- Nano Review
- Open Access
Selective crystallization with preferred lithium-ion storage capability of inorganic materials
© Liu et al; licensee Springer. 2012
- Received: 15 November 2011
- Accepted: 21 February 2012
- Published: 21 February 2012
Lithium-ion batteries are supposed to be a key method to make a more efficient use of energy. In the past decade, nanostructured electrode materials have been extensively studied and have presented the opportunity to achieve superior performance for the next-generation batteries which require higher energy and power densities and longer cycle life. In this article, we reviewed recent research activities on selective crystallization of inorganic materials into nanostructured electrodes for lithium-ion batteries and discuss how selective crystallization can improve the electrode performance of materials; for example, selective exposure of surfaces normal to the ionic diffusion paths can greatly enhance the ion conductivity of insertion-type materials; crystallization of alloying-type materials into nanowire arrays has proven to be a good solution to the electrode pulverization problem; and constructing conversion-type materials into hollow structures is an effective approach to buffer the volume variation during cycling. The major goal of this review is to demonstrate the importance of crystallization in energy storage applications.
- lithium-ion battery
- hollow structure
Materials crystallized with unique sizes and structures are expected to find various novel applications [1–5]. The discovery of novel materials, processes, and phenomena provides fresh opportunities for the development of innovative systems and devices, which is likely to have a profound impact in areas such as energy, electronics, medicine, and biotechnology [6–12]. Batteries are a major technological challenge in the present society as they are a key method to make a more efficient use of energy [13–15]. Although the current lithium-ion battery (LIB) technology has conquered the portable electronic markets and is still improving, the use of LIB in the powering of plug-in electric vehicles or the storage of renewable energies (wind, solar) is still challenging . The performance of LIB depends essentially on the thermodynamics and kinetics of the electrochemical reactions involved in the electrode materials. During the past decade, extensive efforts have been made to developing advanced batteries with large capacity, high energy and power densities, high safety, long cycle life, fast response, and low cost [17–20]. These developments rely on new ways to prepare electrode materials via eco-efficient processes; achieving these goals will require the inputs of multiple disciplines.
Insertion reaction mechanism:(1)
Li-alloy reaction mechanism:(2)(3)
Conversion reaction mechanism:(4)
Insertion-type materials containing cobalt are the most studied cathodes for LIB . They show high stability in a high-voltage range; however, cobalt has limited availability in nature and is toxic, which is a tremendous drawback for mass manufacturing. Manganese offers a low-cost substitution with a high thermal threshold and excellent rate capabilities but limited cycling behavior . Olivines are nontoxic and have a moderate capacity with low fade due to cycling, but their conductivity is quite low . Alloy anodes have high capacities but show a dramatic volume change in charging and discharging, resulting in poor cycling behavior , a similar problem also found in conversion-type materials .
Nanostructuring electrode materials has been proven to be an effective strategy to alleviate these above problems [27–31]. There are several advantages associated with the development of nanomaterials for LIBs , which include (1) better accommodation of the strain of lithium insertion/removal, improving cycle performance; (2) new reactions which are not possible in bulk materials may happen; (3) better electrode/electrolyte contact, and (4) short path lengths for electron and Li+ transport. Here, we summarize recent scientific research and development of LIB electrode materials upon novel nanoscience and nanotechnology progresses. The focus is on research activities toward the selective crystallization of inorganic materials with preferred shapes, sizes, and structures, which can influence ionic diffusion and transport, electron transfer, surface/interface interaction, and the electrochemical reactions. The effect of selective crystallization on the LIB performances of electrode materials is discussed in detail according to different Li storage mechanisms. The current review shows that the selective crystallization route plays a predominant role in the development of next-generation LIBs.
Insertion-type materials involve most cathode materials and some anode materials (such as graphite, Li4Ti5O12, and TiO2). The first generation of LIB uses LiCoO2 and graphite as the positive and negative electrodes; the redox operation of both versus lithium is based on intercalation reactions. Alternative materials such as LiMn2O4, LiFePO4, and Li4Ti5O12 have also reached the market at different levels, bringing about incremental improvements in performance . Nonetheless, all these materials have intrinsic capacity limitations, which are derived from their redox mechanisms and structural aspects, i.e., the intrinsic redox activity of the transition metals and the changes the crystal structure can withstand. Such limitation handicaps the device in terms of energy density. Power density of these cathode materials with bulk sizes is also generally low due to the high level of polarization at high charge/discharge rates . Therefore, the selective crystallization approach was introduced to overcome these shortcomings by decreasing diffusion paths for mass transport and increasing the surface area for charge transfer.
Besides increasing capacity, a high cell voltage resulting from a high (cathode) and low (anode) standard redox potential of the respective electrode redox reaction can also greatly improve the energy density of LIB. Due to the redox potential of an intercalation compound which mainly tracks the iono-covalency of the metal-X bonding, selective crystallization of cathode materials with fluorine substitution appears to be quite an attractive route to increase the material redox voltage as F is very electronegative . Recently, Barpanda et al. reported a polyanionic material that crystallizes in the triplite structure Li(Fe1-δMnδ)SO4F . An open-circuit voltage of 3.9 V has been achieved, exceeding that of LiFePO4 by 450 mV. Also, this new triplite phase is capable of reversibly releasing and reinserting 0.7 to 0.8 Li ions with a volume change of only 0.6% (compared with 7% and 10% for LiFePO4 and LiFeSO4F, respectively), to give a capacity of 125 mAh g-1. Such a material could become a promising cathode to replace LiFePO4. These new types of polyanionic compound, having the triplite structure, provide valuable information in the search for even better cathode materials.
