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Analog synaptic devices have made significant advances based on various electronic materials that can realize the biological synapse properties of neuromorphic computing. Ferroelectric (FE) HfO2-based materials with nonvolatile and low power consumption characteristics are being studied as promising materials for application to analog synaptic devices. The gradual reversal of FE multilevel polarization results in precise changes in the channel conductance and allows analogue synaptic weight updates. However, there have been few studies of FE synaptic devices doped with La, Y, and Gd. Furthermore, an investigation of interface quality is also crucial to enhance the remnant polarization (Pr), synaptic conductance linearity, and reliability characteristics. In this study, we demonstrate improved FE and artificial synaptic characteristics using an atomic layer-deposited (ALD) lanthanum-doped HfO2 (La:HfO2) and TaN electrode in the structure of an FE thin-film transistor (ITO/IGZO/La:HfO2/TaN), where indium-tin oxide (ITO) and indium-gallium-zinc oxide (IGZO) were used as source/drain and channel materials, respectively. Improved Pr and lower surface roughness were achieved by doped HfO2 and ALD TaN thin films. This synaptic transistor shows long-term potentiation and long-term depression with 200 levels of conductance states, high linearity (Ap, 0.97; Ad, 0.86), high Gmax/Gmin (â¼6.1), and low cycle-to-cycle variability. In addition, a pattern recognition accuracy higher than 90% was achieved in an artificial neural network simulation.
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The use of elemental doping in lithium cobalt oxide (LCO) cathode material at high cutoff voltage is a widely adopted technique in the field of rechargeable batteries to mitigate multiple unfavorable phase transitions. However, there is still a lack of fundamental understanding regarding the rationality of each doping element implemented in this method, specifically considering the various thermodynamic stability and phase transitions. Herein, we investigated the effect of Ti doping on an O2 phase LCO (LCTO) cathode material that exhibited enhanced rate performance. We suggest that the incorporation of Ti into an O2 phase LCO results in the mitigation of multiple-phase transitions and the improvement of phase stability, thereby yielding a high-rate-capable cathode material. Through a combination of experimental and computational calculations, we demonstrate that Ti doping improves the thermodynamic stability and kinetics of Li-ions during the cycling process.
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An intriguing mechanism for enabling fast Na kinetics during oxygen redox (OR) is proposed to produce high-power-density cathodes for sodium-ion batteries (SIBs) based on the P2-type oxide models, Na2/3 [Mn6/9 Ni3/9 ]O2 (NMNO) and Na2/3 [Ti1/9 Mn5/9 Ni3/9 ]O2 (NTMNO) using the "potential pillar" effect. The critical structural parameter of NTMNO lowers the Na migration barrier in the desodiated state because the electrostatic repulsion of O(2p)O(2p) that occurs between transition metal layers is combined with the chemically stiff Ti4+ (3d)O(2p) bond to locally retain the strong repulsion effect. The NTMNO interlayer distance moderately decreases upon charging with oxygen oxidation, whereas that of NMNO decreases at a much faster rate, which can be explained by the dependence of OR activity on the coordination environment. Fundamental electrochemical experiments clearly indicate that the Ti doping of the bare material significantly improves its rate capability during OR, and detailed electrochemical and structural analyses show much faster Na kinetics for NTMNO than for NMNO. A systematic comparison of the two cathode oxides based on experiments and first-principles calculations establishes the "potential pillar" concept of not only improving the sluggish Na kinetics upon OR reaction but also harnessing the full potential of the anionic redox for high-power-density SIBs.
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Cation migration often occurs in layered oxide cathodes of lithium-ion batteries due to the similar ion radius of Li and transition metals (TMs). Although Na and TM show a big difference of ion radius, TMs in layered cathodes of sodium-ion batteries (SIBs) can still migrate to Na layer, leading to serious electrochemical degeneration. To elucidate the origin of TM migration in layered SIB cathodes, we choose NaCrO2 , a typical layered cathode suffering from serious TM migration, as a model material and find that the TM migration is derived from the random desodiation and subsequent formation of Na-free layer at high charge potential. A Ru/Ti co-doping strategy is developed to address the issue, where the doped active Ru is first oxidized to create a selective desodiation and the doped inactive Ti can function as a pillar to avoid complete desodiation in Ru-contained TM layers, leading to the suppression of the Na-free layer formation and subsequent enhanced electrochemical performance.
