CN102263273B - Self-respiration microfluid fuel cell based on positive displacement three-dimensional anode catalysis - Google Patents
Self-respiration microfluid fuel cell based on positive displacement three-dimensional anode catalysis Download PDFInfo
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Abstract
The invention provides a self-respiration microfluid fuel cell based on positive displacement three-dimensional anode catalysis. The fuel cell comprises a baseboard, a top plate, a cathode electrode, an anode electrode, a spacer rod, an inlet end plate and an outlet end plate, wherein the inlet end plate and the outlet end plate are respectively arranged on the front end and rear end of the baseboard, and the top plate is arranged on the top of the baseboard. The fuel cell is characterized in that a channel is arranged on the baseboard, an electrolyte inlet and a fuel inlet are arranged on the inlet end plate, an outlet is arranged on the outlet end plate, and the outlet, the electrolyte inlet and the fuel inlet are communicated with the channel; an electrolyte enters the channel through the electrolyte inlet, and a fuel enters the channel through the fuel inlet; the lower part of the channel is provided with the anode electrode, wherein the anode electrode comprises an anode bar in which a conducting material is used as a matrix, and a catalyst is deposited on the surface of a conducting material; and the spacer rod is arranged on the upper part of the cathode electrode, an air respiration hole is arranged on the top plate, the air respiration hole is opposite to the channel, and the cathode electrode is arranged above the spacer rod.
Description
Technical field
The present invention relates to the microfluid fuel cell, be specifically related to the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell of positive displacement.
Background technology
Microfluid fuel cell (Microfluidic fuel cell), also claim the fuel cell (Laminar flow-based fuel cell) based on laminar flow or do not have membrane cell (Membraneless fuel cell), it is the characteristics of utilizing fluid to flow at the minute yardstick underflow, make two fluid streams that comprise fuel and oxidant respectively separate naturally, can work at normal temperatures and pressures.Compare with traditional fuel cell, the microfluid fuel cell does not need proton exchange membrane, not only have compact conformation, advantage that cost is low, and avoided the fuel infiltration relevant with film, film is dry, film is degenerated and problem such as negative electrode water management, make it become the substitute electric power that fields such as portable electric appts, microsensor, microrobot have potentiality, yet existing microfluid fuel cell performance and fuel availability are all lower, have seriously restricted its development and application.
In the microfluid fuel cell, electrode adopts the plate armature (US2006003217 that is positioned at the microchannel wall usually, WO2006031268-A2, US20060210867), the viscous effect of fluid is much larger than the inertia effect under minute yardstick, surface force has substantially exceeded body force, therefore, carrying out along with reaction, the anode and cathode reactant constantly consumes, and makes that reactant concentration constantly reduces near electrode, forms depletion boundaries layer (Depletion boundary layer), seriously restrict the transmission of anode and cathode reactant to electrode, reduced fuel availability and battery performance.Adopt the three-diemsnional electrode structure of graphite rod to be applied to whole vanadium oxide reduction microfluid fuel cell (E. Kjeang, J. McKechnie, D. Sinton, et al. J. Power Sources, 2007,168 (2): 379-390.), adopt oxidation-reduction pair V
2+/ V
3+And VO
2+/ VO
2 +Be dissolved in the dilute sulfuric acid and act as a fuel respectively and oxidant, compare with the plate electrode design, increased the specific area of reaction electrode, make battery performance and fuel availability all obtain raising to a certain degree.But because vanadium-containing water and discarded object are the important sources of soil pollution of vanadium, must handle the waste liquid of whole vanadium oxide reduction microfluid fuel cell for reducing pollution of vanadium, complexity and auxiliary energy consumption that this has just increased whole system are unfavorable for the microminiaturization of battery.By contrast, organic substance such as formic acid, methyl alcohol act as a fuel have the energy density height, cheap, source advantage such as abundanter, be widely used in the microfluid fuel cell, and the microfluid fuel cell that yet there are no the three-dimensional anode construction of positive displacement that adopts this class A fuel A occurs.
