“…Even so, comparing the R elec at the lithiated state to that of the delithiated state, the lower values obtained at 5.0 V suggested that the LNMO becomes less electronically insulator by extracting Li + ‐ion. This is related to the fact that the conducting domains become rapidly interconnected [45,47,51,52] . The mentioned phase transitions of LNMO_0 % N 2 seem to be suppressed by nitrogen doping, as suggested the R elec , (Figure 10b).…”
Section: Resultsmentioning
confidence: 76%
“…This is related to the fact that the conducting domains become rapidly interconnected. [45,47,51,52] The mentioned phase transitions of LNMO_0 % N 2 seem to be suppressed by nitrogen doping, as suggested the R elec , (Figure 10b). This is due to the fact that the ChemElectroChem diffusion of Li + -ion enhances the stability of the charge transfer interfaces via decreasing lattice mismatch and structural stress upon the charge and discharge.…”
Section: Electrochemical Investigationmentioning
confidence: 65%
“…The selected sequences of Nyquist plots corresponding to the relevant potentials for the LNMO_0 % N 2 are shown in Figure 8, while Nyquist plots for the LNMO_50 % N 2 are illustrated in Figure 9. The Nyquist plots present the typical features of cathode electrodes for LIBs [45–48] . It can be observed at a glance that the LNMO_50 % N 2 shows one order of magnitude lower overall resistance values compared to that of the LNMO_0 % N 2 .…”
Section: Resultsmentioning
confidence: 92%
“…The Nyquist plots present the typical features of cathode electrodes for LIBs. [45][46][47][48] It can be observed at a glance that the LNMO_50 % N 2 shows one order of magnitude lower overall resistance values compared to that of ChemElectroChem the LNMO_0 % N 2 . However, both cells show a similar trend during operation.…”
Delivering a commercial high‐voltage spinel LiNi0.5Mn1.5O4 (LNMO) cathode electrode for Li‐ion batteries would result in a significant step forward in terms of energy density. However, the structural ordering of the spinel and particle size have considerable effects on the cathode material's cyclability and rate capability, which are crucial challenges to address. Here, a novel mid‐frequency alternating current dual magnetron sputtering method was presented, using different Ar‐N2 gas mixtures ratios for the process gas to prepare various LNMO thin films with highly controlled morphology and particle size; as determined from X‐ray diffraction, Raman spectroscopy and electron microscopy. It resulted in enhanced cycling and rate performance. This processing method delivered N‐containing LNMO thin film electrodes with up to 15 % increased discharge capacity at 1 C (120 mAh g−1) with respect to standard LNMO (grown under only Ar gas flow) thin film electrodes, along with outstanding rate performance up to 10 C (99 mAh g−1) in the operating voltage window 3.5–4.85 V vs. Li+/Li. Besides, electrochemical impedance spectroscopy results showed that the intricate phase transitions present in standard LNMO electrodes were almost suppressed in N‐containing LNMO thin films grown under different Ar‐N2 gas flow mixtures.
“…Even so, comparing the R elec at the lithiated state to that of the delithiated state, the lower values obtained at 5.0 V suggested that the LNMO becomes less electronically insulator by extracting Li + ‐ion. This is related to the fact that the conducting domains become rapidly interconnected [45,47,51,52] . The mentioned phase transitions of LNMO_0 % N 2 seem to be suppressed by nitrogen doping, as suggested the R elec , (Figure 10b).…”
Section: Resultsmentioning
confidence: 76%
“…This is related to the fact that the conducting domains become rapidly interconnected. [45,47,51,52] The mentioned phase transitions of LNMO_0 % N 2 seem to be suppressed by nitrogen doping, as suggested the R elec , (Figure 10b). This is due to the fact that the ChemElectroChem diffusion of Li + -ion enhances the stability of the charge transfer interfaces via decreasing lattice mismatch and structural stress upon the charge and discharge.…”
Section: Electrochemical Investigationmentioning
confidence: 65%
“…The selected sequences of Nyquist plots corresponding to the relevant potentials for the LNMO_0 % N 2 are shown in Figure 8, while Nyquist plots for the LNMO_50 % N 2 are illustrated in Figure 9. The Nyquist plots present the typical features of cathode electrodes for LIBs [45–48] . It can be observed at a glance that the LNMO_50 % N 2 shows one order of magnitude lower overall resistance values compared to that of the LNMO_0 % N 2 .…”
Section: Resultsmentioning
confidence: 92%
“…The Nyquist plots present the typical features of cathode electrodes for LIBs. [45][46][47][48] It can be observed at a glance that the LNMO_50 % N 2 shows one order of magnitude lower overall resistance values compared to that of ChemElectroChem the LNMO_0 % N 2 . However, both cells show a similar trend during operation.…”
Delivering a commercial high‐voltage spinel LiNi0.5Mn1.5O4 (LNMO) cathode electrode for Li‐ion batteries would result in a significant step forward in terms of energy density. However, the structural ordering of the spinel and particle size have considerable effects on the cathode material's cyclability and rate capability, which are crucial challenges to address. Here, a novel mid‐frequency alternating current dual magnetron sputtering method was presented, using different Ar‐N2 gas mixtures ratios for the process gas to prepare various LNMO thin films with highly controlled morphology and particle size; as determined from X‐ray diffraction, Raman spectroscopy and electron microscopy. It resulted in enhanced cycling and rate performance. This processing method delivered N‐containing LNMO thin film electrodes with up to 15 % increased discharge capacity at 1 C (120 mAh g−1) with respect to standard LNMO (grown under only Ar gas flow) thin film electrodes, along with outstanding rate performance up to 10 C (99 mAh g−1) in the operating voltage window 3.5–4.85 V vs. Li+/Li. Besides, electrochemical impedance spectroscopy results showed that the intricate phase transitions present in standard LNMO electrodes were almost suppressed in N‐containing LNMO thin films grown under different Ar‐N2 gas flow mixtures.
