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Ib tug carousel uas qhia peb slides nyob rau tib lub sij hawm.Siv cov nyees khawm dhau los thiab Tom ntej kom txav mus los ntawm peb qhov swb ib zaug, lossis siv cov khawm slider thaum kawg kom txav mus los ntawm peb qhov swb ib zaug.
Tus nqi siab ntawm tag nrho-vanadium ntws-los ntawm redox roj teeb (VRFBs) txwv lawv txoj kev siv dav.Kev txhim kho cov kinetics ntawm electrochemical tshuaj tiv thaiv yuav tsum tau ua kom lub zog tshwj xeeb thiab lub zog efficiency ntawm VRFB, yog li txo tus nqi ntawm kWh ntawm VRFB.Hauv kev ua haujlwm no, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 thiab C76 / HWO, tau muab tso rau ntawm cov ntaub ntawv carbon electrodes thiab sim ua electrocatalysts rau VO2 + / VO2 + redox cov tshuaj tiv thaiv.Field emission scanning electron microscopy (FESEM), zog 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 ( ntsuas FT.)Nws tau pom tias qhov sib ntxiv ntawm C76 fullerenes rau HWO tuaj yeem txhim kho electrode kinetics los ntawm kev nce hluav taws xob conductivity thiab muab oxidized functional pawg ntawm nws nto, yog li txhawb VO2 + / VO2 + redox cov tshuaj tiv thaiv.HWO / C76 composite (50 wt% C76) ua pov thawj yog qhov kev xaiv zoo tshaj plaws rau VO2 + / VO2 + cov tshuaj tiv thaiv nrog ΔEp ntawm 176 mV, thaum tsis kho cov ntaub ntawv carbon (UCC) yog 365 mV.Tsis tas li ntawd, HWO / C76 composite tau pom qhov cuam tshuam tseem ceeb ntawm cov kab mob chlorine evolution cov tshuaj tiv thaiv vim yog W-OH pab pawg ua haujlwm.
Kev mob siab rau tib neeg kev ua haujlwm thiab kev hloov pauv sai sai tau ua rau muaj kev xav tau hluav taws xob tsis tu ncua, uas tau nce li ntawm 3% ib xyoos ib zaug.Tau ntau xyoo lawm, kev siv cov fossil fuels thoob plaws los ua lub zog tau ua rau cov pa roj carbon monoxide emissions uas ua rau lub ntiaj teb sov sov, dej thiab huab cua phem, ua rau tag nrho cov ecosystems.Raws li qhov tshwm sim, kev nkag mus ntawm cov cua huv thiab rov ua dua tshiab thiab lub hnub ci zog yuav tsum ncav cuag 75% ntawm tag nrho cov hluav taws xob los ntawm 20501. Txawm li cas los xij, thaum cov khoom siv hluav taws xob los ntawm cov khoom siv txuas ntxiv dua li 20% ntawm tag nrho cov tsim hluav taws xob, daim phiaj yuav tsis ruaj khov.
Ntawm txhua lub zog cia khoom xws li hybrid vanadium redox flow battery2, tag nrho-vanadium redox flow roj teeb (VRFB) tau tsim qhov nrawm tshaj plaws vim nws muaj ntau yam zoo thiab suav tias yog qhov kev daws teeb meem zoo tshaj plaws rau lub sijhawm ntev zog (txog 30 xyoo).) Kev xaiv ua ke nrog lub zog tauj dua tshiab4.Qhov no yog vim kev sib cais ntawm lub zog thiab lub zog ntom ntom, cov lus teb ceev, lub neej ntev tau them nyiaj rau $ 939-420 US Dollars Per KWH.roj teeb raws 4.
Txawm li cas los xij, lawv qhov kev lag luam loj loj tseem raug txwv los ntawm lawv cov peev txheej tseem ceeb, feem ntau vim yog cov cell stacks 4,5.Yog li, kev txhim kho pawg kev ua tau zoo los ntawm kev nce cov kinetics ntawm ob lub ntsiab lus ib nrab tuaj yeem txo cov pawg loj thiab yog li txo nqi.Yog li ntawd, kev hloov hluav taws xob ceev ceev mus rau qhov chaw electrode yog qhov tsim nyog, uas nyob ntawm tus qauv tsim, muaj pes tsawg leeg thiab cov qauv ntawm cov electrode thiab yuav tsum tau ceev faj optimization6.Txawm hais tias muaj cov tshuaj lom neeg zoo thiab electrochemical stability thiab cov hluav taws xob zoo ntawm cov pa roj carbon electrodes, lawv cov kinetics tsis kho tau qeeb vim tsis muaj cov pa oxygen ua haujlwm thiab hydrophilicity7,8.Yog li ntawd, ntau yam electrocatalysts tau ua ke nrog carbon-based electrodes, tshwj xeeb tshaj yog cov pa roj carbon nanostructures thiab hlau oxides, txhawm rau txhim kho kinetics ntawm ob lub electrodes, yog li ua kom cov kinetics ntawm VRFB electrode.