Since oxygen have oxidation-reduction potential higher, easily obtain, product is water, need not to carry out advantage such as reprocessing, cathode side at the microfluid fuel cell adopts dissolved oxygen as oxidant (US7435503 mostly, US20060003217, WO2006031268-A2, US20060228622, US20060210867, US20040058217), but the diffusion coefficient that it is less and lower oxygen concentration have seriously limited the mass transfer of cell cathode side oxygen, have greatly reduced battery performance.Consider that the aerial diffusion coefficient of oxygen is than high four orders of magnitude in solution, its concentration also is higher than the concentration of oxygen in solution, the researcher has proposed microfluid fuel cell (the R.S. Jayashree of air self-respiration type cathode construction, L. Gancs, E.R. Choban, et al. JACS, 2005,127 (48): 16758-16759.), negative electrode adopts gas-diffusion electrode, directly be exposed in the air, not only strengthened the oxygen mass transfer of cathode side, also reduced the parasitic energy consumption of entire cell system, battery performance also improves greatly, be that the employing dissolved oxygen is 5 times of oxidant under similarity condition, but because anode-side still adopts the plate electrode structure, the carrying out along with reaction still can form the depletion boundaries layer near anode electrode, the mass transfer that this has limited the anode reaction thing greatly has a strong impact on from breathing the microfluid fuel cell performance.
Summary of the invention
Technical problem to be solved by this invention is to provide positive displacement the three-dimensional anode-catalyzed microfluid of breathing certainly fuel cell, to obtain higher fuel availability and battery performance.
In order to solve the problems of the technologies described above, technical scheme of the present invention is that the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell of a kind of positive displacement comprises base plate, top board, cathode electrode, anode electrode, spacer rod, sheet inlet and outlet end plate; Wherein, sheet inlet and outlet end plate are separately positioned on the rear and front end of base plate, top board is arranged on the top of base plate, be characterized in: be provided with conduit at base plate, sheet inlet is provided with electrolyte import and fuel inlet, the outlet end plate is provided with outlet, and outlet is as the outlet of intact fuel, product and electrolyte of unreacted; Outlet, electrolyte import and fuel inlet all communicate with conduit, electrolyte enters conduit by the electrolyte import, fuel enters conduit by fuel inlet, anode electrode is placed in bottom at conduit, this anode electrode comprises anode stub, this anode stub adopts electric conducting material as matrix, and at the electric conducting material surface deposition catalyst is arranged; Top at anode electrode is placed with spacer rod, be provided with the aerial respiration hole at top board, the aerial respiration hole is relative with conduit, cathode electrode is arranged on the top of spacer rod, be coated with eelctro-catalyst in the one side near the cathode electrode of spacer rod, the another side of cathode electrode directly is exposed in the air by the aerial respiration hole.
Because anode electrode comprises anode stub, this anode stub adopts electric conducting material as electrode matrix, and by electrochemical deposition method catalyst deposit is made in the electric conducting material surface; With anode stub layering regular arrangement in conduit as anode electrode, therefore, in conduit, form the three-dimensional anode-catalyzed structure of positive displacement, fuel flows by the micro-pore between the anode stub, flow in the micro-pore of electrolyte between spacer rod, fuel mixes by diffusion at the liquid/liquid interface place that forms with electrolyte, the flow velocity of control fuel and electrolyte makes two fluid streams form Laminar Flow in conduit, guarantee fuel can not diffuse to cathode electrode simultaneously and the fuel infiltration phenomenon takes place, fuel is oxidized on the anode electrode surface, and discharge proton and electronics simultaneously, proton arrives cathode electrode by electrolyte, electronics arrives cathode electrode by external circuit, the fuel that unreacted is intact, product and electrolyte are discharged battery by the outlet on the outlet end plate.At cathode side, adopt carbon paper or carbon cloth as cathode electrode, simultaneously spray eelctro-catalyst Pt/C at the cathode electrode near spacer rod, directly be exposed in air by the aerial respiration hole cathode electrode another side, airborne oxygen is delivered to the catalyst surface of cathode electrode by diffusion and free convection mode, with proton and electronics generation electrochemical reducting reaction generation water.
The present invention adopts the three-dimensional anode-catalyzed structure of positive displacement in anode-side, increased the specific area of electrode reaction, simultaneously, adopt the self-respiration type electrode structure at cathode side, utilize oxygen higher diffusion coefficient and advantage of concentration in air, thereby reach the purpose of strengthening anode and cathode reactant mass transfer, accelerating electrochemical reaction speed;
According to the three-dimensional anode-catalyzed preferred version of breathing the microfluid fuel cell certainly of positive displacement of the present invention, described spacer rod is graphite rod or carbon-point.
