Constructing a robust integrated surface structure for enhancing the performance of Li-rich Mn-based oxides cathodes

Gao, Xianggang; Li, Shihao; Zhang, Haiyan; Zhang, Shuai; Chang, Shilei; Li, Simin; Lai, Yanqing; Zhang, Zhian

doi:10.1016/j.mtener.2022.101152

Cited by 15 publications

(8 citation statements)

References 46 publications

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“…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. Unlike LLO, the NaBF 4 -treated samples display a new peak at approximately 18.7°, ascribed to Li x B y O z , confirming the presence of B in the bulk material . Parts b and c of Figure S3 illustrate changes in cell parameters a and c .…”

Section: Resultssupporting

confidence: 84%

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%

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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“…The value of I(003)/I(104) of all the samples is larger than 1.2, indicating the low cation mixing. [ 11 ] In addition, the left‐shift peaks of (003) and (104) ascribe to the enlarged d‐spacing and Li + slab, ascribing to the extraction of oxygen atoms after surface defect construction. [ 9b,12 ] The increasing interplanar spacing is beneficial for the fast Li + diffusion and to enhance the fast‐charging capability.…”

Section: Resultsmentioning

confidence: 99%

Local Electronic Structure Modulation Enables Fast‐Charging Capability for Li‐Rich Mn‐Based Oxides Cathodes With Reversible Anionic Redox Activity

Gao

Zhang

et al. 2023

Adv Funct Materials

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Anionic and cationic redox chemistries boost ultrahigh specific capacities of Li‐rich Mn‐based oxides cathodes (LRMO). However, irreversible oxygen evolution and sluggish kinetics result in continuous capacity decay and poor rate performance, restricting the commercial fast‐charging cathodes application for lithium ion batteries. Herein, the local electronic structure of LRMO is appropriately modulated to alleviate oxygen release, enhance anionic redox reversibility, and facilitate Li+ diffusion via facile surface defect engineering. Concretely, oxygen vacancies integrated on the surface of LRMO reduce the density of states of O 2p band and trigger much delocalized electrons to distribute around the transition metal, resulting in less oxygen release, enhancing reversible anionic redox and the MnO6 octahedral distortion. Besides, partially reduced Mn and lattice vacancies synchronously stimulate the electrochemical activity and boost the electronic conductivity, Li+ diffusion rate, and fast charge transfer. Therefore, the modified LRMO exhibits enhanced cyclic stability and fast‐charging capability: a high discharging capacity of 212.6 mAh·g−1 with 86.98% capacity retention after 100 cycles at 1 C is obtained and to charge to its 80%, SOC is shortened to 9.4 min at 5 C charging rate. This work will draw attention to boosting the fast‐charging capability of LRMO via the local electronic structure modulation.

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“…Coating materials should meet the following requirements: (i) high stability of physical and chemical properties; (ii) resistance against electrolyte corrosion; and (iii) high ionic conductivity. The major LRMO surface coating materials reported to date include oxides [ 66 ], fluorides [ 67 ], phosphates [ 68 ], Li + conductors [ 69 ], and conductive polymers [ 70 ].…”

Section: Modification Strategiesmentioning

confidence: 99%

Modification Strategies of High-Energy Li-Rich Mn-Based Cathodes for Li-Ion Batteries: A Review

Xi,

Sun,

et al. 2024

Molecules

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Li-rich manganese-based oxide (LRMO) cathode materials are considered to be one of the most promising candidates for next-generation lithium-ion batteries (LIBs) because of their high specific capacity (250 mAh g−1) and low cost. However, the inevitable irreversible structural transformation during cycling leads to large irreversible capacity loss, poor rate performance, energy decay, voltage decay, etc. Based on the recent research into LRMO for LIBs, this review highlights the research progress of LRMO in terms of crystal structure, charging/discharging mechanism investigations, and the prospects of the solution of current key problems. Meanwhile, this review summarizes the specific modification strategies and their merits and demerits, i.e., surface coating, elemental doping, micro/nano structural design, introduction of high entropy, etc. Further, the future development trend and business prospect of LRMO are presented and discussed, which may inspire researchers to create more opportunities and new ideas for the future development of LRMO for LIBs with high energy density and an extended lifespan.

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Constructing a robust integrated surface structure for enhancing the performance of Li-rich Mn-based oxides cathodes

Cited by 15 publications

References 46 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

Local Electronic Structure Modulation Enables Fast‐Charging Capability for Li‐Rich Mn‐Based Oxides Cathodes With Reversible Anionic Redox Activity

Modification Strategies of High-Energy Li-Rich Mn-Based Cathodes for Li-Ion Batteries: A Review

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