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Oxygen redox (OR) reactions in sodium layered oxide cathodes have been studied intensively to harness their full potential in achieving high energy density for sodium-ion batteries (SIBs). However, OR triggers a large hysteretic voltage during discharge after the first charge process for OR-based oxides, and its intrinsic origin is unclear. Therefore, in this study, an in-depth reinvestigation on the fundamentals of the reaction mechanism in Na[Li1/3Mn2/3]O2 with a Mn/Li ratio (R) of 2 was performed to determine the factors that polarize the OR activity and to provide design rules leading to nonhysteretic oxygen capacity using first-principles calculations. Based on thermodynamic energies, the O2-/O22- and O2-/On- conditions reveal the monophasic (0.0 ≤ x ≤ 4/6) and biphasic (4/6 ≤ x ≤ 1.0) reactions in Na1-x[Li2/6Mn4/6]O2, but each stability at x = 5/6 is observed differently. The O-O bond population elucidates that the formation of an interlayer O-O dimer is a critical factor in triggering hysteretic oxygen capacity, whereas that in a mixed layer provides nonhysteretic oxygen capacity after the first charge. In addition, the migration of Li into the 4h site in the Na metallic layer contributes less to the occurrence of voltage hysteresis because of the suppression of the interlayer O-O dimer. These results are clearly elucidated using the combined-phase mixing enthalpies and chemical potentials during the biphasic reaction. To compare the Mn oxide with R = 2, Na1-x[Li1/6Mn5/6]O2 tuned with R = 5 was investigated using the same procedure, and all the impeding factors in restraining the nonhysteretic OR were not observed. Herein, we suggest two strategies based on three types of OR models: (i) exploiting the migration of Li ions for the suppression of the interlayer O-O dimer and (ii) modulating the Mn/Li ratio for controlling the OR participation, which provides an exciting direction for nonhysteretic oxygen capacities for SIBs and lithium-ion batteries.
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Nonhysteretic redox capacity is a critical factor in achieving high energy density without energy loss during cycling for rechargeable battery electrodes, which has been considered a major challenge in oxygen redox (OR) for Li-excess layered oxide cathodes for lithium-ion batteries (LIBs). Until recently, transition metal migration into the Li metal layer and the formation of O-O dimers have been considered major factors affecting hysteretic oxygen capacity. However, Li-excess layered oxides, particularly Ru oxides, exhibit peculiar voltage hysteresis that cannot be sufficiently described by only these factors. Therefore, this study aims to unlock the critical impeding factors in restraining the non-polarizing oxygen capacity of Li-excess layered oxides (herein, Li2RuO3) that exhibit reversible OR reactions. First, Li2RuO3 undergoes an increase in the chemical potential fluctuation as both the thermodynamic material instability and vacancy content increase. Second, the chemical compression of O-O bonds occurs at the early stage of the OR reaction (0.5 ≤ x ≤ 0.75) for Li1-xRu0.5O1.5, leading to flexible voltage hysteresis. Finally, in the range of 0.75 ≤ x ≤ 1.0, for Li1-xRu0.5O1.5, the formation of an O(2p)-O(2p)* antibonding state derived from the structural distortion of the RuO6 octahedron leads to the irreversibility of the OR reaction and enhanced voltage hysteresis. Consequently, our study unlocks the new decisive factor, namely, the structural distortion inducing the O(2p)-O(2p)* antibonding state, of the hysteretic oxygen capacity and provides insights into enabling the full potential of the OR reaction for Li-excess layered oxides for advanced LIBs.
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Neuromorphic computing has garnered significant attention because it can overcome the limitations of the current von-Neumann computing system. Analog synaptic devices are essential for realizing hardware-based artificial neuromorphic devices; however, only a few systematic studies in terms of both synaptic materials and device structures have been conducted so far, and thus, further research is required in this direction. In this study, we demonstrate the synaptic characteristics of a ferroelectric material-based thin-film transistor (FeTFT) that uses partial switching of ferroelectric polarization to implement analog conductance modulation. For a ferroelectric material, an aluminum-doped hafnium oxide (Al-doped HfO2) thin film was prepared by atomic layer deposition. As an analog synaptic device, our FeTFT successfully emulated short-term plasticity and long-term plasticity characteristics, such as paired-pulse facilitation and spike timing-dependent plasticity. In addition, we obtained potentiation/depression weight updates with high linearity, an on/off ratio, and low cycle-to-cycle variation by adjusting the amplitude and number of input pulses. In the simulation trained with optimized potentiation/depression conditions, we achieved a pattern recognition accuracy of approximately 90% for the Modified National Institute of Standard and Technology (MNIST) handwritten data set. Our results indicated that ferroelectric transistors can be used as an alternative artificial synapse.
