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Mtengo wokwera kwambiri wa mabatire a all-vanadium flow-through redox (VRFBs) umachepetsa kugwiritsidwa ntchito kwawo kofala.Kupititsa patsogolo ma kinetics a electrochemical reactions ndikofunikira kuti muwonjezere mphamvu zenizeni ndi mphamvu za VRFB, potero kuchepetsa mtengo wa kWh wa VRFB.Mu ntchitoyi, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 ndi C76 / HWO, adayikidwa pamagetsi a nsalu ya carbon ndi kuyesedwa ngati electrocatalysts kwa VO2 +/VO2+ redox reaction.Field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDX), high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier transform Spectroscopy (FTIR) ndi miyeso yolumikizana.Zapezeka kuti kuwonjezera kwa C76 fullerenes ku HWO kungathe kusintha ma electrode kinetics poonjezera mphamvu yamagetsi ndi kupereka magulu ogwira ntchito oxidized pamwamba pake, potero kulimbikitsa VO2 +/VO2+ redox reaction.The HWO/C76 composite (50 wt% C76) idakhala chisankho chabwino kwambiri pakuchita kwa VO2 +/VO2+ ndi ΔEp ya 176 mV, pomwe nsalu ya kaboni yosatulutsidwa (UCC) inali 365 mV.Kuphatikiza apo, gulu la HWO / C76 linawonetsa kulepheretsa kwakukulu pakusintha kwachilengedwe kwa chlorine chifukwa cha gulu la W-OH.
Ntchito zazikulu za anthu komanso kusintha kwachangu kwa mafakitale kwadzetsa kufunikira kwakukulu kwa magetsi, komwe kukuchulukirachulukira pafupifupi 3% pachaka1.Kwa zaka zambiri, kufalikira kwa mafuta oyaka mafuta monga gwero la mphamvu kwachititsa kuti mpweya wowonjezera kutentha utuluke, zomwe zimapangitsa kutentha kwa dziko, kuipitsidwa kwa madzi ndi mpweya, zomwe zikuwopseza chilengedwe chonse.Chotsatira chake, kulowa kwa mphepo yoyera ndi yowonjezereka komanso mphamvu ya dzuwa ikuyembekezeka kufika 75% ya magetsi onse pofika chaka cha 20501. Komabe, pamene gawo la magetsi kuchokera kuzinthu zongowonjezwdwa likuposa 20% ya mphamvu zonse zamagetsi, gululi limakhala losakhazikika.
Pakati pa machitidwe onse osungira mphamvu monga hybrid vanadium redox flow battery2, all-vanadium redox flow battery (VRFB) yapanga mofulumira kwambiri chifukwa cha ubwino wake wambiri ndipo imatengedwa kuti ndi njira yabwino yothetsera mphamvu yosungira nthawi yaitali (pafupi zaka 30).) Zosankha kuphatikiza ndi mphamvu zongowonjezwdwa4.Izi zimachitika chifukwa cha kulekanitsidwa kwa mphamvu ndi kachulukidwe ka mphamvu, kuyankha mofulumira, moyo wautali wautumiki, ndi mtengo wochepa wapachaka wa $ 65 / kWh poyerekeza ndi $ 93-140 / kWh kwa Li-ion ndi mabatire a lead-acid ndi 279-420 US dollars pa kWh.batire motsatana 4.
Komabe, malonda awo akuluakulu amakakamizikabe ndi ndalama zawo zotsika mtengo, makamaka chifukwa cha ma cell stacks4,5.Chifukwa chake, kuwongolera magwiridwe antchito powonjezera ma kinetics azinthu ziwiri za theka kumatha kuchepetsa kukula kwa stack ndikuchepetsa mtengo.Chifukwa chake, kusuntha kwa ma elekitironi mwachangu kupita kumtunda ndikofunikira, zomwe zimatengera kapangidwe kake, kapangidwe kake ndi kapangidwe ka electrode ndipo zimafunikira kukhathamiritsa mosamala6.Ngakhale kukhazikika kwamankhwala ndi electrochemical komanso kukhazikika kwamagetsi kwamagetsi a carbon electrode, kinetics yawo yosagwiritsidwa ntchito imakhala yaulesi chifukwa cha kusowa kwamagulu ogwiritsira ntchito mpweya ndi hydrophilicity7,8.Chifukwa chake, ma electrocatalyst osiyanasiyana amaphatikizidwa ndi ma elekitirodi opangidwa ndi kaboni, makamaka ma carbon nanostructures ndi oxides zitsulo, kuti apititse patsogolo ma kinetics a maelekitirodi onse awiri, potero akuwonjezera ma kinetics a electrode ya VRFB.
