Solid State Ionics for Batteries
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The conductivities of glasses, ionic liquids and polymer electrolytes rather unexpectedly display the same first-universality features on the frequency scale. As regards the temperature dependence, however, there is an important difference between glasses and 'non-Arrhenius' materials.
After a thermally activated elementary displacement of a mobile ion, its immediate backward motion appears to be non-activated in the 'non-Arrhenius' materials while it is activated in a glass. Therefore, the position of the high-frequency end of the dispersion of the conductivity, marking the inverse of the time when backward 'roll-back' movement sets in, does not depend on temperature. The resulting dc conductivity is indeed very close to VTF.
The mobile lithium ions are contained in the polymer coil. In these materials, the charge carriers are alkali ions in their hydrated state. A stunning property of this polymeric electrolyte is the reported absence of any conductivity dispersion. A probable explanation is the following. The lithium ions would thus diffuse almost randomly within the regions of space available for them.
In nanosized systems such as nano-composites and thin films level 3d , surfaces and interfaces play a paramount role in creating unexpectedly pronounced, sometimes even dramatic, ionic and electronic conductivity effects.
Energy level diagram for a mixed conductor MX with Frenkel disorder in the cation lattice, showing level bending at the equilibrium contact to a second phase. Top: ionic disorder.
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Bottom: electronic disorder in upside-down representation. The chemical potential of M is indicated by the two-headed arrow on the right-hand side. Basic relationships can be read from the diagram. The most important aspect is, of course, the constancy of the electrochemical potentials of metal ions and electrons in the region of varying electric potential. They also cancel in the distance of the two ionic levels from each other. However, if positive charges are accumulated at the interface, this will result in a position-dependent electric potential and thus in a level bending as shown in the figure.
Consequently, cation vacancies will be enriched and interstitial ions will be depleted in the space-charge zone in front of the interface. Evidently, it consists of two components. One of them is motionally narrowed, while the other is not, the former being caused by highly mobile lithium ions located in the interfacial regions, the latter being due to less mobile lithium ions within the crystallites.
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By courtesy of Heitjans and Indris. Many more examples can be given. These include the effects of grain boundaries in both cation and anion conductors. In nano-crystalline materials, the interfacial effects may completely dominate. If the material is coarse-grained, it contains a large number of oxygen vacancies, but only few excess electrons, and exhibits oxygen conduction. However, when prepared in nano-crystalline form, the material becomes an electronic conductor. In the bulk, the oxygen vacancies by far exceed the free electrons in number density, but this is reversed in the immediate vicinity of the grain boundary.
It is, however, also conceivable that the dopant ions are not mobile, their number density remaining spatially constant. In thin-film systems, lateral conductivities increase with inverse film thickness because the space-charge layers occupy an ever larger fraction of the cross section.
In international common usage, however, expressions such as 'solid electrolytes' and 'fast ion transport in solids' continued to be more customary.
They were replaced by 'Solid State Ionics' only about two decades later, when the proceedings of the Tokyo Solid State Ionics conference were published in the journal Solid State Ionics. The first international conference on this topic was held at Belgirate, Italy, in September Undoubtedly, the most renowned scientist attending was Carl Wagner. Notably, the solid electrolytes used up to the time of the Belgirate meeting had mostly been based on, or related to, AgI and doped ZrO 2 ; the beta alumina family had been discovered only a few years prior to the meeting.
In van Gool's own words, the most important achievement of the conference was that scientists, until then working as individuals, formed a nucleus that was going to shape the field of solid electrolytes in the years to come 6. In retrospect, the Belgirate conference is indeed remembered for marking a point in time when Solid State Ionics became a truly international endeavor, with scientists in many countries closely cooperating and, as it were, setting out to new shores.
The new initiatives taken included in particular the quest for new materials and new technologies. Regarding new materials, the impression conveyed at Belgirate was that 'we have only scratched the surface' 7. The truth of this assessment was to become obvious in the decades to follow.
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Regarding new technologies for possible applications, the message was twofold. On one hand, a long list of devices could be envisaged, including not only batteries, fuel cells and sensors but also ionic pumps, ion-transport membranes and ionic capacitors with high power densities.
On the other hand, it was only realistic to foresee that considerable technological problems would be awaiting along the way. The second and third were conferences held in the United States, namely at Lake Geneva, Wisconsin, in and at Gatlinburg, Tennessee, in The fourth meeting in the series was again held at Belgirate, Italy, marking the year anniversary of the first, in To cite Bruce UK 8 , 'Topics that were central or even dominant in the field in , such as intercalation electrodes and polymer electrolytes, had been in their infancy or not yet born in '.
While polymer electrolytes had in fact been unknown in , the intercalation concept had just come into existence. At the same meeting, the Bordeaux France group of Hagenmuller and Delmas introduced a lithium battery for electrical engine vehicles, in which reversible 'rocking chair' intercalation processes were occurring at both electrodes The interesting possibility of a paddle-wheel-type interaction between translationally mobile cations and rotationally mobile anions, e.
