CN101635532B - Method for converting free energy stored in ion concentration gradient form into electric energy - Google Patents
Method for converting free energy stored in ion concentration gradient form into electric energy Download PDFInfo
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- CN101635532B CN101635532B CN2009100915461A CN200910091546A CN101635532B CN 101635532 B CN101635532 B CN 101635532B CN 2009100915461 A CN2009100915461 A CN 2009100915461A CN 200910091546 A CN200910091546 A CN 200910091546A CN 101635532 B CN101635532 B CN 101635532B
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- raceway groove
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Abstract
The invention discloses a method for converting free energy stored in an ion concentration gradient form into electric energy. In the method, a substrate provided with nano-pores, nano-flow channels or micro-flow channels is arranged in electrolytes having ion concentration gradient at both ends of the substrate, and through the ionic selectivity of the nano-pores, the nano-flow channels or the micro-flow channels, cations and anions in the electrolytes are separated to form current, and free energy stored in an ion concentration gradient form is converted into electric energy. The method can be used for developing new clean energy. An energy supply unit prepared by the method has nano-scale dimension, can be used for providing energy for other nano-scale devices in a microenvironment, and has a good application prospect in the integrated aspect of a nano-scale device system.
Description
Technical field
The present invention relates to the method that a kind of free energy is converted into electric energy, particularly relate to and a kind ofly will be converted into the method for electric energy with the free energy of ion concentration gradient form storage.
Background technology
Exist in many organisms can accumulate with conversion environment in the functional structure of energy, such as by all kinds of optionally ion channel (ion channel) and the ionic pumps (ion pump) of having.One of them example is electric eel fish (electric eel), and it can produce huge electric energy output and be used for hunting or defending oneself.Under the inspiration of this in vivo micro-nano functional structure, modern nano-fabrication technique can help the human conversion that realizes this class clean environment energy to electric energy.
The fluid passage (solid-state nanofluidicchannel) that development in recent years is got up based on the nanoscale of solid material, owing to have bigger specific area, and have remainder electric charge (surface charge) on the vias inner walls usually, surface charge plays conclusive effect for the ion transport characteristic of receiving in the fluid passage.Because the existence of surface charge, can preferentially be transported than ion with the ion of surface charge contrary sign with the surface charge jack per line, this characteristic is commonly called ion selectivity.When receiving when having ion concentration gradient in the solution at circulation road two ends, ion in the solution diffuses through under the promotion of its concentration gradient when receiving circulation road near surface electric double layer (electrical double layer), under the effect of surface charge separation of charge takes place.Receive the ion selectivity that circulation road forms a kind of means that positive and negative charge effectively separates in the environment solution that make are provided by charged, can utilize this separation of charge effect that is caused by ion selectivity, the free energy that electrolyte solution intermediate ion concentration gradient form is stored transforms into electric energy.
Summary of the invention
The purpose of this invention is to provide and a kind ofly will be converted into the method for electric energy with the free energy of ion concentration gradient form storage.
Provided by the inventionly will be converted into the method for electric energy with the free energy of ion concentration gradient form storage, be will offer nano-pore, the matrix of stream raceway groove or miniflow raceway groove received places the two ends of described matrix to have the electrolyte of ion concentration gradient, utilize nano-pore, receive the ion selectivity of stream raceway groove or miniflow raceway groove, zwitterion in the described electrolyte is separated, thereby the formation net current finishes describedly will be converted into the method for electric energy with the free energy of ion concentration gradient form storage.
This method comprises the charged nano-pore with ion selectivity of two essential condition: a, inwall or little/receive stream raceway groove; B, nano-pore, the ion concentration gradient that flows raceway groove or miniflow raceway groove two ends of receiving.
Wherein, the matrix that offers nano-pore is polymeric membrane or pellumina; The thickness of described polymeric membrane or pellumina is 100 nanometers to 100 micron, and the density of nano-pore is 1 to 10 on the described polymeric membrane
12Individual/cm
2, the physical dimension of described nano-pore is 1 nanometer to 10 micron.The material that constitutes polymeric membrane is selected from least a in PETG film, polyimide film and the polycarbonate membrane.This nano-pore be shaped as cylindricality, taper or biconial.
Offering and receiving the matrix of stream raceway groove or miniflow raceway groove is silicone substrate film; The described yardstick of receiving stream raceway groove or miniflow raceway groove cross section is 5 nanometers to 100 micron, and length is 1 micron to 1 centimetre.The material that constitutes silicone substrate film is selected from least a in silicon, silicon dioxide and the silicon nitride.This cross section of receiving stream raceway groove or miniflow raceway groove is an arbitrary shape, as rectangle.
