304 capillary tube Nanocomposites Raws li Tungsten Oxide / Fullerene li Electrocatalysts thiab Inhibitors ntawm Parasitic VO2 + / VO2 + Reactions hauv Mixed Acids

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Stainless hlau 304 Coil Tube Chemical Composition

304 Stainless Hlau Chev Tube yog ib hom austenitic chromium-nickel alloy.Raws li Stainless Hlau 304 Coil Tube Chaw Tsim Tshuaj, cov khoom tseem ceeb hauv nws yog Cr (17% -19%), thiab Ni (8% -10.5%).Txhawm rau txhim kho nws cov kev tiv thaiv corrosion, muaj me me ntawm Mn (2%) thiab Si (0.75%).

Stainless hlau 304 Coil Tube Mechanical Properties

Cov yam ntxwv ntawm 304 stainless hlau coil tube yog raws li hauv qab no:

• Tensile zog: ≥515MPa
• Tawm zog: ≥205MPa
• Elongation: ≥30%

Kev Siv & Kev Siv Cov Hlau Stainless 304 Coil Tube

Tus nqi siab ntawm vanadium redox flow batteries (VRFBs) txwv lawv txoj kev siv dav.Lub kinetics ntawm electrochemical cov tshuaj tiv thaiv yuav tsum tau txhim kho nyob rau hauv thiaj li yuav ua rau kom lub zog ceev thiab lub zog efficiency ntawm VRFB, yog li txo tus nqi 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 Hloov Spectroscopy (FTIR) thiab kev ntsuas lub kaum sab xis.Nws tau pom tias qhov sib ntxiv ntawm C76 fullerene rau HWO tuaj yeem txhim kho cov kinetics ntawm cov electrode nrog kev hwm rau VO2 + / VO2 + redox cov tshuaj tiv thaiv los ntawm kev nce cov conductivity thiab muab cov pa oxygen-muaj cov pab pawg ua haujlwm ntawm nws qhov chaw.HWO / C76 composite (50 wt% C76) ua pov thawj tias yog qhov tsim nyog tshaj plaws rau VO2 + / VO2 + cov tshuaj tiv thaiv nrog ΔEp ntawm 176 mV piv rau 365 mV rau cov ntaub ntawv tsis kho carbon (UCC).Tsis tas li ntawd, HWO / C76 composite tau pom qhov tseem ceeb inhibition ntawm cov kab mob chlorine evolution cov tshuaj tiv thaiv vim yog W-OH cov pab pawg ua haujlwm.
Kev mob siab rau tib neeg kev ua haujlwm thiab kev lag luam hloov pauv sai tau ua rau muaj kev xav tau hluav taws xob tsis tu ncua, uas tau loj hlob ntawm kwv yees li 3% hauv ib xyoos.Tau ntau xyoo lawm, kev siv fossil fuels ntau dhau los ua lub zog tau ua rau muaj cov pa roj carbon monoxide emissions, ua rau lub ntiaj teb sov sov, dej thiab huab cua ua paug, hem tag nrho cov ecosystems.Raws li qhov tshwm sim, los ntawm 2050 qhov sib koom ntawm lub zog tauj dua tshiab thiab hnub ci zog tau kwv yees kom ncav cuag 75% ntawm tag nrho cov hluav taws xob1.Txawm li cas los xij, thaum tsim hluav taws xob txuas ntxiv dua 20% ntawm tag nrho cov hluav taws xob tsim hluav taws xob, kab sib chaws yuav tsis ruaj khov 1. Kev tsim kho lub zog txuag hluav taws xob yog qhov tseem ceeb rau qhov kev hloov pauv no, vim lawv yuav tsum khaws cov hluav taws xob ntau dhau thiab sib npaug thiab kev xav tau.
Ntawm txhua lub zog khaws cia xws li hybrid vanadium redox flow batteries2, tag nrho cov roj teeb vanadium redox flow batteries (VRFBs) yog qhov zoo tshaj plaws vim lawv cov txiaj ntsig zoo 3 thiab suav tias yog qhov kev daws teeb meem zoo tshaj plaws rau lub sijhawm ntev zog (~ 30 xyoo).Kev siv cov khoom siv hluav taws xob tauj dua tshiab 4.Qhov no yog vim kev sib cais ntawm lub zog thiab lub zog ceev, cov lus teb nrawm, lub neej ntev thiab muaj roj teeb txhua xyoo thiab 279-420 USD / KWH./kWh roj teeb raws 4.
