Useful Work For Heat Warm Account

Part 1. Some terms and definitions.

The electromotive force (emf) is the field strength integral of the external forces over the section containing the current source ... The external forces in the galvanic cells act on the boundaries between the electrolytes and the electrodes. They also act on the interface between two dissimilar metals and cause a contact potential difference between them [5, p. 193, 191]. The sum of the potential jumps at all circuit interfaces is equal to the potential difference between the conductors at the ends of the circuit, and is called the electromotive force of the conductor chain ... A circuit consisting only of conductors of the first kind is equal to the potential jump between the first and last conductors when they are in direct contact (Volta's law) ... If the circuit is properly open, then the emf. This chain is equal to zero. The law of the Volta is not applicable to the correctly opened circuit of conductors, which includes at least one electrolyte ... It is obvious that only the conductor chains, including at least one conductor of the second kind, are electrochemical elements (or electrochemical chains of elements) [1, p. 490 - 491].

Polyelectrolytes are polymers capable of dissociating into ions in solution, with a large number of periodically recurring charges in one macromolecule ... The cross-linked polyelectrolytes (ion exchangers, ion exchange resins) do not dissolve, but only swell, while retaining the dissociation ability [6, p. 320 - 321]. Polyelectrolytes dissociating into negatively charged macroions and H + ions are called polyacids, and dissociating into positively charged macroions and OH-ions are called poly-bases.

The Donnan potential is the equilibrium potential difference arising on the phase boundary between two electrolytes in the case when this boundary is permeable not for all ions. The impermeability of the boundary for certain ions can be due, for example, to the presence of a membrane with very narrow pores that are impassable for particles exceeding a certain size. The selective permeability of the interphase boundary also arises if some ions are so firmly bound in one of the phases that they can not leave it at all. This is how ionogenic or ion-exchange groups fixed by homopolar bonds in a molecular lattice or matrix behave in ion-exchange resins. A solution inside such a matrix forms together with it one phase; The solution outside it is the second [7, p. 77].

A double electric layer (DES) is the set of two oppositely charged layers, located at a certain distance from each other, arising at the interface of phases [7, p. 96].

Peltier effect is the release or absorption of heat at the contact of two dissimilar conductors, depending on the direction of the electric current flowing through the contact [2, p. 552].

Part 2. Using the heat of the environment in the electrolysis of water.

Let us consider the mechanism of the appearance in the chain of an electrochemical element (hereinafter Element), schematically depicted in Fig. 1, an additional emf due to the internal contact potential difference (CRP) and the Donnan effect (a brief description of the essence of the Donnan effect, the internal IF and the associated heat of Peltier is given in the third part of the article).

Fig. 1. Schematically represented electrochemical element: 1 - cathode, contacts with solution 3, electrochemical reactions of reduction of cations of electrolyte proceed on its surface, it is made of chemically inert strongly doped n-semiconductor. The part of the cathode that connects it to an external voltage source is metallized; 2-anode, contacts solution 4, electrochemical oxidation reactions of anions of electrolyte proceed on its surface, it is made of chemically inert heavily doped p-semiconductor. A part of the anode connecting it to an external voltage source is metallized; 3 - cathode space, polyelectrolyte solution dissociating in water to negatively charged macro-ions R- and positively charged small counterions K + (in the example considered, these are hydrogen ions H + ); 4 - anode space, a solution of polyelectrolyte dissociating in water to positively charged macroions R + and negatively charged small counterions A- (in the example considered this is hydroxide ions OH- ); 5 - membrane (diaphragm), impermeable to macromolecules (macroions) of polyelectrolytes, but completely permeable for small counterions of K + , A- and water molecules, divides spaces 3 and 4; Yevnesh is an external source of tension.

