CN208272026U - Electro-chemical systems, cathode, battery - Google Patents
Electro-chemical systems, cathode, battery Download PDFInfo
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- CN208272026U CN208272026U CN201820542336.4U CN201820542336U CN208272026U CN 208272026 U CN208272026 U CN 208272026U CN 201820542336 U CN201820542336 U CN 201820542336U CN 208272026 U CN208272026 U CN 208272026U
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
The utility model discloses electro-chemical systems, cathode, batteries.Specifically, the utility model relates to a kind of electro-chemical systems, comprising: shell limits reaction compartment in the shell；And modularization electrode assembly, the modularization electrode assembly is arranged in the reaction compartment, the modularization electrode assembly further comprises: hollow type cathode slot, the hollow type cathode slot includes: multiple air cathodes, the multiple air cathode is arranged on the side wall of the hollow type cathode slot, the air cathode includes multiple sub- cathodes, and the sub- cathode includes the catalyst layer containing atom level dispersed metal catalyst；Anode, the anode are electrically connected with the air cathode.The catalytic activity of the air cathode is good as a result, metal utilization is high, low in cost；The biggish air cathode of area can easily be prepared；Multiple air cathodes and anode are incorporated into same reaction compartment, the electricity generation performance of the electro-chemical systems is further improved.
Description
Technical field
The utility model relates to environment, material, energy fields.In particular it relates to electro-chemical systems, cathode, battery.
Background technique
Environmental problem and energy problem are that contemporary society develops two hang-ups faced, take into account the energy while purifying sewage
Recycling is the new challenge that sewage disposal technology faces.Using Microbial fuel electro-chemical systems as the bioelectrochemistry system of Typical Representative
System is a kind of emerging sewage disposal technology, can convert electric energy for the chemical energy in pollutant while handling sewage,
Using being attached to the electricity-producing microorganism of anode for the oxidation operation in sewage, while cathode receives electronics to complete hydrogen reduction anti-
It answers.
However, the performance of current electro-chemical systems is still to be improved.
Utility model content
The utility model be based on inventor couple on the fact that and problem discovery and understanding make:
Inventors have found that the generally existing electricity generation performance of current electro-chemical systems is poor and the higher problem of production cost.
Inventor by further investigation and many experiments discovery, this be by electro-chemical systems, the catalyst efficiency of cathode compared with
Caused by difference and higher cost.Especially in bioelectrochemical system, the oxygen reduction reaction of cathode is limitation bioelectrochemistry
One of key factor of electricity generation performance of system, what oxygen reduction reaction was mainly driven by cathod catalyst, and currently used for
The catalyst higher cost and catalytic efficiency of cathode are poor, for example, traditional cathode uses platinum carbon as catalyst, platinum price is high
Expensive, scarcity of resources, and when longtime running cathode is contaminated, catalytic performance significant degradation.Also, inventor also found,
Current electro-chemical systems generally contain only an air cathode and an anode, in the process of running, whole electricity production
Limited efficacy.Also, in practical application in industry, when the production biggish air cathode of one bulk area, it is more difficult to guarantee its surface
Planarization and service performance.Therefore, if high catalytic efficiency, stable in catalytic performance and low-cost air can be proposed
Cathod catalyst and air cathode make it play preferable catalysis in electro-chemical systems and bioelectrochemical system and make
With, and the structure for designing new air cathode and electro-chemical systems will largely solve the above problems.
The utility model is intended to solve at least some of the technical problems in related technologies.
In the one aspect of the utility model, the utility model proposes a kind of electro-chemical systems.Specifically, the electrochemistry
System includes: shell, limits reaction compartment in the shell；And modularization electrode assembly, the modularization electrode assembly
It is arranged in the reaction compartment, the modularization electrode assembly further comprises: hollow type cathode slot, the hollow type yin
Pole slot includes: multiple air cathodes, and the multiple air cathode is arranged on the side wall of the hollow type cathode slot, described
Air cathode includes multiple sub- cathodes, and the sub- cathode includes the catalyst layer containing atom level dispersed metal catalyst；Anode,
The anode is electrically connected with the air cathode.The catalytic activity of the air cathode is good as a result, metal utilization is high, at low cost
It is honest and clean etc.；By the way that multiple sub- cathodes are arranged, the biggish air cathode of area, and air cathode surface obtained can be easily prepared
Planarization is high, functional；The electro-chemical systems also pass through setup module polarizing electrode component, by multiple air cathodes and anode
Organic combination further improves the electricity generation performance of the electro-chemical systems in the same reaction compartment.
Specifically, the hollow type cathode slot includes multiple side walls and bottom surface, multiple side walls and institute
State bottom surface and limit hollow space inside the hollow type cathode slot, the side wall close to the hollow space side with
Atmosphere contact.Thus, it is possible to guarantee each air yin in the case where multiple air cathodes are incorporated into the same hollow space
Pole comes into full contact with air reacts, and further improves the electricity generation performance of electro-chemical systems.
Specifically, the anode is arranged between the hollow type cathode slot and the shell.It further mentions as a result,
The high using effect of electro-chemical systems.
Specifically, the modularization electrode assembly further comprises: anode slot, the anode setting are inserted in the anode
On the side wall of slot.Anode slot can be dismantled easily as a result, convenient for replacing to anode, also, when in the system
When being provided with multiple anodes, easily multiple anodes can be arranged in the same anode slot, further improve electrification
The using effect of system.
Specifically, multiple sub- cathodes are in parallel or series.The connection type multiplicity of multiple sub- cathodes as a result, Ke Yigen
According to needing to be combined, to form air cathode, the using effect of electro-chemical systems is further improved.
Specifically, the air cathode further comprises conductive supporting frame, the multiple sub- cathode is set up directly on described
On conductive supporting frame, the conductive supporting frame is electrically connected with the anode.Thus, it is possible to easily enable multiple sub- cathodes with sun
Pole electrical connection, further improves the using effect of electro-chemical systems.
Specifically, the air cathode further comprises multiple conducting wires, the multiple conducting wire and the multiple sub- cathode one
One is correspondingly connected with, and the multiple conducting wire is electrically connected with the anode.Thus, it is possible to easily enable multiple sub- cathodes with
Anode electrical connection, further improves the using effect of electro-chemical systems.
Specifically, the anode is at least one of carbon brush, carbon cloth, carbon paper, carbon felt, active carbon, graphite.When the electrification
When system is bioelectrochemical system, the adhesive ability of microorganism is can be improved in the anode, and can further save the electricity
The cost of chemical system.
Specifically, the anode is plane-shape electrode, the electro-chemical systems further comprise: diaphragm, the diaphragm setting
Between the air cathode and the anode.The diaphragm can slow down the pollution rate of air cathode as a result, further
Improve the electricity generation performance of electro-chemical systems.
Specifically, the catalyst layer includes atom level dispersion Co catalyst, atom level dispersion Fe catalyst or atom
Grade dispersion Ni catalyst.The type of the atom level dispersed metal catalyst is more as a result, from a wealth of sources, further improves sky
The service performance of gas cathode.
In the another aspect of the utility model, the utility model proposes a kind of cathodes.Specifically, the cathode includes: to urge
Agent layer, the catalyst layer include atom level dispersed metal catalyst；Current collection layer；And diffusion layer.Atom level is used as a result,
Oxygen reduction reaction in the dispersed metal catalyst cathode, not only with catalytic activity is good, metal utilization is high, at low cost
The advantages that honest and clean, and when the cathode is used for electro-chemical systems, electronics utilization rate can be improved, and then improve electro-chemical systems
Electricity generation performance.