According to the three-dimensional anode-catalyzed preferred version of breathing the microfluid fuel cell certainly of positive displacement of the present invention, anode stub with graphite rod or carbon-point as matrix, and by electrochemical deposition method with catalyst deposit in graphite rod or carbon-point surface.
According to the three-dimensional anode-catalyzed preferred version of breathing the microfluid fuel cell certainly of positive displacement of the present invention, base plate, top board, sheet inlet and outlet end plate all adopt transparent material to make.
According to the three-dimensional anode-catalyzed preferred version of breathing the microfluid fuel cell certainly of positive displacement of the present invention, described fuel adopts formic acid, formates, methyl alcohol or ethanol.
The three-dimensional anode-catalyzed beneficial effect of breathing the microfluid fuel cell certainly of positive displacement of the present invention is: the present invention adopts the three-dimensional anode-catalyzed structure of positive displacement in anode-side, increased the specific area of electrode reaction, simultaneously, adopt the self-respiration type electrode structure at cathode side, utilize oxygen higher diffusion coefficient and advantage of concentration in air, thereby reach the purpose of strengthening anode and cathode reactant mass transfer, accelerating electrochemical reaction speed; The present invention has improved microfluid fuel cell performance and fuel availability, and can increase the flexibility that battery pack is arranged by radical and the arrangement that changes anode stub and spacer rod, simultaneously, microfluid fuel cell involved in the present invention does not need proton exchange membrane, not only have compact conformation, advantage that cost is low, and can avoid the fuel infiltration relevant with film, film is dry, film is degenerated and problem such as negative electrode water management, have a good application prospect.
Description of drawings
Fig. 1 is the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell structure schematic diagram of positive displacement of the present invention.
Fig. 2 is the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell assembling relationship figure of positive displacement of the present invention.
Fig. 3 is the front view of sheet inlet 9.
Fig. 4 is the cutaway view of Fig. 3.
Fig. 5 is the front view of outlet end plate 6.
Fig. 6 is the layout schematic diagram of conduit inner anode rod 15 and spacer rod 5 among the embodiment one.
Fig. 7 is three-dimensional anode-catalyzed the microfluid fuel cell of breathing certainly and flat fuel cell performance comparison diagram of positive displacement.
Fig. 8 is the three-dimensional anode-catalyzed fuel availability comparison diagram of breathing microfluid fuel cell and flat fuel cell certainly of positive displacement.
Embodiment
Be further described specifically below in conjunction with the present invention of embodiment, but embodiments of the present invention are not limited thereto.
Referring to Fig. 1 to Fig. 6, the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell of a kind of positive displacement comprises base plate 2, top board 7, cathode electrode 1, anode electrode 4, spacer rod 5, sheet inlet 9 and outlet end plate 6; Wherein, base plate 2, top board 7, sheet inlet 9 and outlet end plate 6 all adopt transparent material such as Merlon, polymethyl methacrylate etc. to make; Wherein, sheet inlet 9 and outlet end plate 6 are separately positioned on the rear and front end of base plate 2, top board 7 is arranged on the top of base plate 2, on base plate 2, longitudinally be provided with conduit 12, sheet inlet 9 is provided with electrolyte import 10 and fuel inlet 11, and outlet end plate 6 is provided with outlet 3, and sheet inlet 9 and outlet end plate 6 are provided with a plurality of location holes 16, the quantity of location hole 16 is pressed anode stub 15 and is arranged with spacer rod 5 quantity sums, and location hole 16 is used for fixed anode rod 15 and spacer rod 5; Outlet 3, electrolyte import 10 and fuel inlet 11 all communicate with conduit 12, electrolyte enters conduit 12 by electrolyte import 10 and passage 13, fuel enters conduit 12 by fuel inlet 11 and passage 14, anode electrode 4 is placed in bottom at conduit 12, this anode electrode 4 is arranged by N root anode stub 15 layering rules and constitutes, wherein, N is the natural number more than or equal to 2; This anode stub 15 adopts electric conducting material as matrix, and by electrochemical deposition method catalyst deposit is made in the electric conducting material surface; Be placed with M root spacer rod 5 on the top of anode electrode 4, wherein, M is the natural number more than or equal to 2; The setting of anode stub 15 and spacer rod 5, must guarantee that fuel flows by the micro-pore between the anode stub 15, flow in the micro-pore of electrolyte between spacer rod 5, fuel mixes by diffusion at the liquid/liquid interface place that forms with electrolyte, and the flow velocity of control fuel and electrolyte makes two fluid streams form Laminar Flow in conduit, guarantees that simultaneously fuel can not diffuse to cathode electrode and the fuel infiltration phenomenon takes place; The equivalent diameter that micro-pore between rod and the rod can be set is 0.1 millimeter to 2 millimeters; Be provided with aerial respiration hole 8 at top board 7, aerial respiration hole 8 is relative with conduit 12, cathode electrode 1 is arranged on the top of spacer rod 5, can adopt carbon paper or carbon cloth as cathode electrode 1, at the one side spraying eelctro-catalyst near the cathode electrode 1 of spacer rod 5, the another side of cathode electrode 1 directly is exposed in the air by aerial respiration hole 8.
