CN109888326B - Air self-breathing membraneless microfluidic fuel cell with integral cylindrical anode - Google Patents
Air self-breathing membraneless microfluidic fuel cell with integral cylindrical anode Download PDFInfo
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- CN109888326B CN109888326B CN201910192463.5A CN201910192463A CN109888326B CN 109888326 B CN109888326 B CN 109888326B CN 201910192463 A CN201910192463 A CN 201910192463A CN 109888326 B CN109888326 B CN 109888326B
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Abstract
The invention discloses an air self-breathing membraneless microfluid fuel cell with an integrated cylindrical anode, which comprises a cathode cover plate, a flow channel and a cell bottom plate, wherein a cathode air breathing hole is formed in the cathode cover plate, and an air self-breathing cathode is arranged below the cathode air breathing hole; the method is characterized in that: the flow channel is arranged between the cathode cover plate and the battery bottom plate; a metal round pipe is arranged in the flow passage; the outer surface of the metal round pipe is coated with a catalytic layer; the metal round pipe is arranged in parallel with the air self-breathing cathode; the front part of the metal round pipe is a hollow pipe, and the rest part of the metal round pipe is a solid pipe; a plurality of overflow ports are arranged on the pipe wall at the junction of the hollow pipe and the solid pipe along the circumferential direction; the front end of the metal round pipe is provided with a fuel inlet; a waste liquid outlet is formed in the battery bottom plate; the waste liquid outlet is communicated with the flow channel; the invention can strengthen fuel transmission, is beneficial to system integration and improves the performance of the battery; can be widely applied in the fields of energy, chemical industry, environmental protection and the like.
Description
Technical Field
The invention relates to the field of fuel cells, in particular to an air self-breathing membraneless microfluidic fuel cell with an integrated cylindrical anode.
Background
The lithium ion battery widely used at present has the defects of low theoretical energy density, long charging time, narrow normal use temperature range and the like. Common height of micro fuel cellMethanol or formic acid and the like with energy density are taken as fuels and are obviously higher than the theoretical energy density upper limit of the lithium battery; the adaptability of the operating environment is strong, and the range of the using temperature is wide; chemical energy is directly converted into electric energy, and the theoretical energy conversion efficiency is high; the product has no pollution to the environment. Therefore, micro fuel cells (such as micro direct methanol or formic acid fuel cells) have unique advantages and broad application prospects in the new generation of micro electronic devices and portable instant detection devices. In addition, methanol, formic acid, or the like can convert biomass, reduce CO2The fuel is obtained by the methods and is a renewable and environment-friendly near-zero carbon cycle fuel. However, the micro fuel cell usually uses an ion exchange membrane to separate the liquid fuel and the oxidant, and has technical challenges of high cost, difficult water management, large ohmic loss, severe fuel permeation, membrane aging degradation and the like, which severely limit the development and application of the micro fuel cell.
The membrane-free microfluidics fuel cells (membranneless microfluidics fuel cells) utilize the characteristics that the viscous force of fluid in a microchannel (with the characteristic dimension of 1-1000 mu m) is greater than the inertia force, and the surface force is greater than the volume force (such as gravity), so that two or more streams of fluid form parallel laminar flow in the microchannel to flow, natural separation of fuel and oxidant is realized, and ions can be conducted through a laminar flow interface, thereby removing an ion exchange membrane, simplifying the structure, reducing the cost and avoiding the defects related to the membrane. The introduction of the air self-breathing cathode further eliminates the mass transfer limitation of the cathode caused by the liquid oxidant, and improves the performance of the battery. The membraneless microfluid fuel cell contains the main components such as a flow channel, an electrode and the like in a microchannel, is compatible with the existing micromachining process, and is beneficial to system integration and large-scale manufacturing.
In a typical air self-breathing membraneless microfluidic fuel cell, the fuel and catholyte create parallel laminar flows in the microchannel and a diffusive mixing zone near the laminar interface. In the acid electrolyte, the fuel is oxidized in the anode catalyst layer to generate electrons, protons and CO2The electrons reach the cathode via the load through the external circuit, the protons reach the cathode mainly in an electromigration mode and are subjected to reduction reaction with oxygen to generate water, and CO2After the coalescence bubbles are generated, disturbance is caused to the laminar flow interface, and the battery performance is influenced. In the alkaline electrolyte, fuel is oxidized in the anode catalyst layer to generate electrons, water and carbonate, the carbonate is discharged along with waste liquid, and the electrons reach the cathode through an external circuit to combine with oxygen and water to generate hydroxide ions.