At the another aspect of the utility model, the utility model proposes a kind of batteries.Specifically, before the battery includes:
Cathode described in face；And anode, the anode are electrically connected with the cathode.The battery has mentioned-above cathode as a result,
Possessed whole feature and advantage, and the battery efficiency of fuel cell generation is high, and operation stability is preferable.
Detailed description of the invention
The above-mentioned and/or additional aspect and advantage of the utility model from the description of the embodiment in conjunction with the following figures will
Become obvious and be readily appreciated that, in which:
Fig. 1 shows the structural schematic diagram of the electro-chemical systems according to the utility model one embodiment；
Fig. 2 shows the structural schematic diagram of the sub- cathode according to the utility model one embodiment；
Fig. 3 shows the structural schematic diagram of the sub- cathode according to the utility model another embodiment；
Fig. 4 shows the structural schematic diagram of the sub- cathode according to the utility model another embodiment；
Fig. 5 shows the structural schematic diagram of the sub- cathode according to the utility model another embodiment；
Fig. 6 shows the structural schematic diagram of the air cathode according to the utility model one embodiment；
Fig. 7 shows the structural schematic diagram of the air cathode according to the utility model another embodiment
Fig. 8 shows the structural schematic diagram of the electro-chemical systems according to the utility model another embodiment；
Fig. 9 shows the structural schematic diagram of the electro-chemical systems according to the utility model another embodiment；
Figure 10 shows the structural schematic diagram of the electro-chemical systems according to the utility model another embodiment；
Figure 11 shows the method stream of the preparation atom level dispersed metal catalyst according to the utility model one embodiment
Cheng Tu；
Figure 12 shows the structural schematic diagram of the battery according to the utility model one embodiment；
Figure 13 shows the electricity generation performance of the electro-chemical systems according to some specific embodiments of the utility model and comparative example
Test chart；
Figure 14 shows the electricity production of the bioelectrochemical system according to some specific embodiments of the utility model and comparative example
Performance test figure；And
Figure 15 is shown according to the stable of some specific embodiments of the utility model and the electro-chemical systems of comparative example
Property test chart.
Appended drawing reference:
10: catalyst layer；20: current collection layer；30: diffusion layer；40: supporting layer；100: shell；200: reaction compartment；300:
Modularization electrode assembly；310: hollow type cathode slot；311: side wall；320: air cathode；321: sub- cathode；322: conduction branch
Support；323: conducting wire；330: anode；350: extrernal resistance；360: anode slot；110: cathode；1000: electro-chemical systems.
Specific embodiment
The embodiments of the present invention are described below in detail, examples of the embodiments are shown in the accompanying drawings, wherein from beginning
Same or similar element or element with the same or similar functions are indicated to same or similar label eventually.Below by ginseng
The embodiment for examining attached drawing description is exemplary, and is only used for explaining the utility model, and should not be understood as to the utility model
Limitation.
In the one aspect of the utility model, the utility model proposes a kind of electro-chemical systems.Specifically, with reference to Fig. 1,
The electro-chemical systems 1000 may include: shell 100 and modularization electrode assembly 300, limit reaction compartment in shell 100
200, modularization electrode assembly 300 is arranged in reaction compartment 200.Specifically, during modularization electrode assembly 300 may include:
Empty formula cathode slot 310 and anode 330.Wherein, hollow type cathode slot 310 may include: multiple air cathodes 320, more
A air cathode 320 can be set on the side wall 311 of hollow type cathode slot 310, and air cathode 320 includes multiple sub- cathodes
321, sub- cathode 321 includes the catalyst layer containing atom level dispersed metal catalyst；Anode 330 is electrically connected with air cathode 320
It connects.The catalytic activity of the air cathode 320 is good as a result, metal utilization is high, low in cost etc., also, by the way that multiple sons are arranged
Cathode 321 can easily prepare the biggish air cathode 320 of area, and 320 profile pattern of air cathode obtained
Height, it is functional, it should be noted that in practical application in industry, when the production biggish air cathode of one bulk area, it is more difficult to
Guarantee the planarization and service performance on its surface, specifically, the air cathode 320, lesser by the way that multiple areas are arranged
Sub- cathode 321 can easily prepare large area and air cathode of good performance 320, be more conducive to the electrochemistry system
The industrial applications of system 1000.Specifically, each air cathode 320, may include the son of multiple area equations of array arrangement
Cathode 321.The area of every sub- cathode 321 is all relatively reasonable as a result, simple, fast can prepare and guarantee catalyst layer
Quality.In addition, the electro-chemical systems 1000 are also by setup module polarizing electrode component 300, by multiple air cathodes 320 and
330 organic combination of anode further improves the electricity generation performance of the electro-chemical systems 1000 in the same reaction compartment 200.
Specifically, hollow type cathode slot 310 may include multiple side walls 311 and bottom surface (not shown), it is multiple
Side wall 311 and bottom surface limit hollow space inside hollow type cathode slot 310, side wall 311 close to hollow space one
Side is contacted with atmosphere.Thus, it is possible to guarantee every in the case where multiple air cathodes 320 are incorporated into the same hollow space
A air cathode 320 comes into full contact with air to react, and further improves the electricity generation performance of electro-chemical systems 1000.
Inventors have found that current electro-chemical systems, generally contain only an air cathode and an anode, are transporting
During row, whole efficiency of fuel cell generation is limited.Also, air cathode is generally located on electrochemistry system due to needing to contact atmosphere
On the top surface or side of system.And according to the electro-chemical systems of the utility model embodiment, on the one hand, air cathode uses atom
Grade dispersed metal catalyst carrys out catalytic oxidation-reduction reaction, and catalysis reaction efficiency is high, and stability is good, improves in electro-chemical systems
Electronics utilization rate and electricity generation performance；On the other hand, by the way that hollow type cathode slot is arranged, multiple air cathodes can be set
It sets on the side wall of the hollow type cathode slot, i.e., multiple air cathodes is incorporated into the same electro-chemical systems, is not only saved
Space has been saved, and can guarantee that each air cathode can come into full contact with air, and the hydrogen reduction of each air cathode
Reaction is independent of each other.Electronics utilization rate and the electricity generation performance in electro-chemical systems are further improved as a result,.Also, it is hollow
Formula cathode slot can be dismantled easily, convenient for replacing to electrode, or according to the water situation of actual treatment, adjust
The power (can pass through increase and decrease number of electrodes realize) of whole whole system which thereby enhances the flexibility of the electro-chemical systems and practical
Property.
Specifically, sub- cathode 321 may include: catalyst layer 10 and current collection layer 20 with reference to Fig. 2.Wherein, catalyst layer 10
It is arranged on current collection layer 20, catalyst layer 10 includes atom level dispersed metal catalyst.Thus, it is possible to electronics utilization rate is improved,
And then improve the electricity generation performance of electro-chemical systems.
