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WIREs Energy Environ.
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A comprehensive review on recent advances of polyanionic cathode materials in Na‐ion batteries for cost effective energy storage applications

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Abstract Sustainable and efficient energy storage devices are crucial to meet the soaring global energy demand. In this context, Na‐ion batteries (NIBs) have emerged as one of the excellent alternatives to the Li‐ion batteries, due to the uniform geographical distribution, abundance, cost‐effectiveness, comparable operating voltage as well as similar intercalation chemistry. However, due to larger size of Na and other related issues, a subtle strategy of research is required for the development of electrode materials for NIBs to enhance overall electrochemical performance. Here, we provide a comprehensive review on recent advances of polyanionic cathode materials for NIBs for cost effective and large scale energy storage applications. Owing to their great thermal and chemical stability, high redox potential (inductive effect), and rich structural diversity, polyanionic cathodes have been considered potential candidates in recent years. We cover a large number of polyanionic materials and conclude with the strategies to improve the energy and power density of NIB. This article is categorized under: Energy Research & Innovation > Science and Materials Energy and Development > Science and Materials Energy and Transport > Science and Materials
(a) The Rietveld refined synchrotron X‐ray diffraction pattern, (b) structure of the Na3MnTi(PO4)3 where MnO6 and TiO6 octahedra is presented in blue, the PO4 octahedron in green, and the sodium ions in yellow, (c) galvanostatic charge/discharge curves, (d) capacity retention and Coulombic efficiency of the Na3MnTi(PO4)3 at a constant charge/discharge rate of 0.1 C (Gao et al., 2016); (e) The in‐situ XRD patterns collected during galvanostatic charge/discharge at 50 mA/g, (f) Schematic illustration showing 2 Na+ de‐intercalating from Na3MnTi(PO4)3 during the first charge process, and 3 Na+ intercalating from the framework upon subsequent electrochemical discharge/charge processes (T. Zhu et al., 2019); (g) schematic illustration of the sol–gel route of rGO encapsulated Na3MnTi(PO4)3 C material (J. Li, Peng, et al., 2019). Charge and discharge voltage profiles of Na4MnV(PO4)3 (NMVP) (h) and Na3FeV(PO4)3 (NFVP) (i) at different C‐rates, (j) capacity performance of NMVP and NFVP up to 1000 cycles(Zhou et al., 2016)
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Illustration of Mg doped Na3V2(PO4)3 (H. Li, Tang, et al., 2018)
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(a) The crystal structure of the Na3V2(PO4)3 (NVP), synthesized by solid‐state route, in a standard orientation where the magenta and dark green balls denote the Na1 and Na2 atoms, respectively, peach color denotes oxygen atoms, royal blue and purple correspond to P and V atoms, respectively, as visualized with the VESTA software. (b) Rietveld refined XRD pattern of NVP, synthesized by the solid state route. (c) Raman spectrum of the NVP measured at λ = 514 nm at room temperature. (d) The CV profile and (e) the electrochemical performance (rate capability) of NVP at different rates. (f) In‐situ XRD patterns of NVP cycled between 2.7 and 3.7 V at 0.1 C rate, taken from reference Z. Jian et al. (2013)
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The crystal structure for (a) maricite phase and (b) olivine phase (Moreau et al., 2010); (c) electrochemical performance of NaFePO4 (Oh et al., 2012); (d) synthesis process of carbon coated LiFePO4 and NaFePO4 (Y. Zhu et al., 2013); (e) galvanostatic curves of maricite NaFePO4 at C/20 rate for 200 cycles where the inset shows discharge curves of NaFePO4 as a function of C‐rate (J. Kim, Seo, et al., 2015)
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(a) Energy level diagram for the ionic and covalent bonds., (b) Charge localization of the ionic bond around XO4 tetrahedra (Melot & Tarascon, 2013) and (c) Electronegativity values of B, P, Si, and S elements, as on Pauling scale
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(a) The tree classification of cathode materials for NIBs with one branch corresponding to the division of family of polyanionic compounds and (b) operating potential and capacity of recently studied polyanionic compounds (Ni et al., 2017)
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(a) Working principle of Na‐ion insertion/de‐insertion in NIBs, and the relative energy of the chemical potentials μA, μC, and Eg for open‐circuit with (b) liquid electrolyte and (c) solid electrolyte
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(a) Abundance of the elements in the earth's crust (https://pubs.usgs.gov/fs/2002/fs087‐02/), and (b) Illustration of the Na‐ion battery power system
