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Nanoionics of Advanced Superionic Conductors 306 Ionics 11 (2005) Nanoionics of Advanced Superionic Conductors A.L. Despotuli, A.V. Andreeva and B. Rambabu* Institute of Microelectronics Technology & High Purity Materials RAS, 142432 Chernogolovka, Moscow Region, Russia *Southern University and A&M College, Baton Rouge, Louisiana, 70813 USA ~E-mail: [email protected] (A.L. Despotuli) Abstract. New scientific direction - nanoionics of advanced superionic conductors (ASICs) was proposed. Nanosystems of solid state ionics were divided onto two classes differing by an opposite influence of crystal structure defects on the ionic conductivity oi (energy activation E): 1) nanosystems on the base compounds with initial small o~ (large values of E); and II) nanosystems of ASICs (nano-ASICs) with E = 0.1 eV. The fundamental challenge of nanoionics as the conservation of fast ion transport (FIT) in nano-ASICs on the level of bulk crystal was first recognized and for the providing of FIT in nano- ASICs the conception of structure-ordered (coherent) ASIC//indifferent electrode (IE) hetero- boundaries was proposed. Nano-ASIC characteristic parameter P = d/Xo (d is the thickness of ASIC layer with the defect crystal structure at the heteroboundary, and Ao is the screening length of charge for mobile ions of the bulk of ASIC) was introduced. The criterion for a conservation of FIT in nano-ASIC is P = 1. It was shown that at the equilibrium conditions the contact potentials V at the ASIC//IE coherent heterojunctions in nano-ASICs are V << keT/e. Interface engineering approach "from advanced materials to advanced devices" was proposed as fundamentals for the development of applied nanoionics. The possibility for creation on the base of ASIC//IE coherent heterojunctions of the efficient energy and power devices (sensors and supercapacitors with specific capacity ~10 -~ F/cm 2 and maximal frequencies 10~-109 Hz,) suited for micro(nano)electronics, microsystem technology and 5 Gbit DRAM was pointed out. 1. Introduction introduced and some appropriate fundamentals are for- Dispersoids of ionic conductors [1-3] and ionic con- mulated. Key role of interface design in nanoionics of ductor//electronic conductor heterojunctions [4] are classic ASICs is pointed. It is expected that in next decade the objects of solid state ionics and, at the same time, the nanoionic devices will find a wide application in the objects of nanoionics, as by structure they are nano- sphere of wireless sensor networks (multitude auto- systems. The term and conception of nanoionics as a new nomous sensors that coordinate among themselves and branch of science devoted to a fast ion transport (FIT) in revolutionize information gathering in any type of terrain solid nanosystems was first introduced by [5] in 1992. and conditions). Main applications of nanoionics relate to the creation of new materials, functional structures and devices suited for 2. Two Classes of Solid State Ionic Nano- the storage and conversion energy and information. In the systems and Two Fundamentally Different latest years, the term "nanoionics" ("nano-ionics") came Nanoionics into wide use in scientific articles and denotes also the Solid state ionic conductors (SSIC) with a high level of area of interests of the scientific societies and organiza- unipolar ionic conductivity (Q > 0.001 f2-~cm-~ and the tions [6]. level of electronic conductivity G, is arbitrary) are called In the present article the new scientific direction - superionic conductors (SIC), and solids with oi )> 4, nanoionics of advanced superionic conductors (ASIC) is identified as solid electrolytes (SE). Intersection of SIC f3 Ionics 11 (2005) 3O7 size in nanocomposites. At the sizes of crystallites comparable with a thickness of DEL, the integral values of cri in nanocomposites of "poor" ionic conductors are much higher than in component substances. However, the ion-transport properties (G, E, ni) in the nanocomposites of "poor" ionic conductors are significantly worse (for example, the energy of activation E is 4-8 times large) than in ASICs (c~-AgI, RbAg4Is). Crystal structure of ASICs is close to an optimal one for FIT (oi =, 0.3 ~-lcm-1 at 300 K, E = 0.1 eV). Therefore, the defects of crystal structure should violate almost everywhere in ASIC conditions for FIT. Thus, at the high concentration of defects in nanosystem of "poor" ionic conductors the integral ~ arises, but in ASICs the influence of defects is Fig. 1. Different types of solid state ionic conductors opposite. (SSIC) on the cri- o e diagram [8-10]: SE are the solid In [5], a general approach for description of properties electrolytes where the ionic conductivity ~ >> electronic one o~; SIC are the superionic conductors, ~ > 0.001 f2-Lcm ~, of ionic nanosystem was