Method of catalyzing formaldehyde dehydrogenation with NiPd/porous Ce*CuyOz nano-catalyst

A nano-catalyst and formaldehyde technology, applied in the field of chemical industry, can solve the problems of non-recyclable use, unfavorable large-scale application, and inability to separate catalysts, and achieve the effects of high activity and easy operation.

Inactive Publication Date: 2019-04-23
ANHUI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the homogeneous catalyst cannot separate the catalyst from the reaction system after the reaction, and cannot be recycled, which is not conducive to large-scale application

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0022] Catalyst preparation process

[0023] Dissolve 2mmol cerium nitrate, 7mmol copper nitrate and 15mmol 2-methylimidazole in 200mL methanol to form a homogeneous solution, stir at 20°C for 32h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to a tube Furnace, calcination time 6h at 450℃, calcination atmosphere is 8%O 2 / N 2 , roasted to produce porous CexCuyOz, the prepared porous CexCuyOz placed in a solution containing 1mmol nickel chloride and 0.4mmol potassium chloropalladate, using 0.1mol / L ammonia borane solution at 0 ℃ for 2h, the catalyst was prepared , denoted as NiPd 0.4 / Porous Ce 2 Cu 7 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 0°C, add dropwise 6 g of formaldehyde and sodium hydroxide mixed solution with a molar ratio of 1:0.2, and collect Reaction gas, the selectivity of h...

Embodiment 2

[0027] Catalyst preparation process

[0028] Dissolve 5 mmol cerium nitrate, 4 mmol copper nitrate and 22 mmol 2-methylimidazole in 200 mL methanol to form a homogeneous solution, stir at 35 °C for 20 h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to a tube Furnace, calcination time 3h at 560℃, calcination atmosphere is 14%O 2 / N 2 , roasted to produce porous CexCuyOz, the prepared porous CexCuyOz was placed in a solution containing 1mmol nickel chloride and 0.1mmol potassium chloropalladate, and reduced with 0.24mol / L ammonia borane solution at 6°C for 5h to obtain the catalyst , denoted as NiPd 0.1 / Porous Ce 5 Cu 4 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 30°C, add dropwise 12 g of formaldehyde and sodium hydroxide mixed solution with a molar ratio of 1:0.8, and collect Reaction gas,...

Embodiment 3

[0032] Catalyst preparation process

[0033] Dissolve 3mmol cerium nitrate, 6mmol copper nitrate and 19mmol 2-methylimidazole in 200mL methanol to form a homogeneous solution, stir at 28°C for 24h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to the tube Furnace, calcination time 4h at 520℃, calcination atmosphere is 11%O 2 / N 2 , roasted to produce porous CexCuyOz, the prepared porous CexCuyOz was placed in a solution containing 1mmol nickel chloride and 0.2mmol potassium chloropalladate, and reduced with 0.23mol / L ammonia borane solution at 3°C ​​for 4h to obtain a catalyst , denoted as NiPd 0.2 / Porous Ce 3 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 20°C, add dropwise 11 g of formaldehyde and sodium hydroxide mixed solution with a molar ratio of 1:0.4, and collect Reaction gas, the...

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PUM

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Abstract

The invention discloses a method of catalyzing formaldehyde dehydrogenation with a NiPd / porous Ce*CuyOz nano-catalyst and belongs to the technical field of chemistry and chemical engineering. The method comprises the steps of placing the prepared NiPd / porous Ce*CuyOz nano-catalyst into a reactor, arranging the reactor into water bath, heating the reactor to a certain temperature, then filling themixed liquor of formaldehyde and sodium hydroxide into the reactor for reaction, and collecting produced hydrogen through a drainage method. Compared with existing catalysts and according to the method of catalyzing formaldehyde dehydrogenation with the NiPd / porous Ce*CuyOz nano-catalyst, the NiPd / porous Ce*CuyOz nano-catalyst high in activity, selectivity and stability and applicable to formaldehyde dehydrogenation hydrogen production is prepared by adjusting the molar ratio of Ni and Pd and the molar ratio of precursors of cerium nitrate, cupric nitrate and 2-methylimidazole. When applied toformaldehyde dehydrogenation, the NiPd / porous Ce*CuyOz nano-catalyst can achieve a dehydrogenation conversion rate and a selectivity index to 100% and a reaction TOF (turnover frequency) higher than310 h<-1>, and after being recycled and reused for 4 h, still achieves a reaction TOF higher than 301 h<-1>.

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 formaldehyde dehydrogenation with a NiPd / porous CexCuyOz nanometer catalyst. Background technique [0002] With the rapid development of modern society, energy is the key factor restricting the rapid economic development, especially the serious environmental problems caused by the extensive use of traditional fossil energy, which seriously restricts the progress of human beings. Therefore, the demand for clean and efficient new energy is of great significance to promote the rapid development of society. [0003] Hydrogen energy is known as the green energy of the 21st century, and its converted product is only water and has a high energy density. Promoting the large-scale application of hydrogen energy is of great significance to the current economic development. Among them, efficient hydrogen storage technology is o...

Claims

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Application Information

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IPC IPC(8): C01B3/22B01J23/89
CPCB01J23/002B01J23/894C01B3/22C01B2203/0277C01B2203/1064C01B2203/1211
Inventor 叶明富王嘉佩孙林万超许立信
Owner ANHUI UNIVERSITY OF TECHNOLOGY
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