CN101748422A - Method for preparing alkaline hydrogen peroxide in situ - Google Patents
Method for preparing alkaline hydrogen peroxide in situ Download PDFInfo
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- CN101748422A CN101748422A CN200810229978A CN200810229978A CN101748422A CN 101748422 A CN101748422 A CN 101748422A CN 200810229978 A CN200810229978 A CN 200810229978A CN 200810229978 A CN200810229978 A CN 200810229978A CN 101748422 A CN101748422 A CN 101748422A
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Abstract
The invention relates to a method for preparing alkaline hydrogen peroxide in situ, which is used for taking hydrogen, oxygen and an alkaline solution as raw materials to prepare an alkaline hydrogen peroxide water solution by direct electrocatalysis in situ. The preparing method adopts a membrane reactor, the oxygen and the hydrogen enter cathode and anode by the air inlets of a cathode end plate and an anode end plate and generate electrochemical reaction on the gas diffusion electrode loading with nano electro-catalyst, and the obtained product rapidly enters an electrolyte solution to be beneficial to the enrichment of the hydrogen peroxide. The middle adopts a cation-exchange membrane, so the explosion hazard of direct reaction of the hydrogen and the oxygen is avoided, and the safety is high. The volume of the reactor is small, and the product can be simply separated from reactants. Adopting the gas diffusion electrode loading with the nano electro-catalyst, the preparing method effectively increases the three-phase reaction interface, improves the utilization ratio of the catalyst, and increases the reaction rate. The use of the nano electro-catalyst can effectively reduce the over potential of reaction and energy consumption.
Description
Technical field
The present invention relates to a kind of method for preparing alkaline hydrogen peroxide water solution, more particularly relate to a kind ofly prepare the method for hydrogen peroxide, belong to the energy, catalysis, chemical industry and association area by fuel battery reaction device.
Background technology
Hydrogen peroxide is a kind of important Inorganic Chemicals and fine chemical product, is widely used in that chemical is synthetic, paper pulp, paper and the bleaching of textiles, the processing of metalliferous mineral, a plurality of fields such as environmental protection, electronics, military project and space flight.Along with the fast development of global economy, the Application Areas of hydrogen peroxide is constantly opened up, and its market demand is also in continuous growth, and it is well sold and in short supply market to occur.The more general employing of suitability for industrialized production hydrogen peroxide both at home and abroad is anthraquinone, and further perfect from improving hydrogenation catalyst efficient and aspects such as life-span, reactor efficiency and control technique.In addition, many scientific research institutions, major company and producer are just in active research with develop other brand-new production approach, and these methods mainly contain air cathode method, methyl-benzyl alcohol oxidation style, isopropanol oxidation method and hydrogen-oxygen direct synthesis technique etc.These methods respectively have relative merits, are left to be desired.The hydrogen-oxygen direct synthesis technique comprises that hydrogen-oxygen is mixed into reactor by a certain percentage and carries out catalyzed reaction generation hydrogen peroxide, this method is a kind of direct, the simplest and the most direct and the most most economical synthetic method with environment protection significance, this method has been removed the many equipment and the raw material of anthraquinone needs, installation cost can be than anthraquinone minimizing 50%, product cost also significantly reduces, usually select Pd as catalyzer, aluminium, silicon and carbon also are the auxiliary agents of using always, but hydrogen-oxygen mixed catalytic synthesis method has two main drawbacks, the first, H
2And O
2In a very big concentration range content explosive, therefore need to adjust the ratio of H2 and O2, perhaps add thinner at reaction species; Second, on selection of catalysts, the catalyzer that generally is used to produce hydrogen peroxide also is easy to make simultaneously oxidation of hydrogen Cheng Shui, perhaps make hydrogen peroxide decomposition, potential safety hazard becomes the principal element of restriction hydrogen-oxygen direct synthesis technique preparing hydrogen peroxide, requirement to production technique and equipment is very harsh, also is difficult to realize for the moment industrialization, needs to do further to improve.