Txawm li cas los xij, lawv txoj kev lag luam dav dav txuas ntxiv mus cuam tshuam los ntawm cov nqi tseem ceeb ntawm cov nqi, feem ntau yog vim cov roj teeb 4,5.Yog li, kev txhim kho roj teeb kev ua tau zoo los ntawm kev ua kom cov kinetics ntawm ob qhov kev cuam tshuam ib nrab ntawm tes tuaj yeem txo cov roj teeb loj thiab yog li txo nqi.Yog li ntawd, kev hloov hluav taws xob ceev ceev mus rau qhov chaw electrode yog xav tau, nyob ntawm qhov tsim, muaj pes tsawg leeg thiab cov qauv ntawm cov electrode, uas yuav tsum tau ua tib zoo ua kom zoo.Txawm hais tias carbon-based electrodes muaj tshuaj zoo thiab electrochemical stability thiab hluav taws xob zoo, yog tias tsis kho, lawv cov kinetics yuav qeeb vim tsis muaj cov pa oxygen ua haujlwm thiab hydrophilicity7,8.Yog li ntawd, ntau yam electrocatalysts tau ua ke nrog cov pa roj carbon 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 electrodes.
Ntau cov ntaub ntawv carbon tau raug siv, xws li carbon paper9, carbon nanotubes10,11,12,13, graphene-based nanostructures14,15,16,17, carbon nanofibers18 thiab lwm yam 19,20,21,22,23, tshwj tsis yog rau tsev neeg fullerene. .Hauv peb txoj kev tshawb fawb yav dhau los ntawm C76, peb tau tshaj tawm thawj zaug qhov kev ua haujlwm zoo ntawm electrocatalytic ntawm no fullerene rau VO2 + / VO2 +, piv rau cov ntaub ntawv kub thiab tsis kho cov pa roj carbon monoxide, cov nqi hloov pauv tau txo los ntawm 99.5% thiab 97% 24.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, 38 yog siv vim lawv cov dej ntau ntxiv thiab cov pa oxygen siab.pab pawg.Table S2 qhia txog kev ua haujlwm catalytic ntawm cov hlau oxides hauv VO2 + / VO2 + cov tshuaj tiv thaiv.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, WO3 pom kev txhim kho me ntsis hauv cathode kinetics.Txhawm rau txhim kho cov kev ua haujlwm ntawm WO3, cov txiaj ntsig ntawm kev siv cov tungsten oxide txo qis (W18O49) ntawm kev ua haujlwm zoo electrode raug sim38.Hydrated tungsten oxide (HWO) yeej tsis tau sim hauv VRFB daim ntawv thov, txawm hais tias nws tau pom tias muaj kev ua haujlwm siab dua hauv cov ntawv thov supercapacitor vim muaj cov cation diffusion sai dua piv rau anhydrous WOx39,40.Peb tiam tag nrho-vanadium redox ntws roj teeb siv cov kua qaub sib xyaw ua ke ntawm HCl thiab H2SO4 los txhim kho cov roj teeb kev ua haujlwm 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 kev tsis zoo ntawm peb tiam, yog li nrhiav txoj hauv kev txhawm rau txhawm rau tshuaj xyuas cov tshuaj chlorine tau dhau los ua txoj haujlwm ntawm ntau pawg tshawb fawb.
Ntawm no, VO2 + / VO2 + cov tshuaj tiv thaiv kev ntsuas tau ua tiav ntawm HWO / C76 cov khoom sib xyaw tso rau ntawm cov ntaub ntawv carbon electrodes txhawm rau txhawm rau nrhiav qhov sib npaug ntawm cov hluav taws xob conductivity ntawm cov khoom sib xyaw thiab cov tshuaj tiv thaiv redox kinetics ntawm lub electrode nto thaum suppressing parasitic chlorine deposition.Cov tshuaj tiv thaiv (KVR).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 ntawm cov kua qaub electrolyte (H2SO4 / HCl) los simulate peb tiam VRFB (G3) kom yooj yim thiab tshawb xyuas cov txiaj ntsig ntawm HWO ntawm cov tshuaj tua kab mob chlorine evolution42.