Described nano-pore or the charged mode of stream raceway groove received, can be polymeric membrane or silicone substrate film self with electric charge, also can be polymeric membrane or silicone substrate film electric charge by forming on the surface after the chemical modification, electrically charged be positive charge or negative electrical charge.
Nano-pore, the ion selection mode that flows raceway groove or miniflow raceway groove of receiving that described inwall is charged can be cation or anion and select permeability, and according to the difference of cation or anionic kind, mobility is also different.
Described nano-pore, the ion concentration gradient that flows raceway groove or miniflow raceway groove two ends of receiving are because the concentration difference that electrolyte salt solution concentration difference causes or because the different hydrogen ions that cause of pH value and the concentration difference of hydroxide ion.This ion concentration gradient is 1: 1-1: 10
8, preferred 1: 1-1: 10
4, described electrolyte is soluble-salt, solubility acid or water soluble alkali, is not limited to water miscible electrolyte, only needs to guarantee that salt, acid or alkali have good solvent and is complementary with it and gets final product.
In addition, said method based on receiving the application in galvanic battery or the miniflow battery received of application, especially concentration (as ion concentration) gradient-driven in the energy conversion device (as battery) of circulation road or miniflow raceway groove, also belongs to protection scope of the present invention in preparation.This battery can only be made of a battery unit, wherein, this battery unit is made up of the charged nano-pore of electrode, the electrolyte that has ion concentration gradient, cell wall and inwall, miniflow raceway groove or the stream raceway groove of receiving, and the material of described formation cell wall is any insulating material, as polytetrafluoroethylene.The physical dimension of described nano-pore is 1 nanometer-10 micron; The yardstick of the described cross section of receiving stream raceway groove or miniflow raceway groove is 5 nanometers-100 micron, and length is 1 micron-1 centimetre.The structure of this battery unit as shown in Figure 3.
Provided by the inventionly a kind ofly will be converted into the method for the electric energy that can externally export with the free energy of ion concentration gradient form storage, the ion concentration gradient of the energy source that this method transformed and utilized in solution is the existence form of a kind of Gibbs free energy (Gibbs free energy).It extensively is present in occurring in nature, and reserves are huge, is a kind of recycled energy.Utilizing this technology not produce other harmful gas or solid wastes in energy sources conversion, is a kind of efficient, environmental protection, safety, the free of contamination mode of utilizing the energy.Therefore, this method can be used as the method for a kind of novel clean energy resource of exploitation.In addition, utilize the prepared supply unit size of this method, can be used under microenvironment, aspect nano-device system integrated, have good application prospects to other nano-devices provide energy in the Nano/micron magnitude.
Description of drawings
Fig. 1 is the schematic diagram with the nano-pore on the preparation polymeric membrane.
Fig. 2 is the silica-based miniflow of preparation or the flow chart that flows raceway groove of receiving.
Fig. 3 is the structural representation of battery unit.
Embodiment
The present invention by at the charged nano-pore of inwall, receive stream raceway groove or miniflow raceway groove two ends and construct electrolytical concentration gradient, make zwitterion spontaneously to be diffused into low concentration from high concentration, under the effect of the ion selectivity of nano-pore or micro-nano raceway groove, can collect the net current that produces by diffusion.In this process, do not need additionally to apply mechanical power and come drive fluid, can further promote energy conversion efficiency.This method can will be converted into the electric energy that can be utilized with the free energy of ion concentration gradient form storage from environment solution, the method that provides a kind of novel development of clean energy to utilize, and its schematic diagram is as shown in Figure 1.
Because dissufion current is driven by ions diffusion, so it is along with actuating force, i.e. concentration gradient, increase and increase.The electromotive force at nano-pore or micro-nano raceway groove two ends derives from the liquid junction potential in nano-pore or the raceway groove.Liquid junction potential can be expressed as quantitatively:
E
j＝U
L-U
H＝(t
+-t
-)RT/Fln(α
H/α
L) (1)
T wherein
+And t
-Be respectively cation and anionic number (transference number), the α of transporting
H, α
LBe respectively the chemical activity of two ends solution, R is a universal gas constant, and T is an absolute temperature.This shows that it is to increase with concentration gradient that liquid connects electromotive force.When calculating the liquid junction potential that potassium chloride produces in macroscopical solution with formula (1), t wherein
+=0.49, t
-=0.51, the liquid that KCl produced in macroscopical solution connects electrical potential difference much smaller than the result who measures in nano-pore.Be that the ion selectivity of charged nano-pore of inwall or micro-nano raceway groove has strengthened nano-pore greatly and transports cationic.Along with the increase of surface charge density, the ion selectivity of nano-pore or micro-nano raceway groove further strengthens, and electromotive force can be further improved.