Fuel cell membrane reactor (FCMR) has little, high-effect, the flexible operation of pollution, is convenient to advantages such as control.Fuel cell has been used for car power source, and is about to commercialization, the promotion that these achievements are strong FCMR produce and development, and cause chemistry, chemical research personnel's concern studies show that, this type of reactor internal resistance is less, operation control is flexible.Yet because the complicacy of fuel cell membranes reactor technology, many problems wait to solve, and at different types of reaction, how to design multi-form reactor and electrode catalyst, how to determine that feeding manner and electrode complete processing all need conscientiously to study.Occurred some abroad and utilized fuel cell membranes reactor made hydrogen peroxide and electric energy symbiosis to send out the research report, but all be in the laboratory exploratory stage, reactor size is very little, and the current density that produces in the reaction process is little, and Reactive Mechanism of Electrode it be unclear that.If it is big that reactor size becomes, the mass transfer rule on the porous electrode then will become outstanding during problem of transmission between Potential distribution rule and plate.
Summary of the invention
Technical problem to be solved by this invention provides a kind of newly-designed fuel cell membrane reactor, and utilizes this fuel cell membrane reactor to produce hydrogen peroxide, to solve in the prior art the seriously polluted or characteristics such as set off an explosion easily of hydrogen peroxide manufacture.
The technical solution used in the present invention:
A kind of method of preparing alkaline hydrogen peroxide in situ, it adopts in the electrolyzer that fills alkaline electrolyte solution and carries out, 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 is electrically connected by lead with anode end plate or is electrically connected (cathode end plate is connected by external circuit with anode end plate) with anodal with the negative pole of a 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 by load on carbon paper or the carbon cloth (as; The surface spraying) eelctro-catalyst that has required being used to of cathode and anode reaction to generate hydrogen peroxide constitutes, to promote the carrying out of cathode and anode electrode reaction; In the cathode and anode chamber, be contained with the required alkaline 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.
Oxygen and hydrogen enter the negative electrode and the anode of reactor (fuel cell membrane reactor) respectively by the inlet mouth of cathode end plate, anode end plate, react being loaded with on the anodic gas diffusion electrode of catalyzer, the product of reaction enters the electrolyte solution of cathode compartment and anolyte compartment rapidly, thereby helps the enrichment of hydrogen peroxide; That is: the inlet mouth of hydrogen on anode end plate enters, react being loaded with on the anodic gas diffusion electrode of catalyzer, be dissociated into hydrogen ion and ejected electron, hydrogen ion by ion-exchange membrane very faster than reacting in the alkaline electrolyte solution, generate water, electronics arrives negative electrode and transmits the combination with oxygen generation reduction reaction of advancing by external circuit, the peroxide radical ion that generates under alkaline condition is transferred to enrichment in the solution rapidly.
Described cathode end plate and anode end plate adopt stainless steel, aluminium, copper, gold-plated or silver plated stainless steel plate or are made by the material of the good anti-alkali corrosion of conduction, and it plays the effect of conveyings, distribution reactant gases and afflux.
Described cathode compartment and anolyte compartment are the tetrafluoroethylene groove or the silicon rubber groove of the tolerance alkali corrosion of radial periphery sealing, and it has narrow cavity, is contained with aqueous alkaline electrolyte in it; Between cathode compartment and anolyte compartment cationic exchange membrane, as the Nafion series membranes.
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 electrolyte solution is selected from NaOH or KOH solution.
Described gas diffusion electrode is that loaded with nano level electrocatalyst layers is made on stratum basale, is specially, and substrate is carbon paper or the carbon cloth that hydrophobisation was handled; Then catalyzer and PTFE are made into slurries, are prepared into by spraying, blade coating on the carbon paper or carbon cloth of hydrophobisation processing;
The catalyzer that anode adopted is to be selected from platinum, platinum black, palladium, palladium black or to load on platinum or palladium on the carbon black, loads on platinum black or palladium black on carbon nanotube or the graphite, the alloy of platinum black or palladium black and transition metal, or transition metal oxide WO
3Or NiO
2The carrying capacity of anode catalyst is at 0.1-4mg/cm
2, be preferably 0.4-2mg/cm
2
The catalyzer that negative electrode adopted is selected from carbon black, activated carbon, graphite, nanotube, carbon fiber, the perhaps graphited carbon black of part, and in the said components one or several; The carrying capacity of cathod catalyst is at 1-20mg/cm
2, preferred 1-10mg/cm
2The weight content of PTFE is 20～60% in the catalyst layer, is preferably 25%～50%.
Use the method for above-mentioned fuel cell membranes reactor made hydrogen peroxide, comprise the following steps: to make oxygen and hydrogen to enter into negative electrode and anode by the inlet mouth of cathode and anode end plate respectively, open the electrolyte solution that recycle pump makes cathode compartment and anolyte compartment and maintain a higher concentration, closed external circuit, electrochemical reaction takes place in hydrogen and oxygen on the cathode and anode gas diffusion electrode, the hydrogen peroxide that generates, and be added to rapidly in the electrolyte solution, help the enrichment of hydrogen peroxide.