Vanadium (IV) sulfate oxide hydrate (VOSO4, 99.9%, Alfa-Aeser), sulfuric acid (H2SO4), hydrochloric acid (HCl), dimethylformamide (DMF, Sigma-Aldrich), polyvinylidene fluoride (PVDF, Sigma-Aldrich), sodium Tungsten oxide dihydrate (Na2WO4, 99%, Sigma-Aldrich) thiab hydrophilic carbon daim ntaub ELAT (Fuel Cell Store) tau siv hauv txoj kev tshawb no.
Hydrated tungsten oxide (HWO) tau npaj los ntawm cov tshuaj tiv thaiv hydrothermal uas 2 g ntawm Na2WO4 ntsev tau yaj hauv 12 ml ntawm HO kom txog thaum tau txais cov tshuaj tsis muaj xim, thiab tom qab ntawd 12 ml ntawm 2 M HCl tau ntxiv dropwise kom txog thaum lub teeb daj daj. tau txais.kev ncua.Cov tshuaj tiv thaiv hydrothermal tau nqa tawm hauv Teflon coated stainless hlau autoclave hauv qhov cub ntawm 180 ºC rau 3 teev.Cov residue tau sau los ntawm kev pom, ntxuav 3 zaug nrog ethanol thiab dej, ziab hauv qhov cub ntawm 70 ° C rau ~ 3 h, thiab tom qab ntawd hauv av kom tau txais cov hmoov xiav-grey HWO.
Cov tau txais (tsis kho) carbon daim ntaub electrodes (CCTs) tau siv nyob rau hauv daim ntawv uas lawv tau txais los yog raug kev kho cua sov nyob rau hauv ib lub raj rauv ntawm 450 ° C rau 10 h ntawm qhov cua kub ntawm 15 ° C / min nyob rau hauv cov huab cua. tau txais kev kho UCC (TCC), s Ib yam li yav dhau los ua haujlwm 24. 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 ntawm cov khoom siv hmoov thiab 10 wt% (~ 2.22 mg) ntawm PVDF binder rau ~ 1 ml ntawm DMF npaj rau hauv thiab sonicated rau 1 teev los txhim kho uniformity.Tom qab ntawd 2 mg ntawm C76, HWO thiab HWO-C76 composites tau siv rau kwv yees li 1.5 cm2 ntawm UCC active electrode cheeb tsam.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 qhia 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 zoo dua qub.Tom qab ntawd tag nrho cov electrodes tau qhuav hauv qhov cub thaum hmo ntuj ntawm 60 ° C.Cov electrodes yog ntsuas ua ntej thiab tom qab kom paub tseeb tias cov khoom thauj khoom raug.Txhawm rau kom muaj thaj chaw geometric (~ 1.5 cm2) thiab tiv thaiv qhov nce ntawm vanadium electrolyte rau cov electrodes vim cov nyhuv capillary, nyias txheej ntawm paraffin tau siv rau cov khoom siv.