Utilize method provided by the invention, can prepare the galvanic battery of receiving with the concentration gradient driving, the electrical properties of this battery is measured according to following method: (with the polyimide porous membrane is example, and electrolyte solution is a KCl solution)
1, electromotive force
The film sample that will have a nano-pore is clipped in the middle of as described in Figure 1 the electrolyte tank, adds 1.5 milliliters Klorvess Liquid in each half groove.Keeping the solution concentration of conical nano-pore aperture osculum end is 1mM, and the concentration that contacts conical nano-pore big opening end solution is 1000mM, thereby constructs a concentration gradient of striding nano-pore.
Can measure the electrical potential difference at film two ends with sensitive potentiometer.Measurement electrode is used reference electrode or Ag/AgCl electrode.Can not form because the additional electrical potential difference that concentration difference causes at electrode surface when wherein, using reference electrode; When using the Ag/AgCl electrode, on electrode, will produce additional electrical potential difference.
2, short circuit current
Use said method, the electric current that records during making alive is not short circuit current.
3, electric energy draws
Ionic current is converted to the electric current that in circuit, conducts electricity with reference electrode or Ag/AgCl electrode by metal electron.Can record the electric current and the wire-end voltage of external circuit with galvanometer and voltmeter.
In the method provided by the invention, the nano-pore or the stream raceway groove of receiving all can be prepared according to conventional method, as the macromolecule membrane (composition is: PETG film, polyimide film or Merlon) of 12 micron thickness high-energy heavy ion irradiation, form the ion track of diving with 11.4MeV/u.The film sample that will have the latent track of ion irradiation carries out etching with etching liquid (as NaOH or aqueous sodium hypochlorite solution), forms the nano pore based on macromolecule membrane.Also can utilize MEMS (Micro-Electro-Mechanical Systems) method to prepare silica-based receiving and flow raceway groove or miniflow raceway groove, this method comprises the steps:
(a) get rid of the last layer photoresist on silicon chip, this silicon chip is followed successively by silicon layer and silicon nitride layer from the bottom to top, utilizes photoetching technique to prepare a groove on photoresist.Shown in Fig. 2 a end view, be followed successively by photoresist, silicon nitride and silicon from top to bottom.
(b) with the photoresist be mask, (etching gas is SF6 and CHF3 according to RIE (reactive ion beam etching (RIBE)) method, etching parameters is SF6: CHF3=8sccm: 8sccm, air pressure 30m Torr, radio-frequency power 30W, etch rate are 14.7nm/min) preparation and the same groove of photoresist on silicon nitride.Shown in Fig. 2 b, be followed successively by photoresist, silicon nitride and silicon from top to bottom.
(c) remove photoresist with acetone, shown in Fig. 2 c, be followed successively by silicon nitride and silicon from top to bottom.
(d) be template with the silicon nitride, use the Tetramethylammonium hydroxide etch silicon, on silicon base, obtain nanometer channel.Fig. 2 d is an end view, is followed successively by silicon nitride and silicon from top to bottom, and Fig. 2 d ' is a vertical view.
(e) with PDMS (dimethyl silicone polymer) and silicon based package, the groove that obtains sealing, and on PDMS, prepare solution pool, be used to provide concentration gradient (PDMS is a soft material).Shown in Fig. 2 e end view, be followed successively by PDMS, silicon nitride and silicon from top to bottom, Fig. 2 e ' is a vertical view.
Embodiment 1, polyimides single hole film
With polyimides (polyimide) film of 12 micron thickness high-energy heavy ion irradiation with 11.4MeV/u, form the ion track of diving, the density in hole is single hole.To have the dive film sample of track of ion irradiation and carry out the single face etching with clorox under 50 ℃, forming conical, big opening end and be 1.34 microns, osculum end is the nanometer single hole film of 41 nanometers.
The nano-pore surface is that (COO-) surface negative charge of Gou Chenging, this nano-pore has cation selective by the carboxylic acid ester bond.For the KCl aqueous solution, the easier nano-pore that passes through of potassium ion.At the fixing KCl aqueous solution of 1mM of an end of film, the other end KCl aqueous solution is respectively 10mM, 30mM, 100mM, 300mM, 1000mM, and electromotive force and short circuit current that the nano-pore two ends can produce are respectively: 123mV, 254pA; 170mV, 462pA; 220mV, 889pA; 250mV, 1785pA; 267mV, 3284pA.