Described electrolyte solution is selected from NaOH or KOH solution, and concentration is 1-5M/L, preferred 2M/L.
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 be by adopting catalyzer efficiently, react to drive by self galvanic cell and produce hydrogen peroxide.
Description of drawings
Fig. 1 fuel cell membranes structure of reactor of the present invention synoptic diagram;
The impedance chart that Fig. 2 gets when opening a way for fuel cell membrane reactor of the present invention;
Fig. 3 is the electric current-time diagram of the constant voltage discharge of fuel cell membrane reactor of the present invention.
Embodiment
The present invention is a kind of method of preparing alkaline hydrogen peroxide in situ, is that being used for hydrogen, oxygen and basic solution is raw material, and the electrocatalysis of direct method original position prepares alkaline hydrogen peroxide water solution.It (is the fuel cell membrane reactor that this preparation method adopts film reactor, it is a kind of electrolyzer), oxygen, hydrogen enter negative electrode and anode by the inlet mouth of cathode and anode end plate, have in load on the gas diffusion electrode of nano level eelctro-catalyst electrochemical reaction takes place, products therefrom enters the enrichment that electrolyte solution helps hydrogen peroxide rapidly.Cationic exchange membrane is adopted in the centre, has avoided the explosion hazard of hydrogen-oxygen direct reaction, and safe, reactor volume is little, and product can be separated from reactant simply.Adopt load that the gas diffusion electrode of nano level eelctro-catalyst is arranged, the utilization ratio of catalyzer has been improved at the interface that has effectively increased phase reaction, has increased the speed of reaction.The use of nano level eelctro-catalyst can effectively reduce the overpotential of reaction, effectively reduces energy consumption.
It adopts in the electrolyzer that fills alkaline electrolyte solution and carries out, 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, cathode end plate and anode end plate are electrically connected by lead or are electrically connected with the negative pole and the positive pole of a constant voltage power supply respectively, even cathode end plate is connected by external circuit with anode end plate;
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 by load on carbon paper or the carbon cloth (as; The surface spraying) eelctro-catalyst that has required being used to of cathode and anode reaction to generate hydrogen peroxide constitutes, to promote the carrying out of cathode and anode electrode reaction; In the cathode and anode chamber, be contained with the required alkaline 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.
Oxygen and hydrogen enter the negative electrode and the anode of reactor respectively by the inlet mouth of cathode end plate, anode end plate, the inlet mouth of hydrogen on anode end plate enters, react being loaded with on the anodic gas diffusion electrode of catalyzer, be dissociated into hydrogen ion and ejected electron, hydrogen ion by ion-exchange membrane very faster than reacting in the alkaline electrolyte solution, generate water, electronics passes through external circuit, arrive negative electrode and transmit the combination with oxygen generation reduction reaction of advancing, the peroxide radical ion that generates under alkaline condition is transferred to enrichment in the solution rapidly.
Fuel cell membrane reactor of the present invention, its load have the cathode and anode gas diffusion electrode of catalyzer to be prepared from by following method:
1) carbon paper (or carbon cloth) being carried out hydrophobic handles.Get an amount of 60% ptfe emulsion, standby with distilled water diluting to 1～2%.Carbon paper is weighed earlier, then carbon paper (or carbon cloth) is immersed in the PTFE emulsion fully, take out rapidly and dry, weigh, and calculate the per-cent of the PTFE that has leached thus.The PTFE carrying capacity of anode and cathode carbon paper (carbon cloth) is generally 10～60%, and preferred 20～50%.Then carbon paper (carbon cloth) is put into 350 ℃ of thermal treatment 0.5h of retort furnace, take out the cooling back.
2) in carbon paper or carbon cloth surface preparation microporous layers.According to the area of carbon paper, calculate the quality of required carbon dust, weighing mixes a certain amount of XC-72 and PTFE emulsion, adds an amount of ethanol, and ultrasonic agitation makes slurries, it is applied to the carbon paper surface forms MPL.At last with carbon paper behind 350 ℃ of thermal treatment 0.5h, cooling is taken out.
