Unveiling the migration behavior of lithium ions in NCM/Graphite full cell via in operando neutron diffraction

Wang, Chaoqi; Wang, Rui; Huang, Zhongyuan; Chu, Mihai; Ji, Wenxin; Chen, Ziwei; Zhang, Taolue; Zhai, Jingjun; Lu, Huaile; Deng, Sihao; Chen, Jie; He, Lunhua; Liang, Tianjiao; Wang, Fangwei; Wang, Jun; Deng, Yonghong; Cai, Weihua; Xiao, Yinguo

doi:10.1016/j.ensm.2021.09.032

Cited by 40 publications

(25 citation statements)

References 49 publications

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“…Obviously, the lowest migration barrier is identified when migrating along the O‐A path, which is also regarded as the most likely migration path by the other groups. [ 46–49 ] When Li + migrates along this pathway, the energy barrier decreases by 13.24% (0.355 vs 0.308 eV) after doping with W 6+ (Figure 9g). It is confirmed from the results that W 6+ doping is extremely beneficial to the migration of Li + in the cathode, which helps improve the rate capability.…”

Section: Resultsmentioning

confidence: 99%

Atomic Horizons Interpretation on Enhancing Electrochemical Performance of Ni‐Rich NCM Cathode via W Doping: Dual Improvements in Electronic and Ionic Conductivities from DFT Calculations and Experimental Confirmation

Gao

Huang

Dong

et al. 2022

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270 mAh g −1 , are candidates for the next generation of lithium-ion batteries (LIBs). [7,8] NCM cathodes with high nickel content have attracted increasing attention because of their higher capacities when more nickel cations provide a more electron transfer from Ni 2+ /Ni 3+ and Ni 3+ /Ni 4+ redox pairs. [9,10] Meanwhile, since the relative content of expensive cobalt will be reduced, the production cost will also be decreased. Therefore, it is a trend to increase the proportion of nickel in the ternary system of LiNi 1−x−y Co x Mn y O 2 . [11] However, when the nickel content exceeds 80%, [12,13] the battery suffers from serious capacity degradation during the cycle.The main role of elemental doping is to reduce the mixing of Li and Ni cations and stabilize the crystal structure. It is a feasible approach to slow the capacity decay. Presently, it has been found that W 6+ is a good choice as a doping element. W 6+ has a higher valence and stronger bond energy compared to other ions (such as Al 3+ , Mg 2+ , Ba 2+ , and Zn 2+ ), resulting in a dual functional enhancement of the electronic and cationic conductivities. In 2018, Kim [14] proposed that, after the doping with 1 mol% W into Ni-rich LiNi 0.9 Co 0.05 Mn 0.05 O 2 cathode, the salt rock phase with surface segregation could protect the cathode material from harmful reactions and improve the cycle stability. In 2019, Park [15] reported that 1 mol% W doping in LiNi 0.9 Co 0.05 Mn 0.05 O 2 cathode significantly improved the capacity retention from 60% to 89% after 500 cycles at a 4.3 V cutoff voltage. It was believed that the reason for the cathode performance improvement of the W-doped LiNi 0.9 Co 0.05 Mn 0.05 O 2 in the abovementioned reports was mainly due to the internal stress reduction to stabilize the bulk structure so that the formation of harmful microcracks was inhibited. Shang et al. [16] suggested that adding W stabilized the structure and slowed the diffusion of the rock salt phase from the surface to the interior. However, researchers have conflicting opinions on the effects of the formed rock salt structure after doping. For instance, concerning the abovementioned conflicting opinions, that is, Kim thinks the existence of rock salt phase is good, whereas Shang thinks it is bad. Furthermore, reports on the formation of the rock salt phase by non-W cation doping are controversial. Jianming Zheng et al. [17] believeThe rapid capacity degradation and poor rate capability hinder the application of Rich-Ni layered LiNi x Co y Mn z O 2 (NCM) as cathode materials for highenergy lithium-ion batteries. In this study, density functional theory (DFT) calculations, combined with conventional electrochemical measurements, reveal from the atomic view that the dual improvements in electronic and ionic conductivities are the main facts for the property enhancement. The bandgap of the cathode material is reduced to 1.1623 eV due to the increased number of electrons near the Fermi level after W intercalation. Such improved electronic conductivity subsequently lea...

