In situ multiscale probing of the synthesis of a Ni-rich layered oxide cathode reveals reaction heterogeneity driven by competing kinetic pathways

Park, Hyeokjun; Park, Ha Young; Song, Kyung; Song, Seok Hyun; Kang, Sungsu; Ko, Kun-Hee; Eum, Donggun; Jeon, Yonggoon; Kim, Jihoon; Seong, Won Mo; Kim, Hyungsub; Park, Jungwon; Kang, Kisuk

doi:10.1038/s41557-022-00915-2

Cited by 63 publications

(37 citation statements)

References 59 publications

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“…This provides an estimate that the as-synthesized NCM811 precursor possesses one structural water molecule from calculating the theoretical weight loss value of Ni 0.8 Co 0.1 Mn 0.1 OH·H 2 O (16.3%). The decomposition of Ni 0.8 Co 0.1 Mn 0.1 OH started at around 340 °C and was completed at around 800 °C, along with obtaining Ni 0.8 Co 0.1 Mn 0.1 O and releasing water . Three endothermic peaks in the DSC spectra confirm the three processes observed in TGA: surface water loss around 100 °C, bind water loss around 200–340 °C, and decomposition above 350 °C.…”

Section: Resultssupporting

confidence: 61%

“…The decomposition of Ni 0.8 Co 0.1 Mn 0.1 OH started at around 340 °C and was completed at around 800 °C, along with obtaining Ni 0.8 Co 0.1 Mn 0.1 O and releasing water. 51 Three endothermic peaks in the DSC spectra confirm the three processes observed in TGA: surface water loss around 100 °C, bind water loss around 200–340 °C, and decomposition above 350 °C.…”

Section: Resultsmentioning

confidence: 55%

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Scalable Advanced Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials from a Slug Flow Continuous Process

et al. 2022

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Li[Ni0.8Co0.1Mn0.1]O2 (LNCMO811) is the most studied cathode material for next-generation lithium-ion batteries with high energy density. However, available synthesis methods are time-consuming and complex, restricting their mass production. A scalable manufacturing process for producing NCM811 hydroxide precursors is vital for commercialization of the material. In this work, a three-phase slug flow reactor, which has been demonstrated for its ease of scale-up, better synthetic control, and excellent uniform mixing, was developed to control the initial stage of the coprecipitation of NCM811 hydroxide. Furthermore, an equilibrium model was established to predict the yield and composition of the final product. The homogeneous slurry from the slug flow system was obtained and then transferred into a ripening vessel for the necessary ripening process. Finally, the lithium–nickel–cobalt–manganese oxide was obtained through the calcination of the slug flow-derived precursor with lithium hydroxide, having a tap density of 1.3 g cm–3 with a well-layered structure. As-synthesized LNCMO811 shows a high specific capacity of 169.5 mAh g–1 at a current rate of 0.1C and a long cycling stability of 1000 cycling with good capacity retention. This demonstration provides a pathway toward scaling up the cathode synthesis process for large-scale battery applications.

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Section: Resultssupporting

confidence: 61%

Section: Resultsmentioning

confidence: 55%

Scalable Advanced Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials from a Slug Flow Continuous Process

et al. 2022

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“…From a comparison of LNO and Nb-LNO after cycling in Figure c,d, it is evident that the incorporation of Nb helps to suppress the formation of these defects during cycling. These defects are demonstrably linked to various mechanisms of electrochemical performance degradation, including rock-salt-phase formation and progressive intragranular cracking. − …”

Section: Resultsmentioning

confidence: 99%

“…Previous work suggests that formation of such defects during high-temperature calcination may result from incomplete lithiation of the hydroxide precursor due to kinetically competing thermal decomposition and topotactic lithiation reactions. 41 In contrast, no such defects are apparent in the Nb-LNO immediately after calcination, which may be due to shortened lithium diffusion paths associated with reduced primary particle size. The substantially increased prevalence of nanopore defects shown in Figure 4c confirms that the majority are formed during electrochemical cycling, rather than calcination.…”

Section: Postmortem Analysesmentioning

confidence: 99%

Surface Stabilization of Cobalt-Free LiNiO₂ with Niobium for Lithium-Ion Batteries

