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首页> 外文期刊>RSC Advances >Structural elucidation of NASICON (Na3Al2P3O12) based glass electrolyte materials: effective influence of boron and gallium
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Structural elucidation of NASICON (Na3Al2P3O12) based glass electrolyte materials: effective influence of boron and gallium

机译：基于NASICON（Na3Al2P3O12）的玻璃电解质材料的结构阐明：硼和镓的有效影响

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摘要

Understanding the conductivity variations induced by compositional changes in sodium super ionic conducting (NASICON) glass materials is highly relevant for applications such as solid electrolytes for sodium (Na) ion batteries. In the research reported in this paper, NASICON-based NCAP glass (Na _(2.8) Ca _(0.1) Al _(2) P _(3) O _(12) ) was selected as the parent glass. The present study demonstrates the changes in the Na ~(+) ion conductivity of NCAP bulk glass with the substitution of boron (NCABP: Na _(2.8) Ca _(0.1) Al _(2) B _(0.5) P _(2.7) O _(12) ) and gallium (NCAGP: Na _(2.8) Ca _(0.1) Al _(2) Ga _(0.5) P _(2.7) O _(12) ) for phosphorus and the resulting structural variations found in the glass network. For a detailed structural analysis of NCAP, NCABP and NCAGP glasses, micro-Raman and magic angle spinning-nuclear magnetic resonance (MAS-NMR) spectroscopic techniques (for ~(31) P, ~(27) Al, ~(23) Na, ~(11) B and ~(71) Ga nuclei) were used. The Raman spectrum revealed that the NCAP glass structure is more analogous to the AlPO _(4) mesoporous glass structure. The ~(31) P MAS-NMR spectrum illustrated that the NCAP glass structure consists of a high concentration of Q ~(0) (3Al) units, followed by Q ~(0) (2Al) units. The ~(27) Al MAS-NMR spectrum indicates that alumina exists at five different sites, which include AlO _(4) units surrounded by AlO _(6) units, Al(OP) _(4) , Al(OP) _(5) , Al(OAl) _(6) and Al(OP) _(6) , in the NCAP glass structure. The ~(31) P, ~(27) Al and ~(11) B MAS-NMR spectra of the NCABP glass revealed the absence of B–O–Al linkages and the presence of B _(3) –O–B _(4) –O–P _(4) linkages which further leads to the formation of borate and borophosphate domains. The ~(71) Ga MAS-NMR spectrum suggests that gallium cations in the NCAGP glass compete with the alumina cations and occupy four (GaO _(4) ), five (GaO _(5) ) and six (GaO _(6) ) coordinated sites. The Raman spectrum of NCAGP glass indicates that sodium cations have also been substituted by gallium cations in the NCAP glass structure. From impedance analysis, the dc conductivity of the NCAP glass (～3.13 × 10 ~(?8) S cm ~(?1) ) is slightly decreased with the substitution of gallium (～2.27 × 10 ~(?8) S cm ~(?1) ) but considerably decreased with the substitution of boron (～1.46 × 10 ~(?8) S cm ~(?1) ). The variation in the conductivity values are described based on the structural changes of NCAP glass with the substitution of gallium and boron.
机译：理解由钠超离子导电（NASICON）玻璃材料的成分变化引起的电导率变化与诸如钠（Na）离子电池的固体电解质等应用非常相关。在本文报道的研究中，选择了基于NASICON的NCAP玻璃（Na _（2.8）Ca _（0.1）Al _（2）P _（3）O _（12））作为母玻璃。本研究表明NCAP大块玻璃的Na〜（+）离子电导率随硼的取代而变化（NCABP：Na _（2.8）Ca _（0.1）Al _（2）B _（0.5）P _（ 2.7）O _（12））和镓（NCAGP：Na _（2.8）Ca _（0.1）Al _（2）Ga _（0.5）P _（2.7）O _（12））及其生成的结构玻璃网络中发现的变化。对于NCAP，NCABP和NCAGP玻璃的详细结构分析，采用微拉曼和魔角旋转核磁共振（MAS-NMR）光谱技术（〜（31）P，〜（27）Al，〜（23）Na ，〜（11）B和〜（71）Ga核）。拉曼光谱显示，NCAP玻璃结构更类似于AlPO_（4）介孔玻璃结构。 〜（31）P MAS-NMR光谱表明，NCAP玻璃结构由高浓度的Q〜（0）（3Al）单元，然后是Q〜（0）（2Al）单元组成。 〜（27）Al MAS-NMR光谱表明氧化铝存在于五个不同的位置，其中包括被AlO _（6）单元包围的AlO _（4）单元，Al（OP）_（4），Al（OP）_ （5）在NCAP玻璃结构中为Al（OAl）_（6）和Al（OP）_（6）。 NCABP玻璃的〜（31）P，〜（27）Al和〜（11）B MAS-NMR光谱显示不存在B–O–Al键和B_（3）–O–B _ （4）–OP–（4）键进一步导致形成硼酸盐和硼磷酸盐域。 〜（71）Ga MAS-NMR光谱表明，NCAGP玻璃中的镓阳离子与氧化铝阳离子竞争，并占据四个（GaO _（4）），五个（GaO _（5））和六个（GaO _（6） ）协调的网站。 NCAGP玻璃的拉曼光谱表明，NCAP玻璃结构中的钠阳离子也已被镓阳离子取代。从阻抗分析来看，NCAP玻璃的直流电导率（〜3.13×10〜（？8）S cm〜（？1））随镓的取代而降低（〜2.27×10〜（？8）S cm〜（？1））。 （？1）），但随着硼的取代而显着降低（〜1.46×10〜（？8）S cm〜（？1））。基于NCAP玻璃的结构变化（用镓和硼替代）描述了电导率值的变化。

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