Synthesis of Na ion‐electron mixed conductor Na3Zr2Si2PO12 by doping with transition metal elements (Co, Fe, Ni)

Luo, Jing; Zhao, Guo Ping; Qiang, Wenjiang; Huang, Baotong

doi:10.1111/jace.18325

Cited by 12 publications

(9 citation statements)

References 51 publications

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“…This is detrimental for their applications in batteries because a wide electrochemical stability window is desired for solid‐state electrolytes. Meanwhile, previous literature on cobalt dopants focused on changes in ionic conductivity, and the reported ionic conductivity data was not remarkable [34–36] . By having optimized the experimental conditions for the cobalt doping strategy, we discover that the cobalt doping exhibits an excellent performance.…”

Section: Introductionmentioning

confidence: 89%

“…Meanwhile, previous literature on cobalt dopants focused on changes in ionic conductivity, and the reported ionic conductivity data was not remarkable. [34][35][36] By having optimized the experimental conditions for the cobalt doping strategy, we discover that the cobalt doping exhibits an excellent performance. Additionally, we have identified the factors that lead to the previously observed poor performance of cobalt-doping strategy.…”

Section: Introductionmentioning

confidence: 99%

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Machine Learning Guided Cobalt‐doping Strategy for Solid‐state NASICON Electrolytes

et al. 2023

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The solid‐state battery (SSB) is a promising direction to address the inherent safety problems in commercial batteries and energy storage systems. However, the development of SSBs is still hider of the low ionic conductivity of solid‐state electrolytes. Based on a machine learning (ML) method, a cobalt‐doping strategy was developed for the Na3.2Zr2Si2.2P0.8O12 (NASICON) compound by training on NASICON‐type solid electrolyte data. The cobalt‐doping strategy efficiently improves the NASICONs’ ionic conductivity to ∼2.63 mS/cm with low activation energy at ∼0.245 eV. The grain‐boundary ionic conductivity reaches ∼11.00 mS/cm without extra densification of the pellet. The NASICON's structures were studied by the Rietveld and the bond‐valence methods. The calculations and observed structural transitions confirm that the cobalt‐doping strategy promotes the structural transition and adjusts the structure to a better performance state. The doping strategy predicted by the ML model is consistent with our experimental results, providing very useful guidance for improving ionic conductivity of NASICON electrolytes.

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Section: Introductionmentioning

confidence: 89%

Section: Introductionmentioning

confidence: 99%

Machine Learning Guided Cobalt‐doping Strategy for Solid‐state NASICON Electrolytes

et al. 2023

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“…As a result, the examination of NASICON electrolytes' mechanical properties has emerged as a critical area of research 7,[17][18][19][20][21][35][36][37] .…”

Section: Fig 1 a Succinct History Of Nasicon Solid Electrolytesmentioning

confidence: 99%

“…This seminal work has catalyzed a growing interest in the field, evidenced by a consistent annual increase in related research. The predominant strategies to enhance the mechanical properties of NASICON electrolytes encompass a variety of approaches: doping [17][18][19] , compositional modification 7 , incorporation of sintering aids 20 , and use of more-recently broadly adopted fabrication techniques such as microwave-assisted sintering 39 and a hybrid fabrication method that combines tape-casting and hot-pressing 35 . These methodologies have been instrumental in significantly improving the mechanical robustness of NASICON electrolytes.…”

Section: Current Research Status On the Mechanical Properties Of Nasiconmentioning

confidence: 99%

Correlation between mechanical properties and ionic conductivity of sodium superionic conductors: a relative density-dependent relationship

Cheng,

Yang,

Liu

et al. 2024

Preprint

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Sodium superionic conductors (NASICON) are pivotal for the functionality and safety of solid-state sodium batteries. Their mechanical properties and ionic conductivity are key performance metrics, yet their interrelation remains inadequately understood. Addressing this gap is vital for concurrent enhancements in both properties. This study summarizes recent literature on NASICON solid electrolytes Na1+xZr2SixP3-xO12 (NZSP, 0≤x≤3), highlighting the mechanical properties and ionic conductivity, and identifies a positive correlation between mechanical strength, in particular hardness, and ionic conductivity at ambient temperatures. Microstructural analysis reveals that a range of factors, including relative density, grain size, secondary phases, and crystallographic structures, significantly influence material properties. Notably, an increase in relative density uniquely contributes to simultaneous enhancements in both ionic conductivity and mechanical strength. Consequently, future research should prioritize enhancing the relative density of NASICON solid electrolytes, possibly employing advanced techniques, including sol-gel process, spark plasma sintering (SPS), and microwave-assisted sintering. The correlation between mechanical properties and ionic conductivity observed in NASICON solid electrolytes extends to other high-temperature sintered oxide electrolytes like Li7La3Zr2O12 (LLZO). This investigation not only suggests a potential linkage between these crucial properties but also guides subsequent strategies for refining solid electrolytes for advanced battery technologies.

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“…Other metrics, such as electrochemical stability and interfacial compatibility should also be considered among the key parameters. Research efforts in the past decades have been mainly focused on ceramic‐type oxides with relatively high ionic conductivity, including NASICON (such as Na 3 Zr 2 Si 2 PO 12 [ 3 ] ), Garnet (such as Li 7 La 3 Zr 2 O 12 [ 4 ] ), and LiPON (such as Li 3.6 PO 3.4 N 0.6 [ 5 ] ). In addition to the relatively low ionic conductivity (e.g., in the range of 10 −4 –10 −5 S cm −1 at room temperature (RT)), unfavorable mechanical properties such as low fracture toughness are also challenges with most of these ceramic electrolytes.…”

Section: Introductionmentioning

confidence: 99%

Frameworked Electrolytes: A Pathway Towards Solid Future of Batteries

Sun,

Wang,

Yuan

et al. 2023

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All‐solid‐state batteries (ASSBs) represent a highly promising next‐generation energy storage technology owing to their inherently high safety, device reliability, and potential for achieving high energy density in the post‐ara of lithium‐ion batteries, and therefore extensive searches are ongoing for ideal solid‐state electrolytes (SSEs). Though promising, there is still a huge barrier that limits the large‐scale applications of ASSBs, where there are a couple of bottleneck technical issues. In this perspective, a novel category of electrolytes known as frameworked electrolytes (FEs) are examined, where the solid frameworks are intentionally designed to contain 3D ionic channels at sub‐nano scales, rendering them macroscopically solid. The distinctive structural design of FEs gives rise to not only high ionic conductivity but also desirable interfaces with electrode solids. This is achieved through the presence of sub‐nano channels within the framework, which exhibit significantly different ion diffusion behavior due to the confinement effect. This perspective offers a compelling insight into the potential of FEs in the pursuit of ASSBs, where FEs offer an exciting opportunity to overcome the limitations of traditional solid‐state electrolytes and propel the development of ASSBs as the holy grail of energy storage technology.

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Synthesis of Na ion‐electron mixed conductor Na₃Zr₂Si₂PO₁₂ by doping with transition metal elements (Co, Fe, Ni)

Cited by 12 publications

References 51 publications

Machine Learning Guided Cobalt‐doping Strategy for Solid‐state NASICON Electrolytes

Machine Learning Guided Cobalt‐doping Strategy for Solid‐state NASICON Electrolytes

Correlation between mechanical properties and ionic conductivity of sodium superionic conductors: a relative density-dependent relationship

Frameworked Electrolytes: A Pathway Towards Solid Future of Batteries

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