CN101748423A - Efficient electrochemical reactor of electro-catalysis in-situ hydrogen peroxide - Google Patents
Efficient electrochemical reactor of electro-catalysis in-situ hydrogen peroxide Download PDFInfo
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- CN101748423A CN101748423A CN200810229979A CN200810229979A CN101748423A CN 101748423 A CN101748423 A CN 101748423A CN 200810229979 A CN200810229979 A CN 200810229979A CN 200810229979 A CN200810229979 A CN 200810229979A CN 101748423 A CN101748423 A CN 101748423A
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Abstract
The invention discloses an efficient electrochemical reactor of electro-catalysis in-situ hydrogen peroxide. The reactor consists of a two-cavity reaction system and an external circuit. A solid polymer electrolyte membrane is arranged in the middle of the two-cavity reaction system and can separate a cathode reaction and an anode reaction. The two-cavity reaction system mainly comprises a cathode end plate, a cathode gas diffusion electrode, a cathode chamber, an ion exchange membrane, an anode chamber, an anode gas diffusion electrode and an anode end place from left to right. The external circuit consists of an ammeter, a voltmeter and a variable resistor. The reactor effectively improves a three-phase reaction interface and a reaction rate by utilizing the gas diffusion electrodes loaded with a catalyst. Electrolyte in the cathode and anode chambers for participating in the reaction can rapidly diffuse a reaction product in a solution, so that the reaction products are enriched and the concentration of the reaction product is improved. A current and the reaction speed can be adjusted by adjusting the variable resistor. The electrolyte at a cathode and at an anode can circulate under the action of a circulating pump to maintain a higher conductivity of the system and the high reaction rate of the electrode reaction.
Description
Technical field
The present invention relates to electrochemical reactor, relate to a kind of electrochemical reactor of new and effective electro-catalysis in-situ hydrogen peroxide.
Background technology
Hydrogen peroxide is a kind of eco-friendly strong oxidizer, chemical bleaching reagent, is the source product of a series of important superoxide simultaneously.Along with the raising of environmental requirement, it is widely used in fields such as chemical industry, medicine, food, electronics, environmental protection, is just replacing traditional potassium bichromate, potassium permanganate becomes a kind of emerging " cleaning oxidizer ", more and more is subjected to people's attention.Normally used hydrogen peroxide is by the anthraquinone production of chemistry, and this method is a working fluid with the organic solvent that contains 2-ethyl-anthraquinone, feeds hydrogen, oxygen, circulate between quinhydrones and quinone, and hydrolysis obtains hydrogen peroxide.But residual alkyl-anthraquinone in this method product has limited the raising of finished product concentration of hydrogen peroxide; Unit operation is many, the production cost height; And having used multiple high toxicity organic raw material and solvent in the process, by product comprises organic carcinogen matter such as trichloromethane, dioxin.Therefore, a kind of green synthesis process of producing hydrogen peroxide of development is imperative.Research by the direct synthesize hydrogen peroxide of hydrogen-oxygen causes people's attention.But this method adopts noble metal catalyst, very easily sets off an explosion, and poor stability has limited its application.Since the seventies in 20th century, extensively carried out the research of electrochemical in-situ hydrogen reduction synthesize hydrogen peroxide both at home and abroad.The reactor types that is used for electrochemical oxygen reduction generation hydrogen peroxide at present mainly contains: press filter type or plate and frame electrolyzer; The fixed bed of mosaic electrode and fluidized-bed electrolyzer.These electrolyzers can be divided into board-like and the grain bed form by electrode shape wherein.Electrode materials generally adopts graphite, vitreous carbon, carbon tetrafluoroethylene.The subject matter that exists in the application of these reactors is, for last type reactor, the mass transfer effect of oxygen is poor, and current efficiency is low, and the hydrogen peroxide generating rate is low; For back one type reactor, though mass transfer effect improves, the hydrogen peroxide that generates can further decompose at cathode surface, thereby the generating capacity of solution main body is affected.The electrocatalysis synthesize hydrogen peroxide is a kind of green synthesis process that grows up the eighties in 20th century, and the cost of electrochemical synthesis still remains to be reduced.Development along with nanotechnology, combining nano technology and fuel cell electrode technology of preparing, a kind of eco-friendly preparation method----feulcell prototype reactor synthesize hydrogen peroxide is suggested, it has characteristics such as green, energy-saving and environmental protection, attracted vast domestic and international scientific research personnel that it is studied, and along with the attention of country to the energy environment problem, many enterprises also extremely pay close attention to this technology, but rarely found about the play-by-play of this reactor.