Lub teb emission scanning electron microscope (FESEM, Zeiss SEM Ultra 60.5 kV) tau siv los soj ntsuam HWO nto morphology.Zog dispersive X-ray spectroscopy nruab nrog Feii8SEM (EDX, Zeiss AG) tau siv los ua daim ntawv qhia HWO-50% C76 cov ntsiab lus ntawm UCC electrodes.Kev daws teeb meem siab xa hluav taws xob hluav taws xob tsom iav (HR-TEM, JOEL JEM-2100) ua haujlwm ntawm qhov nrawm nrawm ntawm 200 kV tau siv kom tau txais cov duab daws teeb meem siab thiab diffraction rings ntawm HWO hais.Siv Crystallographic Tool Box (CrysTBox) software los txheeb xyuas HWO diffraction rings siv lub ringGUI muaj nuj nqi thiab sib piv cov txiaj ntsig nrog XRD qauv.Cov qauv thiab graphitization ntawm UCC thiab TCC tau txiav txim los ntawm X-ray diffraction (XRD) ntawm tus nqi scan 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.Sib piv cov txiaj ntsig HWO nrog cov txiaj ntsig TEM.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.Fourier hloov infrared spectroscopy (FTIR, siv Perkin Elmer chav kawm KBr FTIR spectrometer) tau ua los txiav txim siab qhov chaw ua haujlwm ntawm HWO thiab HWO-50% C76.Sib piv cov txiaj ntsig 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 lub thev naus laus zis siv peb-electrode cell nrog cov electrolyte concentration ntawm 0.1 M VOSO4 (V4+) yaj hauv 1 M H2SO4 + 1 M HCl (mixed acid).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 tus nqi (ν) ntawm 5, 20, thiab 50 mV / s tau siv rau lub qhov rais muaj peev xwm (0–1) V piv rau SCE rau VO2 + / VO2 +, tom qab ntawd kho ntawm SHE nplai rau zaj duab xis (VSCE = 0.242 V ntsig txog HSE).Txhawm rau tshawb xyuas qhov khaws cia ntawm cov khoom siv hluav taws xob, CV rov ua dua tshiab tau ua ntawm UCC, TCC, UCC-C76, UCC-HWO thiab UCC-HWO-50% C76 ntawm ν sib npaug 5 mV / s.Rau EIS ntsuas rau VO2 + / VO2 + cov tshuaj tiv thaiv redox, ntau zaus ntawm 0.01-105 Hz thiab qhib hluav taws xob hluav taws xob (OCV) cuam tshuam ntawm 10 mV tau siv.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 loj me hauv thaj tsam ntawm 25-50 nm.
X-ray diffraction qauv ntawm HWO qhia peaks (001) thiab (002) ntawm ~ 23.5 ° thiab ~ 47.5 °, raws li, uas yog cov yam ntxwv ntawm nonstoichiometric WO2.63 (W32O84) (PDF 077–0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90°), uas sib raug rau nws cov xim xiav pom tseeb (Fig. 1b)48,49.Lwm qhov siab ntawm kwv yees li 20.5 °, 27.1 °, 28.1 °, 30.8 °, 35.7 °, 36.7 ° thiab 52.7 ° yog ntawm (140), (620), (350), (720), (740), (560).thiab (970) diffraction dav hlau, feem, 49 orthorhombic WO2.63.Songara et al.43 siv tib txoj kev hluavtaws kom tau txais cov khoom dawb, uas yog vim muaj WO3 (H2O) 0.333.Txawm li cas los xij, hauv txoj haujlwm no, vim muaj kev sib txawv, cov khoom siv xiav-grey tau txais, qhia txog kev sib koom ua ke ntawm WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7.7) hauv Å , α = β = γ = 90 °) thiab txo daim ntawv ntawm tungsten oxide.Semiquantitative tsom xam nrog 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 ntawm theem nucleus, TEM duab, FTIR spectra thiab Raman spectra ntawm C76 hais tau nthuav tawm hauv peb daim ntawv dhau los24.Raws li Kawada et al.50,51, X-ray diffraction qauv ntawm C76 qhia cov qauv monoclinic ntawm FCC tom qab tshem tawm cov toluene.
SEM images in fig.2a thiab b qhia txog kev ua tiav ntawm HWO thiab HWO-50% C76 ntawm thiab nruab nrab ntawm cov roj carbon fibers ntawm UCC electrodes.Elemental mapping of tungsten, carbon and oxygen in the SEM image in Fig. 2c yog qhia hauv daim duab.2d-f qhia tias cov tungsten thiab cov pa roj carbon sib xyaw ua ke sib xyaw ua ke (piv txwv li kev faib tawm zoo sib xws) hla cov electrode nto thiab cov khoom sib xyaw tsis sib npaug.vim qhov xwm txheej ntawm txoj kev los nag.
