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Materials 2020, 13, 3453 10 of 58 = 80 mA·g−1) and 59.2 mA·h·g−1 at 30C. The capacity retention of 91.0 % and 75.9 % could be achieved at 1C (800 cycles) and 10C rate (5000 cycles), respectively. Gao et al. used a sol-gel synthesis to obtain 200 nm particles of Na3MnZr(PO4)3 coated in situ with a thin carbon layer. Na3MnZr(PO4)3 crystallizes in the rhombohedral NASICON structure. Used as a cathode, it delivered a capacity of 105 mA·h·g−1 at 0.1C rate, and a capacity retention of 91% was demonstrated at 0.5C after 500 cycles [112]. Therefore, the material was stable enough Materials 2020, 13, x FOR PEER REVIEW 10 of 53 and the particles small enough to avoid any problem related to the JT distortion associated with 3+ Msynnth.esTisheprsoycnetshseshiesreprwocaesssimhpeorertawnats, simincpeorptrainotr, wsinorckespfroiourndwoprokosr feoluecntdropchoeomr eiclaelctreoscuhletsmwiciatlh rseasmulptslewsipthrespaamrpedlesbyprseoplaidre-sdtabtye sroelaicdt-isotna,tewrehaichtiolend, wtohibcihggleedr tpoabrtigicglesr,paanrdticpleos,saibnldypnosnsibulnyifnoormn ucnairfboormn-coaartbionng-sc.oatings. Naa3MnTii((PO4)3/C hollow microspheres with an open andssttaablleNASSIICONffrraameeworrkweerree 343 ssyynnttheessiizzeed bbyyaasspprraayy-d-drryyiningg--aasssiisstteed prroocceesss[[11133]]. . Ass aanaannoodee, ,ththisisccoomppoossititeeddeemoonnssttrraatteedaa −1 −1 −1 −1 ccaappaaccitiytyooff161060mmAA·h·hgg aatt00.2.2CC. .WWhhenencyccylceldedata2tC2,Ct,htehceacpapciatcyitwyawsacsapcacpiatyciotyf 1o1f91m19Am·hA·gh gwitwhi≈th 9≈29%2 %capcapciatycitryetreentteinotnioanftaefrte5r0050c0yclyecsl.es. Naa4Fe3(PO4)2((P2OO7),), wiwthithits itms ixmedixecdrystcarlylisnteallifnreamefwraomrkewroerpkresreenptreedsenbtyedthebyorthoe- 434227 oprythrop-phyorsopphhaotessp,hpaotsese, spseoss3eDsseosd3iuDmsdoidffiumsiodnipffautshiwonaypsaitnhtwhaeysstuidnytchreystauldfryamcreywstoalrkfroafmaetywpoirckal oNf AaStIyCpOicNal-tNypAeSsItCruOcNtu-rtyepaendstrisucthturseaangodoids ctahnudsidaagteooads acacnadthidodateefaosr SaIBcast[h1o1d4e]. fCoarrbSoIBns-c[o1a1t4e]d. Cnarnbosniz-ceodatNeda4nFaen3(oPsOiz4e)d2(PN2Oa7F),ew(PitOh )its(PmOix)e,dwcitrhysitsalmlinixeedfrcarmysetwalolirnkerferapmreeswenotrekdrebpyretsheentoedrthboy- 434227 tpheyrorptho-spyhraotpehso, pspohssaetesse, spo3Dssessosdeisu3mDdsiofdfuiusimondpiffauthswioanypsaitnhtwhaeysstuindythcerystsutadlyfrcarmysetwalofrkamofeawtoyrpkicoafl −1 −1 aNtyApSiIcCalONA-tSyIpCeOsNtr-utycptuersetruscetduraesuasecdatahsoadecadtheloivderdedeliavecraepdacaitcyapoafc1it1y3 oaf n1d1310a8n dm1A08hmgA·ha·tg0.05aCt −1 −1 −1 −1 0a.0n5dC0a.1nCd,0r.e1sCp,ercetsipveclytiv(1eCly=(11C20=m12A0gmA).