Summary of the invention
The electrochemical reactor that the purpose of this invention is to provide a kind of efficient electro-catalysis in-situ hydrogen peroxide, adopting load to have the gas diffusion electrode of effective catalyst and the appropriate design of reactor to improve current efficiency and the growing amount that the electrochemical catalysis original position efficiently generates hydrogen peroxide, thereby cutting down the consumption of energy.
For achieving the above object, the technical solution used in the present invention is:
A kind of efficient electrocatalysis generates the electrochemical reactor of hydrogen peroxide, comprises electrolyzer and constant voltage power supply;
Described electrolyzer from left to right is formed by stacking by cathode end plate, cathode gas diffusion electrode, cathode compartment, ion-exchange membrane, anolyte compartment, anodic gas diffusion electrode, anode end plate successively, and cathode end plate and anode end plate are electrically connected with the negative pole and the positive pole of constant voltage power supply respectively;
On the outer side wall of cathode end plate and anode end plate, be provided with inlet mouth and air outlet, and be provided with the flow field in a side of cathode end plate and the close electrode of anode end plate; Described cathode and anode gas diffusion electrode is made of the eelctro-catalyst that load on the carbon paper (as: surface spraying) has required being used to of cathode and anode reaction to generate hydrogen peroxide, to promote the carrying out of cathode and anode electrode reaction; In the cathode and anode chamber, be contained with the required electrolyte solution of electrolytic reaction;
Have in the top and bottom, anolyte compartment and to be used for changing the required electrolytical aperture of reaction, to keep efficiently carrying out of reaction; Cathode compartment upper end or lower end have aperture, and be airtight at ordinary times, opens when the concentration of sampling or product reaches requirement, takes out aqueous hydrogen peroxide solution.
Described cathode end plate and anode end plate adopt stainless steel, gold-plated or silver plated stainless steel plate to make, the effect that it plays conveying, distributes reactant gases and afflux; In the inlet mouth aerating oxygen of described cathode end plate, in the inlet mouth feeding hydrogen of anode end plate; The reaction ionogen promptly can be acid, also can be aqueous alkaline electrolyte; The aperture of upper end, anolyte compartment or lower end is connected via the ionogen storage tank of a recycle pump with the external world, and ionogen can be circulated, to keep the required electrolytical concentration of reaction a higher constant value; Described cathode compartment and anolyte compartment are the silicon rubber groove of radial periphery sealing, are contained with aqueous electrolyte liquid in it.
Cathode and anode of the present invention is a liquid electrolyte between gas diffusion electrode and solid polymer dielectric film separately, is different from gas diffusion electrode three-in-one component used in the present Proton Exchange Membrane Fuel Cells; This device can also be assembled with the form of pressure filter, is made up of the such reaction member of a plurality of multiple, can effectively save the space, conveniently carries out the amplification of output simultaneously.This device both can pass through impressed voltage, produced hydrogen peroxide with the form of electrolyzer; Also can drive by id reaction and produce hydrogen peroxide by adopting catalyzer efficiently.
The present invention has following advantage:
1) adopts metal end plate in conveying, distribution of gas, also play the effect of afflux, simplified the assembling of reactor.
2) the employing load has the gas diffusion electrode of catalyzer, has increased the utilization ratio of catalyzer, has effectively increased gas, liquid, solid three-phase reaction interface, has improved speed of response.
3) this device cathode and anode is a liquid electrolyte between gas diffusion electrode and solid polymer dielectric film separately, is different from gas diffusion electrode three-in-one component used in the present Proton Exchange Membrane Fuel Cells; Inert substance is adopted in the cathode and anode chamber, for the required ionogen of cathode and anode reaction provides storage; The hydrogen peroxide that cathodic reaction produced simultaneously can be transferred in the catholyte rapidly, helps the raising of concentration; Simultaneously in the anode and cathode perforate, can keep ionogen in two chambeies in certain concentration with crossing recycle pump, make reaction maintain efficient state always.
4) reaction medium can be according to actual needs, and device itself is not stipulated acid, the alkalescence of medium.5) reactor is isolated by solid polymer dielectric film, so substrate can not compete in same catalytic site, and explosion hazard reduces, and security improves, and reactor volume is little, and product can be separated from reactant simply.
6) the exercisable temperature of electrochemical reactor is far below the temperature of the catalytic process of routine.