SEM images of deposited HWO particles (a) and HWO-C76 particles (b).EDX daim duab qhia uploaded rau HWO-C76 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).Lub HWO ua qauv qhia txog nanocube morphology raws li qhia hauv daim duab 3a thiab kom meej meej hauv daim duab 3b.Los ntawm kev nthuav cov nanocube rau qhov sib txawv ntawm qhov chaw xaiv, cov qauv grating thiab diffraction dav hlau txaus siab rau Bragg txoj cai tuaj yeem pom tau raws li pom hauv daim duab 3c, lees paub qhov crystallinity ntawm cov khoom.Nyob rau hauv inset rau Fig. 3c qhia qhov deb d 3.3 Å coj mus rau lub (022) thiab (620) diffraction dav hlau nyob rau hauv lub WO3 (H2O) 0.333 thiab W32O84, 43, 44, 49 theem, feem.Qhov no yog ua raws li qhov kev soj ntsuam XRD 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 lub nplhaib qauv 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-ntu ntawm 3.30, 3.17, 2.38, 1.93, thiab 1.69 Å tau pom, uas yog raws li XRD tus nqi ntawm 3.30, 3.17, 2 .45, 1.63. thiab 1.Å, 44, 45, ob.
(a) HR-TEM duab ntawm HWO, (b) qhia cov duab loj.Cov duab ntawm lub dav hlau grating tau pom nyob rau hauv (c), thiab inset (c) qhia cov duab loj ntawm cov dav hlau thiab lub caij d 0.33 nm sib raug rau (002) thiab (620) dav hlau.(d) HWO nplhaib qauv qhia cov dav hlau txuam nrog WO3 (H2O) 0.333 (dawb) thiab W32O84 (xiav) theem.
XPS tsom xam tau ua los txiav txim siab qhov chaw chemistry thiab oxidation xeev ntawm tungsten (Figures S1 thiab 4).Lub spectrum ntawm qhov dav-ntau XPS scan ntawm lub synthesized HWO yog qhia nyob rau hauv daim duab.S1, qhia tias muaj tungsten.XPS nqaim-scan spectra ntawm lub ntsiab W 4f thiab O 1s qib tau pom hauv daim duab.4a a b,ua.W 4f spectrum raug muab faib ua ob lub voj voog sib txuas sib txuas nrog lub zog khi ntawm lub xeev oxidation W. Lub ncov W 4f5 / 2 thiab W 4f7 / 2 ntawm kev khi lub zog ntawm 37.8 thiab 35.6 eV belongs rau W6 +, thiab cov peaks W. 4f5/2 thiab W 4f7/2 ntawm 36.6 thiab 34.9 eV yog tus yam ntxwv ntawm W4+ xeev, feem.Lub xub ntiag ntawm lub xeev oxidation (W4 +) ntxiv qhia txog kev tsim cov uas tsis yog-stoichiometric WO2.63, thaum lub xub ntiag ntawm W6+ qhia tias stoichiometric WO3 vim yog WO3 (H2O) 0.333.Cov ntaub ntawv haum tau pom 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, muab qhov sib txawv ntawm ob lub thev naus laus zis.Ob txoj hauv kev muab cov ntaub ntawv ntau yam nrog qhov tseeb tsawg, tshwj xeeb yog XRD.Tsis tas li ntawd, ob txoj hauv kev txheeb xyuas qhov sib txawv ntawm cov khoom siv vim XRD yog ib txoj hauv kev loj thaum XPS yog txoj hauv kev uas tsuas yog mus txog ob peb nanometers.O 1s spectrum 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 sib koom ua ke ntawm cov 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 zoo ib yam vim muaj HWO, tab sis qhov kev siv ntawm cov peaks txawv vim qhov sib txawv ntawm cov qauv siv thaum npaj rau kev tsom xam (Fig. 5a ).HWO-50% C76 Tag nrho cov fullerene 24 peaks yog qhia tshwj tsis yog rau lub ncov tungsten oxide.Paub meej hauv daim duab.5a qhia tau hais tias ob qho tib si kuaj pom muaj qhov dav dav dav ntawm ~ 710 / cm, ntaus nqi rau OWO stretching vibrations hauv HWO