The main factor currently limiting further improvements in membrane-less microfluidic fuel cell performance is the anode surface fuel concentration boundary layer. The fluid in the membraneless microfluidic fuel cell flows in a laminar flow mode, and the diffusion and transmission direction of the fuel is perpendicular to the flow direction. Whereas Peclet (Peclet) numbers are generally higher (>2000) in membraneless microfluidic fuel cells, so that convective transport in the flow direction is much stronger than diffusive transport in the transverse direction. Under the influence, the fuel concentration reduction of the anode surface caused by the consumption of the electrochemical reaction cannot be effectively supplemented, so that a region (namely a fuel concentration boundary layer) with gradually reduced fuel concentration appears on the anode surface along the flow direction, the fuel transmission is severely limited, and the further improvement of the cell performance is limited.
To enhance fuel delivery, several proposals have been made by researchers at home and abroad. 1) oritiz-Orteg et al (e.oritiz-Ortega et al, Lab on a Chip,2014) increase fuel concentration and enhance fuel mass transfer. However, the increased fuel concentration enhances diffusion/convection transport of the fuel to the cathode, and when the fuel contacts the cathode catalyst layer, mixed potential and parasitic current are generated, which seriously degrade the performance of the cell. In addition, due to the existence of the fuel concentration boundary layer, a large amount of fuel in the main flow region cannot participate in the reaction and is directly discharged out of the cell, so that the fuel utilization rate is extremely low. 2) Bazylak et al (a. Bazylak et al, Journal of Power Sources,2005) increase anode fuel flow rates, thereby thinning the fuel concentration boundary layer, increasing the concentration gradient, and enhancing fuel mass transfer. However, too high a flow rate can cause flow instability, disturb laminar interfaces, enhance mixing and cause fuel permeation. 3) Ahme et al (d.h. Ahme et al, International Journal of energy research,2010) arrange a micro-convex structure on the anode surface such that the fuel fluid near the anode surface generates micro-convection, thereby enhancing fuel mass transfer. However, this approach may enhance convective mixing at the laminar flow interface, causing fuel permeation. 4) Lim et al (k.g. Lim et al, Biosensors and Bioelectronics,2007) employ a discontinuous anode electrode, thereby disrupting the continuous generation of a fuel concentration boundary layer. But this solution would reduce the effective electrode area and reduce the battery output. 5) kjeang et al (e.kjeang et al, Electrochimica Acta,2008) use a permeable porous anode to enhance fuel mass transfer in a convective manner, however on the one hand the hydraulic retention time of the fuel in the thin catalytic layer is short and the reaction rate is limited; on the other hand, an additional anode flow channel is required, which reduces the volume energy or power density and is not favorable for system integration. 6) Wang et al (y.wang et al, Applied Energy,2015) uses gaseous methanol vapor as fuel, but this solution requires a larger fuel vaporization chamber, reduces volumetric Energy or power density and is not conducive to system integration. In addition, studies (w.r.merida et al, Journal of Power Sources,2001) have demonstrated that the use of curved electrolyte-electrode interfaces can effectively increase the volumetric Power density of the membraneless fuel cell, while curved electrodes facilitate the integration and amplification of the cell.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides an air self-breathing membraneless microfluidic fuel cell with an integrated cylindrical anode.