7) selectivity of process mainly changes electrode potential by change external resistance or additional power source or realizes by the catalyzer that changes electrode.Can apply external voltage, electrolytic reaction takes place in electrolyzer; Also can drive, the galvanic cell reaction takes place in electrolyzer by the electrochemical reaction of self.
8) this reaction unit promptly can singlely amplify, and also can be made up of the such reaction member of a plurality of multiple by the form assembling of pressure filter, can effectively save the space, to adapt to the demand that enlarges of producing.
Description of drawings
Fig. 1 is one of structural representation of the present invention.
Fig. 2 is two of a structural representation of the present invention.
Embodiment
Now in conjunction with the accompanying drawings the utility model is described further.
It is made up of this electrochemical reaction following major portion: (1) yin, yang end plate one side has the air inlet port and the port of giving vent to anger, another time near electrode has the flow field, the effect that play conveying, distributes reactant gases and afflux, general stainless steel or gold-plated stainless steel or the silver-plated stainless steel of handling through special corrosion protection that adopt, can tolerate strong acid, alkaline corrosion, in the side near gas diffusion electrode is the flow field of the certain flow pattern of processing, effectively disperses gas; (2) cathode and anode gas diffusion electrode, substrate are carbon paper or the carbon cloth that hydrophobisation is handled, and Catalytic Layer has the catalyzer of catalytic capability for all, and by spraying, coating, sputter or other known method for preparing gas diffusion electrode are prepared from.Anode active material generally adopts the carbon of high-specific surface area to carry platinum or platinum black, and negative electrode is a gac, carbon black, polyacrylonitrile, carbon nanotube, graphite, the gac of the graphited high specific area of part, carbon fiber, Au/C, or Pd/C or their mixture.(3) cathode and anode chamber, be generally chemically inert material, and easily processing comprises that tetrafluoroethylene or silastic material make, can be according to the different mining of reaction system with acidic electrolyte bath or alkaline electrolyte, cavity perforate up and down simultaneously, can pass through the effective cyclic electrolysis matter of pump, make electrolytical concentration maintain certain value, increase conductive capability, convenient simultaneously sampling, the concentration of detection product.(4) polymer dielectric film, acid-alkali-corrosive-resisting allows positively charged ion to pass through, and stops negatively charged ion to pass through, and can effectively separate the cathode and anode reaction, is generally cationic exchange membrane, as commercial Nafion series membranes and other cationic exchange membrane.
Promising two chamber reaction systems of this reactor and external circuit are formed, and are solid polymer dielectric film in the middle of the two chamber reaction systems, can separate the cathode and anode reaction.Two chamber reaction systems mainly contain from left to right: 1 cathode end plate, and 2 cathode gas diffusion electrodes, 3 cathode compartments, 4 ion-exchange membranees, 5 anolyte compartments, 6 anode diffusion electrodes, 7 anode end plates are formed; External circuit is by reometer, and voltmeter and variohm are formed.Yin, yang end plate one side has the air inlet port and the port of giving vent to anger, and the opposite side of close electrode has the flow field, the effect that play conveying, distributes reactant gases and afflux.The load of cathode and anode gas diffusion electrode own has the eelctro-catalyst of cathode and anode reaction, can utilize the advantage of gas diffusion electrode, and more three-phase reaction interface is provided, and more reactive behavior site is provided.Be respectively applied in cathode cavity, the anode cavities and hold negative electrode, the ionogen of anodic reaction.During reaction, pump into required ionogen to the cathode and anode reaction chamber respectively by recycle pump, as KOH solution, NaOH solution.Inlet mouth by the cathode and anode end plate is carried O to cathode and anode respectively
2, H
2Regulate electric current, the speed of conditioned reaction by regulating variohm.This device can also be assembled with the form of pressure filter, is made up of the such reaction member of a plurality of multiple, can effectively save the space, conveniently carries out the amplification of output simultaneously.This device both can pass through additional power source, produced hydrogen peroxide with the form of electrolyzer; Also can drive by id reaction and produce hydrogen peroxide by adopting catalyzer efficiently.