proposed (nanoionics con- and o~ is arbitrary; ASIC are the advanced superionic ception). It is based on the using of the P = d/L ~ 1 conductors oi > 0.1 ~ fcm-~, and cr is arbitrary; SIC n SE are dimensionless parameter (d is the thickness of boundary the superionic conductors & solid electrolytes, ~ > 0.001 if2-lcm ~, and oi >~q; ASIC fq SE are the advanced superionic domain of SSIC with the peculiar properties, and the L - conductors & solid electrolytes, cr~ > 0.1 if2-lcm ~, and o, ~>% characteristic size of the SSIC nanostructure). For nano- systems of "poor" ionic conductors with DEL it can be d ~- )~D and P = )~o/L. However, if DEL is absent then SE is a group of SIC & SE, simultaneously. Among the others characteristic values should be used instead of 3,D. SICs there is a subgroup with a record high level of Two examples can be mentioned. In a fuel cell the effec- unipolar ~. This subgroup can be called as advanced tive functioning of catalyst demands that the diffusion superionic conductors (ASIC). There is a subgroup ASIC length of proton (d) be comparable with the size of ca- fq SE, i.e. compounds with o, ~ % (examples are: ct- talyst particle (L). Also, at the solid-state synthesis of AgI, ct-RbAg4Is, CsAg4Br3_xIz§ Rb4Cu16IvCl13 and some new compounds in the nano-physical-chemical systems others). For instance, the Rb4Cu16IvC113 is ASIC & SE [6,13-16], dissolution of metals in SSICs is accompanied with recorded high crj (~ 0.34 if2-~crn-~ at 300 K, and by the simultaneous insertion of electrons and ions and activation energy of ionic conductivity E = 0,1 eV) [7]. local electro-neutrality in the layer with peculiar pro- All types of SSICs are presented on the ~,-cr~ diagram perties remains. Therefore, instead of ~.D it is necessary to (Fig. 1). use, for example, a critical radius of a new phase crystal On the boundaries of ionic crystals the double electric nucleus, the average size of crystallite and others similar layers (DEL) with a high concentration of defects always values. exist. It is a consequence of different values of work The calculation of ~-D for the c~-RbAg4I~ ASIC (300 function for different kind of ions [11]. The thickness of K, and concentration of mobile ions ~ 10 28 m -3) according DEL is an order of Debye length )~ and is defined by a to the Debye formula: concentration of mobile ions ne. In the work [1] an en- hanced ionic conductivity cri in nanocomposites (dis- )~o ~ (eeo k8 T/e2 ni) 1/2, (1) persoids) with components of small initial crg was discovered. Such an effect is due to the high density of (e0 = 8.8x 10 -~2 F/m; e is the dielectric constant, 1 for DELs with high values of Oe. vacuum; kB is the Boltzmann's constant, 1.4x10 -23 jK-l; Two classes of SSICs can be distinguished. In the T = 300 K; e is the electronic charge, 1.6x10 -19 C) class of substances with small ~ ("poor" ionic results in value for )~D ~ 0.05 nm, which is less than the conductors), for instance, LiI (at 300 K ere ~ 5.5x10 -7 size of Ag+-ion. It indicates the need for another formula f2-~cm-1, and energy activation E > 0.4 eV [12]), the (see, for example, [17]) for the calculation of the value of ~,o is about ~60 nm that is an order of a grain screening length (/LQ). 308 Ionics 11 (2005) In the RbAg4I5 ASIC, the oscillation frequencies of thickness of transition defect layer was introduced in [34]. mobile Ag+-ions in the potential minimums of crystalline The work [35] was devoted to the development of ad- relief are ~10 J2 s -~ and the Ag+-ions jump over the sorption relaxation model (relaxation of DEL in ASICs). potential barriers (= 0.1 eV) between neighboring In this model, the slow diffusion processes (large values crystallographic positions with the frequencies ~101~ s -~. of energy activation E) on electrode are attributed to the According to [18], in the RbAg4I5 ASIC the concentration movement of ionic defects. However, all above-mentioned of Ag+-ions in the state of flying over potential barriers is models and conceptions are phenomenological and macro- of the order of ~10 26 m -3. For these ions the Debye's scopic and they do not take into account the concrete formula yields ~,o ~ 0.5 nm (the size of ion is several atomic structure of heteroboundaries. Such structures in a times less) and (1) can be using for estimation of number of cases can have a size comparable with ~e in screening length. If the potential of indifferent electrode the volume of ASIC. (IE) at the RbAg4Is/IE heterojunction changes then the Atomic structure of homo- and heterophase boundaries Ag+-ions (flying under potential barriers) will form the and the analysis of appropriate processes are in a focus of DEL with the thickness ~-D ~ 0.5 nm during the time material science during decades. Terms and approaches as interval At ~ 10-j~ s.
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