Ober

Mesnier

Manthiram

2023

ACS Appl. Mater. Interfaces

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Lithium nickel oxide (LiNiO2) is a promising next-generation cathode material for lithium-ion batteries (LIBs), offering exceptionally high specific capacity and reduced material cost. However, the poor structural, surface, and electrochemical stabilities of LiNiO2 result in rapid loss of capacity during prolonged cycling, making it unsuitable for application in commercial LIBs. Herein, we demonstrate that incorporation of a small amount of niobium effectively suppresses the structural and surface degradation of LiNiO2. The niobium-treated LiNiO2 retains 82% of its initial capacity after 500 cycles in full cells with a graphite anode compared to 73% for untreated LiNiO2. We utilize a facile method for incorporating niobium, which yields Li x NbO y phase formation as a surface coating on the primary particles. Through a combination of X-ray diffraction, electron microscopy, and electrochemical analyses, we show that the resulting niobium coating reduces active material loss over long-term cycling and enhances lithium-ion diffusion kinetics. The enhanced structural integrity and electrochemical performance of the niobium-treated LiNiO2 are correlated to a reduction in the formation of nanopore defects during cycling compared to the untreated LiNiO2.

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“…Hence in the case of LFP, like for several other compounds, XRPD was a crucial tool to spark subsequent studies focused on understanding electrochemical reaction pathways. Very recently, XRPD has also been applied to investigate synthesis reaction mechanisms and thermal stabilities of electrode materials for rechargeable batteries [77][78][79][80][81][82]. A review article in this focus issue highlights the importance of understanding synthesis reaction mechanisms and shows several key examples using in situ heating XRPD experiments [83].…”

Section: Progress In Experimentsmentioning

confidence: 99%

Advances and challenges in multiscale characterizations and analyses for battery materials

Bianchini

Lacivita

Seo

2022

Journal of Materials Research

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Rechargeable ion batteries are efficient energy storage devices widely employed in portable to largescale applications such as electric vehicles and grids. Electrochemical reactions within batteries are complex phenomena, and they are strongly dependent on the battery materials and systems used. These electrochemical reactions often include detrimental irreversible reactions at various length scales from atomic-to macro-scales, which ultimately determine the overall electrochemical behavior of the system. Understanding such reaction mechanisms is a critical component to improve battery performance. To help this effort, this review article discusses recent advances and remaining challenges in both computational and experimental approaches to better understand dynamic electrochemical reactions in batteries across multiple length scales. Important related findings from this focus issue will also be highlighted. The aim of our focus issue is to contribute to the battery community towards having better understanding of complex reactions occurring in battery devices and of computational and experimental methods to investigate them.

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In situ multiscale probing of the synthesis of a Ni-rich layered oxide cathode reveals reaction heterogeneity driven by competing kinetic pathways

Cited by 63 publications

References 59 publications

Scalable Advanced Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials from a Slug Flow Continuous Process

Scalable Advanced Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials from a Slug Flow Continuous Process

Surface Stabilization of Cobalt-Free LiNiO₂ with Niobium for Lithium-Ion Batteries

Advances and challenges in multiscale characterizations and analyses for battery materials

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In situ multiscale probing of the synthesis of a Ni-rich layered oxide cathode reveals reaction heterogeneity driven by competing kinetic pathways

Cited by 63 publications

References 59 publications

Scalable Advanced Li(Ni0.8Co0.1Mn0.1)O2 Cathode Materials from a Slug Flow Continuous Process

Scalable Advanced Li(Ni0.8Co0.1Mn0.1)O2 Cathode Materials from a Slug Flow Continuous Process

Surface Stabilization of Cobalt-Free LiNiO2 with Niobium for Lithium-Ion Batteries

Advances and challenges in multiscale characterizations and analyses for battery materials

Contact Info

Product

Resources

About

Scalable Advanced Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials from a Slug Flow Continuous Process

Scalable Advanced Li(Ni_0.8Co_0.1Mn_0.1)O₂ Cathode Materials from a Slug Flow Continuous Process

Surface Stabilization of Cobalt-Free LiNiO₂ with Niobium for Lithium-Ion Batteries