Synergistic regulation of kinetic reaction pathway and surface structure degradation in single-crystal high-nickel cathodes

Shen, Jixue; Bao, Zhenan; He, Xinyou; Xiao, Biaobiao; Xiao, Zhiming; Xiao, Li

doi:10.1016/j.jcis.2022.08.184

Cited by 23 publications

(6 citation statements)

References 47 publications

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“…The measured lattice spacing is 0.477 nm, which is assigned to the (003) plane of the SC83. 39,40 The amorphous B 2 O 3 coatings with the thickness of 1.4 nm are observed on the surface of the SC83 particles, which agrees with the calculated thickness derived from the ICP-OES results. B is detected at the surface of the 6B SC83 particles, while the atomic concentration of B in the bulk of the 6B SC83 particles is much lower, which further validates the existence of B 2 O 3 coatings (Fig.…”

Section: Resultssupporting

confidence: 86%

“…The surface morphology of the 6B SC83 particles is shown in Figure 2b using high-resolution TEM (HR-TEM). The measured lattice spacing is 0.477 nm, which is assigned to the (003) plane of the SC83 39,40 . The amorphous B 2 O 3 coatings with the thickness of 1.4 nm are observed on the surface of the SC83 particles, which agrees with the calculated thickness derived from the ICP-OES results.…”

Section: Resultsmentioning

confidence: 94%

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Stabilization of the surface and lattice structure for LiNi_0.83Co_0.12Mn_0.05O₂via B₂O₃ atomic layer deposition and post-annealing

Li,

Xiang,

et al. 2024

Energy Adv.

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Section: Resultssupporting

confidence: 86%

Section: Resultsmentioning

confidence: 94%

Stabilization of the surface and lattice structure for LiNi_0.83Co_0.12Mn_0.05O₂via B₂O₃ atomic layer deposition and post-annealing

Li,

Xiang,

et al. 2024

Energy Adv.

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“…As displayed in Figure a, the secondary spherical SNCM particles have been completely broken, which is caused by the unavoidable anisotropic stress changes during long‐term cycling processes. [ 37 ] The intergranular cracks provide the path for electrolyte penetration, exacerbating the degree of parasite reactions. Thus, these SNCM broken particle shows a rough surface, which may be related to the residue of electrolyte derivatives (Figure S3a, Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

Strong Oxidizing Molten Salts for Strengthening Structural Restoration Enabling Direct Regeneration of Spent Layered Cathode

Xiao,

Yang,

et al. 2024

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As a mainstream technology for recycling spent lithium‐ion batteries, direct regeneration is rapidly developed due to its high efficiency and green characteristics. However, efficient reuse of spent LiNixCoyMn1‐x‐yO2 cathode is still a significant challenge, as the rock salt/spinel phase on the surface hinders the Li replenishment and phase transformation to the layered structure. In this work, the fundamental understanding of the repair mechanism is confirmed that the oxidizing atmosphere is the crucial factor that can greatly improve the rate and degree of phase restoration. Particularly, a ternary‐component molten salt system (LiOH‐Li2CO3‐LiNO3) is proposed for direct regeneration of LiNi0.5Co0.2Mn0.3O2 (NCM523), which can in situ generate the strong oxidizing intermediate of superoxide radicals. Additionally, it shows a liquid‐like reaction environment at a lower temperature to acceclerate the transport rate of superoxide‐ions. Therefore, the synergistic effect of LiOH‐Li2CO3‐LiNO3 system can strengthen the full restoration of rock salt/spinel phases and achieve the complete Li‐supplement. As anticipated, the regenerated NCM523 delivers a high cycling stability with a retention of 91.7% after 100 cycles, which is even competitive with the commercial NCM523. This strategy provides a facile approach for the complete recovery of layer structure cathode, demonstrating a unique perspective for the direct regeneration of spent lithium‐ion batteries.