Ntxiv nrog rau peb cov haujlwm dhau los ntawm C76, peb thawj zaug tau tshaj tawm cov kev ua haujlwm zoo ntawm electrocatalytic ntawm no fullerene rau VO2 + / VO2 +, them nyiaj hloov pauv, piv rau cov ntaub ntawv kub thiab tsis kho cov pa roj carbon.Kev tiv thaiv yog txo los ntawm 99.5% thiab 97%.Kev ua haujlwm catalytic ntawm cov ntaub ntawv carbon rau VO2 + / VO2 + cov tshuaj tiv thaiv piv rau C76 yog qhia hauv Table S1.Ntawm qhov tod tes, ntau cov hlau oxides xws li CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 thiab WO331, 32, 33, 34, 35, 36, 37 tau siv vim lawv cov dej noo ntau ntxiv thiab muaj cov pa oxygen ntau ntxiv., 38., ib.Kev ua haujlwm catalytic ntawm cov hlau oxides hauv VO2 + / VO2 + cov tshuaj tiv thaiv yog nthuav tawm hauv Table S2.WO3 tau siv rau hauv cov haujlwm tseem ceeb vim nws cov nqi qis, kev ruaj ntseg siab hauv cov kua qaub tawm, thiab kev ua haujlwm siab catalytic31,32,33,34,35,36,37,38.Txawm li cas los xij, kev txhim kho hauv cathodic kinetics vim WO3 yog qhov tsis tseem ceeb.Txhawm rau txhim kho cov conductivity ntawm WO3, cov nyhuv ntawm kev siv txo tungsten oxide (W18O49) ntawm cathodic kev ua haujlwm tau raug sim38.Hydrated tungsten oxide (HWO) yeej tsis tau sim hauv VRFB daim ntawv thov, txawm hais tias nws nthuav tawm kev ua haujlwm ntau ntxiv hauv cov ntawv thov supercapacitor vim muaj cation diffusion sai dua piv rau anhydrous WOx39,40.Lub tiam thib peb vanadium redox flow roj teeb siv cov kua qaub sib xyaw ua ke ntawm HCl thiab H2SO4 los txhim kho roj teeb kev ua tau zoo thiab txhim kho cov solubility thiab stability ntawm vanadium ions hauv electrolyte.Txawm li cas los xij, cov tshuaj tiv thaiv kab mob chlorine evolution tau dhau los ua ib qho tsis zoo ntawm peb tiam, yog li kev tshawb nrhiav txoj hauv kev los cuam tshuam cov tshuaj chlorine tshuaj ntsuam xyuas tau dhau los ua qhov tseem ceeb ntawm ntau pawg tshawb fawb.
Ntawm no, VO2 + / VO2 + kev ntsuam xyuas cov tshuaj tiv thaiv tau ua tiav ntawm HWO / C76 cov khoom sib xyaw tso rau ntawm cov pa roj carbon electrodes txhawm rau txhawm rau nrhiav qhov sib npaug ntawm cov hluav taws xob conductivity ntawm cov khoom sib xyaw thiab cov redox kinetics ntawm electrode nto thaum suppressing parasitic chlorine evolution.teb (CER).Hydrated tungsten oxide (HWO) nanoparticles tau tsim los ntawm txoj kev yooj yim hydrothermal.Kev sim tau ua nyob rau hauv ib qho kev sib xyaw acid electrolyte (H2SO4 / HCl) los simulate peb tiam VRFB (G3) rau kev ua tau zoo thiab tshawb xyuas cov txiaj ntsig ntawm HWO ntawm cov tshuaj tiv thaiv kab mob chlorine evolution.
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 tungsten oxide 2Aldrich 9, NWO 9% sodium tungsten oxide dihydrate (NWO) daim ntaub ELAT (Fuel Cell Store) tau siv rau hauv txoj kev tshawb no.
Hydrated tungsten oxide (HWO) tau npaj los ntawm hydrothermal cov tshuaj tiv thaiv 43 uas 2 g ntawm Na2WO4 ntsev tau yaj hauv 12 ml ntawm H2O kom muab cov tshuaj tsis muaj xim, tom qab ntawd 12 ml ntawm 2 M HCl tau ntxiv dropwise kom muab cov xim daj daj.Cov slurry tau muab tso rau hauv Teflon coated stainless hlau autoclave thiab khaws cia rau hauv qhov cub ntawm 180 ° C. rau 3 teev rau hydrothermal cov tshuaj tiv thaiv.Cov seem tau sau los ntawm kev pom, ntxuav 3 zaug nrog ethanol thiab dej, ziab hauv qhov cub ntawm 70 ° C rau ~ 3 teev, thiab tom qab ntawd triturated kom muab cov hmoov xiav-grey HWO.