Ed. From the Donnan effect

For clarity, an aqueous solution of a polyacid ( R-H + ) was chosen as the electrolyte of the cathode space (3, Fig. 1), and an aqueous solution of the poly-base ( R + OH- ) was used as the electrolyte of the anodic space (4, Fig. As a result of the dissociation of the polyacid, in the cathode space, near the cathode surface (1, Fig. 1), there is an increased concentration of H + ions. The positive charge arising in the immediate vicinity of the cathode surface is not compensated for by the negatively charged macroions R- , They can not come close to the surface of the cathode due to their size and the presence of a positively charged ionic atmosphere (for more details, see the description of the Donnan effect in Appendix 1 of the third part of the article). Thus, the boundary layer of the solution, which is in direct contact with the surface of the cathode, has a positive charge. As a result of electrostatic induction, a negative charge of conduction electrons appears on the surface of the cathode bordering the solution. Those. At the interface between the surface of the cathode and the solution, a DES appears. The field of this DELP pushes the electrons from the cathode into the solution.

Similarly, at the anode (2, figure 1), the boundary layer of the solution in the anode space (4, Fig. 1), which is in direct contact with the anode surface, has a negative charge, and a positive charge appears on the surface of the anode bordering the solution. Those. At the interface between the surface of the anode and the solution, there is also a DES. The field of this DES is pushing electrons from the solution - into the anode.

Thus, the DES fields at the interfaces of the cathode and the anode with the solution, supported by the thermal diffusion of the solution ions, are two internal sources of the emf acting in concert with the external source, i.e. Pushing negative charges in the contour counter-clockwise.

The dissociation of a polyacid and a poly-base also causes thermal diffusion through the membrane (5, Fig. 1) of H + ions from the cathode space to the anode space, and OH- ions from the anode space to the cathode space. Macroions of R + and R- polyelectrolytes can not move through the membrane, therefore on it, from the cathode space, there is an excessive negative charge, and from the side of the anode space - an excess positive charge, i.e. There is another DPS caused by the Donnan effect. Thus, an internal emf also appears on the membrane, acting in concert with the external source and maintained by the thermal diffusion of the solution ions.

In our example, the voltage across the membrane can reach 0.83 Volts, because This corresponds to a change in the potential of the standard hydrogen electrode from -0.83 to 0 volts upon transition from the alkaline medium of the anode space to the acidic medium of the cathode space. For details, see Appendix 1 of the third part of the article.

Ed. From internal IF

In the Element of the emf. Occurs, among other things, at the point of contact between the anode semiconductors and the cathode with their metal parts serving to connect an external voltage source. This emf Is due to internal IF. The internal IF does not create, in contrast to the outer surface, a field in the space around the contacting conductors, i.e. Does not affect the motion of charged particles outside the conductors. The n-semiconductor / metal / p-semiconductor structure is well known and is used, for example, in thermoelectric Peltier modules. The value of the emf Such a construction at room temperature can reach values of the order of 0.4-0.6 volts [5, p. 459; 2, p. 552]. The fields in the contacts are directed in such a way that they push the electrons counter-clockwise in the circuit, i.e. Operate in concert with an external source. In this case, the electrons increase their energy level, absorbing Peltier heat from the medium.

The internal IF, which arises from the diffusion of electrons at the points of contact between the electrodes and the solution, on the contrary, pushes the electrons clockwise in the circuit. Those. When electrons move in the Element in a counter-clockwise direction, Peltier heat must be released in these contacts. But since The transition of electrons from the cathode to the solution and from the solution to the anode is necessarily accompanied by an endothermic reaction of formation of hydrogen and oxygen, then Peltier heat is not released into the medium, but reduces the endothermic effect, i.e. As it were, "canned" in the enthalpy of formation of hydrogen and oxygen. For more details see Appendix 2 of the third part of the article.

Carriers of current (electrons and ions) move in the contour of the Element not along closed trajectories, no charge in the Element moves along a closed contour. Each electron produced by the anode from the solution (during the oxidation of OH-ions to oxygen molecules) and passing through the external circuit to the cathode, volatilizes together with hydrogen molecules (during the reduction of H + ions). Similarly, H + and OH- ions do not move in a closed loop, but only up to the corresponding electrode, and then volatilize in the form of molecules of hydrogen and oxygen. Those. And ions and electrons, move each in their environment in the accelerating fields of DES, and at the end of the path, when they reach the electrode surface, they unite into molecules, transforming all stored energy into chemical bonding energy, and exit the circuit!

