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Method for catalyzing formaldehyde dehydrogenation by using AgPd/porous CexCuyOz nano-catalyst

A nano-catalyst and formaldehyde technology, applied in the field of chemical industry, can solve problems such as unsatisfactory effects, and achieve the effect of simple operation and high activity

Inactive Publication Date: 2019-05-10
ANHUI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

But the effect is not ideal

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0020] Catalyst preparation process

[0021] Dissolve 3 mmol cerium nitrate, 5 mmol copper nitrate and 18 mmol 2-methylimidazole in 200 mL methanol to form a homogeneous solution, stir at 15 °C for 27 h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to a tube furnace , at 480°C for 5 hours, and the firing atmosphere is 5% O 2 / N 2 , roasted to produce porous CexCuyOz, the prepared porous CexCuyOz was placed in a solution containing 1mmol silver nitrate and 0.3mmol potassium chloropalladate, and reduced with 0.13mol / L ammonia borane solution at -2°C for 4h to obtain a catalyst , denoted as AgPd 0.3 / Porous Ce 3 Cu 5 Oz nano-catalyst, airtight storage.

[0022] Dehydrogenation process

[0023] 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 at -5°C, and add dropwise 3.5 g of formaldehyde and sodium hydroxide mixed solution with a molar ratio of 1:0.6 , collect the reaction gas...

Embodiment 2

[0025] Catalyst preparation process

[0026] Dissolve 7 mmol of cerium nitrate, 2 mmol of copper nitrate and 24 mmol of 2-methylimidazole in 200 mL of methanol to form a homogeneous solution, stir at 33 °C for 18 h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to a tube Furnace, firing time at 530°C for 2h, firing atmosphere is 11%O 2 / N 2 , roasted to obtain porous CexCuyOz, the prepared porous CexCuyOz was placed in a solution containing 1mmol silver nitrate and 0.6mmol potassium chloropalladate, and reduced with 0.26mol / L ammonia borane solution at 3°C ​​for 2h to obtain a catalyst. denoted as AgPd 0.6 / Porous Ce 7 Cu 2 Oz nano-catalyst, airtight storage.

[0027] Dehydrogenation process

[0028] 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 7 g of formaldehyde and sodium hydroxide mixed solution with a molar ratio of 1:1.2, and collect Reaction g...

Embodiment 3

[0030] Catalyst preparation process

[0031] Dissolve 3 mmol cerium nitrate, 4 mmol copper nitrate and 19 mmol 2-methylimidazole in 200 mL methanol to form a homogeneous solution, stir at 28 °C for 24 h, centrifuge to obtain Ce-Cu-MOF, transfer Ce-Cu-MOF to a tube Furnace, calcination time 4h at 520℃, calcination atmosphere is 9%O 2 / N 2 , roasted to obtain porous CexCuyOz, the prepared porous CexCuyOz was placed in a solution containing 1mmol silver nitrate and 0.4mmol potassium chloropalladate, and reduced with 0.23mol / L ammonia borane solution at 3°C ​​for 4h to obtain a catalyst. denoted as AgPd 0.4 / Porous Ce 3 Cu 4 Oz nano-catalyst, airtight storage.

[0032] Dehydrogenation process

[0033] Put 50 mg of the above-mentioned catalyst into a tubular reactor, then place the tubular reactor in a water bath to control the reaction temperature to 18° C., add dropwise 6.5 g of formaldehyde and sodium hydroxide mixed solution with a molar ratio of 1:1.1, The reaction gas...

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Abstract

The invention discloses a method for catalyzing formaldehyde dehydrogenation by using an AgPd / porous CexCuyOz nano-catalyst and belongs to the technical field of chemical engineering. The method comprises the following steps: placing the prepared AgPd / porous CexCuyOz nano-catalyst into a reactor; placing the reactor into water bath and rising to a certain temperature; adding a mixed solution of formaldehyde and sodium hydroxide into the reactor for reaction; adopting a draining method for collecting the generated hydrogen. Different from the present catalyst, the nano-catalyst with high activity, high selectivity and high stability used for generating hydrogen by formaldehyde dehydrogenation can be prepared by adjusting molar ratio of metal Ag to Pd and molar ratio of carrier precursor cerium nitrate to cupric nitrate to 2-methylimidazole in the catalyst according to the invention. When the catalyst is used for formaldehyde dehydrogenation reaction, dehydrogenation conversion rate andselectivity are both 100%, TOF value of reaction is more than 330h-1, and the TOF value of reaction is still more than 323h-1 after 4h reuse.

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 AgPd / porous CexCuyOz nanometer catalyst. Background technique [0002] Formaldehyde (HCHO) is an important chemical hydride newly discovered in recent years. It has chemical properties and is liquid at room temperature. It can make good use of existing energy devices and is regarded as the most promising fuel cell hydrogen energy. One of the supply materials. However, there are two paths for the decomposition of formaldehyde: one is direct decomposition to generate hydrogen and carbon monoxide, and carbon monoxide extremely poisons hydrogen fuel cell catalysts; the other is to generate hydrogen and carbon dioxide through hydrolysis, which is an ideal way to release hydrogen energy. The key to regulating the reaction pathway of formaldehyde dehydrogenation lies in the design of effici...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C01B3/22B01J23/89
Inventor 叶明富王嘉佩万超许立信张代林
Owner ANHUI UNIVERSITY OF TECHNOLOGY
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