Cov tau txais (tsis kho) carbon daim ntaub electrodes (CCT) tau siv raws li yog los yog cua sov kho nyob rau hauv ib lub raj rauv ntawm 450 ° C nyob rau hauv cov huab cua nrog ib tug kub ntawm 15 ºC / min rau 10 teev kom tau txais kev kho mob CCs (TCC).raws li tau piav nyob rau hauv tsab xov xwm 24 dhau los.UCC thiab TCC raug txiav rau hauv electrodes kwv yees li 1.5 cm dav thiab 7 cm ntev.Kev ncua ntawm C76, HWO, HWO-10% C76, HWO-30% C76 thiab HWO-50% C76 tau npaj los ntawm kev ntxiv 20 mg .% (~ 2.22 mg) ntawm PVDF binder rau ~ 1 ml DMF thiab sonicated rau 1 teev los txhim kho uniformity.2 mg ntawm C76, HWO thiab HWO-C76 composites tau ua ntu zus mus rau UCC active electrode cheeb tsam ntawm kwv yees li 1.5 cm2.Tag nrho cov catalysts tau thauj mus rau UCC electrodes thiab TCC tau siv rau kev sib piv nkaus xwb, raws li peb cov haujlwm dhau los tau pom tias kev kho cua sov tsis tas yuav tsum tau 24.Kev xav txog kev daws teeb meem tau ua tiav los ntawm kev txhuam 100 µl ntawm kev ncua (load 2 mg) kom muaj txiaj ntsig ntau dua.Tom qab ntawd tag nrho cov electrodes tau qhuav hauv qhov cub ntawm 60 ° C. thaum hmo ntuj.Cov electrodes yog ntsuas rau pem hauv ntej thiab rov qab los xyuas kom meej cov khoom thauj khoom.Txhawm rau kom muaj thaj chaw geometric (~ 1.5 cm2) thiab tiv thaiv qhov nce ntawm vanadium electrolyte mus rau electrode vim cov nyhuv capillary, nyias txheej ntawm paraffin tau siv rau cov khoom siv.
Field emission scanning electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) tau siv los soj ntsuam HWO nto morphology.Lub zog dispersive X-ray spectrometer nruab nrog Feii8SEM (EDX, Zeiss Inc.) tau siv los qhia HWO-50% C76 cov ntsiab lus ntawm UCC electrodes.Ib qho kev daws teeb meem siab kis tau tus mob electron microscope (HR-TEM, JOEL JEM-2100) ua haujlwm ntawm qhov nrawm nrawm ntawm 200 kV tau siv los ua duab ntau dua HWO hais thiab diffraction rings.Crystallography Toolbox (CrysTBox) software siv lub ringGUI muaj nuj nqi los tshuaj xyuas HWO nplhaib diffraction qauv thiab sib piv cov txiaj ntsig nrog XRD qauv.Cov qauv thiab graphitization ntawm UCC thiab TCC tau soj ntsuam los ntawm X-ray diffraction (XRD) ntawm qhov ntsuas ntawm 2.4 ° / min los ntawm 5 ° txog 70 ° nrog Cu Kα (λ = 1.54060 Å) siv Panalytical X-ray diffractometer (Model 3600).XRD qhia cov qauv siv lead ua thiab theem ntawm HWO.PANalytical X'Pert HighScore software tau siv los ua kom haum HWO peaks rau tungsten oxide maps muaj nyob rau hauv database45.HWO cov txiaj ntsig tau muab piv nrog TEM cov txiaj ntsig.Cov tshuaj muaj pes tsawg leeg thiab lub xeev ntawm HWO cov qauv raug txiav txim los ntawm X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).CASA-XPS software (v 2.3.15) tau siv rau qhov siab tshaj plaws deconvolution thiab cov ntaub ntawv tsom xam.Txhawm rau txiav txim siab cov pab pawg ua haujlwm saum npoo ntawm HWO thiab HWO-50% C76, kev ntsuas tau siv Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, siv KBr FTIR).Cov txiaj ntsig tau muab piv nrog XPS cov txiaj ntsig.Kev ntsuas lub kaum sab xis (KRUSS DSA25) kuj tau siv los ua tus yam ntxwv ntawm qhov ntub dej ntawm cov electrodes.
Rau txhua qhov kev ntsuas electrochemical, Biologic SP 300 workstation tau siv.Cyclic voltammetry (CV) thiab electrochemical impedance spectroscopy (EIS) tau siv los kawm cov electrode kinetics ntawm VO2 + / VO2 + redox cov tshuaj tiv thaiv thiab cov nyhuv ntawm reagent diffusion (VOSO4 (VO2 +)) ntawm cov tshuaj tiv thaiv.Ob txoj kev siv peb-electrode cell nrog ib qho electrolyte concentration ntawm 0.1 M VOSO4 (V4+) hauv 1 M H2SO4 + 1 M HCl (sib tov ntawm acids).Tag nrho cov ntaub ntawv electrochemical tau nthuav tawm yog IR kho.Ib qho saturated calomel electrode (SCE) thiab platinum (Pt) coil tau siv los ua tus siv thiab counter electrode, feem.Rau CV, scan nqi (ν) ntawm 5, 20, thiab 50 mV / s tau siv rau VO2 + / VO2 + qhov rais qhov rais rau (0–1) V vs. SCE, tom qab ntawd kho rau SHE rau zaj duab xis (VSCE = 0.242 V vs. HSE).Txhawm rau kawm txog kev tuav pov hwm ntawm electrode, rov ua CVs rov ua dua ntawm ν 5 mV / s rau UCC, TCC, UCC-C76, UCC-HWO, thiab UCC-HWO-50% C76.Rau kev ntsuas EIS, qhov ntau zaus ntawm VO2 + / VO2 + redox cov tshuaj tiv thaiv yog 0.01-105 Hz, thiab qhov hluav taws xob perturbation ntawm qhov qhib-circuit voltage (OCV) yog 10 mV.Txhua qhov kev sim tau rov ua dua 2-3 zaug kom ntseeg tau qhov sib xws ntawm cov txiaj ntsig.Lub heterogeneous tus nqi tsis tu ncua (k0) tau txais los ntawm Nicholson txoj kev 46,47.