All considered internal sources of emf. Element, reduce the cost of an external source for the electrolysis of water. Thus, the heat of the environment, absorbed by the Element in the course of its work to maintain diffusion DPS, is used to reduce the costs of the external source, i.e. Increases the efficiency of electrolysis.

Electrolysis of water without an external source.

When considering the processes occurring in the Element shown in Fig. 1, the parameters of the external source were not taken into account. Let its internal resistance be equal to Rn, and the voltage Einesh = 0. Ie. The electrodes of the Element are closed to a passive load (Figure 5). In this case, the directions and values of the fields of the DEL that arise at the interfaces between the phases in the Element will remain the same.

Fig. 5. Instead of Yevnesh (Figure 1), the passive load Rn is switched on.

Let us determine the conditions for the spontaneous flow of current in such an Element. The change in the Gibbs potential, in accordance with the formula (1) of Appendix 1 of the third part of the article:

Δ G rep = ( ΔH obre - П ) + Q обр

If П > Δ H обр + Q обр = 284,5 - 47,2 = 237,3 (kJ / mol) = 1,23 (eV / molecule),

Then Δ G obre <0 and a spontaneous process is possible.

We will further take into account that in the Element, the formation of hydrogen occurs in an acid medium (electrode potential 0 V), and oxygen in an alkaline (electrode potential 0.4 Volt). Such electrode potentials are provided by the membrane (5, figure 5), the voltage at which it should be 0.83 Volts. Those. The energy necessary for the formation of hydrogen and oxygen will decrease by 0.83 (eV / molecule). Then the condition for the possibility of a spontaneous process will be:

P > 1.23 - 0.83 = 0.4 (eV / molecule) = 77.2 (kJ / mol) (2)

We get that the energy barrier for the formation of hydrogen and oxygen molecules can be overcome without using an external voltage source. Those. Already at P = 0.4 (eV / molecule), i.e. With an internal IF of 0.4 Volts electrodes, the Element will be in a state of dynamic equilibrium, and any (even small) change in the conditions of this equilibrium will cause a current in the circuit.

Another obstacle in the way of reactions at the electrodes is the activation energy, but it is eliminated by the tunnel effect, which arises because of the small gap between the electrodes and the solution [7, p. 147-149].

Thus, starting from energy considerations, we find that the spontaneous current in the Element shown in Fig. 5, is possible. But what physical causes can this current cause? These reasons are listed below:

1. The probability of the transition of electrons from the cathode to the solution is higher than the probability of their transition from the anode to the solution, since The cathode n-semiconductor has many free electrons with a high energy level, and the p-semiconductor of the anode is only a "hole", and these "holes" are at the energy level below the level of the cathode electrons;

2. The membrane maintains an acid medium in the cathode space, and an alkaline medium in the anode chamber. In the case of inert electrodes, this leads to the fact that the cathode acquires a larger electrode potential than the anode. Consequently, electrons must move along the external circuit from the anode to the cathode;

3. The surface charge of solutions of polyelectrolytes arising from the Donnan effect creates on the boundaries an electrode / solution of the field such that the field at the cathode facilitates the release of electrons from the cathode into the solution and the field at the anode is the entrance of electrons from the solution to the anode;

4. The equilibrium of direct and reverse reactions on electrodes (exchange currents) is shifted towards direct reactions of reduction of H + ions at the cathode and oxidation of OH-ions at the anode, because They are accompanied by the formation of gases (H2 and O2), which can easily leave the reaction zone (the Le Chatelier principle).

Experiments.

To quantify the voltage on the load from the Donnan effect, an experiment was performed in which the cathode of the Element consisted of activated carbon with an external graphite electrode and the anode from a mixture of activated carbon and anionite AB-17-8 with an external graphite electrode. The electrolyte is an aqueous solution of NaOH, the anodic and cathodic spaces are separated by synthetic felt. At the open external electrodes of this Element, there was a voltage of about 50 mV. When connected to an external load element of 10 ohm, a current of about 500 μA was fixed. With an increase in the ambient temperature from 20 to 30 ° C, the voltage at the external electrodes increased to 54 mV. The increase in voltage with increasing ambient temperature confirms that the source of the emf. Is diffusion, i.e. Thermal motion of particles.