Specifically, with reference to Fig. 3 and Fig. 4, sub- cathode 321 may further include diffusion layer 30, and diffusion layer 30 can be with
Air is in contact (not shown), so that reduction reaction occurs using the oxygen in air, and then realizes the sub- cathode 321
Use function.Specifically, diffusion layer 30 can be set in side of the current collection layer 20 far from catalyst layer 10 with reference to Fig. 3, and with electricity
It solves liquid and contacts (not shown).Diffusion layer 30 is contacted with air as a result, so that oxygen can diffuse in the sub- cathode 321,
Current collection layer 20 is for being enriched with electric current simultaneously, and improves the electric conductivity of sub- cathode 321, and catalyst layer 10 is urged in atom level dispersed metal
Under agent effect, reduction reaction occurs using electronics and oxygen, and then the using effect of the sub- cathode 321 can be improved.
Specifically, the sub- cathode 321, which can also have a structure that diffusion layer 30 is in contact with air, (schemes with reference to Fig. 4
In be not shown), catalyst layer 10 is formed in side of the diffusion layer 30 far from air, and it is separate that current collection layer 20 is formed in catalyst layer 10
The side of diffusion layer 30, and with electrolyte contacts (not shown).And then the using effect of sub- cathode 321 can be improved.
In order to further increase the using effect of sub- cathode 321, specifically, sub- cathode 321 can also be into one with reference to Fig. 5
Step has supporting layer 40, and supporting layer 40 can be formed between catalyst layer 10 and diffusion layer 30, and supporting layer 40 can be by
Stainless (steel) wire is formed.Thus, it is possible to be that sub- cathode 321 provides more good support construction, and supports by supporting layer 40
Layer 40 is located at the two sides of catalyst layer 10 with current collection layer 20, and then can provide good protection for catalyst layer 10, prevents
Only 10 dusting of catalyst layer in actual use is lost and is adversely affected to the using effect of the sub- cathode 321.This
Outside, the supporting layer 40 being made of stainless (steel) wire can also further increase the electric conductivity of the sub- cathode 321, and then can be further
Improve the performance of the sub- cathode 321.
Specifically, multiple sub- cathodes 321 can connect or parallel connection.The connection type multiplicity of multiple sub- cathodes as a result,
It can according to need and be combined, to form air cathode 320, further improve the using effect of electro-chemical systems.
Specifically, multiple sub- cathodes 321 can directly be set when hollow type cathode slot 310 is formed by conductive material
It sets on the side wall of hollow type cathode slot 310；Specifically, when hollow type cathode slot 310 is formed by electrically non-conductive material,
Such as when being formed by plastics, with reference to Fig. 6, air cathode 320 may further include conductive supporting frame 322, multiple sub- cathodes 321
It can be set on conductive supporting frame 322, conductive supporting frame 322 is electrically connected with anode 330.Specifically, conductive supporting frame 322
Material is not particularly limited, as long as sub- cathode 321 can be made to fix and electrically conductive on its surface.For example, conductive supporting
Frame 322 can be stainless (steel) wire.Thus, it is possible to which multiple sub- cathodes 321 is easily enabled to be electrically connected with anode 330, further mention
The high using effect of electro-chemical systems 1000.
Specifically, when hollow type cathode slot 310 is formed by electrically non-conductive material, such as when being formed by plastics, reference
Fig. 7 can not also use conductive material to form conductive supporting frame, but in such a way that conducting wire is set, realize multiple sub- cathodes 321
It is in series or in parallel: air cathode 320 may further include multiple conducting wires 323, multiple conducting wires 323 and multiple sub- cathodes
321 correspond, and are electrically connected with anode 330.Thus, it is possible to which multiple sub- cathodes 321 are set up directly on hollow type cathode
On the side wall 311 of slot, each sub- cathode 321 then is electrically connected with anode 330 by multiple conducting wires, simplifies preparation work
Skill, and further improve the using effect of electro-chemical systems 1000.
Inventors have found that atom level dispersed metal catalyst has the active site of high degree of dispersion, therefore it is catalyzed
Active good, high catalytic efficiency, and metal utilization is high, and cost is relatively low.Inventor passes through further investigation and many experiments hair
It is existing, atom level dispersed metal catalyst can be applied in cathode, and be applied to electro-chemical systems and bioelectrochemistry
In system, so as to improve the oxygen reduction reaction efficiency of cathode, the electronics utilization rate in electro-chemical systems is improved, and then promoted
The electricity generation performance of electro-chemical systems.Also, inventors have found that above-mentioned sub- cathode construction, is particularly conducive to atom level dispersed metal
The attachment of catalyst.Under above-mentioned sub- cathode construction, not only can be easy be fixed on atom level dispersed metal catalyst is urged
Catalyst layer in agent layer, and after fixing also has preferable stability.Also, atom level dispersed metal catalyst is for yin
In extremely, also there is preferable catalytic action using the reduction reaction that air carries out for cathode.
Specifically, atom level dispersed metal catalyst may include carrier and the active metal that is supported on carrier.Tool
Body, the concrete type of carrier is not particularly limited, as long as atom level dispersed metal catalyst can be made more to be evenly dispersed in
Wherein, specifically, carrier can be graphene, mesoporous carbon, carbon nanotube, carbon black or active carbon etc..Specifically, active
The specific type of metal is not particularly limited, as long as energy catalytic oxidation-reduction reaction, specifically, active metal may include
At least one of Fe, Co and Ni.Specifically, active metal can be unit metal, such as single Co, single Ni are single
Fe, or double base metal, such as Fe/Co double base metal, Fe/Ni double base metal, Co/Ni double base metal, active metal
It can also be ternary metal, such as Fe/Co/Ni ternary metal.The type of the atom level dispersed metal catalyst is more as a result,
It is from a wealth of sources, and the hydrogen reduction efficiency of the air cathode is improved, reduce production cost.
Specifically, the specific number of air cathode 320 is not particularly limited, those skilled in the art can be according to practical need
It is configured.For example, 2-10 air cathode 320 can be set, 2,3 or 4 air cathodes 320 can be set.
Specifically, the specific number of anode 330 is also not particularly limited, for example, 1-10 anode 330 can be set, 1 can be set
A, 2,3 or 4 anodes 330.Specifically, air cathode 320 and the connection type of anode 330 are not particularly limited, only
Each air cathode 320 is wanted to have anode 330 connected to it.Specifically, air cathode 320 can be with anode 330
Connect one to one, can also be connect with multiple air cathode 320 and 1 anodes 330, can also with 1 air cathode 320 with it is multiple
Anode 330 connects.Specifically, the shape of hollow type cathode slot 310 is not particularly limited, those skilled in the art can basis
The number of the air cathode 320 wanted to set up is reasonably designed.Specifically, hollow type cathode slot 310 can be three
Prismatic, hexahedron type or octahedral figure.For example, specifically, hollow type cathode slot 310 can be hexahedron with reference to Fig. 1
Type, 2 air cathodes, 320,2 air cathodes 320 can be set on the side wall 311 of hollow type cathode slot opposite to be set
It sets, can also be disposed adjacent.Specifically, with reference to Fig. 8, it can also be in 4 side walls of the hexahedron hollow type cathode slot 310
4 air cathodes 320 are set on 311.Specifically, hollow type cathode slot 310 can be triangular prism-shaped, 3 skies with reference to Fig. 9
Gas cathode 320 can be set on 3 side walls of the triangular prism hollow type cathode slot 310.
Specifically, the material of anode 330 is not particularly limited, and when the electro-chemical systems are bioelectrochemical system, sun
As long as pole 330 is conducive to microorganism attachment.Specifically, anode 330 can be carbon brush, carbon cloth, carbon paper, carbon felt, active carbon
And at least one of graphite.Specifically, may include a carbon brush in anode 330, multiple groups carbon brush also can be set.It is similar
Ground can be monolayer carbon cloth when anode is carbon cloth, or combination be spaced apart with diaphragm, with multilayer carbon cloth.By
This, can be further improved microorganism in the adhesive ability of anode, and can save the cost of the electro-chemical systems.