Hydrated tungsten oxide (HVO) tau ua tiav los ntawm txoj kev hydrothermal.SEM image in fig.1a qhia tau hais tias qhov tso nyiaj HWO muaj pawg ntawm nanoparticles nrog qhov ntau thiab tsawg ntawm 25-50 nm.
X-ray diffraction qauv ntawm HWO qhia peaks (001) thiab (002) ntawm ~ 23.5 ° thiab ~ 47.5 °, ntsig txog, uas yog cov yam ntxwv ntawm nonstoichiometric WO2.63 (W32O84) (PDF 077–0810, a = 21.4 Å, 8. β = γ = 90 °), uas sib haum rau lawv cov xim ntshiab xiav (Fig. 1b) 48.49.Lwm cov peaks ntawm kwv yees li 20.5 °, 27.1 °, 28.1 °, 30.8 °, 35.7 °, 36.7 ° thiab 52.7 ° tau muab rau (140), (620), (350), (720), (740), (560 °).) ) thiab (970) diffraction dav hlau orthogonal rau WO2.63, feem.Tib txoj kev hluavtaws tau siv los ntawm Songara li al.43 kom tau txais cov khoom dawb, uas yog vim muaj WO3 (H2O) 0.333.Txawm li cas los xij, hauv kev ua haujlwm no, vim muaj cov xwm txheej sib txawv, cov khoom siv xiav-grey tau txais, qhia tias WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90° .)Semiquantitative tsom xam siv X'Pert HighScore software pom 26% WO3 (H2O) 0.333: 74% W32O84.Txij li W32O84 muaj W6+ thiab W4+ (1.67:1 W6+:W4+), kwv yees cov ntsiab lus ntawm W6+ thiab W4+ yog li 72% W6+ thiab 28% W4+, raws li.SEM dluab, 1-thib ob XPS spectra nyob rau theem nucleus, TEM cov duab, FTIR spectra, thiab Raman spectra ntawm C76 hais tau nthuav tawm hauv peb tsab xov xwm dhau los.Raws li Kawada li al., 50,51 X-ray diffraction ntawm C76 tom qab tshem tawm ntawm toluene pom cov qauv monoclinic ntawm FCC.
SEM images in fig.2a thiab b qhia tias HWO thiab HWO-50% C76 tau ua tiav zoo tso rau thiab nruab nrab ntawm cov roj carbon fibers ntawm UCC electrode.EDX daim duab qhia chaw ntawm tungsten, carbon, thiab oxygen ntawm SEM cov duab hauv daim duab.2c yog qhia hauv daim duab.2d-f qhia tias cov tungsten thiab cov pa roj carbon sib npaug sib npaug (qhia qhov kev faib tawm zoo sib xws) dhau ntawm tag nrho cov electrode nto thiab cov khoom sib xyaw tsis sib xws vim qhov xwm txheej ntawm txoj kev tso nyiaj.
SEM images of deposited HWO particles (a) and HWO-C76 particles (b).EDX daim ntawv qhia ntawm HWO-C76 loaded ntawm UCC siv thaj tsam hauv daim duab (c) qhia txog kev faib tawm ntawm tungsten (d), carbon (e), thiab oxygen (f) hauv cov qauv.
HR-TEM tau siv rau cov duab loj loj thiab cov ntaub ntawv crystallographic (Daim duab 3).HWO qhia txog nanocube morphology raws li qhia nyob rau hauv daim duab 3a thiab kom meej meej nyob rau hauv daim duab 3b.Los ntawm kev nthuav cov nanocube rau qhov sib txawv ntawm cov cheeb tsam xaiv, ib tus tuaj yeem pom cov qauv grating thiab diffraction dav hlau uas txaus siab rau Bragg txoj cai, raws li qhia hauv daim duab 3c, uas lees paub qhov crystallinity ntawm cov khoom.Nyob rau hauv inset rau Fig. 3c qhia qhov kev ncua deb d 3.3 Å coj mus rau lub (022) thiab (620) diffraction dav hlau pom nyob rau hauv lub WO3 (H2O) 0.333 thiab W32O84 theem, ntsig txog 43,44,49.Qhov no zoo ib yam nrog XRD tsom xam uas tau piav qhia saum toj no (Daim duab 1b) txij li qhov pom ntawm lub dav hlau nyob deb d (Fig. 3c) sib raug rau qhov siab tshaj XRD hauv HWO qauv.Cov qauv rings kuj pom nyob rau hauv daim duab.3d, qhov twg txhua lub nplhaib sib raug rau ib lub dav hlau nyias.Lub dav hlau WO3 (H2O) 0.333 thiab W32O84 yog xim dawb thiab xiav, raws li, thiab lawv qhov sib thooj XRD peaks kuj pom nyob rau hauv daim duab 1b.Thawj lub nplhaib uas pom nyob rau hauv daim duab lub nplhaib sib raug rau thawj lub cim ncov nyob rau hauv x-ray qauv ntawm (022) los yog (620) diffraction dav hlau.Los ntawm (022) mus rau (402) rings, d-spacing tus nqi yog 3.30, 3.17, 2.38, 1.93, thiab 1.69 Å, raws li XRD tus nqi ntawm 3.30, 3.17, 2, 45, 1.93.thiab 1.66 Å, uas yog sib npaug rau 44, 45, raws li.