Embodiment 2, silica-based single nanochannel
Prepare silica-based single nanochannel according to following step:
(a) get rid of the last layer photoresist on silicon chip, this silicon chip is followed successively by silicon layer and silicon nitride layer from the bottom to top, utilizes photoetching technique to prepare a groove on photoresist.Shown in Fig. 2 a end view, be followed successively by photoresist, silicon nitride and silicon from top to bottom.
(b) with the photoresist be mask, (etching gas is SF according to RIE (reactive ion beam etching (RIBE)) method
6And CHF
3, etching parameters is SF
6: CHF
3=8sccm: 8sccm, air pressure 30m Torr, radio-frequency power 30W, etch rate are 14.7nm/min) preparation and the same groove of photoresist on silicon nitride.Shown in Fig. 2 b, be followed successively by photoresist, silicon nitride and silicon from top to bottom.
(c) remove photoresist with acetone, shown in Fig. 2 c, be followed successively by silicon nitride and silicon from top to bottom.
(d) be template with the silicon nitride, on silicon base, use the Tetramethylammonium hydroxide etch silicon, obtain length, width and highly be respectively the nanometer channel of 100 microns, 10 microns and 50 nanometers.Fig. 2 d is an end view, is followed successively by silicon nitride and silicon from top to bottom, and Fig. 2 d ' is a vertical view.
(e) with PDMS (dimethyl silicone polymer) and silicon based package, the groove that obtains sealing, and on PDMS, prepare solution pool, be used to provide concentration gradient (PDMS is a soft material).Shown in Fig. 2 e end view, be followed successively by PDMS, silicon nitride and silicon from top to bottom, Fig. 2 e ' is a vertical view.
In addition, according to last identical method, only in step (d), on silicon base, use the Tetramethylammonium hydroxide etch silicon, obtain length, width and highly be respectively the micron groove of 100 microns, 10 microns and 5 microns.
Utilize the single nanometer of silica-based cylindricality or the micron vias inner walls of method for preparing electronegative, have cation selective.When the KCl at the nano-channel two ends aqueous solution is respectively 1mM and 1000mM, can produce the electromotive force of 150mV and 5 microamperes short circuit current.When the KCl aqueous solution at micron raceway groove two ends was respectively 1mM and 1000mM, the electromotive force and 20 that can produce 10mV was received the short circuit current of peace.
Embodiment 3, PETG (PET) single hole film
With the pet film of 12 micron thickness high-energy heavy ion irradiation, form the ion track of diving with 11.4MeV/u.This is had dive pet film sample of track of ion irradiation carry out the single face etching with the 9M/L sodium hydrate aqueous solution under 25 ℃, forming conical, big opening end is that 760 nanometers, osculum end are the nanometer single hole film of 37 nanometers.
This nano-pore surface is that (COO-) surface negative charge of Gou Chenging, this nano-pore has cation selective by the carboxylic acid ester bond.For the KF aqueous solution, the easier nano-pore that passes through of potassium ion.At the fixing KF solution of 1mM of an end of film, the other end KF aqueous solution is respectively 10mM, 30mM, 100mM, 300mM, 1000mM, and electromotive force and short circuit current that the nano-pore two ends can produce are respectively: 115mV, 226pA; 156mV, 412pA; 198mV, 796pA; 221mV, 1688pA; 233mV, 2877pA.
Embodiment 4, Merlon (PC) single hole film
With the polycarbonate film of 12 micron thickness high-energy heavy ion irradiation, form the ion track of diving with 11.4MeV/u.This is had dive polycarbonate film sample of track of ion irradiation carry out two-sided etching with the 5M/L sodium hydrate aqueous solution under 25 ℃, forming diconical, big opening end is that 100 nanometers, osculum end are the nanometer single hole film of 80 nanometers.
The nano-pore surface is that (COO-) surface negative charge of Gou Chenging, this nano-pore has cation selective by the carboxylic acid ester bond.For the LiCl aqueous solution, the easier nano-pore that passes through of lithium ion.At the fixing LiCl aqueous solution of 1mM of an end of film, the other end LiCl aqueous solution is respectively 10mM, 30mM, 100mM, 300mM, 1000mM, and electromotive force and short circuit current that the nano-pore two ends can produce are respectively: 61mV, 122pA; 83mV, 216pA; 112mV, 415pA; 124mV, 895pA; 129mV, 1457pA.