3) supported catalyst according to the area of carbon paper, calculates the amount of required catalyzer.Then catalyzer is mixed with a certain amount of PTFE emulsion, by the method for spraying or blade coating, catalyzer in the load.Then under nitrogen protection, 350 ℃ of thermal treatment 0.5h, the amount of control anode catalyst is 0.1-4mg/cm
2, preferred 0.4-2mg/cm
2The amount of control cathode catalyzer is 1-20mg/cm
2. preferred 1-10mg/cm
2. the content of control PTFE is 20～60%, preferred 25～40%.
Vucan XC-72 with 2100 ℃ of pyroprocessing is a cathod catalyst, and catalyst loading is 1mg/cm2; Pt/C is an anode catalyst, and the carrying capacity of catalyzer is 0.4mg (Pt)/cm
2., gold-plated stainless steel is the anode and cathode end plate, and advancing anode hydrogen gas pressure is 0.01MPa, and flow is 76ml/min; Advancing the negative electrode oxygen pressure is 0.01MPa, and flow is 76ml/min, 25 ℃ of service temperatures, and ionogen is the KOH solution of 2mol/L, ionogen does not circulate.After the external circuit closure, under this condition, the generating rate of hydrogen peroxide is 0.1mol/Lcm
2, current density 20mA/cm
2
Vucan XC-72 with 2100 ℃ of pyroprocessing is a cathod catalyst, and catalyst loading is 2mg/cm
2Pt/C is an anode catalyst, and the carrying capacity of catalyzer is 0.4mg (Pt)/cm
2., gold-plated stainless steel is the anode and cathode end plate, and advancing anode hydrogen gas pressure is 0.01MPa, and flow is 76ml/min; Advancing the negative electrode oxygen pressure is 0.01MPa, and flow is 76ml/min, 25 ℃ of service temperatures, and ionogen is a 2mol/LKOH solution, ionogen does not circulate.After the external circuit closure, under this condition, the generating rate of hydrogen peroxide is 0.3mmol/Lcm
2, current density 40mA/cm
2
Vucan XC-72 with 2100 ℃ of pyroprocessing is a cathod catalyst, and catalyst loading is 3mg/cm2; Pt/C is an anode catalyst, and the carrying capacity of catalyzer is 0.4mg (Pt)/cm
2., gold-plated stainless steel is the anode and cathode end plate, and advancing anode hydrogen gas pressure is 0.01MPa, and flow is 76ml/min; Advancing the negative electrode oxygen pressure is 0.01MPa, and flow is 76ml/min, 25 ℃ of service temperatures, and ionogen is a 2mol/LKOH solution, ionogen does not circulate.After the external circuit closure, apply the voltage of 1V for the reactor two ends by constant current power supply, under this condition, the generating rate of hydrogen peroxide is 0.2mmol/Lcm
2, current density 30mA/cm
2
Claims (8)
1. the method for a preparing alkaline hydrogen peroxide in situ, it is characterized in that: it adopts in the electrolyzer that fills alkaline electrolyte solution and carries out, 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 by lead or are electrically connected with the negative pole and the positive pole of a 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 carbon paper or the carbon cloth 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 alkaline 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. method according to claim 1, it is characterized in that: make oxygen and hydrogen pass through cathode end plate respectively, the inlet mouth of anode end plate enters the fuel cell membrane reactor, the inlet mouth of hydrogen on anode end plate enters, react being loaded with on the anodic gas diffusion electrode of catalyzer, be dissociated into hydrogen ion and ejected electron, hydrogen ion by ion-exchange membrane very faster than reacting in the alkaline electrolyte solution, generate water, electronics passes through external circuit, arrive negative electrode and transmit the combination with oxygen generation reduction reaction of advancing, the peroxide radical ion that generates under alkaline condition is transferred to enrichment in the solution rapidly.
3. method according to claim 1, it is characterized in that: described cathode end plate (1) and anode end plate (7) adopt stainless steel, aluminium, copper, gold-plated or silver plated stainless steel plate or are made by the material of the good anti-alkali corrosion of conduction, and it plays the effect of conveyings, distribution reactant gases and afflux.
4. method according to claim 1 is characterized in that: described cathode compartment (3) and anolyte compartment (5) are contained with aqueous electrolyte liquid for the tetrafluoroethylene groove or the silicon rubber groove of the tolerance alkali corrosion of radial periphery sealing in it.
5. method 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.
6. method according to claim 1 is characterized in that: described electrolyte solution is selected from NaOH or KOH solution.
