A novel boron-doping approach for long-term cycling life of Li-rich layered cathode

Ren, Zhimin; Li, Guohua; Bai, Xiangtao; Hu, Wei; Li, Xiaoyan; He, Haocheng; Chang, Zenghua; Liu, Yang; Wang, Zhenyao; Liang, Zhanshuo; Guo, Lihao; Gao, Zhao; Wang, Jiantao

doi:10.1016/j.electacta.2023.142630

Cited by 5 publications

(4 citation statements)

References 44 publications

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“…Initially, cell parameter c increases and then decreases, indicating that, with increasing B content, some B occupies octahedral interstices in the TM layer sites, resulting in a reduction in cell parameter c due to the smaller radius of B in contrast to the TM. This finding, along with previous studies, strongly suggests that B doping occurs between both the tetrahedral interstitial of the packed O in the TM layer and Li layer site and the octahedral interstice in the TM layer sites . Similarly, the negative shift of the crystal plane (003) (Figure k) of the modified material in contrast to LLO indicates intentional doping of the bulk material with F and Na, as further supported by the increase in cell parameters a and c , as shown in Table .…”

Section: Resultssupporting

confidence: 84%

“…This finding, along with previous studies, 22 strongly suggests that B doping occurs between both the tetrahedral interstitial of the packed O in the TM layer and Li layer site and the octahedral interstice in the TM layer sites. 19 Similarly, the negative shift of the crystal plane (003) (Figure 1k) of the modified material in contrast to LLO indicates intentional doping of the bulk material with F and Na, 23 as further supported by the increase in cell parameters a and c, as shown in Table 1. Furthermore, Table 1 reveals a higher degree of Li + /Ni 2+ mixing in 2-BNF-LLO and 3-BNF-LLO in contrast to LLO, which could be attributed to the entry of Ni 2+ into Li vacancies created during the sintering process, resulting in the observed difference in Li + /Ni 2+ mixing.…”

Section: Resultsmentioning

confidence: 67%

“…To investigate the impact of NaBF 4 treatment on the crystal structure of LLO, X-ray diffraction (XRD) analysis was carried out on untreated LLO and NaBF 4 -treated samples (1-BNF-LLO, 2-BNF-LLO, and 3-BNF-LLO). The results, shown in Figure S3a, show peaks corresponding to the typical α-NaFeO 2 structure (space group: R 3̅ m ) . Additionally, a weaker peak in the 20–23° range is attributed to the monoclinic stage Li 2 MnO 3 (space group: C 2/ m ) .…”

Section: Resultsmentioning

confidence: 97%

“…The results, shown in Figure S3a, show peaks corresponding to the typical α-NaFeO 2 structure (space group: R3̅ m). 19 Additionally, a weaker peak in the 20−23°range is attributed to the monoclinic stage Li 2 MnO 3 (space group: C2/m). 20 Interestingly, the splitting of the (006)/(012) and (018)/(110) peaks indicates that NaBF 4 treatment preserved the material's bulk structure, maintaining its distinct layered attributes.…”

Section: Resultsmentioning

confidence: 99%

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In Situ Surface Reaction for the Preparation of High-Performance Li-Rich Mn-Based Cathode Materials with Integrated Surface Functionalization

Su,

Guo,

Xie

et al. 2024

ACS Appl. Mater. Interfaces

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Li-rich Mn-based cathode materials (LLOs) are often faced with problems such as low initial Coulombic efficiency (ICE), limited rate performance, voltage decay, and structural instability. Addressing these problems with a single approach is challenging. To overcome these limitations, we developed an LLO with surface functionalization using a simple fabrication method. This two-step process involved a liquid-stage NaBF 4 treatment followed by an in situ chemical reaction during sintering. This reaction led to the creation of oxygen vacancies (O V ), spinel structures, and doping with Na at the Li site, B at the tetrahedral interstitial spaces of O in both the transition-metal (TM) layer and Li layers as well as the octahedral interstices in the TM layer, and F at the O site. We have carried out a thorough study and employed density functional theory calculations to reveal the hidden mechanisms. The treatment not only increases the electrical conductivity but also changes the oxygen charge environment and inhibits lattice oxygen activity. Surprisingly, the B−O bond is so strong that it prevents the migration of TM within the tetrahedral interstitial spaces of O in both the TM and Li layers, hence stabilizing its structure. This bonding interaction strengthens the transition of the TM 3d and O 2p states to lower energy levels, thus causing an increase in the redox potentials. Hence, a rise in the operating voltage occurs. Of special importance, this therapy dramatically increases the ICE to 90.29% and keeps a specified capacity of 203.3 mAh/g after 100 cycles at 1C, which is an excellent capacity retention of 89.94%. This study introduces ideas and methods to tackle the challenges associated with LLOs in batteries. It also provides compelling evidence for the development of high-energy-density Li-ion batteries.

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Section: Resultssupporting

confidence: 84%

Section: Resultsmentioning

confidence: 67%

Section: Resultsmentioning

confidence: 97%

Section: Resultsmentioning

confidence: 99%

See 2 more Smart Citations

In Situ Surface Reaction for the Preparation of High-Performance Li-Rich Mn-Based Cathode Materials with Integrated Surface Functionalization

Su,

Guo,

Xie

et al. 2024

ACS Appl. Mater. Interfaces

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Modification of Lithium‐Rich Manganese Oxide Materials: Coating, Doping and Single Crystallization

Li,

Zhang,

Liang

et al. 2024

Batteries & Supercaps

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The increasing demand for portable electronics, electric vehicles and energy storage devices has spurred enormous research efforts to develop high‐energy‐density advanced lithium‐ion batteries (LIBs). Lithium‐rich manganese oxide (LRMO) is considered as one of the most promising cathode materials because of its high specific discharge capacity (>250 mAh g⁻¹), low cost, and environmental friendliness, all of which are expected to propel the commercialization of lithium‐ion batteries. However, practical applications of LRMO are still limited by low coulombic efficiency, significant capacity and voltage decay, slow reaction kinetics, and poor rate performance. This review focus on recent advancements in the modification methods of LRMO materials, systematically summarizing surface coating with different physical properties (e.g., oxides, metal phosphates, metal fluorides, carbon, conductive polymers, lithium compound coatings, etc.), ion doping with different doping sites (Li sites, TM sites, O sites, etc.), and single crystal structures. Finally, the current states and issues, key challenges of the modification of LRMO are discussed, and the perspectives on the future development trend base on the viewpoint of the commercialization of LRMO are also provided.

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The mechanism of the impact of Li2MnO3 with dual-edged sword functionality on the cyclic performance of lithium-rich manganese-based cathode materials

Su,

Guo,

Xie

et al. 2025

Journal of Energy Storage

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A novel boron-doping approach for long-term cycling life of Li-rich layered cathode

Cited by 5 publications

References 44 publications

In Situ Surface Reaction for the Preparation of High-Performance Li-Rich Mn-Based Cathode Materials with Integrated Surface Functionalization

In Situ Surface Reaction for the Preparation of High-Performance Li-Rich Mn-Based Cathode Materials with Integrated Surface Functionalization

Modification of Lithium‐Rich Manganese Oxide Materials: Coating, Doping and Single Crystallization

The mechanism of the impact of Li2MnO3 with dual-edged sword functionality on the cyclic performance of lithium-rich manganese-based cathode materials

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