lattice qauv, thiab lub xub pwg nyom ntawm ~ 840 / cm, ntaus nqi rau WO.lub ntse band ntawm ~ 1610 / cm yog hais txog qhov khoov kev co ntawm OH, thiab lub dav haum band ntawm ~ 3400 / cm yog hais txog lub stretching vibration ntawm OH nyob rau hauv lub hydroxyl pawg 43.Cov txiaj ntsig no zoo ib yam nrog XPS spectrum hauv daim duab 4b, qhov twg WO pab pawg ua haujlwm tuaj yeem muab cov chaw ua haujlwm 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, yog li ua kom cov hydrophilicity ntawm electrode, yog li txhawb kev sib hloov thiab hloov hluav taws xob.Tus qauv HWO-50% C76 qhia tau hais tias C76 ncov ntxiv raws li qhia hauv daim duab.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 ntsuas lub kaum sab xis tau siv raws li qhia hauv daim duab 5b, c.Lub HWO electrode tam sim ntawd nqus cov tee dej, qhia tias superhydrophilicity vim muaj cov pab pawg ua haujlwm OH.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 electrochemical, 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 OH pawg 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 tsis pub cov chlorine gas uas tshwm sim thaum VO2 + / VO2 + cov tshuaj tiv thaiv hauv cov kua qaub sib xyaw, thaum C76 yuav ntxiv rau qhov xav tau VO2 + / VO2 +.HWO suspensions muaj 10%, 30% thiab 50% C76 tau siv rau UCC electrodes nrog tag nrho cov load ntawm txog 2 mg / cm2.
Raws li qhia hauv daim duab.6, kinetics ntawm VO2 + / VO2 + cov tshuaj tiv thaiv ntawm cov electrode nto tau tshuaj xyuas siv CV hauv cov kua qaub sib xyaw electrolytes.Currents yog qhia raws li I / Ipa los pab txhawb kev sib piv ntawm ΔEp thiab Ipa / Ipc.Ntau yam catalysts tau ncaj qha los 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 qho nyuaj nrog qhov tseeb muaj pes tsawg leeg ntawm HWO thiab C76 yuav tsum muaj cov haujlwm zoo tshaj plaws thiab muaj peev xwm siab tshaj plaws los tiv thaiv cov tshuaj chlorine.Nws tau pom tias tom qab nce C76 cov ntsiab lus, cov khoom siv hluav taws xob ntawm cov hluav taws xob 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 tau muab rho tawm los ntawm Nyquist zajlus hauv daim duab 6d ( rooj S3), qhov uas nws tau pom tias cov nqi RCT poob qis nrog cov ntsiab lus ntawm C76.Cov txiaj ntsig no kuj zoo ib yam nrog Lee txoj kev tshawb fawb uas ntxiv cov pa roj carbon mesoporous rau mesoporous WO3 txhim kho tus nqi hloov pauv kinetics ntawm VO2 + / VO2 + 35.Qhov no qhia tau hais tias cov tshuaj tiv thaiv zoo tuaj yeem nyob ntawm ntau yam ntawm cov khoom siv hluav taws xob (C = C daim ntawv cog lus) 18,24,35,36,37.Vim qhov kev hloov pauv hauv kev sib koom ua ke ntawm geometry ntawm [VO(H2O)5]2+ thiab [VO2(H2O)4]+, C76 tuaj yeem txo cov lus teb overstrain los ntawm kev txo cov ntaub so ntswg zog.Txawm li cas los xij, qhov no yuav tsis ua tau nrog HWO electrodes.
(a) Cyclic voltammetric cwj pwm ntawm UCC thiab HWO-C76 composites nrog txawv HWO: C76 ratios nyob rau hauv VO2 + / VO2 + cov tshuaj tiv thaiv nyob rau hauv 0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl electrolyte (ntawm ν = 5 mV / s).(b) Randles-Sevchik thiab (c) Nicholson's VO2 + / VO2+ txoj kev kwv yees diffusion efficiency thiab tau txais k0 qhov tseem ceeb (d).