Kuphatikiza pa ntchito yathu yapitayi pa C76, tidayamba kunena za ntchito yabwino kwambiri ya electrocatalytic ya fullerene iyi ya VO2+/VO2+, kutumiza ndalama, poyerekeza ndi nsalu yotenthetsera komanso yopanda mpweya.Kukana kumachepetsedwa ndi 99.5% ndi 97%.Kuchita kwamphamvu kwa zida za kaboni pakuchita kwa VO2+/VO2+ poyerekeza ndi C76 kukuwonetsedwa mu Table S1.Kumbali ina, ma oxides ambiri achitsulo monga CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 ndi WO331, 32, 33, 34, 35, 36, 37 akhala akugwiritsidwa ntchito chifukwa chakuchulukira kwawo konyowa komanso kugwira ntchito kwa okosijeni wambiri., 38. gulu.Ntchito yothandiza ya ma oxides achitsulo awa mumayendedwe a VO2+/VO2+ akuwonetsedwa mu Table S2.WO3 yakhala ikugwiritsidwa ntchito pazinthu zambiri chifukwa cha mtengo wake wotsika mtengo, kukhazikika kwapamwamba muzofalitsa za acidic, ndi ntchito yothandiza kwambiri31,32,33,34,35,36,37,38.Komabe, kusintha kwa cathodic kinetics chifukwa cha WO3 ndikochepa.Kupititsa patsogolo kayendedwe ka WO3, zotsatira zogwiritsira ntchito kuchepetsedwa kwa tungsten oxide (W18O49) pa ntchito ya cathodic inayesedwa38.Hydrated tungsten oxide (HWO) sinayesedwepo mu ntchito za VRFB, ngakhale ikuwonetsa ntchito yowonjezereka mu ntchito za supercapacitor chifukwa cha kufalikira kwa cation mofulumira poyerekeza ndi anhydrous WOx39,40.Batire ya m'badwo wachitatu ya vanadium redox flow flow imagwiritsa ntchito ma electrolyte osakanikirana a asidi opangidwa ndi HCl ndi H2SO4 kuwongolera magwiridwe antchito a batri ndikuwongolera kusungunuka ndi kukhazikika kwa ma ion vanadium mu electrolyte.Komabe, chisinthiko cha parasitic chlorine chakhala chimodzi mwazovuta za m'badwo wachitatu, kotero kufunafuna njira zoletsa kuwunika kwa chlorine kwakhala cholinga chamagulu angapo ofufuza.
Apa, kuyesa kwa VO2+/VO2+ kunachitika pamagulu a HWO/C76 omwe adayikidwa pamagetsi ansalu ya kaboni kuti apeze kukhazikika pakati pa madulidwe amagetsi a ma kompositi ndi redox kinetics yapamtunda wa elekitirodi ndikupondereza chisinthiko cha parasitic chlorine.yankho (CER).Hydrated tungsten okusayidi (HWO) nanoparticles anali apanga ndi losavuta hydrothermal njira.Kuyesera kunachitika mu osakaniza asidi electrolyte (H2SO4/HCl) kutsanzira m'badwo wachitatu VRFB (G3) kuti n'zothandiza ndi kufufuza zotsatira za HWO pa parasitic klorini chisinthiko anachita.
Vanadium (IV) sulfate hydrate (VOSO4, 99.9%, Alfa-Aeser), sulfuric acid (H2SO4), hydrochloric acid (HCl), dimethylformamide (DMF, Sigma-Aldrich), polyvinylidene fluoride (PVDF, Sigma)-Aldrich), sodium Tungstenphilic oxide, 9 hydrochloric acid, 9 hydrochloric dihydrate nsalu ELAT (Fuel Cell Store) anagwiritsidwa ntchito mu phunziroli.
Hydrated tungsten oxide (HWO) inakonzedwa ndi hydrothermal reaction 43 momwe 2 g ya mchere wa Na2WO4 inasungunuka mu 12 ml ya H2O kuti ipereke njira yopanda mtundu, ndiye 12 ml ya 2 M HCl inawonjezeredwa dropwise kuti apereke kuyimitsidwa kwachikasu.The slurry anaikidwa mu Teflon yokutidwa zosapanga dzimbiri autoclave ndi kusungidwa mu uvuni pa 180 ° C. kwa 3 hours chifukwa hydrothermal reaction.Chotsaliracho chinasonkhanitsidwa ndi kusefera, kutsukidwa katatu ndi ethanol ndi madzi, zouma mu uvuni pa 70 ° C kwa ~ 3 maola, ndiyeno triturated kupereka buluu-imvi HWO ufa.
Ma electrode a nsalu ya carbon (CCT) omwe adapezedwa (osagwiritsidwa ntchito) adagwiritsidwa ntchito monga momwe amachitira kapena kutentha mu ng'anjo ya chubu pa 450 ° C mumlengalenga ndi kutentha kwa 15 ºC / min kwa maola 10 kuti apeze ma CC (TCC).monga tafotokozera m'nkhani yapitayi24.UCC ndi TCC zidadulidwa kukhala maelekitirodi pafupifupi 1.5 cm mulifupi ndi 7 cm utali.Kuyimitsidwa kwa C76, HWO, HWO-10% C76, HWO-30% C76 ndi HWO-50% C76 anakonzedwa powonjezera 20 mg .% (~ 2.22 mg) wa PVDF binder kwa ~ 1 ml DMF ndi sonicated kwa ola limodzi kuti apititse patsogolo kufanana.2 mg ya C76, HWO ndi HWO-C76 zophatikizika zidagwiritsidwa ntchito motsatizana ku UCC yogwira ma elekitirodi dera pafupifupi 1.5 cm2.Zothandizira zonse zidakwezedwa pa ma elekitirodi a UCC ndipo TCC idagwiritsidwa ntchito pofananiza zokha, monga momwe ntchito yathu yapitayi idawonetsa kuti chithandizo cha kutentha sichinali chofunikira24.Kukhazikika kwamalingaliro kunatheka potsuka 100 µl ya kuyimitsidwa (katundu wa 2 mg) kuti mukhale ndi mphamvu zambiri.Kenako maelekitirodi onse anaumitsidwa mu uvuni pa 60 ° C. usiku wonse.Ma elekitirodi amayezedwa kutsogolo ndi kumbuyo kuti atsimikizire kuti katundu wanyamula.Kuti mukhale ndi malo enaake a geometric (~ 1.5 cm2) ndikuletsa kukwera kwa vanadium electrolyte ku electrode chifukwa cha mphamvu ya capillary, parafini yopyapyala inayikidwa pazitsulo zogwira ntchito.