In the case of anode materials, the formation of a solid-electrolyte-interface (SEI) layer on which metallic lithium is deposited during a fast charge of the battery should also be a concern. The dendrites can grow to short-circuit the battery and ignite the electrolyte. Therefore, safety concerns have led to a search for anode materials having a redox couple in the range of 1.0 to 1.5 eV below the Fermi energy of lithium. The spinel Li4Ti5O12 is reported to be a stable anode operating on the Ti(IV)/Ti(III) redox couple located at 1.5 V versus Li+/Li. It is capable of a fast charge and a long cycle life because no SEI layer is formed [46–48]. However, it has a low specific capacity (approximately 140 mAh g-1), and the high redox potential (1.5 V) reduces the energy density of a cell using this anode. On the basis of these considerations, different niobium-based oxides such as KNb5O13 and K6Nb10.8O30 have been investigated, which exhibit a reversible Li insertion toward the targeted voltage range of 1.0 to 1.5 V versus Li+/Li [49, 50]. More recently, the mixed titanium-niobium oxides such as TiNb2O7 have been selectively crystallized as the anode for lithium batteries with some similar electrochemical properties [51, 52]. Notably, carbon-coated TiNb2O7 gives a reversible specific capacity of approximately 285 mAh g-1 cycled between 1.0 and 2.5 V versus Li+/Li with a Coulombic efficiency over 98% . These new-type anodes provided promising candidates for batteries with high rate, high cycle life, and better safety.
From the above discussion, it is evident that selective crystallization of insertion-type materials into nanosized particles and shapes with specific facets can effectively enhance the lithium-ion diffusion rate and improve their cycling performance; these improvements are all closely related to the crystal structure and reaction mechanisms of this kind of materials. As an alternative route, tuning the crystal structure by selective atom substitution can also improve the energy density of LIB by increasing the cell voltage.
Interstitial-free, 3D transition-metal oxides (MxOy, M = Fe, Co, Ni, Mn, Cu, etc.) are capable of incorporating more than one Li per 3D metal, hence giving high Li storage capacities . The Li storage mechanism of the MxOy differs from the Li-intercalation and Li-alloying mechanisms. Transition-metal oxides are reduced to metal in the lithiation process (Equation 4). During the first reduction of the metal oxide, highly reactive metallic nanodomains embedded in a Li2O matrix can be generated in situ, which contributed to the reversibility of this reaction . Based on this mechanism, reversible lithium storage proceeds more easily with the nanostructured oxides. Therefore, selective crystallization of transition-metal oxides has a significant role for their LIB performances. Similar to the Li-alloying process, the conversion reaction leads to volume variation upon the electrochemical cycling. Conceptually, approaches such as constructing hollow structures or nano-compositing are applicable to conversion-type anode materials as well.
The use of transition-metal oxides as conversion-type electrodes holds the promise of higher energy density and wealth of compounds, but capacity fading needs to be overcome before practical use in LIB; bulk electrodes fail within a few charge/discharge cycles due to the large volumetric change that occurs during lithiation and delithiation. Selective crystallization into specific structures and composites can have a major impact on the performance and cyclability of the conversion-type anode. Nanoscale morphologies have the potential to achieve long cycling lifetimes and good reversibility as stress management and formation of a stable passivation layer during cycling can be achieved.
Selective crystallization of electrode materials into nanostructures has presented the opportunity to design novel energy-storage materials for the next-generation, high-performance LIBs with higher energy density, higher power density, and longer cycle life. Due to the high surface area and specific configuration of nanostructured materials, these electrodes can provide high lithium-ion flux across the interface, short diffusion pathways for both Li ions and electrons, abundant active sites for Li storage, and high freedom for volume change during electrochemical charge/discharge process. In this review article, three categories of LIB electrode materials were discussed. The first one is insertion-type materials, which can store Li through an intercalation process. The improved storage ability is closely related to their surface area, crystallinity, as well as the orientation of these crystallites. In the second group, alloying-type materials such as Sn and Si were presented. Nanostructuring these bulk materials into nanowire arrays and dispersing these elements into rigid matrices have been proven to be effective approaches to overcome the poor cycling problems. The third category is conversion-type materials. Their large-scale application is also hindered by the rapid capacity decay during charging/discharging because of the significant volume change. Nanostructures with hollow interiors and nanocomposites have been developed to address this problem. For a specific material, it is hard to achieve a structure which own all advantaged features, and for different materials, the effect of the crystallization feature is not identical; therefore, much necessary work still needs to be done to give a more comprehensive understanding of the relationship between nanostructures and their performances.
To realize widespread commercial applications, controlled and large-scale fabrication of nanostructures is required, in which selective crystallization should play a vital role. The future directions of electrode materials for LIBs should focus on exploring new types of lithium-ion redox couples with different electrode reaction mechanisms and designing novel structures and morphologies in order to further increase battery energy/power densities, enhance charge/discharge rate capability, improve service life and safety, and reduce the cost at the same time. The 3D nanoarchitectured cells, in which pillared anodes and cathodes are interdigitated, have already attracted much interest. Developing flexible electrodes and all-solid batteries is a strong demand for meeting the various requirements of modern gadgets, which will also be an important feature of research in future years.
Financial support from the National Natural Science Foundation of China (Nos. 50872016, 20973033, and 51125009) and the National Natural Science Foundation for Creative Research Group (No. 20921002) are acknowledged.
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