For conveniently installing and being connected, stretch out respectively outside sheet inlet 9 and the outlet end plate 6 at the two ends of described anode electrode 4, and an end of cathode electrode 1 is drawn.
In specific embodiment, spacer rod 5 and anode stub 15 basis material equal diameters; Because graphite rod and carbon-point cost are low, described spacer rod 5 all adopts graphite rod or carbon-point with the basis material of anode stub 15, and, anode stub 15 also by electrochemical deposition method with catalyst deposit in graphite rod or carbon-point surface; Spacer rod 5 also can adopt metal bar or other non-metallic rods, and anode stub 15 also can adopt the conducting metal rod.
The three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell of a kind of positive displacement of the present invention can adopt pluralities of fuel, as abundant liquid state organics in source such as formic acid, formates, methyl alcohol, ethanol, anode catalyst is decided according to fuel, need use acidic electrolyte bath with the acid during for fuel, can use alkaline electrolyte with the alkaloids during for fuel, can use acidity or alkaline electrolyte when being fuel with alcohols or salts substances, the eelctro-catalyst of cathode electrode 1 spraying can adopt Pt/C.
Below in conjunction with specific embodiment, and referring to Fig. 7 and Fig. 8, performance of the present invention and fuel availability are described.Wherein:
Fig. 7 is three-dimensional anode-catalyzed the microfluid fuel cell of breathing certainly and flat fuel cell performance comparison diagram of positive displacement.Wherein, the A line is flat fuel cell performance curve; The B line is the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell performance curve of positive displacement when adopting acidic electrolyte bath; The C line is the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell performance curve of positive displacement when adopting alkaline electrolyte
Fig. 8 is the three-dimensional anode-catalyzed fuel availability comparison diagram of breathing microfluid fuel cell and flat fuel cell certainly of positive displacement.Wherein, the A line is the fuel availability curve of flat fuel cell; The B line is the three-dimensional anode-catalyzed fuel availability curve of breathing the microfluid fuel cell certainly of positive displacement when adopting acidic electrolyte bath; The C line is the three-dimensional anode-catalyzed fuel availability curve of breathing the microfluid fuel cell certainly of positive displacement when adopting alkaline electrolyte
Embodiment one:
In this embodiment, conduit 12 long 40 mm, its cross section is 2.5 mm * 6.3 mm, is furnished with 12 anode stubs 15 in the conduit 12 as anode electrode 4, is furnished with 8 spacer rods 5 above anode stub 15, anode stub 15 is seen Fig. 6 with the layout of spacer rod 5; Between two adjacent anode stubs, between two adjacent spacer rods 5 and adjacent anode stub and the centre-to-centre spacing between the spacer rod 5 be 0.9 mm, and adopt diameter be the graphite rod of 0.5 mm as the matrix of spacer rod 5 and anode stub 15, and by electrochemical deposition method catalyst P d is deposited on the graphite rod surface and makes anode electrode 4; Adopt that 1 M formic acid solution acts as a fuel, 0.5 M sulfuric acid solution is as electrolyte.The performance of the battery of present embodiment and fuel availability are respectively shown in B line among Fig. 7 and Fig. 8.As can be seen from the figure, under equal conditions, adopt positive displacement of the present invention three-dimensional anode-catalyzed breathe certainly the microfluid fuel cell performance be about adopt planar anode breathe 2.5 times of microfluid fuel cell performance certainly; Adopt the three-dimensional anode-catalyzed microfluid fuel-cell fuel utilance of breathing certainly of positive displacement of the present invention also to increase than the fuel availability of breathing the microfluid fuel cell certainly that adopts planar anode.