To quantify the stress on a load from an internal metal / semiconductor PKR, an experiment was performed in which the cathode of the Element consisted of synthetic graphite powder with an external graphite electrode and the anode was made of boron carbide powder (B4C, p-semiconductor) with an external graphite electrode. The electrolyte is an aqueous solution of NaOH, the anodic and cathodic spaces are separated by synthetic felt. At the open external electrodes of this Element, there was a voltage of about 150 mV. When connected to an External load element of 50 kΩ, the voltage dropped to 35 mV. Such a strong voltage drop is due to the low intrinsic conductivity of boron carbide and, as a consequence, the high internal resistance of the Element. An investigation of the voltage versus temperature for an Element of this construction was not carried out. This is due to the fact that, for a semiconductor, depending on its chemical composition, the degree of doping and other properties, the temperature change in different ways can affect its Fermi level. Those. The effect of temperature on the emf Element (increase or decrease), in this case, depends on the materials used, so this experiment is not indicative.

At the moment, another experiment is continuing, in which the cathode of the Element is made of a mixture of activated carbon powder and cationite KU-2-8 with an external stainless steel electrode, and an anode from a mixture of activated carbon powder and anionite AB-17-8 with an external electrode from of stainless steel. Electrolyte - an aqueous solution of NaCl, the anodic and cathodic spaces are separated by synthetic felt. Since October 2011, the external electrodes of this Element have been in a short-circuit condition with a passive ammeter. The current, which shows the ammeter, about a day after switching on, decreased from 1 mA - to 100 mkA (which, apparently, is connected with the polarization of the electrodes), and has not changed since then.

In the practical experiments described above, in connection with the inaccessibility of more efficient materials, the results obtained are substantially lower than theoretically possible. In addition, it is necessary to take into account that part of the total internal emf. The element is always consumed to maintain electrode reactions (production of hydrogen and oxygen) and can not be measured in an external circuit.

Conclusion .

Summarizing the above, we can conclude that nature allows us to convert heat energy into useful energy or work, while using as a "heater" the environment and not having a "refrigerator". Thus, the Donnan effect and internal IFR transform the thermal energy of the motion of charged particles into the energy of the electric field of the DES, and endothermic reactions convert thermal energy into chemical energy.

The Element, considered by us, consumes heat and water from the environment, but releases electricity, hydrogen and oxygen! Moreover, the process of electricity consumption, and the use of hydrogen as fuel, returns water and heat back to the environment!

Part 3. Applications.

In this section, the impact of Donnan's equilibrium, internal IFR at the metal / semiconductor interface, and Peltier heat on redox reactions and electrode potentials in the Element is discussed in more detail.

Potential of Donnan (Appendix No. 1)

Let us consider the mechanism of the appearance of the Donnan potential for polyelectrolyte. After the dissociation of the polyelectrolyte, its small counterions begin, under the action of diffusion, to leave the volume occupied by the macromolecule. Directional diffusion of small counterions from the volume of the polyelectrolyte macromolecule to the solvent occurs due to their increased concentration in the bulk of the macromolecule in comparison with the rest of the solution. Further, if, for example, small counterions are negatively charged, this leads to the fact that the internal parts of the macromolecule acquire a positive charge, and the solution directly adjacent to the volume of the macromolecule is negative. Those. Around a positively charged volume of a macroion, there appears, as it were, an "ionic atmosphere" of small counterions-charged negatively. The termination of the growth of the charge of the ionic atmosphere occurs when the electrostatic field between the ionic atmosphere and the volume of the macroion equilibrates the thermal diffusion of small counterions. The resultant equilibrium potential difference between the ionic atmosphere and the macroion is Donnan's potential. Potential Donnan is also called membrane potential, because A similar situation occurs on a semipermeable membrane, for example, when it separates an electrolyte solution in which there are ions of two kinds - capable and not able to pass through it, from a pure solvent.