Munda wa emission scanning electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) unagwiritsidwa ntchito kuyang'ana kapangidwe ka HWO pamwamba.Makina owonera mphamvu a X-ray okhala ndi Feii8SEM (EDX, Zeiss Inc.) adagwiritsidwa ntchito kupanga mapu azinthu za HWO-50%C76 pamagetsi a UCC.Ma electron microscope (HR-TEM, JOEL JEM-2100) omwe amagwira ntchito pamagetsi othamanga a 200 kV adagwiritsidwa ntchito kufanizira tinthu tating'ono ta HWO ndi mphete za diffraction.Pulogalamu ya Crystallography Toolbox (CrysTBox) imagwiritsa ntchito ntchito ya ringGUI kusanthula mawonekedwe a HWO ring diffraction ndikufanizira zotsatira ndi mawonekedwe a XRD.Mapangidwe ndi graphitization ya UCC ndi TCC idawunikidwa ndi X-ray diffraction (XRD) pamlingo wa 2.4 ° / min kuchokera ku 5 ° mpaka 70 ° ndi Cu Kα (λ = 1.54060 Å) pogwiritsa ntchito Panalytical X-ray diffractometer (Model 3600).XRD idawonetsa mawonekedwe a kristalo ndi gawo la HWO.Pulogalamu ya PANalytical X'Pert HighScore idagwiritsidwa ntchito kufananitsa nsonga za HWO ndi mamapu a tungsten oxide omwe amapezeka mu database45.Zotsatira za HWO zidafaniziridwa ndi zotsatira za TEM.Kapangidwe ka mankhwala ndi mawonekedwe a HWO zitsanzo adatsimikiziridwa ndi X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).Pulogalamu ya CASA-XPS (v 2.3.15) idagwiritsidwa ntchito pakuchepetsa kwambiri komanso kusanthula deta.Kuti mudziwe magulu ogwirira ntchito a HWO ndi HWO-50% C76, miyeso idapangidwa pogwiritsa ntchito mawonekedwe a Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, pogwiritsa ntchito KBr FTIR).Zotsatira zinafaniziridwa ndi zotsatira za XPS.Miyezo yolumikizirana (KRUSS DSA25) idagwiritsidwanso ntchito kuwonetsa kunyowa kwa ma elekitirodi.
Pamiyezo yonse yama electrochemical, malo ogwirira ntchito a Biologic SP 300 adagwiritsidwa ntchito.Cyclic voltammetry (CV) ndi electrochemical impedance spectroscopy (EIS) anagwiritsidwa ntchito pofufuza ma elekitirodi kinetics a VO2+/VO2+ redox reaction ndi zotsatira za reagent diffusion (VOSO4(VO2+)) pa mlingo anachita.Njira zonse ziwirizi zinagwiritsa ntchito selo la electrode katatu ndi electrolyte ndende ya 0.1 M VOSO4 (V4+) mu 1 M H2SO4 + 1 M HCl (kusakaniza kwa ma asidi).Deta yonse ya electrochemical yoperekedwa ndi IR yokonzedwa.Ma electrode a calomel electrode (SCE) ndi platinamu (Pt) adagwiritsidwa ntchito ngati cholumikizira ndi chowerengera, motsatana.Kwa CV, ma scan rates (ν) a 5, 20, ndi 50 mV / s adagwiritsidwa ntchito pawindo la VO2 +/VO2 + la (0-1) V vs. SCE, kenaka kusinthidwa kuti SHE apange chiwembu (VSCE = 0.242 V vs. HSE) .Kuti muphunzire kasungidwe ka ntchito ya electrode, ma CV obwerezabwereza adachitidwa pa ν 5 mV/s kwa UCC, TCC, UCC-C76, UCC-HWO, ndi UCC-HWO-50% C76.Pamiyezo ya EIS, ma frequency osiyanasiyana a VO2+/VO2+ redox reaction anali 0.01-105 Hz, ndipo kusokoneza kwamagetsi pamagetsi otseguka (OCV) kunali 10 mV.Kuyesera kulikonse kunabwerezedwa nthawi 2-3 kuti zitsimikizire kuti zotsatira zake zikugwirizana.Zosintha zosasinthika (k0) zidapezedwa ndi njira ya Nicholson46,47.