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An intriguing redox chemistry via oxygen has emerged to achieve high-energy-density cathodes and has been intensively studied for practical use of anion-utilization oxides in A-ion batteries (A: Li or Na). However, in general, the oxygen redox disappears in the subsequent discharge with a large voltage hysteresis after the first charge process for A-excess layered oxides exhibiting anion redox. Unlike these hysteretic oxygen redox cathodes, the two Na-excess oxide models Na2IrO3 and Na2RuO3 unambiguously exhibit nonhysteretic oxygen capacities during the first cycle, with honeycomb-ordered superstructures. In this regard, the reaction mechanism in the two cathode models is elucidated to determine the origin of nonhysteretic oxygen capacities using first-principles calculations. First, the vacancy formation energies show that the thermodynamic instability in Na2IrO3 increases at a lower rate than that in Na2RuO3 upon charging. Second, considering that the strains of Ir-O and Ru-O bonding lengths are softened after the single-cation redox of Ru4+/Ru5+ and Ir4+/Ir5+, the contribution in the oxygen redox from x = 0.5 to 0.75 is larger in Na1-xRu0.5O1.5 than that in Na1-xIr0.5O1.5. Third, the charge variations indicate a dominant cation redox activity via Ir(5d)-O(2p) for x above 0.5 in Na1-xIr0.5O1.5. Its redox participation occurred with the oxygen redox, opposite to the behavior in Na1-xRu0.5O1.5. These three considerations imply that the chemical weakness of Ir(5d)-O(2p) leads to a more redox-active environment of Ir ions and reduces the oxygen redox activity, which triggers the nonhysteretic oxygen capacity during (de)intercalation. This provides a comprehensive guideline for design of reversible oxygen redox capacities in oxide cathodes for advanced A-ion batteries.
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A breakthrough utilizing an anionic redox reaction (O2-/On-) for charge compensation has led to the development of high-energy cathode materials in sodium-ion batteries. However, its reaction results in a large voltage hysteresis due to the structural degradation arising from an oxygen loss. Herein, an interesting P2-type Mn-based compound exhibits a distinct two-phase behavior preserving a high-potential anionic redox (≈4.2 V vs Na+/Na) even during the subsequent cycling. Through a systematic series of experimental characterizations and theoretical calculations, the anionic redox reaction originating from O 2p-electron and the reversible unmixing of Na-rich and Na-poor phases are confirmed in detail. In light of the combined study, a critical role of the anion-redox-induced two-phase reaction in the positive-negative point of view is demonstrated, suggesting a rational design principle considering the phase separation and lattice mismatch. Furthermore, these results provide an exciting approach for utilizing the high-voltage feature in Mn-based layered cathode materials that are charge-compensated by an anionic redox reaction.
RESUMEN
A new paradigm based on an anionic O2-/On- redox reaction has been highlighted in high-energy density cathode materials for sodium-ion batteries, achieving a high voltage (â¼4.2 V vs Na/Na+) with a large anionic capacity during the first charge process. The structural variations during (de)intercalation are closely correlated with stable cyclability. To determine the rational range of the anion-based redox reaction, the structural origins of Na1-xRu0.5O1.5 (0 ≤ x ≤ 1.0) were deduced from its vacancy (â¡)/Na atomic configurations, which trigger different interactions between the cations and anions. In the cation-based Ru4+/Ru5+ redox reaction, the â¡ solubility into fully sodiated Na2RuO3 predominantly depends on the crystallographic 4h site when 0.0 ≤ x ≤ 0.25, and the electrostatic repulsion of the linear O2--â¡-O2- configuration is accompanied by the increased volumetric strain. Further Na extraction (0.25 ≤ x ≤ 0.5) induces a compensation effect, leading to Na2/3[Naâ¡Ru2/3]O2 with the â¡ formation of 2b and 2c sites, which drastically reduce the volumetric strain. In the O2-/On- anionic redox region (0.5 ≤ x ≤ 0.75), Na removal at the 4h site generates a repulsive force in O2--â¡-O2- that increases the interlayer distance. Finally, in the 0.75 ≤ x ≤ 1.0 region, the anionic O charges are unprotected by repulsive forces, and their consumption causes severe volumetric strain in Na1-xRu0.5O1.5. Coupling our mechanistic understanding of the structural origin with the â¡- and Na-site preferences and the electrostatic interaction between lattice O and vacancies in Na1-xRu0.5O1.5, we determined the rational range of the anionic redox reaction in layered cathode materials for rechargeable battery research.