Specifically, the concrete shape of anode 330 is not particularly limited, and when anode 330 is plane-shape electrode, such as carbon
Paper or carbon cloth, electro-chemical systems 1000 may further include the diaphragm being arranged between air cathode 320 and anode 330
(not shown).It specifically, the specific material of diaphragm is not particularly limited, such as can be glass fibre, plastic wire, nylon
Cloth etc..The diaphragm can prevent contact between air cathode and anode from short circuit occurs as a result, further shorten cathode and sun
Vertical range between pole improves electrode reaction efficiency, the ion diffusion between intensifier electrode, while slowing down air cathode pollution
Rate.Specifically, those skilled in the art can according to the actual situation, to the electro-chemical systems according to the utility model embodiment
Corresponding adjustment is made, more suitable structure is selected to form electro-chemical systems, as long as meeting previously described practical according to this
The feature of new embodiment.
Specifically, the set-up mode of anode 330 and position are not particularly limited, for example, anode 330 can be set with reference to Fig. 1
It sets between hollow type cathode slot 310 and shell 100.The using effect of electro-chemical systems is further improved as a result,.Tool
Body, with reference to Figure 10, modularization electrode assembly 300 may further include anode slot 360, and anode 330 also can be set
On the side wall of anode slot 360.Specifically, anode slot 360 can be arranged with Wrap round hollow type cathode slot 310, anode as a result,
Slot 360 can be dismantled easily, convenient for replacing to electrode.Also, when in system including multiple anodes 330,
Easily multiple anodes 330 can be incorporated into the same electro-chemical systems by the way that anode slot 360 is arranged, not only saved empty
Between, it is independent of each other, (can also can be led between each anode according to the water situation of actual treatment, the power for adjusting whole system
Cross the realization of increase and decrease number of electrodes).The using effect of electro-chemical systems 1000 is further improved as a result,.
Specifically, electro-chemical systems 1000 may further include multiple extrernal resistances 350, extrernal resistance 350 is arranged in air cathode
Between 320 and anode 330, and it is electrically connected with air cathode 320 and anode 330.Specifically, electro-chemical systems 1000 are transported
Total resistance value of multiple extrernal resistances 350 when row is not particularly limited, for example, can be 0 ohm, i.e. short circuit operation, or nothing
It is poor big, i.e. open running, or 2-1000 ohm.The using effect of electro-chemical systems is further improved as a result,.
It should be noted that concrete type is not particularly limited according to the electro-chemical systems of the utility model embodiment,
As long as oxygen reduction reaction occurs for its cathode.It such as can be fueled electrochemical system, Microbial fuel electro-chemical systems, micro-
Biological electrolytic cell or microorganism desalination electro-chemical systems etc., and according to the electro-chemical systems of the utility model embodiment,
Application scenarios are very extensive, such as can be used for handling sanitary sewage, trade effluent etc., and it leads to the organic matter in sewage
Crossing microorganism conversion is that electric energy generates available energy, low energy consumption and high-efficient while eliminating pollution.
Specifically, the preparation method of atom level dispersed metal catalyst is not particularly limited, if can make active metal with
The monoatomic form dispersion of metal.For example, synthetic method, metal organic frame can be assisted by infusion process, etching method, light
The preparation atom level dispersed metal catalyst such as synthetic method is assisted, the atom level dispersed metal catalyst in catalyst layer can as a result,
With with a variety of preparation methods, therefore it is easier to obtain, and can easily be applied in cathode, improves cathode oxygen
The efficiency of reduction reaction.
Specifically, atom level dispersed metal catalyst can be and prepare at low ambient temperatures.Thus, it is possible to easily make
Standby atom level dispersed metal catalyst of good performance, further increases the service performance of the cathode.Specifically, molten using low temperature
Liquid synthetic method prepares atom level dispersed metal catalyst, extensive, high metal load capacity preparation may be implemented, to improve gold
The effective rate of utilization for belonging to atom, reduces the application cost of metallic catalyst.Specifically, inhibiting to be nucleated using ultralow temperature liquid phase, make
The concentration for obtaining GOLD FROM PLATING SOLUTION category atom is lower than the nucleation limiting threshold value of metallic monomer concentration, to obtain dispersing gold containing atom level
The solution of category, and atom level dispersed metal catalyst is obtained by further loading process.Thus, it is possible in ultralow temperature solution
Atom level dispersed metal catalyst is synthesized in environment on a large scale.
Specifically, each step for the method for preparing catalyst is described in detail below,
Specifically, with reference to Figure 11, this method comprises:
S100: metallic compound and the first solvent are mixed to form metal front liquid solution
Specifically, in this step, metallic compound and the first solvent are mixed to form metal front liquid solution.Specifically
, metallic compound can be the soluble compound of at least one of Fe, Co and Ni, and the first solvent may include water, second
Alcohol, ethylene glycol, acetone, chloroform, ether, tetrafluoro hydrogen mutters, at least one of dimethylformamide and formaldehyde.Thus, it is possible to will
Above-mentioned solute and solvent are mixed to form metal front liquid solution, the source as atom fraction dispersed metallic in subsequent step.Tool
Body, the concentration of metal front liquid solution can be 0.001-1.0mol/L, specifically can for 0.005mol/L,
0.008mol/L、0.01mol/L、0.02mol/L、0.05mol/L、0.08mol/L、1.0mol/L。
Specifically, may include at least one of Fe, Co and Ni by atom level dispersed metal prepared by this method.Need spy
It does not mentionlet alone bright, can be unit metal catalyst by the atom level dispersed metal of this method preparation, for example, practical new according to this
The specific embodiment of type can use this method preparation atom level dispersed metal iron catalyst, or prepare original using this method
Sub- grade dispersed metal Co catalysts, or atom level dispersed metal Raney nickel is prepared using this method.Specifically, by this method
The atom level dispersed metal of preparation can also be double base metallic catalyst, for example, specific embodiment according to the present utility model, it can
To disperse using iron/cobalt double base metallic catalyst of this method preparation atom level dispersion, or using this method preparation atom level
Iron/nickel double base metallic catalyst, or using this method preparation atom level dispersion cobalt/nickel double base metallic catalyst.Specifically
, it can also be ternary metallic catalyst by the atom level dispersed metal of this method preparation, for example, tool according to the present utility model
Body embodiment can use iron/cobalt/nickel ternary metallic catalyst of this method preparation atom level dispersion.Thus, it is possible to using should
The preparation of method realization unit, double base and ternary metallic catalyst.
Specific embodiment according to the present utility model, metallic compound can be the soluble compound of Fe, Huo Zhewei
The soluble compound of Co, perhaps for the soluble compound of Ni or be Fe, Co mixing soluble compound,
Perhaps for Fe, Ni mixing soluble compound perhaps for Co, Ni mixing soluble compound or be Fe, Co,
The soluble compound of Ni mixing.Thus, it is possible to difference preparation unit, double base and ternary metallic catalyst.