Hydrated tungsten oxide (HVO) yapangidwa bwino ndi njira ya hydrothermal.Chithunzi cha SEM1a ikuwonetsa kuti HWO yosungidwa imakhala ndi magulu a nanoparticles okhala ndi makulidwe a 25-50 nm.
Mawonekedwe a X-ray diffraction a HWO amasonyeza nsonga (001) ndi (002) pa ~ 23.5 ° ndi ~ 47.5 °, motero, zomwe zimakhala ndi mawonekedwe a nonstoichiometric WO2.63 (W32O84) (PDF 077-0810, a = 21.4 Å Å γ =, b Å 8 = , b Å 8 = , b = Å 8 = , b = 1 = 1 = Å , b = 1 = 1 = 1, b = 1 = 1 = 1 = 1 = 1. 90 °), yomwe imagwirizana ndi mtundu wawo wabuluu womveka bwino (mkuyu 1b) 48.49.Mapiri ena pafupifupi 20.5 °, 27.1 °, 28.1 °, 30.8 °, 35.7 °, 36.7 ° ndi 52.7 ° adapatsidwa (140), (620), (350), (720), (740), (560 °).)) ndi (970) diffraction ndege orthogonal ku WO2.63, motsatana.Njira yopangira yomweyi idagwiritsidwa ntchito ndi Songara et al.43 kuti apeze chopangidwa choyera, chomwe chidachitika chifukwa cha kukhalapo kwa WO3(H2O) 0.333.Komabe, mu ntchitoyi, chifukwa cha zikhalidwe zosiyanasiyana, mankhwala a buluu-imvi anapezedwa, kusonyeza kuti WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90 °) ndi mawonekedwe ochepetsedwa a oxide.Kusanthula kwa semiquantitative pogwiritsa ntchito pulogalamu ya X'Pert HighScore kunawonetsa 26% WO3(H2O)0.333:74% W32O84.Popeza W32O84 ili ndi W6+ ndi W4+ (1.67:1 W6+:W4+), zomwe zikuyerekezeredwa za W6+ ndi W4+ ndi pafupifupi 72% W6+ ndi 28% W4+, motsatana.Zithunzi za SEM, mawonekedwe a 1-sekondi XPS pamlingo wapakati, zithunzi za TEM, mawonekedwe a FTIR, ndi mawonekedwe a Raman a tinthu tating'ono ta C76 adawonetsedwa m'nkhani yathu yapitayi.Malingana ndi Kawada et al.,50,51 X-ray diffraction ya C76 pambuyo pochotsa toluene inasonyeza mawonekedwe a monoclinic a FCC.
Zithunzi za SEM mu mkuyu.2a ndi b akuwonetsa kuti HWO ndi HWO-50% C76 adayikidwa bwino ndi pakati pa ma fiber a carbon a UCC electrode.Mapu a EDX a tungsten, kaboni, ndi mpweya pazithunzi za SEM mumkuyu.2c ikuwonetsedwa mkuyu.2d-f kusonyeza kuti tungsten ndi kaboni ndizosakanikirana (zosonyeza kugawa kofanana) pamtunda wonse wa electrode ndipo chophatikizikacho sichimayikidwa mofanana chifukwa cha chikhalidwe cha njira yoyikamo.
Zithunzi za SEM za tinthu tating'ono ta HWO (a) ndi HWO-C76 (b).Mapu a EDX pa HWO-C76 atayikidwa pa UCC pogwiritsa ntchito malo omwe ali pachithunzi (c) akuwonetsa kugawidwa kwa tungsten (d), carbon (e), ndi mpweya (f) mu chitsanzo.
HR-TEM idagwiritsidwa ntchito pojambula kukweza kwakukulu ndi chidziwitso cha crystallographic (Chithunzi 3).HWO imasonyeza morphology ya nanocube monga momwe tawonetsera mkuyu 3a komanso momveka bwino mu Chithunzi 3b.Mwa kukulitsa nanocube chifukwa cha diffraction ya madera osankhidwa, munthu akhoza kuwona mawonekedwe a grating ndi ndege zowonongeka zomwe zimakwaniritsa lamulo la Bragg, monga momwe tawonetsera mkuyu 3c, yomwe imatsimikizira crystallinity ya zinthu.M'magawo a Chithunzi 3c amasonyeza mtunda wa d 3.3 Å wofanana ndi (022) ndi (620) ndege zowonongeka zomwe zimapezeka mu WO3 (H2O) 0.333 ndi W32O84 magawo, motsatira43,44,49.Izi zimagwirizana ndi kusanthula kwa XRD komwe kufotokozedwa pamwambapa (mkuyu 1b) popeza mtunda wa ndege wowonera d (mkuyu 3c) umagwirizana ndi nsonga yamphamvu kwambiri ya XRD pachitsanzo cha HWO.Zitsanzo mphete zikuwonetsedwanso mkuyu.3d, pomwe mphete iliyonse imagwirizana ndi ndege yosiyana.Ndege za WO3 (H2O) 0.333 ndi W32O84 zimakhala zoyera ndi zabuluu, motero, nsonga zawo za XRD zogwirizana nazo zikuwonetsedwanso mkuyu 1b.Mphete yoyamba yomwe ikuwonetsedwa pa chithunzi cha mphete ikufanana ndi nsonga yoyamba yodziwika bwino pazithunzi za x-ray ya (022) kapena (620) ndege yosokoneza.Kuchokera pa (022) mpaka (402) mphete, d-spacing values ​​​​ndi 3.30, 3.17, 2.38, 1.93, ndi 1.69 Å, mogwirizana ndi XRD values ​​​​ya 3.30, 3.17, 2, 45, 1.93.ndi 1.66 Å, yomwe ili yofanana ndi 44, 45, motsatira.
