Significant Capacity and Cycle‐Life Improvement of Lithium‐Ion Batteries through Ultrathin Conductive Film Stabilized Cathode Particles

Patel, Rajankumar L.; Xie, Hui; Park, Jong‐Hyun; Asl, Hooman Yaghoobnejad; Choudhury, Amitava; Liu, Xinhua

doi:10.1002/admi.201500046

Cited by 38 publications

(47 citation statements)

References 47 publications

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“…In our recent study, we employed the use of optimally thick CeO 2 film prepared by ALD on LiMn 2 O 4 particles, which showed a 24% increase in initial capacity and 95% capacity retention, when tested at a 1C rate for 1,000 cycles at room temperature. 30 In addition to that, the conductive effects of CeO 2 ALD films were studied and compared with uncoated substrates and insulating coating materials. 31 We found that the ceria ALD coated material showed much improved ionic and electronic conductivities, as compared to the Al 2 O 3 and ZrO 2 ALD coated LiMn 2 O 4 samples.…”

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confidence: 99%

Ultrathin Conductive CeO₂Coating for Significant Improvement in Electrochemical Performance of LiMn_1.5Ni_0.5O₄Cathode Materials

Patel

Palaparty

Liu

2016

J. Electrochem. Soc.

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LiMn 1.5 Ni 0.5 O 4 (LMNO) has a huge potential for use as a cathode material in electric vehicular applications. However, it could face discharge capacity degradation with cycling at elevated temperatures due to attacks by hydrofluoric acid (HF) from the electrolyte, which could cause cationic dissolution. To overcome this barrier, we coated 3-5 micron sized LMNO particles with a ∼3 nm optimally thick and conductive CeO 2 film prepared by atomic layer deposition (ALD). This provided optimal thickness for mass transfer resistance, species protection, and mitigation of cationic dissolution at elevated temperatures. After 1,000 cycles of chargedischarge between 3.5 V-5 V (vs. Li + /Li) at 55 • C, the optimally coated sample, 50Ce (50 cycles of CeO 2 ALD coated) had a capacity retention of ∼97.4%, when tested at a 1C rate, and a capacity retention of ∼83% at a 2C rate. This was compared to uncoated LMNO particles that had a capacity retention of only ∼82.7% at a 1C rate, and a capacity retention of ∼40.8% at a 2C rate. Lithium ion batteries have emerged as potential candidates for replacement of Ni-Cd batteries in electric vehicles because of their high intrinsic energy densities combined with their ease of portability. This potential creates a need for the development of new or modified cathode and anode materials that possess high energy density, long cycle life, excellent capacity retention, and a large voltage window for operation. For electric vehicles, in particular, the upper voltage cutoff window on the cathode side should be ∼5 V vs. Li + /Li. Lithium manganese nickel oxide LiMn 1.5 Ni 0.5 O 4 (LMNO) has emerged in the research community as a potential cathode material for use in electric vehicles due to its large theoretical capacity of ∼148 mAhg −1 , a high working voltage of ∼4.7 V vs. Li + /Li, and a high energy density. 1,2However, LMNO suffers from high capacity fade during performance at elevated temperatures because Mn dissolves due to generation of hydrofluoric acid (HF) in the electrolyte. 3-5The coating of surface protective layers on pristine LMNO particles has been extensively studied in literature. [6][7][8][9][10][11][12][13][14][15][16][17][18][19][20] These layers provide a shield from the HF, and prevent rapid capacity fade, leading to improved cycling performance and capacity retention. Of the different surface coating techniques, atomic layer deposition (ALD) has inherent advantages that provide conformal, pin-hole free, size-tunable ultrathin films 21 and, thus, provide high capacity retention and a long life cycle. The ALD process involves a sequence of self-limiting reactions that result in a coating of one monolayer at a time. This enables size tunability at the sub-nanometer level and promotes conformity in the films. Materials like Al 2 O 3 , 17 MgF 2 , 22 TiO 2 , 18 and LiAlO 2 10 have been studied as coating materials prepared by ALD on LMNO. Even though, these materials have provided effective mitigation of cationic dissolution, the ionic conductivity of such protective layers ...

