous solution, stir at 35°C for 26h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to a tube furnace, at 520°C for 2.5 hours, and the firing atmosphere is 11% O 2 / N 2 , roasted to produce porous CexCuyOz, the prepared porous CexCuyOz placed in a solution containing 1mmol nickel nitrate, 0.3mmol silver nitrate and 0.7mmol potassium chloropalladate solution, using 0.34mol / L ammonia borane solution at -4 ° C for 5h , namely the prepared catalyst, denoted as NiAg 0.3 PD 0.7 / Porous Ce 5 Cu 6 Oz nano-catalyst, airtight storage.

[0029] Dehydrogenation process

[0030] Put 50 mg of the above catalyst into a tubular reactor, then place the tubular reactor in a water bath to control the reaction temperature to 70°C, add dropwise 4 g of a mixture of formic acid and sodium formate with a molar ratio of 1:2.9, and ...

Embodiment 3

[0032] Catalyst preparation process

[0033] Dissolve 4mmol cerium nitrate, 6mmol copper nitrate and 33mmol 2-methylimidazole in 200mL methanol to form a homogeneous solution, stir at 28°C for 29h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to the tube Furnace, calcination time 4h at 510℃, calcination atmosphere is 15%O 2 / N 2 , roasted to obtain porous CexCuyOz, the prepared porous CexCuyOz was placed in a solution containing 1 mmol of nickel nitrate, 0.2 mmol of silver nitrate and 0.5 mmol of potassium chloropalladate, and reduced with 0.32 mol / L ammonia borane solution at 2 ° C for 4 h, That is, the catalyst is obtained, which is recorded as NiAg 0.2 PD 0.5 / Porous Ce 4 Cu 6 Oz nano-catalyst, airtight storage.

[0034] Dehydrogenation process

[0035] Put 50 mg of the above catalyst into a tubular reactor, then place the tubular reactor in a water bath to control the reaction temperature to 60°C, add dropwise 3 g of a mixture of formic acid and sodium format...

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PUM

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Abstract

The invention discloses a method for catalyzing dehydrogenation of formic acid through an NiAgPd/porous CexCuyOz nano catalyst, and belongs to the technical field of chemistry and chemical engineering. The method comprises the steps that the prepared nano catalyst is placed in a reactor, the reactor is placed in a water bath and heated to a certain temperature, then mixed liquor of formic acid andsodium formate is added into the reactor for reaction, and generated hydrogen is collected by a drainage method. Compared with existing catalysts, according to the method, the nano catalyst with highactivity, high selectivity and high stability for dehydrogenation of formic acid to prepare hydrogen can be prepared by adjusting the molar ratios of metals Ni, Ag and Pd in the catalyst and the molar ratios of carrier precursors comprising cerium nitrate, copper nitrate and 2-methylimidazole. When the catalyst is used for dehydrogenation reaction of formic acid, the dehydrogenation conversion rate and selectivity are both 100%, the reaction TOF value is larger than 190h<-1>, and the reaction TOF value is still larger than 184h<-1> even after 3h of cyclic use.

Description

technical field [0001] The invention belongs to the technical field of chemistry and chemical engineering, and in particular relates to a method for catalyzing formic acid dehydrogenation with a NiAgPd / porous CexCuyOz nanometer catalyst. Background technique [0002] Energy is an important support for the rapid development of human society. In particular, the large-scale utilization of traditional fossil energy has caused increasingly serious environmental pollution. The above problems force us to seek new renewable and clean energy. Hydrogen energy is considered to be a clean and green energy that promotes the energy revolution in the 21st century. At present, the key to its large-scale application lies in the development of efficient hydrogen storage technology. [0003] Formic acid has attracted widespread attention as an efficient hydrogen storage material, and the development of efficient dehydrogenation catalysts is the key to the large-scale application of this techn...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/89C01B3/22
CPCB01J23/002B01J23/894B01J2523/00C01B3/22B01J2523/18B01J2523/17B01J2523/3712B01J2523/824B01J2523/847
Inventor 万超徐蒙吴胜华王嘉佩许立信张代林
Owner ANHUI UNIVERSITY OF TECHNOLOGY
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