(a) Chithunzi cha HR-TEM cha HWO, (b) chikuwonetsa chithunzi chokulitsa.Zithunzi za ndege zopangira grating zikuwonetsedwa mu (c), mkati (c) zikuwonetsa chithunzi chokulirapo cha ndege ndi phula d la 0.33 nm lolingana ndi (002) ndi (620) ndege.(d) Chitsanzo cha mphete cha HWO chosonyeza ndege zogwirizana ndi WO3 (H2O) 0.333 (zoyera) ndi W32O84 (buluu).
Kusanthula kwa XPS kudachitika kuti adziwe momwe chemistry ndi oxidation state of tungsten (Zithunzi S1 ndi 4).Mitundu yosiyanasiyana ya XPS scan ya HWO yopangidwa ikuwonetsedwa mu Chithunzi S1, kuwonetsa kukhalapo kwa tungsten.Mawonekedwe a XPS ang'onoang'ono a W 4f ndi O 1s core levels akuwonetsedwa mu Mkuyu.4a ndi b, motsatana.Sipekitiramu ya W 4f imagawanika kukhala mipiringidzo iwiri yozungulira yogwirizana ndi mphamvu zomangirira za W oxidation state.ndi W 4f7/2 pa 36.6 ndi 34.9 eV ndi khalidwe la W4+ boma la 40, motero.0.333.Zomwe zayikidwa zikuwonetsa kuti maperesenti a atomiki a W6+ ndi W4+ ndi 85% ndi 15%, motsatana, omwe ali pafupi ndi zomwe zikuyerekezedwa kuchokera ku data ya XRD poganizira za kusiyana kwa njira ziwirizi.Njira zonsezi zimapereka chidziwitso chochepa kwambiri, makamaka XRD.Komanso, njira ziwirizi zimasanthula magawo osiyanasiyana azinthuzo chifukwa XRD ndi njira yochulukirapo pomwe XPS ndi njira yapamtunda yomwe imayandikira ma nanometer ochepa.Mawonekedwe a O 1s amagawidwa nsonga ziwiri pa 533 (22.2%) ndi 530.4 eV (77.8%).Yoyamba ikufanana ndi OH, ndipo yachiwiri ndi zomangira za okosijeni mu lattice mu WO.Kukhalapo kwa magulu ogwira ntchito a OH kumagwirizana ndi mphamvu za hydration za HWO.
Kusanthula kwa FTIR kudachitikanso pamiyeso iwiriyi kuti awone kukhalapo kwamagulu ogwira ntchito ndikugwirizanitsa mamolekyu amadzi mumpangidwe wa HWO wa hydrated.Zotsatira zimasonyeza kuti chitsanzo cha HWO-50% C76 ndi zotsatira za FT-IR HWO zimawoneka zofanana chifukwa cha kukhalapo kwa HWO, koma kukula kwa nsonga kumasiyana chifukwa cha kuchuluka kwa zitsanzo zomwe zimagwiritsidwa ntchito pokonzekera kusanthula (mkuyu 5a).) HWO-50% C76 imasonyeza kuti nsonga zonse, kupatulapo nsonga ya tungsten oxide, zimagwirizana ndi fullerene 24. Mwatsatanetsatane mu mkuyu.5a ikuwonetsa kuti zitsanzo zonsezi zikuwonetsa gulu lolimba kwambiri lokhala ndi ~ 710/cm lomwe limalumikizidwa ndi ma oscillation a OWO mu HWO lattice kapangidwe, ndi phewa lolimba pa ~ 840/cm lotchedwa WO.Potambasula ma vibrate, gulu lakuthwa pafupifupi 1610/cm limadziwika ndi kugwedezeka kwa OH, pomwe gulu lalikulu la mayamwidwe pafupifupi 3400/cm limalumikizidwa ndi kugwedezeka kwa OH m'magulu a hydroxyl43.Zotsatira izi zimagwirizana ndi mawonekedwe a XPS mu Fig.4b, komwe magulu ogwira ntchito a WO atha kupereka masamba omwe akugwira ntchito pakuchita kwa VO2+/VO2+.
Kusanthula kwa FTIR kwa HWO ndi HWO-50% C76 (a), kunawonetsa magulu ogwira ntchito komanso miyeso yolumikizirana (b, c).