The technical scheme of the invention is as follows: an air self-breathing membraneless microfluidic fuel cell with an integrated cylindrical anode comprises a membraneless microfluidic fuel cell main body, wherein the membraneless microfluidic fuel cell main body comprises a cathode cover plate, an air self-breathing cathode, a flow channel, a cylindrical anode and a cell bottom plate, wherein a cathode air breathing hole is formed in the cathode cover plate and is arranged above the air self-breathing cathode; the method is characterized in that: the flow channel is arranged between the cathode cover plate and the battery bottom plate; the front end of the flow channel is provided with an electrolyte inlet; a metal round pipe is arranged in the flow passage; the outer surface of the metal round pipe is coated with a catalyst layer; the cylindrical anode consists of a metal round pipe and a catalyst layer; the metal round pipe and the flow channel are arranged in parallel with the air self-breathing cathode; the front part of the metal round pipe is a hollow pipe, and the rest part of the metal round pipe is a solid pipe; a plurality of annular through grooves are arranged on the pipe wall at the junction of the hollow pipe and the solid pipe along the circumferential direction to be used as overflow ports; the front end of the metal round pipe is provided with a fuel inlet; the liquid fuel overflows from the overflow port and forms adherent flow on the surface of the metal round pipe; a waste liquid outlet is formed in the battery bottom plate; the waste liquid outlet is communicated with the flow channel.
The cathode of the invention directly reduces oxygen in the air under acidic condition and combines electrons and hydrogen ions to generate water, and reduces oxygen under alkaline condition and combines electrons and water to generate hydroxyl ions; the metal round pipe is used as an anode substrate and a fuel conveying channel; can directly catalyze and oxidize the fuel and generate electrons and hydrogen ions or carbonates; the fuel overflows from the overflow port at a low speed and flows into the flow channel, and the fuel flows along the surface of the metal round pipe under the influence of the flowing action of the electrolyte; and oxidation reaction occurs on the surface of the anode catalyst layer.
The patent provides an air self-breathing membraneless microfluidic fuel cell with an integrated cylindrical anode, and an air self-breathing cathode is adopted to eliminate mass transfer limitation of a cathode oxidant (oxygen); the integrated cylindrical anode is used as a fuel flow channel and an anode electrode at the same time, so that the integration level is further improved; the effective anode reaction area is increased by adopting a cylindrical anode; the fuel is input from a metal round pipe, flows in the pipe firstly, then flows into the flow channel in an overflow mode at a low speed through the annular through groove on the surface of the cylindrical anode, and forms a thin layer to flow tightly attached to the surface of the metal round pipe due to the hydraulic aggregation effect of electrolyte fluid, so that the mass transfer of the fuel is enhanced, and the fuel permeation to the cathode is reduced; in addition, the fuel thin layer is directly covered on the anode catalytic active site, which is beneficial to improving the fuel utilization rate.
According to the preferable scheme of the air self-breathing membraneless microfluidic fuel cell with the integrated cylindrical anode, the metal round tubes are arranged in the flow channel in a single or multiple parallel mode.
According to the preferred scheme of the air self-breathing membraneless microfluidic fuel cell with the integrated cylindrical anode, a plurality of layers of liquid flow ports are arranged on the wall of the hollow tube part of the metal round tube in a layered mode; each layer of liquid flow port is composed of a plurality of annular through grooves arranged on the same circumferential wall surface.
According to a preferred embodiment of the air self-breathing membraneless microfluidic fuel cell with an integral cylindrical anode according to the present invention, the air self-breathing cathode consists of hydrophobic carbon paper, a smoothening layer and a Pt/C catalytic layer.
The air self-breathing membraneless microfluidic fuel cell with the integrated cylindrical anode has the beneficial effects that:
1) the anode cylindrical electrode is simultaneously used as a fuel channel, so that the integration level is improved, and the energy density of the system is further improved. The anode electrode, the anode fuel flow channel, the main flow channel and the cathode electrode are all contained in one micro channel, and system integration is facilitated.
2) The adoption of the integrated cylindrical anode increases the effective reaction area, enhances the fuel transmission and reduces the fuel permeation by utilizing the hydraulic aggregation effect, and is beneficial to improving the performance of the cell.
3) The effective volume of the battery is reduced, the transmission distance of hydrogen ions is shortened, the transmission resistance of the hydrogen ions is reduced, the volume power density of the battery is improved, and the miniaturization and system integration are facilitated.
4) The electrolyte has good performance in acid/alkali electrolyte and good adaptability and flexibility.
5) The oxygen which is cheap and easy to obtain in the air is directly used as the oxidant, so that the operation cost of the battery is effectively reduced.
6) The invention has simple structure, does not need complex micro-channels and fuel diaphragms, can realize fuel operation and avoids fuel permeation.
The invention can be widely applied to the fields of energy, chemical industry, environmental protection and the like.