Tsis tsuas yog HWO-50% C76 nthuav tawm yuav luag tib yam kev ua haujlwm electrocatalytic li C76 rau VO2 + / VO2+ cov tshuaj tiv thaiv, tab sis, qhov nthuav ntxiv, nws tseem txwv tsis pub cov evolution ntawm cov roj chlorine piv rau C76, raws li qhia hauv daim duab.6a, ntxiv rau kev qhia lub voj voog me me hauv daim duab.6g (qis RCT).C76 tau pom qhov pom tseeb dua Ipa / Ipc dua li HWO-50% C76 (Table S3), tsis yog vim kev txhim kho cov tshuaj tiv thaiv rov qab, tab sis vim yog sib tshooj nrog cov tshuaj chlorine txo qhov siab tshaj ntawm 1.2 V piv rau SHE.Qhov kev ua tau zoo tshaj plaws ntawm HWO-50% C76 yog ntaus nqi los ntawm kev sib koom ua ke ntawm qhov tsis zoo ntawm cov khoom siv hluav taws xob C76 thiab cov dej ntub dej siab thiab cov catalytic functionalities ntawm W-OH ntawm HWO.Txawm hais tias tsawg dua chlorine emission yuav txhim kho kev them nqi ntawm lub xov tooj ntawm tes, txhim kho kinetics yuav ua rau kom muaj txiaj ntsig ntawm tag nrho cov xov tooj ntawm tes.
Raws li kev sib npaug 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), tooj. ntawm electrons hloov coefficient (α) thiab scanning ceev (ν).Txhawm rau kawm txog kev coj tus cwj pwm diffusion tswj ntawm cov khoom siv kuaj, kev sib raug zoo ntawm IP thiab ν1/2 tau npaj thiab qhia 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).Vim lub diffusion coefficient tsis tu ncua (≈ 4 × 10–6 cm2 / s) 52, qhov sib txawv ntawm txoj kab nqes ncaj qha qhia qhov sib txawv ntawm α thiab yog li sib txawv ntawm cov hluav taws xob hloov mus rau electrode nto, nrog C76 thiab HWO -50 % C76, nthuav qhia qhov chaw siab tshaj plaws (siab tshaj plaws electron hloov chaw).
Qhov ntsuas qis zaus Warburg slopes (W) qhia hauv Table S3 (Fig. 6d) muaj qhov tseem ceeb ze rau 1 rau tag nrho cov ntaub ntawv, qhia zoo meej diffusion ntawm redox particles thiab paub meej tias tus cwj pwm linear ntawm IP piv rau ν1/2 rau CV .kev ntsuas.Rau HWO-50% C76, Warburg txoj kab nqes deviates los ntawm kev sib koom ua ke mus rau 1.32, qhia txog kev koom tes tsis yog los ntawm ib nrab ntawm qhov tsis muaj qhov kawg ntawm cov reactants (VO2+), tab sis kuj muaj peev xwm nyias-txheej cwj pwm nyob rau hauv tus cwj pwm diffusion 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 los ntawm plotting lub dimensionless kinetic parameter Ψ ua ib tug muaj nuj nqi ntawm ΔEp raws li ib tug muaj nuj nqi ntawm ν−1/2 siv lub S2 kab zauv.Table S4 qhia qhov tshwm sim Ψ qhov tseem ceeb rau txhua yam khoom siv electrode.Npaj cov txiaj ntsig (Daim duab 6c) kom tau txais k0 × 104 cm / s (sau ib sab ntawm txhua kab thiab nthuav tawm hauv Table S4) siv qhov sib npaug S3 rau txoj kab nqes ntawm txhua daim phiaj.HWO-50% C76 tau pom tias muaj qhov chaw siab tshaj (Fig. 6c) thiab yog li qhov siab tshaj k0 tus nqi ntawm 2.47 × 10–4 cm / s.Qhov no txhais tau hais tias cov electrode no muab cov kinetics ceev tshaj plaws raws li CV thiab EIS cov txiaj ntsig hauv daim duab 6a thiab d thiab Table S3.Tsis tas li ntawd, k0 qhov tseem ceeb kuj tau txais los ntawm Nyquist plots (Fig. 6d) ntawm Equation S4 siv cov 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 ntawm k0 txawv vim qhov sib txawv ntawm txhua txoj kev, nws tseem qhia tau hais tias tib qhov kev txiav txim ntawm qhov loj thiab qhia qhov sib xws.