“…Bare and modified cathode powders, labeled as b-LNMO and m-LNMO, respectively, were synthesized by a common synthetic route, corresponding to the citric acid sol–gel method. , For m-LNMO, lithium acetate [Li(CH 3 COO)·2H 2 O], nickel acetate [Ni(CH 3 COO) 2 ·4H 2 O], and manganese acetate [Mn(CH 3 COO) 2 ·4H 2 O], with the addition of magnesium acetate tetrahydrate [Mg(CH 3 COO) 2 ·4H 2 O] and zirconium(IV) acetate hydroxide [Zr(OH) y ·(CH 3 COO) x , x + y ∼ 4] for the modified powder, were dissolved in distilled water in stoichiometric amounts corresponding to the expected composition “LiNi 0.5 Mn 1.47 Mg 0.025 Zr 0.025 O 4 ”. A slight overall (Ni + Mn + dopants) over-stoichiometry was introduced, in order to possibly foster the formation of a Zr oxide coating phase, as previously observed for layered cathodes. , Citric acid (CA), as a chelating agent, was then added to the solution, with a molar ratio of CA/total metal cations of 1:1 (all materials from Sigma–Aldrich, purity ≥ 99%).…”
There is an enormous
drive for moving toward cathode material research
in LIBs due to the proposal of zero-emission electric vehicles together
with the restriction of cathode materials in design. LiNi
0.5
Mn
1.5
O
4
(LNMO) attracts great research interests
as high-voltage Co-free cathodes in LIBs. However, a more extensive
study is required for LNMO due to its poor electrochemical performance,
especially at high temperature, because of the instability of the
LNMO interface. Herein, we design structural modifications using Mg
and Zr to alleviate the above-mentioned drawbacks by limiting Mn dissolution
and tailoring interstitial sites (which are shown by structural and
electrochemical characterizations). This strategy enhances the cycle
life up to 1000 cycles at both 25 and 50 °C. In addition, a thorough
characterization by impedance spectroscopy is applied to give an insight
into the electronic and ionic transport properties and the intricate
phase transitions occurring upon oxidation and reduction.
With the increasing demand for low-cost and environmentally friendly energy, the application of rechargeable lithium-ion batteries (LIBs) as reliable energy storage devices in electric cars, portable electronic devices and space satellites is on the rise. Therefore, extensive and continuous research on new materials and fabrication methods is required to achieve the desired enhancement in their electrochemical performance. Battery active components, including the cathode, anode, electrolyte, and separator, play an important role in LIB functionality. The major problem of LIBs is the degradation of the electrolyte and electrode materials and their components during the charge‒discharge process. Atomic layer deposition (ALD) is considered a promising coating technology to deposit uniform, ultrathin films at the atomic level with controllable thickness and composition. Various metal films can be deposited on the surface of active electrodes and solid electrolyte materials to tailor and generate a protective layer at the electrode interface. In addition, synthesis of microbatteries and novel nanocomplexes of the cathode, anode, and solid-state electrolyte to enhance the battery performance can all be attained by ALD. Therefore, the ALD technique has great potential to revolutionize the future of the battery industry. This review article provides a comprehensive foundation of the current state of ALD in synthesizing and developing LIB active components. Additionally, new trends and future expectations for the further development of next-generation LIBs via ALD are reported.
Graphical Abstract
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