NaCl–NaF和NaCl–LiF的二价通量介导的混合价（V 3 + / 4 +）NASICON型Na 3 V 2（PO 4）2 F 2.5 O 0.5和Na 2.4 Li 0.6 V 2（PO 4）2 F 2.5 O 0.5用于高度可逆的钠离子和锂离子存储,ACS Applied Energy Materials

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NaCl–NaF和NaCl–LiF的二价通量介导的混合价（V ^{3 + / 4 +}）NASICON型Na ₃ V ₂（PO ₄）₂ F _2.5 O _0.5和Na _2.4 Li _0.6 V ₂（PO ₄）₂ F _2.5 O _0.5用于高度可逆的钠离子和锂离子存储
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-02-02 , DOI: 10.1021/acsaem.0c02622
Thamodaran Partheeban ₁ , Baskar Senthilkumar ₂ , Vanchiappan Aravindan ₃ , Srinivasan Madhavi ₄ , Manickam Sasidharan ₁

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近年来，对于锂离子电池和钠离子电池均可使用的坚固的电极材料的开发引起了极大的兴趣。特别是，探索性晶体的生长在实现新的化学成分和发现其内在特性方面提供了很多奖励。在此，我们报道了一种NASICON型氟氧化钒钒酸钠固溶体，Na ₃ V ₂（PO ₄）₂ F _2.5 O _0.5（NVPF），及其部分经Li交换的Na _2.4 Li _0.6 V ₂（PO ₄）₂ F _2.5 O _0.5（NLVPF）晶体是通过一锅固态通量技术首次分别使用二元NaCl-NaF和NaCl-LiF通量。通过对通量，通量比和温度的性质进行的对照实验表明，NaCl和NaF / LiF盐不仅在阳离子/阴离子来源方面，而且从形态学角度看作为结构导向剂都起着至关重要的作用。X射线衍射（XRD）Rietveld精制，X射线光电子能谱（XPS）和²³ Na固态NMR证实了Na ₃ V ₂（PO ₄）₂的晶体结构，相纯度，晶格参数和混合价F _2.5 O _0.5及其锂取代的类似物。对合成的NVPF和NLVPF构造阴极的电化学性能的研究分别提供了117和118 mAh g ^–1相对于Li / Li ^+的初始放电容量，而在Na离子配置下提供了107和110 mAh g ^–1的容量（vs Na / Na ⁺）在0.1C的速率下。NVPF和NLVPF电极均通过保持75和86 mAh g ^–1（vs Li / Li ⁺）表现出长期稳定性，在以1C速率循环400次后，分别具有94％和95％以上的保留率。目前的发现强烈表明，通量法是以可扩展的方式合成用于混合离子电池的阴极材料的潜在方法之一。

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Binary NaCl–NaF and NaCl–LiF Flux-Mediated Growth of Mixed-Valence (V3+/4+) NASICON-Type Na3V2(PO4)2F2.5O0.5 and Na2.4Li0.6V2(PO4)2F2.5O0.5 for Highly Reversible Na- and Li-Ion Storage

Development of robust electrode materials that can work for both Li- and Na-ion batteries received enormous interest in recent times. Especially, exploratory crystal growth offers much reward in realizing new chemical compositions and the opportunity to uncover their intrinsic properties. Herein, we report a NASICON-type sodium vanadium oxy-fluorophosphate solid solution, Na₃V₂(PO₄)₂F_2.5O_0.5 (NVPF), and its partial Li-exchanged Na_2.4Li_0.6V₂(PO₄)₂F_2.5O_0.5 (NLVPF) crystals by one-pot solid-state flux techniques using binary NaCl–NaF and NaCl–LiF fluxes, respectively, for the first time. Controlled experiments with the nature of flux, flux ratios, and temperatures reveal that NaCl and NaF/LiF salts play a critical role, not only as cation/anion sources but also as a structure-directing agent from a morphological perspective. X-ray diffraction (XRD) Rietveld refinement, X-ray photoelectron spectroscopy (XPS), and ²³Na solid-state NMR confirm the crystal structure, phase purity, lattice parameter, and mixed valency of Na₃V₂(PO₄)₂F_2.5O_0.5 and its Li-substituted analogue. Investigation of the electrochemical properties of as-synthesized NVPF and NLVPF constructed cathode delivered initial discharge capacities of 117 and 118 mAh g^–1 vs Li/Li⁺, respectively, while in Na-ion configuration provided capacities of 107 and 110 mAh g^–1 (vs Na/Na⁺) at 0.1C rate. Both the NVPF and NLVPF electrodes demonstrate long-term stability by retaining 75 and 86 mAh g^–1 (vs Li/Li⁺), with over 94 and 95% retentions, respectively, after 400 cycles at 1C rate. The present findings strongly suggest that the flux method is one of the potential approaches to synthesize the cathode materials for hybrid-ion batteries in a scalable manner.

更新日期：2021-02-22

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