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Manganese-based spinel cathode materials for sodium-ion batteries (SIBs) are promising candidates for next-generation batteries; especially, Na[Ni0.5Mn1.5]O4 (NNMO) should get attention because of its relatively high operating voltage and firm octahedral host structure. Here, first-principles calculations and the phase field method are used to elucidate the reasons for the low performance of NNMO compared with Li[Ni0.5Mn1.5]O4, and we determine the requirements for realizing high-performance cathode materials for SIBs. Owing to the Ni2+/Ni4+ double redox, NNMO could operate at a high voltage; however, the large Na+ increases the local site energy of the redox center, promoting electron extraction from the redox center, leading to unexpected voltage loss. Additionally, the homogeneous free energy confirms that NNMO would undergo phase separation into fully intercalated and deintercalated phases, inducing lattice misfits along the interfaces of the two phases. Particularly, a higher phase transition barrier and large Na+ cause fast phase separation, inducing increased polarization and severe stress field upon cycling. The present analysis with comprehensive first-principles calculations and the phase field method provides three critical factors toward high electrochemical performance: (i) strengthening Ni-O bonding to avoid undesirable voltage loss, (ii) increasing the vacancy/Na solubility during (de)sodiation to enhance cyclability, and (iii) suppressing the structural distortion during (de)sodiation to prevent mechanical failure. Based on these crucial points, additionally, we suggest the M-pillared Na1-xMx[Ni0.5Mn1.5]O4 (monovalent or divalent species, M), where the M works to strengthen the redox center for improved energy density and to alleviate the drastic structural change and voltage hysteresis for better cyclability, would have superior electrochemical performance as a cathode material for SIBs.
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Redox reactions of oxygen have been considered critical in controlling the electrochemical properties of lithium-excessive layered-oxide electrodes. However, conventional electrode materials without overlithiation remain the most practical. Typically, cationic redox reactions are believed to dominate the electrochemical processes in conventional electrodes. Herein, we show unambiguous evidence of reversible anionic redox reactions in LiNi1/3 Co1/3 Mn1/3 O2 . The typical involvement of oxygen through hybridization with transition metals is discussed, as well as the intrinsic oxygen redox process at high potentials, which is 75 % reversible during initial cycling and 63 % retained after 10â cycles. Our results clarify the reaction mechanism at high potentials in conventional layered electrodes involving both cationic and anionic reactions and indicate the potential of utilizing reversible oxygen redox reactions in conventional layered oxides for high-capacity lithium-ion batteries.
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Recently, the substitution of inactive elements has been reported as a promising strategy for improving the structural stability and electrochemical performance of layered cathode materials for sodium-ion batteries (SIBs). In this regard, we investigated the positive effects of inactive Ti substitution into O3-type NaFe0.25Ni0.25Mn0.5O2 based on first-principles calculations and electrochemical experiments. After Ti substitution, Na[Ti0.03(Fe0.25Ni0.25Mn0.5)0.97]O2 exhibits improved capacity retention and rate capability compared with Ti-free NaFe0.25Ni0.25Mn0.5O2. Such an improvement is primarily attributed to the enhanced structural stability and lowered activation energy for Na+ migration, which is induced by Ti substitution in the host structure. Based on first-principles calculations of the average net charges and partial densities of states, we suggest that Ti substitution effectively enhances the binding between transition metals and oxygen by increasing the oxygen electron density, which in turn lowers the energy barrier of Na+ migration, leading to a notable enhancement in the rate capability of Na[Ti0.03(Fe0.25Ni0.25Mn0.5)0.97]O2. Compared with other inactive elements (e.g., Al and Mg), Ti is a more suitable substituent for improving the electrochemical properties of layered cathode materials because of its large total charge variation contributing to capacity. The results of this study provide practical guidelines for developing highly reliable layered cathode materials for SIBs.