Drawings
Fig. 1 is a front view of an air self-breathing membraneless microfluidic fuel cell with an integral cylindrical anode.
Fig. 2 is a top view of fig. 1.
Fig. 3 is a left side view of fig. 1.
Fig. 4 is a schematic view of the arrangement of the overflow 7.
Detailed Description
Referring to fig. 1 to 4, an air self-breathing membraneless microfluidic fuel cell with an integrated cylindrical anode comprises a membraneless microfluidic fuel cell body, wherein the membraneless microfluidic fuel cell body comprises a cathode cover plate 2, an air self-breathing cathode 4, a flow channel 5, a cylindrical anode 8 and a cell bottom plate 9, and the cathode cover plate, the flow channel and the cell bottom plate 9 are all made of plastics; a cathode air breathing hole 3 is arranged on the cathode cover plate 2, and the cathode air breathing hole 3 is arranged above the air self-breathing cathode 4; the flow channel 5 is arranged between the cathode cover plate 2 and the battery bottom plate 9; the front end of the flow channel 5 is provided with an electrolyte inlet 6, and a metal round pipe 1 is arranged in the flow channel 5; the outer surface of the metal round tube 1 is coated with a Pd/Nafion catalyst layer by adopting a repeated electrochemical deposition method; the metal round tube 1 and the Pd/Nafion catalyst layer form the cylindrical anode 8; the metal round pipe 1, the flow channel 5 and the air self-breathing cathode 4 are arranged in parallel; the front part of the metal round tube 1 is a hollow tube, and the rest part is a solid tube; a plurality of annular through grooves are arranged on the pipe wall at the junction of the hollow pipe and the solid pipe along the circumferential direction to be used as overflow ports 7; the annular through groove is a rectangular annular hole with the width of 10-1000 microns; the front end of the metal round pipe 1 is provided with a fuel inlet 11; the liquid fuel overflows from the overflow port and forms adherent flow on the surface of the metal round pipe 1; a waste liquid outlet 10 is arranged on the battery bottom plate 9; the waste liquid outlet 10 is in communication with the flow channel 5.
In the specific embodiment, the metal round tubes 1 are arranged in a single piece or in parallel in the flow passage.
Referring to fig. 4, a plurality of layers of liquid flow ports are arranged on the wall of the hollow pipe part of the metal round pipe 1 in a layered manner; each layer of liquid flow port is composed of a plurality of annular through grooves arranged on the same circumferential wall surface.
The air self-breathing cathode 4 consists of hydrophobic carbon paper, a leveling layer and a Pt/C catalytic layer.
When the microfluid fuel cell is operated, a certain flow such as 50 mul min is introduced from the metal round tube 1-1The liquid fuel after deoxygenation can adopt a mixed solution of 5M formic acid and 1M dilute sulfuric acid; the electrolyte with a certain flow rate such as 1M dilute sulfuric acid solution is introduced into the flow channel 5 from the electrolyte inlet 6, and the liquid fuel overflows from the overflow port 7 at a low speedFlows into the flow channel 5, flows closely to the surface of the metal round tube 1, and is convectively/diffusively transferred to the surface catalyst layer of the metal round tube 1. In the acid electrolyte, an anode catalyst layer catalyzes formic acid molecules to generate electrochemical oxidation to generate hydrogen ions, electrons and carbon dioxide, the hydrogen ions reach a cathode in an electromigration mode, the electrons reach the cathode through an external circuit through a load, and carbon dioxide bubbles are discharged from a waste liquid outlet at the downstream of a flow channel. Oxygen in the air is transmitted to the Pt/C catalytic layer through hydrophobic carbon paper with a porous structure, and electrochemical reduction is carried out on the cathode Pt/C catalytic layer to combine hydrogen ions and electrons to generate water. In the alkaline electrolyte, the anode Pt/C catalyst layer catalyzes formate ions to generate electrochemical oxidation to generate water, electrons and carbonate, the electrons reach the cathode through an external circuit by loading, and the carbonate is dissolved in the water and is discharged from a waste liquid outlet.