7. method according to claim 1 is characterized in that: described gas diffusion electrode is that loaded with nano level electrocatalyst layers is made on stratum basale, is specially, and substrate is carbon paper or the carbon cloth that hydrophobisation was handled; Then catalyzer and PTFE are made into slurries, are prepared into by spraying, blade coating on the carbon paper or carbon cloth of hydrophobisation processing;
The catalyzer that anode adopted is to be selected from platinum, platinum black, palladium, palladium black or to load on platinum or palladium on the carbon black, loads on platinum black or palladium black on carbon nanotube or the graphite, the alloy of platinum black or palladium black and transition metal, or transition metal oxide WO
3Or NiO
2The carrying capacity of anode catalyst is at 0.1-4mg/cm
2
The catalyzer that negative electrode adopted is selected from carbon black, activated carbon, graphite, nanotube, carbon fiber, the perhaps graphited carbon black of part, and in the said components one or several; The carrying capacity of cathod catalyst is at 1-20mg/cm
2The weight content of PTFE is 20～60% in the catalyst layer.
8. method according to claim 7 is characterized in that: the carrying capacity of anode catalyst is preferably 0.4-2mg/cm
2, the preferred 1-10mg/cm of the carrying capacity of cathod catalyst
2The content of PTFE is preferably 25%～50% in the catalyst layer.
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| CN108779560A (en) * | 2016-03-17 | 2018-11-09 | Hpnow爱普斯学会 | Electrochemical cell for the vapor-phase reactant in liquid environment |
| CN110306203A (en) * | 2019-07-09 | 2019-10-08 | 郑州大学 | A kind of cathode generates the electrochemical appliance and method of the hydrogen peroxide organic wastewater of anode processing simultaneously |
| CN110306205A (en) * | 2019-07-09 | 2019-10-08 | 郑州大学 | A kind of gas-diffusion electrode and preparation method thereof |
| CN110760876A (en) * | 2019-08-19 | 2020-02-07 | 天津大学 | For efficiently synthesizing H2O2Three-chamber reactor device |
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| CN115198288A (en) * | 2021-03-24 | 2022-10-18 | 中国科学院福建物质结构研究所 | Integrated device and method for producing high-purity hydrogen peroxide by water-oxygen photoelectrocatalysis |
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| CN107200384A (en) * | 2017-07-13 | 2017-09-26 | 陕西科技大学 | A kind of carbon fiber electrode preparation method of efficient production hydrogen peroxide treatment organic wastewater |
| CN108085714A (en) * | 2018-01-12 | 2018-05-29 | 齐鲁工业大学 | A kind of preparation method and applications of novel gas diffusion electrodes |
| CN110835765A (en) * | 2018-08-17 | 2020-02-25 | 中国科学院大连化学物理研究所 | Catalyst and device for preparing high-purity hydrogen through electrocatalysis water-vapor shift reaction |
| CN110835765B (en) * | 2018-08-17 | 2021-01-22 | 中国科学院大连化学物理研究所 | Catalyst and device for preparing high-purity hydrogen through electrocatalysis water-vapor shift reaction |
| CN112996952A (en) * | 2018-10-12 | 2021-06-18 | 塞尼斯有限责任公司 | Electrolysis device and method for producing dry hydrogen peroxide |
| CN110306203A (en) * | 2019-07-09 | 2019-10-08 | 郑州大学 | A kind of cathode generates the electrochemical appliance and method of the hydrogen peroxide organic wastewater of anode processing simultaneously |
| CN110306205A (en) * | 2019-07-09 | 2019-10-08 | 郑州大学 | A kind of gas-diffusion electrode and preparation method thereof |
| CN110306205B (en) * | 2019-07-09 | 2021-06-29 | 郑州大学 | Gas diffusion electrode and preparation method thereof |
| CN110306203B (en) * | 2019-07-09 | 2021-08-06 | 郑州大学 | Electrochemical device and method for generating hydrogen peroxide at cathode and simultaneously carrying out anodic treatment on organic wastewater |
| CN110760876A (en) * | 2019-08-19 | 2020-02-07 | 天津大学 | For efficiently synthesizing H2O2Three-chamber reactor device |
| CN115198288A (en) * | 2021-03-24 | 2022-10-18 | 中国科学院福建物质结构研究所 | Integrated device and method for producing high-purity hydrogen peroxide by water-oxygen photoelectrocatalysis |
| CN113871668A (en) * | 2021-09-24 | 2021-12-31 | 中国科学院山西煤炭化学研究所 | Reversible battery system and method based on hydrogen peroxide electrochemical cycle |
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