Potential Donnan can be considered as the limiting case of diffusion potential, when the mobility of one of the ions (in our case of macroions) is zero. Then, according to [1, p. 535], taking the counterion charge equal to unity:

E d = ( RT / F ) Ln ( a1 / a2 ), where

Ed is Donnan's potential;

R - Universal gas constant;

T - Thermodynamic temperature;

F - Faraday constant;

A1 , a2 - the activity of counterions in the contacting phases.

In our Element, where the membrane separates the solutions of the poly-base (pH = Lg a 1 = 14) and polyacids (pH = Lg a 2 = 0), the Donnan potential on the membrane at room temperature ( T = 300 0K) will be:

E = ( RT / F ) (Lg a 1 - Lg a 2 ) Ln (10) = (8.3 * 300/96500) * (14-0) * Ln (10) = 0.83 Volta

Potential Donnan increases in direct proportion to the temperature increase. For a diffusion cell, Peltier heat is the only source for the production of useful work, so it is not surprising that for such elements, the emf. Increases with increasing temperature. In the diffusion elements, for the production of work, the heat of Peltier is always taken from the environment. When the current flows through the DPS formed by the Donnan effect, in the direction coinciding with the positive direction of the DEL field (ie, when the DES field commits positive work), heat is absorbed from the medium to produce this work.

But in the diffusion element, there is a continuous and unidirectional change in the ion concentrations, which ultimately leads to equalization of the concentrations and the stopping of the directed diffusion, in contrast to Donnan's equilibrium, in which, in the case of quasistatic currents, the ion concentration, once reaching a certain value, remains unchanged .

In Fig. 2 is a diagram of the change in oxidation-reduction potentials of the reactions of formation of hydrogen and oxygen with a change in the acidity of the solution. The diagram clearly shows that the electrode potential of the formation of oxygen in the absence of OH- ions (1.23 Volts in acid medium) differs from the same potential at a high concentration (0.4 Volts in alkaline medium) by 0.83 Volts. Similarly, the electrode potential of the hydrogen formation in the absence of H + ions (-0.83 Volts in alkaline medium) differs from the same potential at their high concentration (0 Volts in acid medium), also at 0.83 Volts [4, p. 66-67]. Those. It is obvious that 0.83 Volts is required in order to obtain a high concentration of the corresponding ions in water. This means that 0.83 volts is required for the mass dissociation of neutral water molecules into H + and OH-ions. Thus, if the membrane of our Element maintains an acidic medium in the cathode space, and the anode is alkaline, the voltage of its DEL can reach 0.83 Volts, which agrees well with the theoretical calculation given earlier. Such a voltage provides a high conductivity of the space of the DEL membrane due to the dissociation of water inside it into ions.

Fig. 2. The diagram of oxidation-reduction potentials of the reaction

Decomposition of water, as well as H + and OH- ions into hydrogen and oxygen.

KPI and Peltier heat (Appendix No. 2)

"The reason for the Peltier effect is that the average energy of the charge carriers (for the sake of certainty of electrons) participating in electrical conductivity in different conductors is different ... In going from one conductor to another, either the electrons transmit excess energy to the grating, or supplement the lack of energy at its expense (Depending on the direction of the current).

Fig. 3. Peltier effect at the contact of a metal and n-semiconductor: ԐF - Fermi level; ԐC is the bottom of the semiconductor conduction band; ԐV - the ceiling of the valence band; I - positive current direction; Circles with arrows conditionally show electrons.

In the first case, near the contact, it is isolated, and in the second case, the so- Peltier heat. For example, at the semiconductor-metal contact (Fig. 3), the energy of electrons passing from an n-type semiconductor to a metal (left contact) is much higher than the Fermi energy ԐF. Therefore, they violate the thermal equilibrium in the metal. The equilibrium is restored as a result of collisions, in which the electrons thermalize, giving off excess energy to the crystal. Grating. Only the most energetic electrons can go into the semiconductor from the metal (right contact), as a result of which the electron gas in the metal cools. The energy of lattice vibrations is used to restore the equilibrium distribution "[2, p. 552].