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Manganese based layered oxides have received increasing attention as cathode materials for sodium ion batteries due to their high theoretical capacities and good sodium ion conductivities. However, the Jahn-Teller distortion arising from the manganese (III) centers destabilizes the host structure and deteriorates the cycling life. Herein, we report that zinc-doped Na0.833[Li0.25Mn0.75]O2 can not only suppress the Jahn-Teller effect but also reduce the inherent phase separations. The reduction of manganese (III) amount in the zinc-doped sample, as predicted by first-principles calculations, has been confirmed by its high binding energies and the reduced octahedral structural variations. In the viewpoint of thermodynamics, the zinc-doped sample has lower formation energy, more stable ground states, and fewer spinodal decomposition regions than those of the undoped sample, all of which make it charge or discharge without any phase transition. Hence, the zinc-doped sample shows superior cycling performance, demonstrating that zinc doping is an effective strategy for developing high-performance layered cathode materials.
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In an effort to develop high-energy-density cathodes for sodium-ion batteries (SIBs), low-cost, high capacity Na(Li1/3 Mn2/3 )O2 is discovered, which utilizes the labile O 2p-electron for charge compensation during the intercalation process, inspired by Li2 MnO3 redox reactions. Na(Li1/3 Mn2/3 )O2 is systematically designed by first-principles calculations considering the Li/Na mixing enthalpy based on the site preference of Na in the Li sites of Li2 MnO3 . Using the anionic redox reaction (O2- /O- ), this Mn-oxide is predicted to show high redox potentials (≈4.2 V vs Na/Na+ ) with high charge capacity (190 mAh g-1 ). Predicted cathode performance is validated by experimental synthesis, characterization, and cyclic performance studies. Through a fundamental understanding of the redox reaction mechanism in Li2 MnO3 , Na(Li1/3 Mn2/3 )O2 is designed as an example of a new class of promising cathode materials, Na(Li1/3 M2/3 )O2 (M: transition metals featuring stabilized M4+ ), for further advances in SIBs.
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A synergistic approach for advanced cathode materials is proposed. Sodium manganese oxide with a layered-tunnel hybrid structure was designed, synthesized, and subsequently investigated. The layered-tunnel hybrid structure provides fast Na ion diffusivity and high structural stability thanks to the tunnel phase, enabling high rate capability and greatly improved cycling stability compared to that of the pure P2 layered phase while retaining the high specific capacity of the P2 layered phase. The hybrid structure provided a decent discharge capacity of 133.4 mAh g-1 even at 8 C, which exceeds the reported best rate capability for Mn-based cathodes. It also displayed an impressive cycling stability, maintaining 83.3 mAh g-1 after 700 cycles at 10 C. Theoretical calculation and the potentiostatic intermittent titration technique (PITT) demonstrated that this hybrid structure helps enhance Na ion diffusivity during charge and discharge, attaining, as a result, an unprecendented electrochemical performance.
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A fundamental understanding of anomalous redox mechanisms in hexacyanometallate compounds, compared with conventional NaMO2 systems (M: transition metals), is presented based on first-principles calculations and experimental validations. From theoretical calculations, we identified low-spin and high-spin states of Fe ions coordinated by the cyanide group (-CN) with the same oxidation state (Fe2+) in Na2Fe2(CN)6. Considering the site dependency of d electronic spin configurations based on the crystal field theory (CFT) of transition metals (TMs), we calculated the thermodynamic mixing energy using Na2Fe2(CN)6 and Na2Mn2(CN)6 for obtaining a thermodynamically stable phase of Na2FeMn(CN)6. The phase stabilities of Na2Fe2-xMnx(CN)6 among many atomic configurations and lattice parameters originating from octahedral structures (i.e., Fe(CN)6 and Mn(NC)6) are highly dependent on the electronic structures of TMs with spin states. From partial density of states (PDOS) and spatial electron distributions, it was observed that Fe2+ in the low-spin state (t) and Mn2+ in the high-spin states (t and e) in the stable phase lead to higher redox potentials (â¼3.55 V vs. Na/Na+) with the removal of Na+ as compared to that of Na2Fe2(CN)6. In addition, lattice parameters from x = 0 to x = 1 in Na2Fe2-xMnx(CN)6 are increased due to the larger ionic radius of Mn2+ in the high-spin states. On the other hand, Fe2+ in the high-spin states (t and e) and Mn2+ in the low-spin state (t) in the most unstable phase of Na2FeMn(CN)6 would have lower redox potentials. Based on the fundamental correlation between redox potentials and CFT with spin configurations of TMs, we suggest a material design concept for intercalation compounds with higher energy densities for rechargeable battery systems.