Interfacial phenomena, in particular the kinetics of ion-transfer across interfaces, had already been discussed at Belgirate I, e. However, the key role of ion-exchange kinetics at interfaces, in particular at the electrodes of solid state electrochemical cells, was perceived only at Belgirate II, see for instance the contribution by Boukamp et al The Netherlands on the surface oxygen exchange kinetics of solid oxide ion conductors As pointed out by Weppner Germany 16 at Belgirate II, the role played by electronic charge carriers in solid ionic and mixed conductors had previously been underestimated.
Many more steps of progress in the development of Solid State Ionics have been reported at other meetings, some held before, but most of them after Belgirate II. These include in particular the biennial Solid State Ionics series of international conferences. At one of those Solid State Ionics conferences, held at Monterey, California, in , Joop Schoonman The Netherlands gave a most memorable opening address, drawing the attention of the audience to the increasing awareness of environmental factors and limited energy resources, which had led to a profound evolution in the way energy was generated, converted and stored.
This sentence has since been considered a guideline for many activities in the Solid State Ionics community.
The clean-energy environmental issue has indeed spurred the development of new functional materials and solid state electrochemical devices. In the field of applied Solid State Ionics, the years and decades after saw both setbacks and instant success stories. On one hand, the hopeful expectations regarding new battery systems, which had been raised by the discoveries of rubidium silver iodide and the beta aluminas, gradually gave way to more realistic views and solutions. On the other hand, solid electrolytes got successfully employed in cardiac pacemaker batteries and in lambda probes for automobile exhaust sensors.
Both devices are now used around the globe and have thus drawn worldwide attention to applied Solid State Ionics. Although some of these lines of development had their origins outside Europe, all of them are certainly remarkable from a European perspective as well and will, therefore, be briefly sketched in the following.
These cells were capable of operation at both high and low current density and over a wide range of temperatures. Nevertheless, this did not prevent the successful development of all-solid-state cardiac pacemaker batteries employing this solid electrolyte. Since then, the LiI battery has established an excellent record in reliability.
Between this cathode and the lithium-metal anode the thin LiI film was formed by an in situ reaction. This offered the advantage of 'self-healing', with new lithium iodide being formed once cracks occurred in the solid electrolyte. Sodium-sulfur cells, with ceramic beta alumina serving as solid electrolyte between the molten-sodium anode and the molten-sulfur cathode, were for a long while regarded as promising units for electrotraction, since they offered energy densities and, therefore, automobile operating ranges that surpassed the possibilities of conventional lead—acid or nickel—cadmium accumulators roughly by a factor of At that time real market introduction was still expected to be possible around the year Later, however, the further development of sodium-sulfur cells aiming at electrotraction was largely discontinued.
The main reason was the unsolved problem of possible crack formation in the brittle solid electrolyte, entailing a catastrophic chemical reaction of molten sodium with molten sulfur. Here it is comforting that alternate forms of electrotraction, involving either lithium-ion batteries or fuel cells, are rapidly coming into view. Remarkably, Solid State Ionics has provided a special gift for motorists, which Walther Nernst, who was an enthusiastic motorist himself, would have happily appreciated.
Indeed, his two most prominent legacies, the Nernst equation and the Nernst mass, have been united in the concept of the lambda probe, which simultaneously serves the driver, the car and the environment. According to the Nernst equation, its e. Obviously, the standard e. As the oxygen partial pressure in air is sufficiently well defined, the oxygen partial pressure in the exhaust gas is given by the Nernst equation with sufficient accuracy as soon as the cell voltage has been measured. Note that the general shape reflects the principle of a titration curve. In this case, the reference electrode consisted of a layer of AgCl on silver, while the electrolyte was a composite chloride-ion conductor.
In the cell reaction, which is. CO 2 is the only gaseous component, while the three solids are in their standard states. Therefore, according to the Nernst equation, the cell voltage is simply. Like the lambda probe, the sensor is based on YSZ. Within the device, a temperature gradient is applied to a thick-film YSZ layer, and the resulting thermovoltage is measured.
This measured voltage is found to depend on the oxygen partial pressure in a way that is in perfect agreement with theoretical predictions. The technique offers the advantages of little temperature dependence and no cross-sensitivity to a variety of other exhaust gases. Electrolytic cells based on YSZ as a solid electrolyte may also be used to remove oxygen from stationary or streaming gas.
While the electrochemical cells employed in cardiac pacemaker batteries and in lambda probes triggered the first truly international success stories in the field of Solid State Ionics, these have not remained the only ones.
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The predominant aim is to decrease the amount of solar radiation entering and heating up the inside of buildings or cars and thus to reduce the energy expenditure for air conditioning considerably. Another aim, relevant during the winter, is to let windows be transparent for visible light, but reflective in the infrared, thus blocking loss of interior heat. This electrochromic material is typically tungsten oxide, WO 3 , and the reaction that causes darkening is.
A solid lithium-ion conductor separates the electrochromic film from an ion-storage film, e.
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The two films consist of nanomaterials with well-developed nanoporosities, and the resemblance to a thin-film 'rocking chair' secondary battery is obvious. Smart windows have meanwhile been tested and installed in different parts of the world, mostly for alleviating air conditioning loads by means of 'light balancing'. Nanostructured, very large surface area electrodes are also essential in a novel class of electrochemical energy storage devices called electric double-layer capacitors or simply 'supercapacitors'.