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Ultrathin Conductive CeO₂Coating for Significant Improvement in Electrochemical Performance of LiMn_1.5Ni_0.5O₄Cathode Materials

Patel

Palaparty

Liu

2016

J. Electrochem. Soc.

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“…ALD ensures control of film thickness at nanometer level. However, if the ALD film is insulating, such trade-off still exists14, which has also been demonstrated in our recent work and an effective solution was proposed17. It has been demonstrated that coating an optimal thickness of conductive metal oxide films could improve both specific capacity and cycling performance.…”

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confidence: 51%

“…As learned from our previous work17, the drawback of coating on particles is slower species transport. Consequently, a demonstration of performance improvement via ALD coatings at a high C rate is significant because the diffusivity of ions in the solid phase becomes significant as the input current increases.…”

Section: Resultsmentioning

confidence: 83%

“…6c). The details about the fitted parameters are explained elsewhere17. Among the fitted parameters, ohmic resistance (R ohm ), charge-transfer resistance (R ct ), and surface film resistance (R f ) can be used to quantify the polarization behaviors.…”

Section: Resultsmentioning

confidence: 99%

“…It has been demonstrated that coating an optimal thickness of conductive metal oxide films could improve both specific capacity and cycling performance. In our recent work17, ultrathin 3 nm ALD CeO 2 film was coated on LiMn 2 O 4 particles that showed 24% improvement in specific capacity, compared to the uncoated one, and high capacity retention of 96% at room temperature and 95% at an elevated temperature of 55 °C even after 1,000 cycles at a 1C rate. Herein, we propose that iron oxide would be an excellent candidate as the coating layer due to its electrochemical activity, low cost, environmental benignity, and natural abundance.…”

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Employing Synergetic Effect of Doping and Thin Film Coating to Boost the Performance of Lithium-Ion Battery Cathode Particles

Patel

Jiang

Choudhury

et al. 2016

Sci Rep

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Atomic layer deposition (ALD) has evolved as an important technique to coat conformal protective thin films on cathode and anode particles of lithium ion batteries to enhance their electrochemical performance. Coating a conformal, conductive and optimal ultrathin film on cathode particles has significantly increased the capacity retention and cycle life as demonstrated in our previous work. In this work, we have unearthed the synergetic effect of electrochemically active iron oxide films coating and partial doping of iron on LiMn1.5Ni0.5O4 (LMNO) particles. The ionic Fe penetrates into the lattice structure of LMNO during the ALD process. After the structural defects were saturated, the iron started participating in formation of ultrathin oxide films on LMNO particle surface. Owing to the conductive nature of iron oxide films, with an optimal film thickness of ~0.6 nm, the initial capacity improved by ~25% at room temperature and by ~26% at an elevated temperature of 55 °C at a 1C cycling rate. The synergy of doping of LMNO with iron combined with the conductive and protective nature of the optimal iron oxide film led to a high capacity retention (~93% at room temperature and ~91% at 55 °C) even after 1,000 cycles at a 1C cycling rate.

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Atomic Layer Deposition for Lithium‐Based Batteries

Nuwayhid

et al. 2016

Adv Materials Inter

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With the increasing demand for energy at a low cost and minimal environmental impact, the development of next‐generation high‐performance batteries has drawn considerable attention. Owing to the capability of forming conformal coatings of thin films and nanoparticles, atomic layer deposition (ALD) has shown great potential in deposition and surface modification of electrode materials with various nanostructures, deposition of solid‐state electrolyte, and fabrication of electrochemical catalysts. This paper reviews the recent development and applications of ALD in Li‐based batteries, especially beyond Li‐ion systems, and provides suggestions for further development of ALD techniques for these batteries.

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Significant Capacity and Cycle‐Life Improvement of Lithium‐Ion Batteries through Ultrathin Conductive Film Stabilized Cathode Particles

Cited by 38 publications

References 47 publications

Ultrathin Conductive CeO₂Coating for Significant Improvement in Electrochemical Performance of LiMn_1.5Ni_0.5O₄Cathode Materials

Ultrathin Conductive CeO₂Coating for Significant Improvement in Electrochemical Performance of LiMn_1.5Ni_0.5O₄Cathode Materials

Employing Synergetic Effect of Doping and Thin Film Coating to Boost the Performance of Lithium-Ion Battery Cathode Particles

Atomic Layer Deposition for Lithium‐Based Batteries

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Significant Capacity and Cycle‐Life Improvement of Lithium‐Ion Batteries through Ultrathin Conductive Film Stabilized Cathode Particles

Cited by 38 publications

References 47 publications

Ultrathin Conductive CeO2Coating for Significant Improvement in Electrochemical Performance of LiMn1.5Ni0.5O4Cathode Materials

Ultrathin Conductive CeO2Coating for Significant Improvement in Electrochemical Performance of LiMn1.5Ni0.5O4Cathode Materials

Employing Synergetic Effect of Doping and Thin Film Coating to Boost the Performance of Lithium-Ion Battery Cathode Particles

Atomic Layer Deposition for Lithium‐Based Batteries

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Ultrathin Conductive CeO₂Coating for Significant Improvement in Electrochemical Performance of LiMn_1.5Ni_0.5O₄Cathode Materials

Ultrathin Conductive CeO₂Coating for Significant Improvement in Electrochemical Performance of LiMn_1.5Ni_0.5O₄Cathode Materials