S200: reducing agent and the second solvent are mixed to form reducing agent solution
Specifically, in this step, reducing agent and the second solvent are mixed to form reducing agent solution.Specifically, reducing agent
It may include NaBH4、KBH4、N2H4、N2H5OH, formaldehyde, formic acid, ascorbic acid, Na2SO3、K2SO3And H2C2O4At least it
One, the second solvent may include water, ethyl alcohol, ethylene glycol, acetone, chloroform, ether, tetrafluoro hydrogen mutter, dimethylformamide and first
At least one of aldehyde.Thus, it is possible to above-mentioned solute and solvent are mixed to form reducing agent solution, to make in subsequent process also
Former agent solution reacts with metal front liquid solution, and reduction obtains the solution containing atom level dispersed metal.Specifically, reduction
The concentration of agent solution can be 0.001-10.0mol/L, specifically can be 2mol/L, 5mol/L, 7mol/L, 8mol/L.It needs
It is noted that the first solvent and the second solvent are not water simultaneously.
S300: carrier material and third solvent are mixed to form dispersion liquid
Specifically, in this step, carrier material and third solvent are mixed to form dispersion liquid.Specifically, carrier material
It can be the carbon nanomaterial of doping.Specifically, can be formed on the surface of carbon nanomaterial scarce due to the presence of foreign atom
It falls into, so as to increase suction-operated of the carrier material to metallic atom, and then carrier material can be improved to metallic atom
Load capacity.Specific embodiment according to the present utility model, carrier material may include N doping mesoporous carbon (CMK-3), N doping
Graphene and graphite-phase nitrogen carbide (g-C3N4At least one of).Thus, it is possible to obtain high metal load capacity using above-mentioned material
Atom level dispersed metal catalyst.
Specifically, third solvent may include water, ethyl alcohol, ethylene glycol, acetone, chloroform, ether, tetrafluoro hydrogen mutter, dimethyl
At least one of formamide and formaldehyde.Thus, it is possible to above-mentioned solute and solvent are mixed to form dispersion liquid, in subsequent step
The middle Adsorption of solute metallic atom using in dispersion liquid obtains the atom level dispersed metal catalyst of carrier material load.Specifically
, it specifically can be 2.5g/L, 3.5g/L, 4.5g/L, 5.5g/L, 6.5g/ that the concentration of dispersion liquid, which can be 0.1-10g/L,
L、7.5g/L、8.5g/L、9.5g/L。
S400: metal front liquid solution is mixed with reducing agent solution, to obtain containing the molten of atom level dispersed metal
Liquid
Specifically, in this step, metal front liquid solution is mixed with reducing agent solution, to obtain containing atom level
The solution of dispersed metal.Specifically, under -100~0 DEG C of low temperature environment, by metal front liquid solution and reducing agent solution into
Row mixing.It will be appreciated to those of skill in the art that there is the nucleation limit of metallic monomer concentration in solution synthesis process
Threshold value, when being lower than this threshold value, the available solution containing atom level dispersed metal.And in the prior art often with microfluidic methods
Metallic monomer concentration is controlled, the mixed on low speed process of reactant is embodied in: by creating local low concentration, improving specific surface
Product reduces the transmission of the control quality and heat such as diffusion dimension.However the preparation flow of the above method is excessively complicated, yield is lower,
The serious large scale preparation for inhibiting atom level dispersed metal catalyst.
It can be obviously improved nucleating potential barrier specifically, passing through and reducing temperature, effectively inhibit nucleation, divided to improve in solution
The concentration of scattered metallic atom, and it is effectively adsorbed on different carrier surfaces, realize that atom fraction dissipates in ultralow temperature solution environmental
The extensive synthesis of metallic catalyst.Inventors have found that the metal dispersed in solution is former when temperature is higher than above-mentioned temperature range
The concentration of son is lower, and the effective rate of utilization of metallic atom is lower.And when temperature is lower than above-mentioned temperature range, it is dynamic to will lead to reaction
Mechanics and thermodynamics are excessively slow, can not effectively prepare.As a result, within the said temperature range by temperature setting, atom level may be implemented
The extensive synthesis of dispersed metal catalyst.
Specifically, in order to make the reaction process of reducing agent solution and metal front liquid solution within the said temperature range into
Row can be first by metal front liquid solution and reducing agent before to metal front liquid solution and reducing agent solution mixing
Solution keeps the temperature the regular hour in cryogenic box, for example, heat preservation 30min.Thus, it is possible to further increase GOLD FROM PLATING SOLUTION category atom
Concentration, further increase the utilization rate of metallic atom.
Hybrid mode about metal front liquid solution and reducing agent solution is not particularly limited, and those skilled in the art can
To be designed as the case may be.For example, specific embodiment according to the present utility model, can use syringe pump control, it will
Metal front liquid solution is added drop-wise in the reducing agent solution of stirring, or reducing agent solution is added drop-wise to the metal precursor of stirring
In solution, so that metal front liquid solution be made sufficiently to react with reducing agent solution, the solution containing atom level dispersed metal is obtained.
Specifically, atom level dispersed metal may include at least one of Fe, Co and Ni.Thus, it is possible to simply and effectively prepare containing
A variety of atom level dispersed metal catalyst of above-mentioned metal.
Specifically, metal front liquid solution and the opposite amount of reducing agent solution, it can be true by chemical equation
It is fixed, in order to react metal front liquid solution sufficiently with reducing agent solution, the amount of reducing agent solution can be made to be far longer than metal
The amount of precursor solution, to guarantee that the metallic atom in metal precursor solution is completely reduced.
Specifically, metal front liquid solution is added drop-wise in the reducing agent solution of stirring, or reducing agent solution is added dropwise
Into the metal front liquid solution of stirring, wherein drop rate can be 0.5-50mL/h, and stirring rate can be 0-
3000rpm.Thus, it is possible to promote metal front liquid solution sufficiently to react with reducing agent solution, to obtain containing atom fraction
The solution of dispersed metallic.According to the utility model specific embodiment, drop rate can for 2.5mL/h, 7.5mL/h, 15mL/h,
30mL/h、45mL/h。
S500: dispersion liquid is added in the solution containing atom level dispersed metal and is stirred, to obtain atom fraction
Dispersed metallic catalyst
Specifically, in this step, dispersion liquid is added in the solution containing atom level dispersed metal and is stirred, so as to
Obtain atom level dispersed metal catalyst.Specifically, containing atom level dispersed metal solution using the Adsorption of solute in dispersion liquid
In metallic atom, obtain and adulterate nanometer carbon material supported atom level dispersed metal catalyst.Specifically, the carbon nanometer of doping
Material has very strong suction-operated to metallic atom, so as to improve carrier material to the load capacity of metallic atom, improves
The effective rate of utilization of metallic atom.
It is the low temperature at -100~0 DEG C specifically, dispersion liquid is mixed with the solution containing atom level dispersed metal
It is carried out under environment, to guarantee that the metal in the solution containing atom level dispersed metal is adsorbed to carrier in an atomic fashion
On material, and then obtain the atom level dispersed metal catalyst of carrier material load.
Specifically, stirring after dispersion liquid is mixed with the solution containing atom level dispersed metal above-mentioned mixed solution
It mixes, promotes absorption of the carrier material to atom level dispersed metal, centrifugation then is carried out to above-mentioned solution or vacuum filtration is handled,
And be dried at room temperature, to obtain the atom level dispersed metal catalyst of high metal load capacity.Specifically, the speed of stirring
Rate can be 0-3000rpm, and the time of stirring can be 0-300min.