Txhawm rau kom nkag siab qhov zoo tshaj plaws kinetics uas tuaj yeem ua tiav, nws yog ib qho tseem ceeb rau kev sib piv cov khoom siv hluav taws xob zoo tshaj plaws nrog cov khoom siv tsis zoo 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 tshuaj tiv thaiv kab mob chlorine evolution piv rau TCC, raws li qhia los ntawm qhov tseem ceeb tam sim no poob ntawm 1.45 V piv rau pom OHA (Fig. 7 a).Hais txog kev ruaj ntseg, peb xav tias HWO-50% C76 yog lub cev ruaj khov vim tias cov catalyst tau tov nrog PVDF binder thiab tom qab ntawd siv rau cov ntaub ntawv carbon electrodes.Piv rau 50 mV rau UCC, HWO-50% C76 tau pom qhov ua haujlwm siab tshaj plaws ntawm 44 mV tom qab 150 cycles (degradation tus nqi 0.29 mV / voj voog) (Daim duab 7b).Nws yuav tsis yog qhov sib txawv loj, tab sis cov kinetics ntawm UCC electrodes qeeb heev thiab degrades nrog cycling, tshwj xeeb tshaj yog rau cov tshuaj tiv thaiv rov qab.Txawm hais tias qhov thim rov qab ntawm TCC yog qhov zoo dua li ntawm UCC, TCC tau pom tias muaj qhov hloov pauv loj ntawm 73 mV tom qab 150 cycles, uas tej zaum yuav yog vim muaj cov tshuaj chlorine ntau tawm ntawm nws qhov chaw.Los xyuas kom meej tias cov catalyst adheres zoo rau lub electrode nto.Raws li tuaj yeem pom ntawm txhua qhov kev sim electrodes, txawm tias cov uas tsis muaj kev txhawb nqa catalysts muaj qhov sib txawv ntawm kev sib txawv ntawm kev caij tsheb kauj vab, qhia tias kev hloov pauv ntawm kev sib cais thaum caij tsheb kauj vab yog vim cov khoom siv deactivation vim cov tshuaj hloov pauv ntau dua li kev sib cais catalyst.Tsis tas li ntawd, yog tias qhov loj ntawm cov khoom siv hluav taws xob 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 los ntawm 44 mV), vim tias cov substrate (UCC) kuj tsis ua haujlwm rau VO2 + / VO2 +. tshuaj tiv thaiv redox.
Kev sib piv ntawm CV (a) thiab kev ruaj ntseg ntawm cov tshuaj tiv thaiv redox VO2 + / VO2 + (b) ntawm cov khoom siv electrode zoo nrog rau CCC.Hauv electrolyte 0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl, tag nrho cov CVs sib npaug rau ν = 5 mV / s.
Txhawm rau nce kev lag luam zoo nkauj ntawm VRFB thev naus laus zis, kev txhim kho thiab nkag siab txog kinetics ntawm vanadium redox cov tshuaj tiv thaiv yog qhov tseem ceeb rau kev ua kom muaj 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 tab sis cuam tshuam cov tshuaj chlorine evolution hauv cov kua qaub sib xyaw electrolytes.Ntau qhov sib piv ntawm HWO: C76 tau siv los ua kom zoo dua cov kinetics ntawm HWO-raws li electrodes.Ua kom cov ntsiab lus ntawm C76 rau HWO tuaj yeem txhim kho kev hloov pauv hluav taws xob ntawm VO2 + / VO2 + cov tshuaj tiv thaiv ntawm cov hluav taws xob hloov pauv, ntawm cov khoom siv HWO-50% C76 yog cov khoom siv zoo tshaj plaws vim tias nws txo qis cov nqi hloov pauv tsis kam thiab ntxiv chlorine gas evolution piv rau C76.thiab TCC raug tso tawm.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 ntawm HWO-50% C76 tau pom tias yog 0.29mV / lub voj voog nyob rau hauv ntau lub voj voog thaum UCC thiab TCC yog 0.33mV / voj voog thiab 0.49mV / voj voog raws li, ua rau nws ruaj khov 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 txhim kho lub zog efficiency ntawm VRFB, yog li txo tus nqi ntawm nws cov lag luam yav tom ntej.
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