Gulu la OH lingathenso kuchititsa kuti VO2 +/VO2+ ichitike, pamene ikuwonjezera hydrophilicity ya electrode, potero kulimbikitsa kuchuluka kwa kufalikira ndi kusintha kwa ma elekitironi.Monga momwe tawonetsera, chitsanzo cha HWO-50% C76 chikuwonetsa nsonga yowonjezera ya C76.Pamwamba pa ~ 2905, 2375, 1705, 1607, ndi 1445 cm3 akhoza kuperekedwa ku CH, O=C=O, C=O, C=C, ndi CO kutambasula kugwedezeka, motero.Ndizodziwika bwino kuti magulu ogwiritsira ntchito okosijeni C=O ndi CO amatha kukhala malo ogwirira ntchito a redox ya vanadium.Kuyesa ndi kuyerekezera kunyowa kwa ma electrode awiri, miyeso ya angle yolumikizana idatengedwa monga momwe tawonetsera mkuyu 5b, c.Ma electrode a HWO nthawi yomweyo adayamwa madontho amadzi, kuwonetsa superhydrophilicity chifukwa cha magulu ogwira ntchito a OH.HWO-50% C76 imakhala ya hydrophobic kwambiri, yokhala ndi ngodya yolumikizana pafupifupi 135 ° pakadutsa masekondi 10.Komabe, mumiyeso yamagetsi, ma elekitirodi a HWO-50% C76 adanyowa kwathunthu pasanathe mphindi imodzi.Miyezo ya kunyowa imagwirizana ndi zotsatira za XPS ndi FTIR, zomwe zikuwonetsa kuti magulu ambiri a OH pamtunda wa HWO amapangitsa kuti ikhale ya hydrophilic.
Zochita za VO2+/VO2+ za HWO ndi HWO-C76 nanocomposites zinayesedwa ndipo zinkayembekezeredwa kuti HWO idzapondereza kusintha kwa chlorine mu VO2+/VO2+ reaction mu osakaniza asidi, ndipo C76 idzalimbikitsanso VO2+/VO2+ redox yomwe ikufunika.%, 30%, ndi 50% C76 mu kuyimitsidwa kwa HWO ndi CCC yoyikidwa pamagetsi odzaza pafupifupi 2 mg/cm2.
Monga momwe tawonetsera mkuyu.6, ma kinetics a VO2 +/VO2+ reaction pa electrode pamwamba adawunikidwa ndi CV mu osakaniza acidic electrolyte.Mafunde akuwonetsedwa ngati I/Ipa kuti afanizire mosavuta ΔEp ndi Ipa/Ipc pazothandizira zosiyanasiyana mwachindunji pa graph.Zomwe zilipo panopa zikuwonetsedwa mu Chithunzi 2S.Pa mkuyu.Chithunzi 6a chikuwonetsa kuti HWO imawonjezera pang'ono kuchuluka kwa ma elekitironi kutengerapo kwa VO2+/VO2+ redox reaction pamtunda wa elekitirodi ndikupondereza momwe chisinthiko cha parasitic chlorine.Komabe, C76 imakulitsa kwambiri kuchuluka kwa ma elekitironi kutengerapo ndipo imathandizira kusintha kwa chlorine.Chifukwa chake, gulu lopangidwa bwino la HWO ndi C76 likuyembekezeka kukhala ndi ntchito yabwino kwambiri komanso kuthekera kwakukulu koletsa kusinthika kwa klorini.Zinapezeka kuti pambuyo poonjezera zomwe zili mu C76, ntchito ya electrochemical ya electrode yakula bwino, monga momwe zikuwonekera ndi kuchepa kwa ΔEp ndi kuwonjezeka kwa chiwerengero cha Ipa / Ipc (Table S3).Izi zinatsimikiziridwanso ndi ma RCT values ​​​​otengedwa kuchokera ku chiwembu cha Nyquist mu Chithunzi 6d (Table S3), chomwe chinapezeka kuti chikuchepa ndi kuchuluka kwa C76.Zotsatira izi zikugwirizananso ndi kafukufuku wa Li, momwe kuwonjezera kwa mesoporous carbon ku mesoporous WO3 kunawonetsa kusintha kwa ma kinetics pa VO2+/VO2+35.Izi zikuwonetsa kuti kuyankha kwachindunji kungadalire kwambiri pa electrode conductivity (C = C bond) 18, 24, 35, 36, 37. Izi zikhoza kukhala chifukwa cha kusintha kwa geometry yogwirizanitsa pakati pa [VO (H2O) 5] 2+ ndi [VO2 (H2O) 4]+, C76 imachepetsa mphamvu zowonongeka mwa kuchepetsa mphamvu zowonongeka.Komabe, izi sizingakhale zotheka ndi ma elekitirodi a HWO.
(a) Cyclic voltammetric behaviour (ν = 5 mV/s) ya VO2+/VO2+ reaction ya UCC ndi HWO-C76 ma composite okhala ndi HWO:C76 ma ratios osiyanasiyana mu 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik ndi (c) Nicholson VO2+/VO2+ njira yowunikira kufalikira kwabwino komanso kupeza ma k0(d) mikhalidwe.