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“…Based on the complementary advantages of bulk doping and surface modification, some dual-modification strategy were proposed. It has been reported that Mg 2+ doping and surface poly pyrrole (PPy) coating, Ti 4+ doping and TiNb 2 O 7 coating, Nb 5+ near-surface doping and Li 5 La 3 Nb 2 O 12 coating, Zr 4+ doping and LiBO 3 /B 2 O 3 coating, and Zr 4+ doping and La 2 Zr 2 O 7 nanoshell − all play a synergistic role in improving both the structural and interfacial stability. Unfortunately, the present dual-modification strategies have the common problem of complicated multistep reaction routes in the experimental synthesis process .…”

Section: Introductionmentioning

confidence: 99%

Simple Synchronous Dual-Modification Strategy with Zr⁴⁺ Doping and CeO₂ Nanowelding to Stabilize Layered Ni-Rich Cathode Materials

Liu

Yin

Zheng

et al. 2023

ACS Appl. Energy Mater.

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A Ni-rich layered oxide, one promising cathode for lithium-ion batteries (LIBs), exhibits the advantages of low cost and high capacity but suffers from rapid capacity loss due to bulk structural instability and surface side reactions. Herein, a simple synchronous dual-modification strategy with Zr4+ doping and CeO2 nanowelding is proposed to address such issues. Utilizing the migration energy difference of Zr and Ce ions in layered structures, one-step high-temperature sintering of LiNi0.8Co0.1Mn0.1O2 particles with Zr and Ce nitrate distributions enables simultaneous doping of Zr ions in the bulk and CeO2 surface modification. Therein, Zr ions in the bulk occupying the Li sites can improve the Li+ diffusion rate and stabilize the crystal structure, while CeO2 on the surface provides nanowelding between the grain boundaries and resistance to electrolyte erosion. Theoretical calculations and a series of structure/composition characterizations (i.e., neutron scattering, in situ X-ray diffraction, etc.) validated the proposed strategy and its role in stabilizing the Ni-rich cathodes. The synergistic effect of Zr4+ doping and CeO2 nanowelding enables an impressive initial capacity of 187.2 mAh g–1 (2.7–4.3 V vs Li/Li+) with 86.1% retention after 200 cycles at 1 C and rate capabilities of 146.6 and 127.3 mAh g–1 at 5 and 10 C, respectively. Upon increasing the testing temperature to 60 °C, the dual-modified Ni-rich cathode exhibits an initial discharge capacity of 203.5 mAh g–1 with a good retention of 80.8% after 100 cycles at 0.5 C. The present strategy utilizing the migration energy difference of metal ions to achieve synchronous bulk doping and surface modification will offer fresh insights to stabilize layered cathode materials for LIBs, which can be widely used in other kinds of batteries with various cathode materials.

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Synergistic regulation of kinetic reaction pathway and surface structure degradation in single-crystal high-nickel cathodes

Cited by 23 publications

References 47 publications

Stabilization of the surface and lattice structure for LiNi_0.83Co_0.12Mn_0.05O₂via B₂O₃ atomic layer deposition and post-annealing

Stabilization of the surface and lattice structure for LiNi_0.83Co_0.12Mn_0.05O₂via B₂O₃ atomic layer deposition and post-annealing

Strong Oxidizing Molten Salts for Strengthening Structural Restoration Enabling Direct Regeneration of Spent Layered Cathode

Simple Synchronous Dual-Modification Strategy with Zr⁴⁺ Doping and CeO₂ Nanowelding to Stabilize Layered Ni-Rich Cathode Materials

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Synergistic regulation of kinetic reaction pathway and surface structure degradation in single-crystal high-nickel cathodes

Cited by 23 publications

References 47 publications

Stabilization of the surface and lattice structure for LiNi0.83Co0.12Mn0.05O2via B2O3 atomic layer deposition and post-annealing

Stabilization of the surface and lattice structure for LiNi0.83Co0.12Mn0.05O2via B2O3 atomic layer deposition and post-annealing

Strong Oxidizing Molten Salts for Strengthening Structural Restoration Enabling Direct Regeneration of Spent Layered Cathode

Simple Synchronous Dual-Modification Strategy with Zr4+ Doping and CeO2 Nanowelding to Stabilize Layered Ni-Rich Cathode Materials

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Product

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Stabilization of the surface and lattice structure for LiNi_0.83Co_0.12Mn_0.05O₂via B₂O₃ atomic layer deposition and post-annealing

Stabilization of the surface and lattice structure for LiNi_0.83Co_0.12Mn_0.05O₂via B₂O₃ atomic layer deposition and post-annealing

Simple Synchronous Dual-Modification Strategy with Zr⁴⁺ Doping and CeO₂ Nanowelding to Stabilize Layered Ni-Rich Cathode Materials