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Device and method for coupled electro-catalytic hydrogen peroxide production and selective organic matter oxidation

A technology for organic matter and hydrogen oxidation, which is applied in chemical instruments and methods, oxidation preparation of carbonyl compounds, organic chemistry, etc. It can solve the problems of storage and transportation of hydrogen peroxide, low concentration of hydrogen peroxide, and low reaction current density, etc., so as to reduce equipment investment and Operating costs, broad prospects for industrial applications, and the effect of solving safety problems

Pending Publication Date: 2021-07-09
CHONGQING UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0003] However, the reaction current density of electrocatalytic oxygen reduction is usually small, and the concentration of hydrogen peroxide produced is low, which requires further concentration to make products
In addition, there are certain risks in the storage and transportation of hydrogen peroxide

Method used

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  • Device and method for coupled electro-catalytic hydrogen peroxide production and selective organic matter oxidation
  • Device and method for coupled electro-catalytic hydrogen peroxide production and selective organic matter oxidation
  • Device and method for coupled electro-catalytic hydrogen peroxide production and selective organic matter oxidation

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0029] Using air and hydrogen system, the anode and cathode are 0.5mg / cm 2 Functionalized carbon powder and commercial Pt / C with a catalyst active area of ​​4 cm 2 , the organic oxidation catalyst is 0.1g TS-1 molecular sieve. 0.1M K 2 SO 4 The aqueous solution is introduced into the organic catalytic chamber through a peristaltic pump for circulation, and the flow rate is maintained at 0.18ml / min, and the power is turned on. At a current density of 37.5mA / cm 2 Under constant current electrolysis, after 30 minutes of activation to stabilize the system, the solution was collected to titrate the concentration of hydrogen peroxide with potassium iodide; organic raw materials (containing 0.085M phenol, 0.1M K2 SO 4 ) is introduced into the organic catalytic chamber through a peristaltic pump, the total volume of the solution is 20ml, and the flow rate is 0.18ml / min; when the current density is 37.5mA / cm 2 During constant current electrolysis at room temperature, the cell volta...

Embodiment 2

[0031] This example is basically the same as Example 1, except that the concentration of the raw material phenol is enlarged to 0.262M. After the activation is stable, 20ml containing 0.262M phenol, 0.1M K 2 SO 4 The aqueous solution is introduced into the organic catalytic chamber through a peristaltic pump, and at a current density of 37.5mA / cm 2 Under the constant current solution cycle electrolysis for 2h, the cell voltage is about 0.85V, and then power off cycle for 8h. The conversion rate of phenol is about 18.25%, the selectivity of hydroquinone is 94.81%, the ratio of catechol to hydroquinone is 0.73, and the current efficiency is 17.09%.

Embodiment 3

[0033] This example is basically the same as Example 1, except that the concentration of the raw material phenol is enlarged to 0.506M. After the activation is stable, 20ml containing 0.506M phenol, 0.1M K 2 SO 4 The aqueous solution is introduced into the organic catalytic chamber through a peristaltic pump, and at a current density of 37.5mA / cm 2 Under the constant current solution cycle electrolysis for 2h, the cell voltage is about 0.9V, and then cut off the power cycle for 8h. The conversion rate of phenol is about 11.98%, the selectivity of hydroquinone is 94.89%, the ratio of catechol to hydroquinone is 0.69, and the current efficiency is 21.69%.

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Abstract

The invention belongs to the field of electrochemical organic synthesis, and particularly relates to a device and method for device and method for coupled electro-catalytic hydrogen peroxide production and selective organic matter oxidation. According to the invention, the reaction device is composed of an anode chamber, a cathode chamber and an organic catalysis chamber, wherein the cathode chamber contains a catalyst for hydrogen peroxide production through oxygen reduction; the anode chamber contains a water oxidation or hydrogen oxidation catalyst; the organic catalysis chamber contains an organic matter oxidation catalyst; the anode chamber and the organic catalysis chamber are separated by a cation exchange membrane; and the cathode chamber and the organic catalysis chamber are separated by an anion exchange membrane. During working of the device, oxygen or air is introduced into the cathode chamber, hydrogen or water is introduced into the anode chamber, and an organic reactant is introduced into the organic catalysis chamber; and under an electrifying condition, a cathode is subjected to oxygen reduction to obtain OOH<->, an anode is subjected to water oxidation or hydroxide reaction to obtain H< + >, the H<+> enters the middle organic catalysis chamber through the corresponding anion and cation exchange membranes to form H2O2, and organic matters are further oxidized under the action of the catalyst. According to the invention, low-concentration hydrogen peroxide generated by oxygen reduction is directly used for oxidation of the organic matters, so problems in separation, concentration, storage and transportation cost and safety of H2O2 are avoided, and remarkable economic benefits are achieved. When the device is used for phenol oxidation, benzyl alcohol oxidation, furfuryl alcohol oxidation and cyclohexanone conversion, the selectivity of target products including benzenediol, benzaldehyde, furfural and cyclohexanone-oxime is greater than 98%, and corresponding total current efficiency is 21-49%.

Description

technical field [0001] The invention belongs to the field of electrochemical organic synthesis, and in particular relates to a device and method for electrocatalytically generating hydrogen peroxide coupled with selective oxidation of organic matter. Background technique [0002] As a commonly used chemical agent, hydrogen peroxide is recognized as an efficient, green, and environmentally friendly oxidant, and is widely used in the fields of selective oxidation of organic matter, wastewater treatment, and sanitation. In industry, hydrogen peroxide is almost entirely produced by the anthraquinone redox method. Although it has the advantages of mature technology, high single-pass yield, and high safety, it still has the advantages of high investment, complicated process flow, and extensive use of organic solvents. product pollution and environmental pollution. Electrocatalytic oxygen reduction is a greener method for producing hydrogen peroxide. Compared with the anthraquinon...

Claims

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Application Information

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IPC IPC(8): C25B1/30C25B9/21C25B9/23C07C37/60C07C39/08C07C45/29C07C47/54C07D307/48C07C249/04C07C251/44
CPCC25B1/30C07C37/60C07C45/294C07D307/48C07C249/04C07C2601/14C07C39/08C07C47/54C07C251/44
Inventor 魏子栋黄寻张红亮
Owner CHONGQING UNIV
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