(a) HR-TEM duab ntawm HWO, (b) qhia cov duab loj.Cov duab ntawm lub dav hlau grating tau pom nyob rau hauv (c), inset (c) qhia cov duab loj ntawm cov dav hlau thiab lub suab d ntawm 0.33 nm sib raug rau (002) thiab (620) dav hlau.(d) HWO nplhaib qauv qhia dav hlau txuam nrog WO3 (H2O) 0.333 (dawb) thiab W32O84 (xiav).
XPS tsom xam tau ua los txiav txim siab qhov chaw chemistry thiab oxidation xeev ntawm tungsten (Figures S1 thiab 4).Qhov ntau yam XPS scan spectrum ntawm synthesized HWO yog qhia nyob rau hauv daim duab S1, qhia tias muaj tungsten.XPS nqaim-scan spectra ntawm W 4f thiab O 1s core theem tau pom hauv daim duab.4a a b,ua.Lub W 4f spectrum splits rau hauv ob lub kiv-orbit doublets sib haum mus rau lub zog khi ntawm W oxidation xeev.thiab W 4f7/2 ntawm 36.6 thiab 34.9 eV yog cov yam ntxwv ntawm W4+ xeev ntawm 40, raws li.0.333 Nws.Cov ntaub ntawv haum qhia tau hais tias cov atomic feem pua ​​​​ntawm W6+ thiab W4+ yog 85% thiab 15%, feem, uas yog ze rau cov nqi kwv yees los ntawm XRD cov ntaub ntawv xav txog qhov sib txawv ntawm ob txoj kev.Ob txoj hauv kev muab cov ntaub ntawv ntau yam nrog qhov tseeb tsawg, tshwj xeeb yog XRD.Tsis tas li, ob txoj kev no tsom xam qhov sib txawv ntawm cov khoom siv vim XRD yog ib txoj hauv kev loj thaum XPS yog ib txoj hauv kev uas tsuas yog mus txog ob peb nanometers.O 1s spectrum muab faib ua ob lub ncov ntawm 533 (22.2%) thiab 530.4 eV (77.8%).Thawj qhov sib raug rau OH, thiab qhov thib ob rau oxygen bonds hauv lub lattice hauv WO.Lub xub ntiag ntawm OH cov pab pawg ua haujlwm zoo ib yam nrog cov khoom hydration ntawm HWO.
Kev tshuaj xyuas FTIR kuj tau ua tiav ntawm ob qhov qauv no los tshuaj xyuas qhov muaj cov pab pawg ua haujlwm thiab kev sib koom tes dej molecules hauv cov qauv HWO hydrated.Cov txiaj ntsig tau pom tias HWO-50% C76 tus qauv thiab FT-IR HWO cov txiaj ntsig tshwm sim zoo sib xws vim muaj HWO, tab sis qhov kev siv ntawm cov peaks sib txawv vim qhov sib txawv ntawm cov qauv siv rau kev npaj rau kev tsom xam (Fig. 5a).) HWO-50% C76 qhia tau hais tias tag nrho cov peaks, tshwj tsis yog lub ncov ntawm tungsten oxide, muaj feem xyuam rau fullerene 24. Cov ntsiab lus hauv daim duab.5a qhia tau hais tias ob qho tib si kev kuaj pom muaj lub zog dav dav ntawm ~ 710 / cm vim yog OWO stretching oscillations hauv HWO lattice qauv, nrog lub xub pwg nyom ntawm ~ 840 / cm yog ntaus nqi rau WO.Rau stretching vibrations, ib tug ntse band ntawm txog 1610 / cm yog ntaus nqi rau dabtsi yog khoov kev co ntawm OH, thaum ib tug dav absorption band ntawm txog 3400 / cm yog ntaus nqi mus stretching vibrations ntawm OH nyob rau hauv hydroxyl pawg43.Cov txiaj ntsig no zoo ib yam nrog XPS spectra hauv Fig.4b, qhov twg WO pab pawg ua haujlwm tuaj yeem muab qhov chaw nquag rau VO2 + / VO2+ cov tshuaj tiv thaiv.
FTIR tsom xam ntawm HWO thiab HWO-50% C76 (a), qhia cov pab pawg ua haujlwm thiab kev ntsuas lub kaum sab xis (b, c).