Preparation platinum carrying capacity is the gas diffusion electrode of anodic gas diffusion electrode and the graphited XC-72 of part of 0.5mg/cm2.Respectively the anodic gas electrode, Nafion117 film, the cathode diffusion electrode battery of packing into.The NaOH solution of configuration 2Mol/L is injected into the cathode and anode reaction chamber to electrolyte solution respectively.Cathode and anode feeds O respectively
2, H
2, flow is 80mL/min, and the temperature of control battery is about 0 degree, and with the discharge of the form of short circuit, as Fig. 1, the concentration that obtains obtaining at cathode side hydrogen peroxide after two hours is 2%, and maximum current density is 50mA/cm
2
Preparation platinum carrying capacity is 0.5mg/cm
2The anodic gas diffusion electrode and the gas diffusion electrode of the graphited XC-72 of part.Respectively the anodic gas electrode, Nafion117 film, the cathode diffusion electrode battery of packing into.The NaOH solution of configuration 2Mol/L is injected into the cathode and anode reaction chamber to electrolyte solution respectively.Cathode and anode feeds O respectively
2, H
2, flow is 80mL/min, and the temperature of control battery is about 0 degree.The voltage of applying 1V for the reactor two ends by external circuit, as Fig. 2, the concentration that obtains obtaining at cathode side hydrogen peroxide after two hours is 4%, maximum current density is 100mA/cm
2
Claims (5)
1. the electrochemical reactor of an efficient electro-catalysis in-situ hydrogen peroxide is characterized in that: comprise electrolyzer and constant voltage power supply,
Described electrolyzer from left to right is formed by stacking by cathode end plate (1), cathode gas diffusion electrode (2), cathode compartment (3), ion-exchange membrane (4), anolyte compartment (5), anodic gas diffusion electrode (6), anode end plate (7) successively, and cathode end plate (1) and anode end plate (7) are electrically connected with the negative pole and the positive pole of constant voltage power supply respectively;
On the outer side wall of cathode end plate (1) and anode end plate (7), be provided with inlet mouth and air outlet, and be provided with the flow field in a side of cathode end plate (1) and the close electrode of anode end plate (7); Described cathode and anode gas diffusion electrode is made of the eelctro-catalyst that load on the carbon paper has required being used to of cathode and anode reaction to generate hydrogen peroxide, to promote the carrying out of cathode and anode electrode reaction; In the cathode and anode chamber, be contained with the required electrolyte solution of electrolytic reaction;
Have in the top and bottom, anolyte compartment and to be used for changing the required electrolytical aperture of reaction, to keep efficiently carrying out of reaction; Cathode compartment upper end or lower end have aperture, and be airtight at ordinary times, opens when the concentration of sampling or product reaches requirement, takes out aqueous hydrogen peroxide solution.
2. electrochemical reactor according to claim 1 is characterized in that: described cathode end plate (1) and anode end plate (7) adopt stainless steel, gold-plated or silver plated stainless steel plate to make, the effect that it plays conveying, distributes reactant gases and afflux.
3. electrochemical reactor according to claim 1 is characterized in that: in the inlet mouth aerating oxygen of described cathode end plate (1), in the inlet mouth feeding hydrogen of anode end plate (7); The reaction ionogen promptly can be acid, also can be aqueous alkaline electrolyte.
4. electrochemical reactor according to claim 1, it is characterized in that: the aperture of upper end, anolyte compartment or lower end is connected via the ionogen storage tank of a recycle pump with the external world, ionogen can be circulated, to keep the required electrolytical concentration of reaction a higher constant value.
5. electrochemical reactor according to claim 1 is characterized in that: described cathode compartment (3) and anolyte compartment (5) are the silicon rubber groove of radial periphery sealing, are contained with aqueous electrolyte liquid in it.