Claims (12)
1. one kind will be converted into the method for electric energy with the free energy of ion concentration gradient form storage, be will offer nano-pore, the matrix of stream raceway groove or miniflow raceway groove received places the two ends of described matrix to have the electrolyte of ion concentration gradient, utilize described nano-pore, receive the ion selectivity of stream raceway groove or miniflow raceway groove, zwitterion in the described electrolyte is separated, thereby the formation electric current, the free energy of finishing with ion concentration gradient form storage is converted into electric energy; Described nano-pore, the inwall of stream raceway groove or miniflow raceway groove received are all charged.
2. method according to claim 1 is characterized in that: the matrix of the described nano-pore that offers is polymeric membrane or pellumina; The thickness of described polymeric membrane or pellumina is 100 nanometers-100 micron, and the density of nano-pore is 1-10 on the described polymeric membrane
12Individual/cm
2, the physical dimension of described nano-pore is 1 nanometer-10 micron;
Describedly offer that to receive the matrix of stream raceway groove or miniflow raceway groove be silicone substrate film; The described cross section of receiving stream raceway groove or miniflow raceway groove is of a size of 5 nanometers-100 micron, and length is 1 micron-1 centimetre.
3. method according to claim 2 is characterized in that: the material that constitutes described polymeric membrane is selected from least a in PETG film, polyimide film and the polycarbonate membrane;
The material that constitutes described silicone substrate film is selected from least a in silicon, silicon dioxide and the silicon nitride.
4. according to the arbitrary described method of claim 1-3, it is characterized in that: described nano-pore is cylindricality, taper or biconial; The described cross section of receiving stream raceway groove or miniflow raceway groove is an arbitrary shape.
5. method according to claim 1 is characterized in that: described ion concentration gradient is 1: 1-1: 10
8
6. method according to claim 5 is characterized in that: described ion concentration gradient is 1: 1-1: 10
4
7. method according to claim 1 is characterized in that: described electrolyte is soluble-salt, solubility acid or water soluble alkali.
The arbitrary described method of claim 1-7 in preparation based on the application of receiving in the energy conversion device of circulation road or miniflow raceway groove.
9. application according to claim 8 is characterized in that: described energy conversion device is a battery; Described battery be concentration gradient drive receive galvanic battery or miniflow battery.
10. application according to claim 9 is characterized in that: described battery by the charged nano-pore of electrode, the electrolyte that has ion concentration gradient, cell wall and inwall, receive stream raceway groove or miniflow raceway groove and form.
11. application according to claim 10 is characterized in that: the material that constitutes described cell wall is an insulating material; The physical dimension of described nano-pore is 1 nanometer-10 micron; The described cross section of receiving stream raceway groove or miniflow raceway groove is of a size of 5 nanometers-100 micron, and length is 1 micron-1 centimetre.
12. application according to claim 11 is characterized in that: the material that constitutes described cell wall is a polytetrafluoroethylene.
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| CN102611353B (en) * | 2012-04-11 | 2014-09-17 | 武汉大学 | Device for generating electricity by collecting environmental low-grade energy source |
| CN103973170A (en) * | 2014-04-28 | 2014-08-06 | 国家电网公司 | Mechanical energy and electric energy conversion device |
| CN107151646B (en) * | 2017-05-18 | 2021-07-09 | 西安交通大学 | Active biological battery construction method based on generating cells |
| CN109995271B (en) * | 2019-03-19 | 2020-08-04 | 华中科技大学 | Salt concentration gradient driven nano fluid power generation device and preparation and application thereof |
| CN109921686B (en) * | 2019-03-26 | 2020-06-02 | 中国科学院理化技术研究所 | Fluid power generation method and device based on funnel-shaped nanometer pore channel film |
| CN110165939B (en) * | 2019-05-29 | 2020-04-14 | 厦门大学 | Sliding type generator based on double charge layers and power generation method thereof |
| CN114873698B (en) * | 2022-05-31 | 2023-10-20 | 西北农林科技大学 | Capacitive deionization water purification device with regenerated electric energy and manufacturing method of separation bin |
| CN115738769B (en) * | 2022-11-02 | 2024-01-23 | 先进能源科学与技术广东省实验室 | Polyimide gas separation membrane based on ion beam irradiation modification and application thereof |
| CN116032154A (en) * | 2023-01-31 | 2023-04-28 | 北京大学 | Nanometer concentration difference power generation device and preparation and power generation methods thereof |
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