Cov pab pawg OH tuaj yeem ua rau VO2 + / VO2 + cov tshuaj tiv thaiv, thaum ua kom cov hydrophilicity ntawm electrode, yog li txhawb tus nqi ntawm diffusion thiab hloov hluav taws xob.Raws li tau pom, tus qauv HWO-50% C76 qhia qhov ncov ntxiv rau C76.Lub ncov ntawm ~ 2905, 2375, 1705, 1607, thiab 1445 cm3 tuaj yeem muab rau CH, O = C = O, C = O, C = C, thiab CO stretching vibrations, feem.Nws paub zoo tias cov pa oxygen ua haujlwm pab pawg C = O thiab CO tuaj yeem ua haujlwm ua haujlwm rau cov tshuaj tiv thaiv redox ntawm vanadium.Txhawm rau kuaj thiab sib piv cov wettability ntawm ob lub electrodes, kev sib cuag lub kaum sab xis ntsuas tau coj raws li qhia hauv daim duab 5b, c.HWO electrode tam sim ntawd nqus cov tee dej, qhia tias superhydrophilicity vim muaj OH ua haujlwm pab pawg.HWO-50% C76 yog ntau hydrophobic, nrog rau lub kaum sab xis ntawm 135 ° tom qab 10 vib nas this.Txawm li cas los xij, hauv kev ntsuas hluav taws xob hluav taws xob, HWO-50% C76 electrode tau ntub tag nrho hauv tsawg dua ib feeb.Cov kev ntsuas wettability zoo ib yam nrog XPS thiab FTIR cov txiaj ntsig, qhia tias ntau pawg OH ntawm HWO nto ua rau nws muaj dej ntau dua.
VO2 + / VO2 + cov tshuaj tiv thaiv ntawm HWO thiab HWO-C76 nanocomposites tau sim thiab xav tias HWO yuav txwv cov tshuaj chlorine evolution hauv VO2 + / VO2 + cov tshuaj tiv thaiv hauv cov kua qaub sib xyaw, thiab C76 yuav ntxiv cov tshuaj tiv thaiv VO2 + / VO2 + redox cov tshuaj tiv thaiv.%, 30%, thiab 50% C76 nyob rau hauv HWO ncua kev kawm ntawv thiab CCC tso rau ntawm electrodes nrog ib tug tag nrho loading ntawm txog 2 mg / cm2.
Raws li qhia hauv daim duab.6, lub kinetics ntawm VO2 + / VO2 + cov tshuaj tiv thaiv ntawm cov electrode nto tau tshuaj xyuas los ntawm CV hauv cov kua qaub sib xyaw electrolyte.Cov tam sim no tau pom tias yog I / Ipa rau kev sib piv yooj yim ntawm ΔEp thiab Ipa / Ipc rau cov catalysts sib txawv ncaj qha rau ntawm daim duab.Cov ntaub ntawv cheeb tsam cheeb tsam tam sim no tau qhia hauv daim duab 2S.Ntawm daim duab.Daim duab 6a qhia tau hais tias HWO me ntsis nce cov hluav taws xob hloov pauv ntawm VO2 + / VO2 + cov tshuaj tiv thaiv redox ntawm cov electrode nto thiab suppresses cov tshuaj tiv thaiv kab mob parasitic chlorine evolution.Txawm li cas los xij, C76 nce qhov hloov pauv hluav taws xob ntau ntxiv thiab ua rau cov tshuaj chlorine evolution tshwm sim.Yog li ntawd, ib tug raug formulated composite ntawm HWO thiab C76 yuav tsum muaj qhov zoo tshaj plaws kev ua ub no thiab lub peev xwm loj tshaj plaws los inhibit cov tshuaj chlorine evolution.Nws tau pom tias tom qab nce cov ntsiab lus ntawm C76, cov khoom siv hluav taws xob ntawm cov electrodes tau txhim kho, raws li pom los ntawm kev txo qis hauv ΔEp thiab nce hauv Ipa / Ipc piv (Table S3).Qhov no kuj tau lees paub los ntawm RCT qhov tseem ceeb rho tawm los ntawm Nyquist zajlus hauv daim duab 6d (Table S3), uas tau pom tias yuav txo qis nrog nce C76 cov ntsiab lus.Cov txiaj ntsig no kuj zoo ib yam nrog Li txoj kev tshawb fawb, uas ntxiv cov pa roj carbon mesoporous rau mesoporous WO3 tau pom tias muaj kev txhim kho cov nqi hloov pauv kinetics ntawm VO2 + / VO2 + 35.Qhov no qhia tau hais tias cov tshuaj tiv thaiv ncaj qha tuaj yeem nyob ntawm ntau dua ntawm cov electrode conductivity (C = C daim ntawv cog lus) 18, 24, 35, 36, 37. Qhov no kuj tseem yog vim muaj kev hloov pauv hauv kev sib koom tes ntawm geometry ntawm [VO(H2O)5]2+ thiab [VO2(H2O)4]+, C76 txo cov tshuaj tiv thaiv overvoltage.Txawm li cas los xij, qhov no yuav tsis ua tau nrog HWO electrodes.
(a) Cyclic voltammetric cwj pwm (ν = 5 mV / s) ntawm VO2 + / VO2 + cov tshuaj tiv thaiv ntawm UCC thiab HWO-C76 composites nrog txawv HWO: C76 ratios hauv 0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik thiab (c) Nicholson VO2 + / VO2 + txoj hauv kev los ntsuas kev ua haujlwm ntawm diffusion thiab tau txais k0(d) qhov tseem ceeb.