For a metal / p-semiconductor contact, the situation is similar. Because The p-semiconductor conductivity provides holes for its valence band below the Fermi level, then a contact will be cooled in which the electrons move from the p-semiconductor to the metal. Peltier heat, released or absorbed by the contact of the two conductors, is due to the production of negative or positive performance of the internal IF.

We turn on the left contact (Fig. 3), which generates heat of Peltier, an electrolytic cell, for example, an aqueous solution of NaOH (Fig. 4), and the metal and n-semiconductor are chemically inert.

Fig. 4. The left contact of the n-semiconductor and the metal is opened, and an electrolyte solution is placed in this gap. The notation is the same as in Fig. 3.

Since, when the current " I " flows from the n-semiconductor, electrons with higher energy enter the solution than leave the solution into the metal, this excess energy (Peltier heat) should be released in the cell.

The current through the cell can go only in the case of electrochemical reactions taking place in it. If the reactions in the cell are exothermic , Peltier heat is released in the cell, because More to it to disappear there is no place. If the reactions in the cell are endothermic, then the heat of Peltier goes entirely or partially to compensate for the endothermic effect, i. E. On the formation of reaction products. In our example, the total cell response: 2H2O → 2H2 ↑ + O2 ↑ is endothermic, so the heat (energy) of Peltier goes to the creation of H2 and O2 molecules formed on the electrodes. Thus, we get that the Peltier heat, taken from the medium in the right n-semiconductor / metal contact, is not released back into the medium, but is retained in the form of the chemical energy of hydrogen and oxygen molecules. Obviously, the work of an external voltage source, spent on electrolysis of water, in this case will be less than in the case of using identical electrodes that do not cause the Peltier effect.

Regardless of the properties of the electrodes, the electrolytic cell itself can absorb or release Peltier heat when a current passes through it. Under quasi-static conditions, the change in the Gibbs potential of a cell [4, p. 60]:

Δ G = Δ H - T Δ S , where

Δ H is the change in enthalpy of the cell;

T - Thermodynamic temperature;

Δ S - change of cell entropy;

Q = - T Δ S - Peltier cell heat.

For a hydrogen-oxygen cell at T = 298 (K), the enthalpy change ΔHpr = -284.5 (kJ / mol) [8, p. 120], the change in the Gibbs potential [4. from. 60]:

ΔGpr = - zFE = 2 * 96485 * 1.23 = - 237.3 (kJ / mol), where

Z is the number of electrons per molecule;

F is the Faraday constant;

E - emf Galvanic cell.

Consequently

Q pr = - T Δ S pr = Δ G pr - Δ H pr = - 237.3 + 284.5 = 47.2 (kJ / mol)> 0,

those. The hydrogen-oxygen cell emits Peltier's heat into the medium, while increasing its entropy and lowering its own. Then in the reverse process, with the electrolysis of water, which is what happens in our example, the heat of Peltier Q obr = - Q pr = - 47.3 (kJ / mol) will be absorbed by the electrolyte from the external environment.

Let P be the Peltier heat selected from the medium in the right-hand contact of the n-semiconductor / metal. Heat P > 0 should stand out in the cell, but because The reaction of the decomposition of water in the cell is endothermic ( ΔH > 0), then Peltier heat P is used to compensate for the thermal effect of the reaction:

Δ G rep = ( ΔH obre - П ) + Q обр                                                                        (1)

Q depends only on the composition of the electrolyte. Is a characteristic of an electrolytic cell with inert electrodes, and II depends only on the materials of the electrodes.

Equation (1) shows that Peltier heat P , as well as Peltier heat Q , are used to produce useful work. Those. Heat Peltier selected from the environment reduces the cost of an external source of electricity, necessary for electrolysis. The situation when the heat of the medium is a source of energy for the production of useful work is characteristic of all diffusion as well as for many electrochemical elements, examples of such elements are given in [3, p. 248-249].

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