Sikuti HWO-50% C76 yokha inali kuwonetsa pafupifupi ntchito yofanana ya electrocatalytic monga C76 ya VO2 +/VO2+ reaction, koma, chochititsa chidwi kwambiri, inaletsanso kusinthika kwa chlorine poyerekeza ndi C76, monga momwe tawonetsera mkuyu.6d (otsika RCT).C76 anasonyeza apamwamba zikuoneka Ipa/Ipc kuposa HWO-50% C76 (Table S3), osati chifukwa cha bwino anachita reversibility, koma chifukwa cha nsonga zikuphatikizana wa chlorine kuchepetsa anachita ndi SHE pa 1.2 V. The bwino ntchito ya HWO- The 50% C76 amachokera ku synergistic charger ndi mkulu C76 zotsatira zoipa ndi WH-ophatikizika WH ndi mkulu caligt calculical pakati pa WH-charged ndi WH-C76 kwambiri. pa HWO.Kuchepa kwa klorini kumapangitsa kuti ma cell azilipiritsa bwino, pomwe ma kinetics owongolera amathandizira kuti mphamvu yamagetsi yonse ya cell ikhale yabwino.
Malinga ndi equation S1, pamachitidwe a quasi-reversible (ocheperako pang'onopang'ono ma elekitironi) amayendetsedwa ndi kufalikira, nsonga yapano (IP) imadalira kuchuluka kwa ma elekitironi (n), dera la ma elekitirodi (A), coefficient coefficient (D), kuchuluka kwa ma elekitironi kusamutsa coefficient (α) ndi liwiro la sikani (ν).Pofuna kuphunzira khalidwe loyendetsedwa ndi kufalikira kwa zipangizo zoyesedwa, ubale pakati pa IP ndi ν1/2 unakonzedwa ndikuwonetsedwa mu Chithunzi 6b.Popeza zida zonse zikuwonetsa ubale wofananira, zomwe zimayendetsedwa ndi kufalikira.Popeza kuti VO2 +/VO2+ reaction ndi quasi-reversible, kutsetsereka kwa mzere kumadalira kufalikira kwa coefficient ndi mtengo wa α (equation S1).Popeza kuchuluka kwa ma electron kumakhala kosalekeza (≈ 4 × 10-6 cm2/s) 52, kusiyana kwa malo otsetsereka a mzerewo kumawonetsa mikhalidwe yosiyana ya α, motero kutengera kwa ma elekitironi pamtunda wa elekitirodi, komwe kumawonetsedwa kwa C76 ndi HWO -50% C76 Motsetsereka wotsetsereka kwambiri wa ma elekitironi.
Malo otsetsereka a Warburg (W) owerengera mafupipafupi otsika omwe akuwonetsedwa mu Table S3 (mkuyu 6d) ali ndi mfundo pafupi ndi 1 ya zipangizo zonse, kusonyeza kufalikira kwabwino kwa mitundu ya redox ndikutsimikizira khalidwe lapamwamba la IP poyerekeza ndi ν1/ 2. CV imayesedwa.Kwa HWO-50% C76, malo otsetsereka a Warburg amapatuka kuchokera ku 1 kupita ku 1.32, kuwonetsa osati kufalikira kwa theka-malire kwa reagent (VO2+), komanso kuthandizira kotheka kwa khalidwe laling'ono-wochepa thupi ku khalidwe la kufalikira chifukwa cha electrode porosity.
Kuti muwunikenso kusinthika (kuchuluka kwa ma elekitironi) kwa VO2+/VO2+ redox reaction, njira ya Nicholson quasi-reversible reaction idagwiritsidwanso ntchito kudziwa mulingo wokhazikika wa k041.42.Izi zimachitika pogwiritsa ntchito equation ya S2 kuti apange parameter ya kinetic yopanda dimensionless Ψ, yomwe ndi ntchito ya ΔEp, monga ntchito ya ν-1/2.Table S4 ikuwonetsa Ψ zomwe zimapezedwa pamtundu uliwonse wa electrode.Zotsatira (mkuyu 6c) adakonzedwa kuti apeze k0 × 104 cm / s kuchokera kumalo otsetsereka a chiwembu chilichonse pogwiritsa ntchito Equation S3 (yolembedwa pafupi ndi mzere uliwonse ndikuwonetsedwa mu Table S4).HWO-50% C76 inapezeka kuti ili ndi malo otsetsereka kwambiri (mkuyu 6c), motero mtengo wapamwamba wa k0 ndi 2.47 × 10-4 cm / s.Izi zikutanthauza kuti electrode iyi imakwaniritsa kinetics yothamanga kwambiri, yomwe imagwirizana ndi CV ndi EIS zotsatira mu Fig. 6a ndi d ndi Table S3.Kuonjezera apo, mtengo wa k0 unapezedwanso kuchokera ku chiwembu cha Nyquist (Mkuyu 6d) wa Equation S4 pogwiritsa ntchito mtengo wa RCT (Table S3).Zotsatira za k0 izi kuchokera ku EIS ndizofupikitsidwa mu Table S4 komanso zikuwonetsa kuti HWO-50% C76 ikuwonetsa kuchuluka kwa ma elekitironi apamwamba kwambiri chifukwa cha synergistic effect.Ngakhale kuti ma k0 amasiyana chifukwa cha magwero osiyanasiyana a njira iliyonse, amawonetsabe dongosolo lomwelo la ukulu ndikuwonetsa kusasinthika.