Tsis yog tsuas yog HWO-50% C76 nthuav tawm yuav luag tib yam electrocatalytic kev ua haujlwm li C76 rau VO2 + / VO2+ cov tshuaj tiv thaiv, tab sis, qhov nthuav ntxiv, nws kuj tseem txwv cov tshuaj chlorine evolution piv rau C76, raws li qhia hauv daim duab 6a, thiab tseem nthuav tawm Cov Semicircle me hauv daim duab.6d (qis RCT).C76 tau pom qhov pom tseeb siab dua Ipa / Ipc dua HWO-50% C76 (Table S3), tsis yog vim kev txhim kho cov tshuaj tiv thaiv rov qab, tab sis vim yog qhov sib tshooj ntawm cov tshuaj chlorine txo cov tshuaj SHE ntawm 1.2 V. Qhov kev ua tau zoo tshaj plaws ntawm HWO- 50% C76 yog vim muaj kev sib koom ua ke ntawm cov txiaj ntsig zoo thiab cov txiaj ntsig tsis zoo ntawm WO-6. tic functionality on HWM.Tsawg chlorine emission yuav txhim kho cov kev them nqi ntawm tag nrho cov xov tooj ntawm tes, thaum txhim kho kinetics yuav txhim kho qhov ua tau zoo ntawm tag nrho cov xov tooj ntawm tes.
Raws li kab zauv S1, rau quasi-reversible (kuj qeeb electron hloov) cov tshuaj tiv thaiv los ntawm diffusion, lub ncov tam sim no (IP) nyob ntawm tus naj npawb ntawm electrons (n), electrode cheeb tsam (A), diffusion coefficient (D), tus naj npawb ntawm electrons hloov coefficient (α) thiab scanning ceev (ν).Txhawm rau kawm txog tus cwj pwm diffusion-tswj ntawm cov khoom siv kuaj, kev sib raug zoo ntawm IP thiab ν1/2 tau npaj thiab nthuav tawm hauv daim duab 6b.Txij li thaum tag nrho cov ntaub ntawv qhia ib tug linear kev sib raug zoo, cov tshuaj tiv thaiv yog tswj los ntawm diffusion.Txij li thaum VO2 + / VO2 + cov tshuaj tiv thaiv yog quasi-reversible, txoj kab nqes ntawm txoj kab nyob ntawm qhov diffusion coefficient thiab tus nqi ntawm α (sib npaug S1).Txij li thaum lub diffusion coefficient yog tas li (≈ 4 × 10–6 cm2 / s) 52, qhov sib txawv ntawm txoj kab nqes ncaj qha qhia qhov sib txawv ntawm α, thiab yog li cov hluav taws xob hloov hluav taws xob rau ntawm qhov chaw electrode, uas yog qhia rau C76 thiab HWO -50% C76 Steepest electron tus nqi (siab tshaj).
Lub Warburg slopes (W) xam rau qhov tsawg zaus pom nyob rau hauv Table S3 (Fig. 6d) muaj nuj nqis ze rau 1 rau tag nrho cov ntaub ntawv, qhia zoo meej diffusion ntawm redox hom thiab paub meej tias cov linear tus cwj pwm ntawm IP piv rau ν1/2. CV yog ntsuas.Rau HWO-50% C76, Warburg txoj kab nqes deviates ntawm 1 txog 1.32, qhia tsis tau tsuas yog ib nrab infinite diffusion ntawm cov reagent (VO2+), tab sis kuj muaj peev xwm ua tau ntawm cov txheej txheem nyias nyias rau diffusion cwj pwm vim electrode porosity.
Txhawm rau txheeb xyuas qhov thim rov qab (electron hloov pauv tus nqi) ntawm VO2 + / VO2 + cov tshuaj tiv thaiv redox, Nicholson quasi-reversible cov tshuaj tiv thaiv kuj tau siv los txiav txim tus qauv tus nqi tas li k041.42.Qhov no yog ua tiav siv qhov sib npaug S2 los tsim qhov dimensionless kinetic parameter Ψ, uas yog ib qho kev ua haujlwm ntawm ΔEp, ua haujlwm ntawm ν-1/2.Table S4 qhia txog Ψ qhov tseem ceeb tau txais rau txhua yam khoom siv electrode.Cov txiaj ntsig (Fig. 6c) tau npaj kom tau k0 × 104 cm/s los ntawm txoj kab nqes ntawm txhua daim phiaj siv Equation S3 (sau ib sab ntawm txhua kab thiab nthuav tawm hauv Table S4).HWO-50% C76 tau pom tias muaj qhov chaw siab tshaj (Fig. 6c), yog li qhov siab tshaj plaws ntawm k0 yog 2.47 × 10–4 cm / s.Qhov no txhais tau hais tias cov electrode no ua tiav cov kinetics ceev tshaj plaws, uas yog raws li CV thiab EIS cov txiaj ntsig hauv daim duab 6a thiab d thiab hauv Table S3.Tsis tas li ntawd, tus nqi ntawm k0 kuj tau txais los ntawm Nyquist plot (Fig. 6d) ntawm Equation S4 siv tus nqi RCT (Table S3).Cov txiaj ntsig k0 no los ntawm EIS tau sau tseg hauv Table S4 thiab tseem qhia tau tias HWO-50% C76 nthuav tawm qhov hloov pauv hluav taws xob siab tshaj plaws vim muaj kev sib koom ua ke.Txawm hais tias tus nqi k0 txawv vim qhov sib txawv ntawm txhua txoj hauv kev, lawv tseem qhia qhov kev txiav txim ntawm qhov loj thiab qhia qhov sib xws.