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Electrochemical characterizations of the NFS8‐5%CNT//HC full cell: (a) galvanostatic charge/discharge profiles with different C‐rates from 0.1 to 5 C, Comparative study of (b) operating voltages, and (c) energy densities between this work and reported experiments from literature survey. (d) Rate capability at various current rates, (e) cycling efficiency at 0.5 C along with coulombic efficiency. (f) Charge/discharge profile for the 1st, 5th, 100th, 200th, and 500th cycles, and (g) cycling efficiency at 2 C for 1000 cycles in a voltage limit of 1.5–4.2 V, taken from reference S. Li, Song, et al. (2019)
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Synthesis and electrochemical performance of pb21a‐NFS/C composite (a) schematic illustration of pb21a‐NFS/C synthesis from C221‐NFS/C during first cycle; the purple and brown tetrahedron represent SiO4 and FeO4, respectively; Na and O atoms are represented by yellow and blue spheres, respectively, (b) the galvanostatic charge–discharge profile of pb21a‐NFS/C composite at 0.1 C in the voltage window of 1.5–4.5 V, (c) the cycling stability at 0.1 C, (d) the normalized voltage versus capacity behavior, (e) the rate capability at different current densities, taken from reference Bai et al. (2018)
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Crystal structure of Na2VO(SO4)2, where blue colored bipyramids represent the VO6 octahedra, and sulfate tetrahedra, Na and O atoms are shown in yellow, green and red colors, respectively, taken from reference M. Sun et al. (2016)
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Crystal structure of the Na2Fe(SO4)2 · 2H2O illustrating the convoluted Na‐ion migration channels along the b‐axis. The FeO6 octahedra, SO4 tetrahedra, O atoms, and Na atoms are represented in brown, yellow, red, and green colors, respectively, taken from reference Barpanda, Oyama, Ling, and Yamada (2014)
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The electrochemical behavior of NFS‐x%CNTs at 0.1 C rate with NaClO4/EC:PC electrolyte. (a) Galvanostatic charge‐discharge profile in a voltage range of 1.5–4.0 V and, (c) 1.5–4.5 V, (b) the cycling stability and Coulombic efficiencies of electrodes in a voltage range of 1.5–4.0 V and, (d) 1.5–4.5 V, taken from reference Ali et al. (2018)
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(a) The crystal structure of the Na3V2(PO4)2F3 (NVPF) (W. Song et al., 2014); (b) the CV plot of NVPF at a scan rate of 0.5 mV/s for different cycles (W. Song & Liu, 2013).; (c) in‐operando XRD Pattern of NVPF (Bianchini et al., 2015); (d) the crystal structure of Na3V2Oy(PO4)2F3−y (Broux et al., 2016); (e) Galvanostatic charge/discharge profile of Na3V2O2(PO4)2F in the voltage range of 1.0–4.5V, with the extraction of three Na‐ions (Bianchini et al., 2017); (f) In‐situ XRD patterns of Na3V2O2(PO4)2F during charging and discharging (Y. Yin et al., 2017); (g) the rate performance of graphene quantum dots coated Na3V2O2(PO4)2[email protected] for 2000 cycles (G. Deng, Chao, et al., 2016); (h) the structure evolution of the intermediate product of Na3V2(PO4)2F3 by annealing (Z. Yang, Li, et al., 2020)
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(a) Structural of Na4Fe3(PO4)2P2O7; where FeO6 units, PO4 and P2O7 units and Na+ ions are represented by brown, grey and yellow color, respectively (Wood et al., 2015), (b) the rate performances of Na4Mn2Co(PO4)2P2O7/C‐CNTs (NM2CPP/C‐5 wt% CNT) and NM2CPP/C (Tang et al., 2019), (c) the rate capability of Na4Mn1.5Co1.5(PO4)2P2O7 /C in the potential range of 3.0–5.1 V versus Na+/Na at 2 and 5 C rates (Kang et al., 2020), (d) the schematic view of NCPP and Al0.15‐NCPP crystal structures, (e) the charge and discharge curves of Al0.15‐NCPP at 0.5 C rate. (f) the cycling stability of Al0.15‐NCPP at 30 C (X. Liu et al., 2019)
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(a) The XRD pattern and crystal structure of Na2CoP2O7, and (b) the electrochemical performance cycled at C/20 rate with Na metal as anode (Barpanda, Lu, et al., 2013); (c) the galvanostatic charge/discharge profiles of first three cycles with the inset displaying the discharge characteristics, (d) the rate capability along with the charge/discharge profile in the inset at different C rates (H. Li, Chen, et al., 2019)
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(a) The crystal structure and electrochemical performance of Na2FeP2O7 with (b) galvanostatic voltage–composition curves at C/20 rate, and (c) the discharge capacity as a function of rate (discharged up to 2 V), with cells charged to 4 V at C/10 constant rate (Barpanda, Ye et al., 2012); Galvanostatic charge‐discharge curves of Na2FeP2O7 with NaFSA‐C3C1pyrrFSA electrolyte, at current density of 10 mAh/g at (d) 298 K and (e) 363 K, (f). The ratio between the discharge capacity (C) and the reference capacity (C0) as a function of cycling rate between 298 and 363 K (C. Y. Chen, Matsumoto, Nohira, Ding, Yamamoto, & Hagiwara, 2014)
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