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Cited By (11)
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| CN102502925A (en) * | 2011-11-29 | 2012-06-20 | 浙江大学 | Device capable of generating electric energy and simultaneously removing metal ions and method of device |
| CN103695958A (en) * | 2013-12-13 | 2014-04-02 | 南开大学 | Configuration of air diffusion cathode for efficiently producing hydrogen peroxide and preparation method thereof |
| CN105762396A (en) * | 2016-03-03 | 2016-07-13 | 重庆大学 | Flat-plate heat regeneration ammonium battery adopting foam metal electrode |
| CN107317040A (en) * | 2017-06-22 | 2017-11-03 | 清华大学 | The floatation type gas-diffusion electrode reacted for gas consumption and its preparation |
| CN107313068A (en) * | 2016-04-26 | 2017-11-03 | 中国科学院大连化学物理研究所 | A kind of electrochemical method of synthetic acidic hydrogen peroxide |
| CN111472016A (en) * | 2020-04-15 | 2020-07-31 | 中南大学 | Method for preparing hydrogen peroxide by electrolyzing and recovering sodium sulfate waste liquid |
| CN112030182A (en) * | 2020-09-18 | 2020-12-04 | 安徽大学 | Electrochemical device, method for synthesizing hydrogen peroxide by electrochemically decomposing urea and application |
| CN113089002A (en) * | 2021-03-18 | 2021-07-09 | 重庆大学 | Selective oxidation device and method for coupling organic matters through electrocatalysis hydrogen peroxide production |
| CN113481525A (en) * | 2021-06-08 | 2021-10-08 | 中国空间技术研究院 | Electrochemical reactor and electrochemical reaction system |
| CN113774416A (en) * | 2021-11-15 | 2021-12-10 | 广东工业大学 | Gas diffusion cathode and electrochemical reactor for in-situ production of hydrogen peroxide |
| CN113809375A (en) * | 2021-09-28 | 2021-12-17 | 北京化工大学 | Solid electrolyte applied to electrocatalytic oxygen reduction synthesis of hydrogen peroxide and preparation method thereof |
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|---|---|---|---|---|
| US3969201A (en) * | 1975-01-13 | 1976-07-13 | Canadian Patents And Development Limited | Electrolytic production of alkaline peroxide solutions |
| DE4311665C1 (en) * | 1993-04-08 | 1994-08-18 | Metallgesellschaft Ag | Method for preparing alkali metal peroxide solutions |
| CN2698812Y (en) * | 2004-04-21 | 2005-05-11 | 杨凤林 | Electrochemical reactor for in situ hydrogen peroxide generation by electrocatalysis |
| CN101003905A (en) * | 2006-12-22 | 2007-07-25 | 上海应用技术学院 | Membrane reactor of fuel cell, and method for using the reactor to prepare hydrogen dioxide |
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| CN102502925A (en) * | 2011-11-29 | 2012-06-20 | 浙江大学 | Device capable of generating electric energy and simultaneously removing metal ions and method of device |
| CN102502925B (en) * | 2011-11-29 | 2013-11-13 | 浙江大学 | Device capable of generating electric energy and simultaneously removing metal ions and method of device |
| CN103695958A (en) * | 2013-12-13 | 2014-04-02 | 南开大学 | Configuration of air diffusion cathode for efficiently producing hydrogen peroxide and preparation method thereof |
| CN105762396B (en) * | 2016-03-03 | 2018-03-23 | 重庆大学 | A kind of flat hot recycling ammonia battery using foam metal electrode |
| CN105762396A (en) * | 2016-03-03 | 2016-07-13 | 重庆大学 | Flat-plate heat regeneration ammonium battery adopting foam metal electrode |
| CN107313068A (en) * | 2016-04-26 | 2017-11-03 | 中国科学院大连化学物理研究所 | A kind of electrochemical method of synthetic acidic hydrogen peroxide |
| CN107317040A (en) * | 2017-06-22 | 2017-11-03 | 清华大学 | The floatation type gas-diffusion electrode reacted for gas consumption and its preparation |
| CN111472016A (en) * | 2020-04-15 | 2020-07-31 | 中南大学 | Method for preparing hydrogen peroxide by electrolyzing and recovering sodium sulfate waste liquid |
| CN112030182A (en) * | 2020-09-18 | 2020-12-04 | 安徽大学 | Electrochemical device, method for synthesizing hydrogen peroxide by electrochemically decomposing urea and application |
| CN113089002A (en) * | 2021-03-18 | 2021-07-09 | 重庆大学 | Selective oxidation device and method for coupling organic matters through electrocatalysis hydrogen peroxide production |
| CN113481525A (en) * | 2021-06-08 | 2021-10-08 | 中国空间技术研究院 | Electrochemical reactor and electrochemical reaction system |
| CN113809375A (en) * | 2021-09-28 | 2021-12-17 | 北京化工大学 | Solid electrolyte applied to electrocatalytic oxygen reduction synthesis of hydrogen peroxide and preparation method thereof |
| CN113809375B (en) * | 2021-09-28 | 2022-12-27 | 北京化工大学 | Solid electrolyte applied to electrocatalytic oxygen reduction synthesis of hydrogen peroxide and preparation method thereof |
| CN113774416A (en) * | 2021-11-15 | 2021-12-10 | 广东工业大学 | Gas diffusion cathode and electrochemical reactor for in-situ production of hydrogen peroxide |
| CN113774416B (en) * | 2021-11-15 | 2022-03-04 | 广东工业大学 | Gas diffusion cathode and electrochemical reactor for in-situ production of hydrogen peroxide |
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