Txhawm rau kom nkag siab qhov zoo tshaj plaws kinetics tau txais, nws yog ib qho tseem ceeb rau kev sib piv cov khoom siv hluav taws xob zoo nrog UCC thiab TCC electrodes.Rau VO2 + / VO2 + cov tshuaj tiv thaiv, HWO-C76 tsis tsuas yog pom qhov qis tshaj ΔEp thiab rov qab zoo dua, tab sis kuj tseem cuam tshuam cov kab mob parasitic chlorine evolution cov tshuaj tiv thaiv piv rau TCC, ntsuas los ntawm qhov tam sim no ntawm 1.45 V txheeb ze rau SHE (Fig. 7a).Hais txog kev ruaj ntseg, peb xav tias HWO-50% C76 lub cev ruaj khov vim tias cov catalyst tau tov nrog PVDF binder thiab tom qab ntawd siv rau cov ntaub ntawv carbon electrodes.HWO-50% C76 tau pom qhov ua haujlwm siab tshaj plaws ntawm 44 mV (degradation rate 0.29 mV / cycle) tom qab 150 cycles piv rau 50 mV rau UCC (Daim duab 7b).Qhov no yuav tsis yog qhov sib txawv loj, tab sis cov kinetics ntawm UCC electrodes yog qeeb heev thiab degrades nrog cycling, tshwj xeeb tshaj yog rau cov kev xav rov qab.Txawm hais tias qhov thim rov qab ntawm TCC yog qhov zoo dua li ntawm UCC, TCC tau pom tias muaj kev hloov pauv loj ntawm 73 mV tom qab 150 cycles, uas tej zaum yuav yog vim muaj cov tshuaj chlorine ntau ntawm nws qhov chaw.kom cov catalyst adheres zoo rau lub electrode nto.Raws li tuaj yeem pom los ntawm txhua qhov kev sim electrodes, txawm tias cov electrodes uas tsis muaj kev txhawb nqa catalysts tau pom qhov sib txawv ntawm kev sib txawv ntawm kev sib tw, qhia tias qhov kev hloov pauv ntawm kev sib cais thaum caij tsheb kauj vab yog vim kev tsis ua haujlwm ntawm cov khoom los ntawm kev hloov tshuaj es tsis yog catalyst sib cais.Tsis tas li ntawd, yog tias qhov loj ntawm cov khoom catalyst yuav tsum tau muab cais tawm ntawm qhov chaw electrode, qhov no yuav ua rau muaj qhov sib txawv ntawm qhov siab tshaj plaws (tsis yog 44 mV), vim tias cov substrate (UCC) kuj tsis ua haujlwm rau VO2 + / VO2 + redox cov tshuaj tiv thaiv.
Kev sib piv ntawm CV ntawm cov khoom siv electrode zoo tshaj plaws piv rau UCC (a) thiab kev ruaj ntseg ntawm VO2 + / VO2 + redox cov tshuaj tiv thaiv (b).ν = 5 mV/s rau tag nrho CVs hauv 0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl electrolyte.
Txhawm rau nce kev lag luam zoo nkauj ntawm VRFB thev naus laus zis, nthuav dav thiab nkag siab txog kinetics ntawm vanadium redox cov tshuaj tiv thaiv yog qhov tseem ceeb kom ua tiav lub zog ua haujlwm siab.Composites HWO-C76 tau npaj thiab lawv cov txiaj ntsig electrocatalytic ntawm VO2 + / VO2 + cov tshuaj tiv thaiv tau kawm.HWO tau qhia me ntsis kev txhim kho kinetic hauv kev sib xyaw acidic electrolytes tab sis cuam tshuam cov tshuaj chlorine evolution.Ntau qhov sib piv ntawm HWO: C76 tau siv los ua kom zoo dua cov kinetics ntawm HWO-raws li electrodes.Kev nce C76 rau HWO txhim kho cov hluav taws xob hloov pauv kinetics ntawm VO2 + / VO2 + cov tshuaj tiv thaiv ntawm cov hluav taws xob hloov kho, ntawm cov khoom siv HWO-50% C76 yog cov khoom siv zoo tshaj plaws vim nws txo cov nqi hloov pauv thiab ntxiv cov tshuaj chlorine piv rau C76 thiab TCC tso nyiaj..Qhov no yog vim muaj kev sib koom ua ke ntawm C = C sp2 hybridization, OH thiab W-OH ua haujlwm pab pawg.Tus nqi degradation tom qab rov ua dua ntawm HWO-50% C76 tau pom tias yog 0.29 mV / voj voog, thaum qhov degradation ntawm UCC thiab TCC yog 0.33 mV / voj voog thiab 0.49 mV / voj voog, feem, ua rau nws ruaj khov heev.hauv cov kua qaub sib xyaw electrolytes.Cov txiaj ntsig tau nthuav tawm ua tiav paub cov khoom siv hluav taws xob ua haujlwm siab rau VO2 + / VO2 + cov tshuaj tiv thaiv nrog cov kinetics ceev thiab ruaj khov.Qhov no yuav ua rau kom cov zis voltage, yog li ua kom lub zog ua haujlwm ntawm VRFB, yog li txo tus nqi ntawm nws cov lag luam yav tom ntej.
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