·gAt)0..5ACt,0t.h5eCc,athpeaciatpyawciatysw80asm8A0mhAg·ha·gftera4f0te0rc4y0c0lecsy,calensd, −1 −1 aantd20aCt2,0thCe,cthapeaccaiptyacwitayswstailsl6st0ilml6A0hmgA·ha·fgter4a4ft0e0rc4y4c0l0esc,ywclheisc,hwchoricrhescpornredsptonadrsetoenatiroenteonfti6o9n.1o%f. 6(9F.i1g%u.re(F5i)g[u1r1e55,1)1[61]1.5,116]. Figure 5. Performance of nanosized Na4Fe3(PO4)2(P2O7) plates (NFPP-E) and microporous Figure 5. Performance of nanosized Na4Fe3(PO4)2(P2O7) plates (NFPP-E) and microporous Na4Fe3(PO4)2(P2O7) particles (NFPP-C) prepared by sol-gel. (a) Cycling stability of NFPP-E electrodes Na4Fe3(PO4)2(P2O7) particles (NFPP-C) prepared by sol-gel. (a) Cycling stability of NFPP-E electrodes over 250 cycles at 0.2C and 430 cycles at 0.5C. (b) Long-term cycling stability (4400 cycles) at high over 250 cycles at 0.2C and 430 cycles at 0.5C. (b) Long-term cycling stability (4400 cycles) at high rate rate (20C) for both NFPP-E and NFPP-C electrodes. (c) Galvanostatic intermittent titration technique (20C) for both NFPP-E and NFPP-C electrodes. (c) Galvanostatic intermittent titration technique (GITT) curves of NFPP-E material for both charge and discharge processes. The inset is the chemical (GITT) curves of NFPP-E material for both charge and discharge processes. The inset is the chemical diffusion coefficient of Na+ ions as a function of voltage calculated from the GITT profile (after 30 diffusion coefficient of Na+ ions as a function of voltage calculated from the GITT profile (after 30 cycles, current density: 0.05C). (d) The calculated capacitance contribution (shadowed area) to the CV cycles, current density: 0.05C). (d) The calculated capacitance contribution (shadowed area) to the CV curve of NFPP-E at the scan rate of 0.3 mV·s−1. Reproduced with permission from [116]. Copyright curve of NFPP-E at the scan rate of 0.3 mV s−1. Reproduced with permission from [116]. Copyright 2019 Springer Nature. 2019 Springer Nature. The main problem of the NASICON-based cathodes is the low capacity limited to ≈ 100 mA·h·g−1. The main problem of the NASICON-based cathodes is the low capacity limited to ≈ 100 mAh This capacity can be increased by choosing other phosphates. In particular, Na2Fe3(PO4)3/carbon g−1. This capacity can be increased by choosing other phosp−h1ates. In particular, Na2Fe3(PO4)3/carbon nanotube nanocomposite delivered a capacity of 143 mA·h·g , but the problem is shifted to the cycle nanotube nanocomposite delivered a capacity of 143 mA h g−1, but the problem is shifted to the cycle ability, since the capacity was stable over 50 cycles. Partial substitution of Fe for Mn only results in a ability, since the capacity was stable over 50 cycles. Partial substitution of Fe for Mn only results in a decrease of capacity [117]. Fluffy Na0.67FePO4/CNT nanocactus used as a cathode delivered the same capacity, also stable over 50 cycles [118]. Fluorophosphates as cathode materials exhibit similar capacities ≈ 100 mA h g−1 as NASICON, but they have a higher operational voltage so that the loss of energy density is smaller. For instance, orthorhombic Na CoPO F/C delivers a capacity of 107 mA h g−1 with a voltage plateau at 4.3 V [119].PDF Image | Electrode Materials for Sodium-Ion Batteries
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