Specifically, in order to increase the thermal stability of atom level dispersed metal catalyst, this method can also include: that will pass through
The atom level dispersed metal catalyst that above-mentioned steps prepare, which is placed in gaseous environment, to be made annealing treatment.Specifically, gas
Environment can be high vacuum, nitrogen, argon gas or hydrogen-argon-mixed, and the amount of gas can be 50-600sccm, the temperature of annealing
Degree can be 200-1200 DEG C.Thus, it is possible to obtain heat-staple atom level dispersed metal catalyst.Tool about annealing
Body step is not particularly limited, and those skilled in the art can be designed as the case may be.
In summary, the atom level metallic catalyst prepared according to the utility model embodiment using low temperature solution polycondensation,
Have many advantages, such as big density, high yield, high efficiency, strong applicability, and the extensive quotient of atom level metallic catalyst can be significantly reduced
Therefore the cost of industryization application applies it in cathode, not only have many advantages, such as that catalytic activity is good, metal utilization is high, and
And production cost can be reduced.
Specifically, sub- cathode 321 can be through following methods preparation:
(1) 150-300mg carbon black powders are mixed into 650-750mg polytetrafluoroethylene (PTFE) binder, by repeatedly rolling, with branch
Timbering material stainless (steel) wire is tabletted at 4.5-10MPa, and using 340 DEG C of high-temperature stable 10-40min, diffusion can be obtained
Layer 30；
(2) 60-300mg atom level dispersed metal catalyst is mixed with 24-350 μ L polytetrafluoroethylene (PTFE) binder, then
It is uniformly applied to the stainless (steel) wire side of the diffusion layer 30 of step (1) preparation, catalyst layer 10 can be formed；
(3) structure prepared in the current collection layer 20 and step (2) formed stainless (steel) wire is pushed in 4.5-10MPa together
System, and formed in 60-100 DEG C of heating 20-60min, sub- cathode 321 can be obtained.
In summary, not only catalytic activity is good, metal utilization is high, low in cost for the air cathode 321, and prepares work
Skill is simple and easy to do, is suitble to large area production.
Specifically, the electro-chemical systems are when extrernal resistance is 50 ohm, power density can reach 2000mW/m2.The electricity as a result,
The efficiency of fuel cell generation of chemical system is higher, further improves the using effect of the electro-chemical systems.Specifically, the electro-chemical systems
Extrernal resistance be 50 ohm when, power density can reach 2540mW/m2, further improve the use effect of the electro-chemical systems
Fruit.
Specifically, current density decaying of the electro-chemical systems after operation 500 hours is no more than 5%.The electricity as a result,
The operation stability of chemical system is preferable, further improves the using effect of the electro-chemical systems.Specifically, the electrochemistry system
For system after operation 700 hours, the decaying of current density can also be no more than 5%, further illustrate the fortune of the electro-chemical systems
Row stability is preferable, further improves the using effect of the electro-chemical systems.
In the another aspect of the utility model, the utility model proposes a kind of cathodes.Specifically, can with reference to Fig. 3 and
Fig. 4, the cathode may include: catalyst layer, current collection layer and diffusion layer.Wherein, catalyst layer includes atom level dispersed metal
Catalyst.As a result, using the oxygen reduction reaction in the atom level dispersed metal catalyst cathode, not only there is catalytic activity
Well, the advantages that metal utilization is high, low in cost, and when the cathode is used for electro-chemical systems, electronics utilization can be improved
Rate, and then improve the electricity generation performance of electro-chemical systems.
At the another aspect of the utility model, the utility model proposes a kind of batteries.Specifically, with reference to Figure 12, the electricity
Pond includes: mentioned-above cathode and anode, and anode is electrically connected with cathode.The battery has mentioned-above cathode as a result,
Possessed whole feature and advantage, and the battery efficiency of fuel cell generation is high, and operation stability is preferable.
The embodiment of the utility model is explained below in conjunction with embodiment.Under it will be understood to those of skill in the art that
The embodiment in face is merely to illustrate the utility model, and should not be regarded as limiting the scope of the utility model.It is not specified in embodiment
Particular technique or condition, it described technology or conditions or is carried out according to the literature in the art according to product description.
Reagents or instruments used without specified manufacturer is that can buy the conventional products obtained by market.
Embodiment 1: preparation atom level disperses Co catalyst
(1) reaction solution A:0.01M CoCl is configured2Solution, solvent are that water/ethyl alcohol that volume ratio is 1:9 mixes solvent；
Prepare reducing agent solution B: the KOH containing 0.05M 5.0M N2H5OH hydrazine hydrate solution；Formulation vehicle dispersion liquid C:2.5mg mL-1
N doping mesoporous carbon dispersion liquid.
(2) above-mentioned reaction solution A and support dispersion C are placed in cryogenic box, are cooled to subzero 60 DEG C and keep the temperature 30 points
Clock；It is controlled with syringe pump, by the above-mentioned CoCl of 5mL2Reaction solution A is with 0.125mL min-1Rate be added dropwise to the reproducibility of 20mL
In solution B；Above-mentioned mixing liquid the reaction was continued under the conditions of subzero 60 DEG C 2h, is mixed into the above-mentioned support dispersion C of 20mL later, after
Continuous stirring 3-5 hours.
(3) it is filtered using cryogenic vacuum and recycles the monatomic sample of cobalt of mesoporous carbon-loaded obtained in step (2)
And clean, later in natural drying at room temperature.
(4) sample prepared in step (3) being subjected to thermal activation, condition are as follows: 90min is warming up to 900 DEG C, keeps the temperature 60min,
Cooled to room temperature, gas condition are 500sccm high-purity argon gas, can be obtained heat-staple atom level dispersion Co catalyst.
Embodiment 2: the air cathode of the dispersion Co catalyst containing atom level is prepared
The sub- cathode of the dispersion Co catalyst containing atom level is prepared first, and the specific method is as follows:
(1) prepare diffusion layer: by the carbon black powders of 212mg and 705.5mg polytetrafluoroethylene (PTFE) binder, (mass fraction is
60%) it mixes, 1.4mL dehydrated alcohol is added, water bath sonicator 20 seconds, uniform stirring was to having sticking purees.By purees
It is placed on plastic board and is rolled repeatedly with idler wheel 2 times, so that the mixing of diffusion layered material is more evenly, then rolled to fid
Expect to suppress 10min on stainless (steel) wire at 4.5MPa with powder compressing machine, be then placed in 340 DEG C of Muffle furnaces and fire 20min,
It is cooled to room temperature after taking-up.
(2) catalyst layer and sub- cathode are prepared: weighing the atom level dispersion Co catalyst prepared in 60mg embodiment 1,
70 μ L polytetrafluoroethylene (PTFE) binders (mass fraction 60%), 388 μ L deionized waters are added, in agitated under sonication mixing 20s, so
It is uniformly applied on the stainless (steel) wire of diffusion layer afterwards, a piece of stainless (steel) wire (i.e. current collection layer) is covered on it, together in 10MPa
Lower compacting 10min is then placed in 80 DEG C of baking ovens dry 30min, is cooled to room temperature after taking-up, is cut into the circle that diameter is 3cm,
The sub- cathode of the dispersion Co catalyst containing atom level is obtained.
By 9 sub- cathodes using above method preparation by multiple conductor in parallel, obtains the Co containing atom level dispersion and urge
The air cathode of agent.