Taking an air self-breathing direct formic acid microfluidic fuel cell as an example, the reaction in the acid electrolyte is as follows:
anodic oxidation of formic acid
HCOOH→CO2↑+2H++2e-，E0She (standard hydrogen electrode) at-0.198V vs
Cathodic oxygen reduction reaction
O2+4H++4e-→2H2O，E0＝1.229V vs.SHE
General reaction
2HCOOH+O2→2CO2↑+2H2O，ΔE＝1.427V
The reactions that take place in the alkaline electrolyte are as follows:
anodic formate oxidation
Cathodic oxygen reduction reaction
O2+2H2O+4e-→4OH-，E0＝0.4V vs.SHE
General reaction
While embodiments of the invention have been shown and described, it will be understood by those of ordinary skill in the art that: various changes, modifications, substitutions and alterations can be made to the embodiments without departing from the principles and spirit of the invention, the scope of which is defined by the claims and their equivalents.
Claims (4)
1. An air self-breathing membraneless microfluidic fuel cell with an integrated cylindrical anode comprises a membraneless microfluidic fuel cell main body, wherein the membraneless microfluidic fuel cell main body comprises a cathode cover plate (2), an air self-breathing cathode (4), a flow channel (5), a cylindrical anode (8) and a cell bottom plate (9), a cathode air breathing hole (3) is formed in the cathode cover plate (2), and the cathode air breathing hole (3) is formed above the air self-breathing cathode (4); the method is characterized in that: the flow channel (5) is arranged between the cathode cover plate (2) and the battery bottom plate (9); the front end of the flow channel (5) is provided with an electrolyte inlet (6); a metal round pipe (1) is arranged in the flow channel (5); the outer surface of the metal round pipe (1) is coated with a catalyst layer; the cylindrical anode (8) is composed of a metal round pipe (1) and a catalyst layer; the metal round pipe is used as an anode substrate and a fuel conveying channel; the metal round pipe (1) and the flow channel (5) are arranged in parallel with the air self-breathing cathode (4); the front part of the metal round tube (1) is a hollow tube, and the rest part is a solid tube; a plurality of annular through grooves are arranged on the pipe wall at the junction of the hollow pipe and the solid pipe along the circumferential direction to be used as overflow ports; the front end of the metal round pipe (1) is provided with a fuel inlet (11); the liquid fuel overflows from the overflow port and forms adherent flow on the surface of the metal round pipe (1); a waste liquid outlet (10) is formed in the battery bottom plate (9); the waste liquid outlet (10) is communicated with the flow channel (5).
2. The air self-breathing membraneless microfluidic fuel cell with integral cylindrical anode of claim 1, wherein: the metal round pipes (1) are arranged in the flow channel in a single or multiple parallel mode.
3. The air self-breathing membraneless microfluidic fuel cell with integral cylindrical anode of claim 1 or 2, wherein: a plurality of layers of liquid flow ports are arranged on the pipe wall of the hollow pipe part of the metal round pipe (1) in a layered manner; each layer of liquid flow port is composed of a plurality of annular through grooves arranged on the same circumferential wall surface.
4. The air self-breathing membraneless microfluidic fuel cell with integral cylindrical anode of claim 3, wherein: the air self-breathing cathode (4) consists of hydrophobic carbon paper, a leveling layer and a Pt/C catalytic layer.
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| CN110534751B (en) * | 2019-09-04 | 2020-09-01 | 重庆大学 | Stack type passive paper-based micro-fluid fuel cell with oppositely arranged cathode and anode |
| CN110459789B (en) * | 2019-09-06 | 2020-09-01 | 重庆大学 | Single-electrolyte microfluid fuel cell with cathode and anode arranged in concurrent flow |
| CN112531182A (en) * | 2020-12-05 | 2021-03-19 | 重庆大学 | Portable cylindrical membraneless fuel cell with large reaction volume ratio |
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| US7435503B2 (en) * | 2004-06-10 | 2008-10-14 | Cornell Research Foundation, Inc. | Planar membraneless microchannel fuel cell |
| CN103066311B (en) * | 2012-12-11 | 2014-11-26 | 华东理工大学 | Self-driven type micro-fluid membrane less fuel cell based on gravity effects |
| CN109148927B (en) * | 2018-09-04 | 2021-03-19 | 重庆大学 | Air self-breathing membraneless microfluidic fuel cell with immersed microjets |
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