Kuti mumvetsetse bwino ma kinetics omwe adapezedwa, ndikofunikira kufananiza zida zabwino kwambiri zama elekitirodi ndi ma elekitirodi osatsekedwa a UCC ndi TCC.Kwa VO2 +/VO2 + reaction, HWO-C76 sinangowonetsa otsika kwambiri ΔEp komanso kusinthika bwino, komanso kupondereza kwambiri kusinthika kwa parasitic chlorine poyerekeza ndi TCC, monga momwe zimayesedwera pano pa 1.45 V wachibale ndi SHE (Mkuyu 7a).Pankhani ya kukhazikika, tinkaganiza kuti HWO-50% C76 inali yokhazikika mwakuthupi chifukwa chothandizira chinali chosakanikirana ndi PVDF binder ndipo kenako chimagwiritsidwa ntchito pamagetsi a carbon cloth.HWO-50% C76 inawonetsa kusintha kwakukulu kwa 44 mV (kuwonongeka kwa 0.29 mV / cycle) pambuyo pa 150 mizunguliro poyerekeza ndi 50 mV kwa UCC (Chithunzi 7b).Izi sizingakhale kusiyana kwakukulu, koma ma kinetics a maelekitirodi a UCC ndi ochedwa kwambiri ndipo amawononga ndi kupalasa njinga, makamaka chifukwa cha kusintha.Ngakhale kusinthika kwa TCC kuli bwino kwambiri kuposa UCC, TCC idapezeka kuti ili ndi kusintha kwakukulu kwa 73 mV pambuyo pa 150 cycle, zomwe zingakhale chifukwa cha kuchuluka kwa klorini komwe kumapangidwa pamwamba pake.kotero kuti chothandizira amamatira bwino ndi electrode pamwamba.Monga momwe tingawonere kuchokera ku ma electrode onse oyesedwa, ngakhale maelekitirodi opanda zida zothandizira anawonetsa kusinthasintha kosiyanasiyana kwa kupalasa njinga, kutanthauza kuti kusintha kwa kupatukana kwakukulu panthawi yoyendetsa njinga kumachitika chifukwa cha kutsekedwa kwa zinthu zomwe zimayambitsidwa ndi kusintha kwa mankhwala m'malo mwa kupatukana koyambitsa.Komanso, ngati kuchuluka kwa chothandizira particles anali kuti analekanitsidwa ndi elekitirodi pamwamba, izi zingachititse kuwonjezeka kwambiri pachimake kulekana (osati 44 mV), popeza gawo lapansi (UCC) ndi wosagwira ntchito kwa VO2 +/VO2+ redox anachita.
Kuyerekeza kwa CV ya zinthu zabwino kwambiri za electrode poyerekeza ndi UCC (a) ndi kukhazikika kwa VO2 +/VO2+ redox reaction (b).ν = 5 mV/s pa ma CV onse mu 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Kuti muwonjezere kukopa kwachuma kwaukadaulo wa VRFB, kukulitsa ndikumvetsetsa ma kinetics a vanadium redox ndikofunikira kuti mukwaniritse bwino mphamvu zamagetsi.Ma Composites HWO-C76 adakonzedwa ndipo mphamvu yawo ya electrocatalytic pa VO2 +/VO2+ reaction idaphunziridwa.HWO idawonetsa kukwezeka pang'ono kwa kinetic mu ma electrolyte osakanikirana a acidic koma kupondereza kusinthika kwa chlorine.Magawo osiyanasiyana a HWO: C76 adagwiritsidwa ntchito kuti apititse patsogolo ma kinetics a ma elekitirodi a HWO.Kuchulukitsa C76 kupita ku HWO kumapangitsa kuti ma elekitironi asamuke ma kinetics a VO2+/VO2+ pa electrode yosinthidwa, pomwe HWO-50% C76 ndiye chinthu chabwino kwambiri chifukwa amachepetsa kukana kutengera ndalama komanso kupondereza chlorine poyerekeza ndi C76 ndi TCC deposit..Izi zimachitika chifukwa cha mgwirizano pakati pa C=C sp2 hybridization, OH ndi W-OH magulu ogwira ntchito.Chiwopsezo chowonongeka pambuyo pa kukwera njinga mobwerezabwereza kwa HWO-50% C76 kunapezeka kuti ndi 0.29 mV / cycle, pamene kuwonongeka kwa UCC ndi TCC ndi 0.33 mV / cycle ndi 0.49 mV / cycle, motero, kumapangitsa kuti ikhale yolimba kwambiri.mu osakaniza asidi electrolytes.Zotsatira zomwe zaperekedwa zimazindikira bwino zida zama elekitirodi pamachitidwe a VO2+/VO2+ okhala ndi kinetics mwachangu komanso kukhazikika kwakukulu.Izi zidzawonjezera mphamvu yamagetsi, potero kuonjezera mphamvu ya VRFB, motero kuchepetsa mtengo wa malonda ake amtsogolo.
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