Embodiment two
With the difference of embodiment one be: adopt that 0.5 M sodium formate solution acts as a fuel, 1 M sodium hydroxide solution is as electrolyte, the performance of the battery of present embodiment and fuel availability are respectively shown in C line among Fig. 7 and Fig. 8.As can be seen from the figure, adopt the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell performance of positive displacement of the present invention to improve about 50% than A line among flat microfluid fuel cell performance such as Fig. 7; Adopt the three-dimensional anode-catalyzed fuel availability of breathing the microfluid fuel cell certainly of positive displacement of the present invention to be about 2 times of A line among the fuel availability of flat microfluid fuel cell such as Fig. 8.
Can draw from embodiment one and embodiment two, the present invention has improved microfluid fuel cell performance and fuel availability.
Claims (1)
1. the three-dimensional anode-catalyzed microfluid of the breathing certainly fuel cell of positive displacement comprises base plate (2), top board (7), cathode electrode (1), anode electrode (4), spacer rod (5), sheet inlet (9) and outlet end plate (6); Wherein, sheet inlet (9) and outlet end plate (6) are separately positioned on the rear and front end of base plate (2), top board (7) is arranged on the top of base plate (2), it is characterized in that: be provided with conduit (12) at base plate (2), sheet inlet (9) is provided with electrolyte import (10) and fuel inlet (11), outlet end plate (6) is provided with outlet (3), outlet (3), electrolyte import (10) and fuel inlet (11) all communicate with conduit (12), electrolyte enters conduit (12) by electrolyte import (10), fuel enters conduit (12) by fuel inlet (11), anode electrode (4) is placed in bottom at conduit (12), this anode electrode (4) comprises anode stub (15), this anode stub (15) adopts electric conducting material as matrix, and at the electric conducting material surface deposition catalyst is arranged; Be placed with spacer rod (5) on the top of anode electrode (4), be provided with aerial respiration hole (8) at top board (7), aerial respiration hole (8) is relative with conduit (12), cathode electrode (1) is arranged on the top of spacer rod (5), be coated with eelctro-catalyst in the one side near the cathode electrode (1) of spacer rod (5), the another side of cathode electrode (1) directly is exposed in the air by aerial respiration hole (8); Described spacer rod (5) is carbon-point; Described anode stub (15) uses carbon-point as matrix; Described base plate (2), top board (7), sheet inlet (9) and outlet end plate (6) all adopt transparent material to make; Described fuel adopts formic acid, formates, methyl alcohol or ethanol.
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| CN103682372B (en) * | 2013-11-29 | 2016-08-17 | 武汉工程大学 | A kind of carbon nanotubes stereo electrod miniature without membrane cell and preparation method thereof |
| CN105762396B (en) * | 2016-03-03 | 2018-03-23 | 重庆大学 | A kind of flat hot recycling ammonia battery using foam metal electrode |
| CN107768698B (en) * | 2017-10-20 | 2020-03-03 | 重庆大学 | Tiled microfluidic direct methanol fuel cell with permeable exhaustible membrane at anode |
| CN110061259B (en) * | 2019-05-08 | 2020-09-04 | 重庆大学 | Air self-breathing paper-based microfluid fuel cell with embedded anode |
| CN110429309B (en) * | 2019-08-12 | 2020-12-29 | 重庆大学 | Preparation method of membrane-free formic acid fuel cell based on integral carbonaceous self-breathing cathode |
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| US6797422B2 (en) * | 2001-01-25 | 2004-09-28 | Gas Technology Institute | Air-breathing direct methanol fuel cell with metal foam current collectors |
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Non-Patent Citations (2)
| Title |
|---|
| Erik Kjeang，etal.Planar and three-dimensional microfluidic fuel cell architectures based on graphite rod electrodes.《Journal of Power Sources》.2007,第168卷第379-390页. * |
| Ranga S. Jayashree,etal.Air-Breathing Laminar Flow-Based Microfluidic Fuel Cell.《J. AM. CHEM. SOC》.2005,第127卷(第48期),第16758-16759页. * |
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