Embodiment 3: the electro-chemical systems of the dispersion Co catalyst containing atom level are made
Reactor uses double chamber type configuration, and the long 4cm in anode chamber, it is the hole of 1cm that, which there is a diameter at top centre position, is used for
Platinum electrode is placed as anode；The long 2cm of cathode chamber, it is the hole of 1cm that, which there is a diameter in centre, for placing reference electrode, two
Chamber is separated using cation-exchange membrane.Load onto the air of the dispersion Co catalyst containing atom level prepared in titanium sheet and embodiment 2
Cathode after then being fixed with cathode baffle, is fixed in reactor quadrangle with screw rod and screw tightening, then reactor (i.e. electrochemistry
System) it is completed.Electrolyte uses 50mM phosphate buffer.
Comparative example 1: the electro-chemical systems of production nanoparticle catalyst containing Co
Other production method reference implementation examples 3, the difference is that in air cathode in the comparative example, catalyst Co
Nano particle.
Comparative example 2: the electro-chemical systems of production platiniferous C catalyst
Other production method reference implementation examples 3, the difference is that catalyst is platinum in air cathode in the comparative example
C catalyst.
Comparative example 3: electro-chemical systems of the production containing activated-carbon catalyst
Other production method reference implementation examples 3, the difference is that catalyst is to live in air cathode in the comparative example
Property Pd/carbon catalyst.
Electricity generation performance test
Air cathode performance is evaluated using chrono-amperometric voltammetry
Using the electro-chemical systems made in chrono-amperometric voltammetric determination embodiment 3 and comparative example 1-3 cathode also
Primary current.Open circuit is measured since onset potential 0.2V (reference electrode Ag/AgCl) after 3 hours, measures one every 0.1V
Group, destination potential are -0.4V (reference electrode Ag/AgCl), current value stable under each group of potential are taken, with active cathodic face
Product 7cm2Conversion is current density (current density i=U/ (RA), U are output voltage, and R is outer resistance value, and A is cathode area).Ginseng
Figure 13 is examined, under 0.2V to -0.4V same potential, the reduction current of the cathode of the dispersion Co catalyst containing atom level is higher than to be received containing Co
The air cathode of rice grain, platinum carbon and active carbon.By taking -0.4V as an example, the air cathode of the dispersion Co catalyst containing atom level is obtained
Obtained highest current density 26A/m2, and the current density of platinum carbon air cathode is only 16A/m2, it will be apparent that, it is practical according to this
The air cathode of the dispersion Co catalyst containing atom level of new embodiment has more excellent than the traditional electrode being widely used at present
Electric property more.
Embodiment 4: the Microbial fuel electro-chemical systems of the dispersion Co catalyst containing atom level are made
Using carbon brush as anode, adheres to anaerobism and produce electricity bacterium, anode material 450 DEG C of calcining 30min in Muffle furnace are carried out
Pretreatment.Reactor uses single chamber type configuration, and with a thickness of 4cm, position is the hole of 6mm there are two diameter side by side among top,
One is used to place anode carbon brush, another is for placing reference electrode；O-ring and gasket are used between cavity and anode and cathode baffle
Sealing is fixed, and is loaded onto the air cathode of the dispersion Co catalyst containing atom level prepared in titanium sheet and embodiment 2, is then kept off with cathode
After plate is fixed, fixed in reactor quadrangle with screw rod and screw tightening, then reactor (i.e. Microbial fuel electro-chemical systems) group
It installs into.Inoculation source is 50mM phosphate using the Microbial fuel electro-chemical systems anode water outlet operated normally, matrix
Buffer concentration is 1g/L sodium acetate, and 12.5mL/L minerals and 5mL/L vitamin is added.
Comparative example 4: the Microbial fuel electro-chemical systems of production nanoparticle catalyst containing Co
Its production method reference implementation example 4, the difference is that catalyst is received in air cathode in the comparative example for Co
Rice grain.
Comparative example 5: the Microbial fuel electro-chemical systems of production platiniferous C catalyst
Its production method reference implementation example 4, the difference is that catalyst is platinum carbon in air cathode in the comparative example
Catalyst.
Comparative example 6: Microbial fuel electro-chemical systems of the production containing activated-carbon catalyst
Its production method reference implementation example 4, the difference is that catalyst is activity in air cathode in the comparative example
Pd/carbon catalyst.
Electricity generation performance test
Polarization curve is measured using extrernal resistance method is changed
The Microbial fuel electrochemistry made in embodiment 4 and comparative example 4-6 is measured using quick change extrernal resistance method
The polarization curve of system replaces external resistance in the short time that is, in a cycle of operation and reaches stable, and reactor replaces 1g/L
After sodium acetate matrix, stablize under 5000 Ω extrernal resistances one hour, record output voltage and anode potential, is then dropped every 20min
Low external resistance makes external resistance be followed successively by 1000 Ω, 500 Ω, 300 Ω, 200 Ω, 100 Ω, 50 Ω, 30 Ω, 20 Ω, 10 Ω, 5
Ω, 2 Ω, and output voltage and anode potential stable under the resistance are recorded in real time, it can be calculated according to data each outer
Power density P=Ui under resistance, wherein current density i=U/ (RA), U are output voltage, and R is outer resistance value, and A is cathode plane
Product.Using current density i as abscissa, area power density P is ordinate, area power density curve is drawn out, such as Figure 14 institute
It shows.It can be seen from the figure that the cathode maximum power of the Microbial fuel electro-chemical systems of the dispersion Co catalyst containing atom level
Density can reach 2500mW/m2Left and right, the maximum power density of Co nano particle air cathode are 2100mW/m2Left and right, active carbon
The maximum power density of air cathode is 1600mW/m2Left and right, the maximum power density of platinum carbon air cathode are 1500mW/m2It is left
It is right, it is obvious that the maximum power density of the Microbial fuel electro-chemical systems of the dispersion Co catalyst containing atom level is higher than to be received containing Co
The Microbial fuel electro-chemical systems of rice grain, platinum carbon and active carbon.
In summary, the catalytic performance of atom level dispersion Co catalyst is good, and catalytic efficiency is higher, is dispersed using atom level
The electro-chemical systems and Microbial fuel electro-chemical systems of Co catalyst all have preferable electricity generation performance.
Operation stability test
The Microbial fuel electro-chemical systems made to embodiment 4 and comparative example 5 carry out operation stability test, that is, exist
Under the conditions of certain external resistance, output voltage U of the electro-chemical systems when running different time is tested, and calculate according to data
(i=U/ (RA), U are output voltage to current density value i when electro-chemical systems run different time, and R is outer resistance value, and A is cathode
Area), for example, respectively test 50 Ω of electro-chemical systems external resistance under the conditions of, operation 50h, 100h, 150h, 200h, 250h,
Output voltage when 300h, 350h, 400h, 450h, 500h, 550h, 600h, 650h and 700h, in order to further prove to contain
Atom level disperses the stability of the Microbial fuel electro-chemical systems electricity generation performance of Co catalyst, the microorganism of platiniferous C catalyst
Fueled electrochemical system strikes off the biomembrane on air cathode surface after running 200h, continues to test it later when different
Between when output voltage, and calculate its current density value, test result is as illustrated in FIG. 15.It can be seen from the figure that containing original
The Microbial fuel electro-chemical systems of sub- grade dispersion Co catalyst, electricity generation performance is highly stable, hardly follows electro-chemical systems
The variation of runing time and change, after running 700h, current density value is still relatively stable, with starting when compare, almost
Do not decline.And the Microbial fuel electro-chemical systems containing platinum carbon catalyst, with the increase of electro-chemical systems runing time,
Electricity generation performance reduction is obvious, and after running 700h, electricity generation performance is only 65% when originating.Strike off the biomembrane of cathode
Afterwards, the electricity generation performance of the Microbial fuel electro-chemical systems of platiniferous C catalyst increases, and illustrates the sky of platiniferous C catalyst
Gas cathode is easily contaminated, hinders it and contacts with air, hinder the oxygen reduction reaction of cathode, and reduces anode to organic
The capacity of decomposition of object in turn results in the reduction of electro-chemical systems electricity generation performance.And the air yin of the dispersion Co catalyst containing atom level
On extremely, microorganism is not easy to assemble, and contamination resistance is strong, and electricity generation performance is relatively stable, good cycle.Comparison is it is found that atom
The catalytic performance of grade dispersion Co catalyst is good, and stability is very high, the microorganism combustion containing atom level dispersion Co catalyst
Expect that the electricity production stability of electro-chemical systems is preferable.