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Ni-rich LiNi0.8Co0.1Mn0.1O2 layered oxide cathodes have been highlighted for large-scale energy applications due to their high energy density. Although its specific capacity is enhanced at higher voltages as Ni ratio increases, its structural degradation due to phase transformations and lattice distortions during cycling becomes severe. For these reasons, we focused on the origins of crack generation from phase transformations and structural distortions in Ni-rich LiNi0.8Co0.1Mn0.1O2 using multiscale approaches, from first-principles to meso-scale phase-field model. Atomic-scale structure analysis demonstrated that opposite changes in the lattice parameters are observed until the inverse Li content x = 0.75; then, structure collapses due to complete extraction of Li from between transition metal layers. Combined-phase investigations represent the highest phase barrier and steepest chemical potential after x = 0.75, leading to phase transformations to highly Li-deficient phases with an inactive character. Abrupt phase transformations with heterogeneous structural collapse after x = 0.81 (~220 mAh g-1) were identified in the nanodomain. Further, meso-scale strain distributions show around 5% of anisotropic contraction with lower critical energy release rates, which cause not only micro-crack generations of secondary particles on the interfaces between the contracted primary particles, but also mechanical instability of primary particles from heterogeneous strain changes.
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In lithium-ion batteries (LIBs) comprising spinel cathode materials, the dissolution of transition metals (TMs) in the cathodes causes severe cyclic degradation. We investigate the origin and mechanism of surface TM dissolution in high-voltage spinel oxide (LiNi0.5 Mn1.5 O4 ) nanoparticles to find a practical method for its mitigation. Atomic structures of the LiNi0.5 Mn1.5 O4 surfaces are developed, and the electronic structures are investigated by first-principles calculations. The results indicate that titanium is a promising dopant for forming a more stable surface structure by reinforcing metal-oxygen bonds in LiNi0.5 Mn1.5 O4 . Experimentally synthesized LiNi0.5 Mn1.5 O4 with titanium surface doping exhibits improved electrochemical performance by suppressing undesirable TM dissolution during cycles. The theoretical prediction and experimental validation presented here suggest a viable method to suppress TM dissolution in LiNi0.5 Mn1.5 O4 .
Asunto(s)
Nanopartículas del Metal , Elementos de Transición/química , Microscopía Electrónica de Transmisión , Tamaño de la Partícula , Solubilidad , Espectrometría por Rayos X , Propiedades de Superficie , Difracción de Rayos XRESUMEN
A combined study involving experiments and multiscale computational approaches is conducted to propose a theoretical solution for the suppression of the Jahn-Teller distortion which causes severe cyclic degradation. As-synthesized pristine and Al-doped Mn spinel compounds are the focus to understand the mechanism of the cyclic degradation in terms of the Jahn-Teller distortion, and the electrochemical performance of the Al-doped sample shows enhanced cyclic performance compared with that of the pristine one. Considering the electronic structures of the two systems using first-principles calculations, the pristine spinel suffers entirely from the Jahn-Teller distortion by Mn(3+), indicating an anisotropic electronic structure, but the Al-doped spinel exhibits an isotropic electronic structure, which means the suppressed Jahn-Teller distortion. A multiscale phase field model in nanodomain shows that the phase separation of the pristine spinel occurs to inactive Li0Mn2O4 (i.e., fully delithiated) gradually during cycles. In contrast, the Al-doped spinel does not show phase separation to an inactive phase. This explains why the Al-doped spinel maintains the capacity of the first charge during the subsequent cycles. On the basis of the mechanistic understanding of the origins and mechanism of the suppression of the Jahn-Teller distortion, fundamental insight for making tremendous cuts in the cyclic degradation could be provided for the Li-Mn-O compounds of Li-ion batteries.