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Section: Resultsmentioning

confidence: 99%

Atomic Horizons Interpretation on Enhancing Electrochemical Performance of Ni‐Rich NCM Cathode via W Doping: Dual Improvements in Electronic and Ionic Conductivities from DFT Calculations and Experimental Confirmation

Gao

Huang

Dong

et al. 2022

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“…The concentration of the Li/Ni mixing varies during charging and its dependence on the Li content is like a crater due to the competition between delithiation and magnetic frustration. In addition, the Li ion hops zigzag from one tetrahedral site to the next in the charge process 61 …”

Section: Fundamentals Of Anionic Redoxmentioning

confidence: 99%

“…Rong et al 6 also observed the decrease of the O–O bond length in the charged P 2 ‐type Na 0.72 [Li 0.24 Mn 0.76 ]O 2 . Wang et al 61 unveiled the diffusion behavior of the Li ion in layered cathode materials LiNi 0.5 Co 0.2 Mn 0.3 O 2 by in situ NPD. The concentration of the Li/Ni mixing varies during charging and its dependence on the Li content is like a crater due to the competition between delithiation and magnetic frustration.…”

Section: Fundamentals Of Anionic Redoxmentioning

confidence: 99%

Configuration‐dependent anionic redox in cathode materials

et al. 2022

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“…[ 164 ] Nuclear scattering length is relatively stable and does not decrease as the wave transfer vector increases, indicating that the neutron diffraction has a strong penetration. [ 165 ] Unlike high energy XRD, nuclear scattering can avoid generating heat and is less destructive. [ 166 ] Using the operando neutron diffraction (Figure 17d), Liu et al revealed a universal four‐stage structural evolution mechanism for LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes.…”

Section: Characterizationmentioning

confidence: 99%

Single‐Crystalline Cathodes for Advanced Li‐Ion Batteries: Progress and Challenges

Han

Lei

et al. 2022

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Single-crystalline cathodes are the most promising candidates for highenergy-density lithium-ion batteries (LIBs). Compared to their polycrystalline counterparts, single-crystalline cathodes have advantages over liquid-electrolyte-based LIBs in terms of cycle life, structural stability, thermal stability, safety, and storage but also have a potential application in solid-state LIBs. In this review, the development history and recent progress of single-crystalline cathodes are reviewed, focusing on properties, synthesis, challenges, solutions, and characterization. Synthesis of single-crystalline cathodes usually involves preparing precursors and subsequent calcination, which are summarized in the details. In the following sections, the development issues of single-crystalline cathodes, including kinetic limitations, interfacial side reactions, safety issues, reversible planar gliding and micro-cracking, and particle size distribution and agglomeration, are systematically analyzed, followed by current solutions and characterization techniques. Finally, this review is concluded with proposed research thrusts for the future development of singlecrystalline cathodes.

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Unveiling the migration behavior of lithium ions in NCM/Graphite full cell via in operando neutron diffraction

Cited by 40 publications

References 49 publications

Atomic Horizons Interpretation on Enhancing Electrochemical Performance of Ni‐Rich NCM Cathode via W Doping: Dual Improvements in Electronic and Ionic Conductivities from DFT Calculations and Experimental Confirmation

Atomic Horizons Interpretation on Enhancing Electrochemical Performance of Ni‐Rich NCM Cathode via W Doping: Dual Improvements in Electronic and Ionic Conductivities from DFT Calculations and Experimental Confirmation

Configuration‐dependent anionic redox in cathode materials

Single‐Crystalline Cathodes for Advanced Li‐Ion Batteries: Progress and Challenges

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