Embodiment 5: electro-chemical systems of the production containing 2 air cathodes
Other production methods are a difference in that the electrode of the electro-chemical systems uses modularization electrode assembly with embodiment 3,
With reference to Fig. 1, hollow type cathode slot 310 is hexahedron type, and 2 air cathodes 320 are placed on the two of hollow type cathode slot 310
On a side wall, wherein urging containing the dispersion Co catalyst containing atom level prepared as described in Example 2 in air cathode 320
Agent layer is full of air among hollow type cathode slot 310, is inserted into the reaction compartment 200 full of matrix；It again will be each
Cathode 321 is connect with the carbon brush anode 330 of attachment anaerobism electricity production bacterium with conducting wire, and connects extrernal resistance 350, can be prepared by containing 2
The electro-chemical systems of air cathode.
Embodiment 6: electro-chemical systems of the production containing 3 air cathodes
Other production methods are with embodiment 5, with reference to Fig. 9, the difference is that hollow type cathode slot 310 used is trigone
Column type, 3 air cathodes 320 are placed on three side walls of hollow type cathode slot 310, wherein are contained in air cathode 320
The catalyst layer of the dispersion Co catalyst containing atom level prepared as described in Example 2.
Embodiment 7: electro-chemical systems of the production containing 4 air cathodes
Other production methods are with embodiment 4, with reference to Fig. 8, the difference is that 4 air cathodes 320 are placed on hollow type
On four side walls of cathode slot 310, wherein contain the fraction containing atom prepared as described in Example 2 in air cathode 320
Dissipate the catalyst layer of Co catalyst.
The orientation or positional relationship of the instructions such as term " on ", "lower" is based on attached drawing institute in the description of the present invention,
The orientation or positional relationship shown is merely for convenience of description the utility model rather than requires the utility model must be with specific
Orientation construction and operation, therefore should not be understood as limiting the present invention.
In the description of this specification, the description of reference term " one embodiment ", " another embodiment " etc. means to tie
The embodiment particular features, structures, materials, or characteristics described are closed to be contained at least one embodiment of the utility model.
In the present specification, the schematic representation of the above terms does not necessarily have to refer to the same embodiment or example.Moreover, description
Particular features, structures, materials, or characteristics may be combined in any suitable manner in any one or more of the embodiments or examples.
In addition, without conflicting with each other, those skilled in the art can by different embodiments described in this specification or
The feature of example and different embodiments or examples is combined.
Although the embodiments of the present invention have been shown and described above, it is to be understood that above-described embodiment is
Illustratively, it should not be understood as limiting the present invention, those skilled in the art are in the scope of the utility model
Inside it can make changes, modifications, alterations, and variations to the above described embodiments.
Claims (10)
1. a kind of electro-chemical systems characterized by comprising
Shell limits reaction compartment in the shell；And
Modularization electrode assembly, the modularization electrode assembly are arranged in the reaction compartment, the modularization electrode assembly
Further comprise:
Hollow type cathode slot, the hollow type cathode slot include: multiple air cathodes, and the multiple air cathode setting exists
On the side wall of the hollow type cathode slot, the air cathode includes multiple sub- cathodes, and the sub- cathode includes containing atom
The catalyst layer of grade dispersed metal catalyst；
Anode, the anode are electrically connected with the air cathode.
2. electro-chemical systems according to claim 1, which is characterized in that the hollow type cathode slot includes multiple described
Side wall and bottom surface, multiple side walls and the bottom surface limit hollow space inside the hollow type cathode slot,
The side wall is contacted close to the side of the hollow space with atmosphere.
3. electro-chemical systems according to claim 1, which is characterized in that the anode setting is inserted in the hollow type cathode
Between slot and the shell.
4. electro-chemical systems according to claim 1, which is characterized in that the modularization electrode assembly further comprises:
Anode slot, the anode are arranged on the side wall of the anode slot.
5. electro-chemical systems according to claim 1, which is characterized in that multiple sub- cathodes are in parallel or series；
The air cathode further comprises conductive supporting frame, and the multiple sub- cathode is set up directly on the conductive supporting frame
On, the conductive supporting frame is electrically connected with the anode；
The air cathode further comprises multiple conducting wires, and the multiple conducting wire connects one to one with the multiple sub- cathode,
And the multiple conducting wire is electrically connected with the anode.
6. electro-chemical systems according to claim 1, which is characterized in that the anode is carbon brush, carbon paper, carbon felt, activity
At least one of charcoal.
7. electro-chemical systems according to claim 1, which is characterized in that the anode is plane-shape electrode, the electrochemistry
System further comprises: diaphragm, and the diaphragm is arranged between the air cathode and the anode.
8. electro-chemical systems according to claim 1, which is characterized in that the catalyst layer includes that atom level dispersion Co is urged
Agent, atom level dispersion Fe catalyst or atom level disperse Ni catalyst.
9. a kind of cathode characterized by comprising
Catalyst layer, the catalyst layer include atom level dispersed metal catalyst；
Current collection layer；And
Diffusion layer.
10. a kind of battery characterized by comprising
Cathode as claimed in claim 9；And
Anode, the anode are electrically connected with the cathode.
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| CN201820542336.4U CN208272026U (en) | 2018-04-17 | 2018-04-17 | Electro-chemical systems, cathode, battery |
| PCT/CN2018/114155 WO2019200895A1 (en) | 2018-04-17 | 2018-11-06 | Single-atom air cathode, battery, electrochemical system and bioelectrochemical system |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108630950A (en) * | 2018-04-17 | 2018-10-09 | 清华大学 | Monatomic air cathode, battery, electro-chemical systems and bioelectrochemical system |
| CN111446476A (en) * | 2020-04-14 | 2020-07-24 | 中国船舶重工集团公司第七二五研究所 | Long-term power supply device for sediment type microbial fuel cell |
-
2018
- 2018-04-17 CN CN201820542336.4U patent/CN208272026U/en active Active
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108630950A (en) * | 2018-04-17 | 2018-10-09 | 清华大学 | Monatomic air cathode, battery, electro-chemical systems and bioelectrochemical system |
| CN111446476A (en) * | 2020-04-14 | 2020-07-24 | 中国船舶重工集团公司第七二五研究所 | Long-term power supply device for sediment type microbial fuel cell |
| CN111446476B (en) * | 2020-04-14 | 2022-12-02 | 中国船舶重工集团公司第七二五研究所 | Long-term power supply device for sediment type microbial fuel cell |
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