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Litsenyehelo tse batlang li phahame tsa li-betri tsohle tsa vanadium flow-through redox (VRFBs) li fokotsa tšebeliso ea tsona e pharaletseng.Ho ntlafatsa kinetics ea karabelo ea electrochemical ho hlokahala ho eketsa matla a khethehileng le matla a VRFB, kahoo ho fokotsa litšenyehelo tsa kWh ea VRFB.Mosebetsing ona, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 le C76 / HWO, li ile tsa kenngoa ka li-electrode tsa lesela la carbon 'me tsa lekoa e le li-electrocatalysts bakeng sa VO2 +/VO2+ redox reaction.Field emission scanning electron microscopy (FESEM), eneji 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) le litekanyo tsa angle tsa ho kopana.Ho fumanoe hore tlatsetso ea C76 fullerenes ho HWO e ka ntlafatsa kinetics ea electrode ka ho eketsa conductivity ea motlakase le ho fana ka lihlopha tse sebetsang tse nang le oxidized holim'a eona, ka hona ho khothalletsa VO2 +/VO2+ redox reaction.HWO/C76 composite (50 wt% C76) e ipakile e le khetho e ntle ka ho fetisisa bakeng sa karabelo ea VO2+/VO2+ ka ΔEp ea 176 mV, athe lesela la khabone le sa sebetsoang (UCC) e ne e le 365 mV.Ho phaella moo, motsoako oa HWO / C76 o bontšitse phello e kholo ea ho thibela phetoho ea likokoana-hloko tsa chlorine ka lebaka la sehlopha se sebetsang sa W-OH.
Ts'ebetso e matla ea batho le phetoho e potlakileng ea indasteri e lebisitse tlhokeho e phahameng e ke keng ea thijoa ea motlakase, e ntseng e eketseha ka hoo e ka bang 3% ka selemo1.Ka lilemo tse mashome, tšebeliso e pharalletseng ea libeso e le mohloli oa matla e lebisitse ho ntšoeng ha likhase tse futhumatsang lefatše tse tlatsetsang ho futhumaleng ha lefatše, tšilafalo ea metsi le moea, e leng ho sokelang tikoloho eohle.Ka lebaka leo, ho kenella ha moea o hloekileng le o tsosolositsoeng le matla a letsatsi ho lebeletsoe ho fihla ho 75% ea kakaretso ea motlakase ka 20501. Leha ho le joalo, ha karolo ea motlakase e tsoang mehloling e tsosolositsoeng e feta 20% ea kakaretso ea tlhahiso ea motlakase, marang-rang a fetoha a sa tsitsang.
Har'a lisebelisoa tsohle tsa polokelo ea matla tse kang hybrid vanadium redox flow battery2, betri ea "vanadium redox flow" (VRFB) e tsoetse pele ka potlako ka lebaka la melemo ea eona e mengata 'me e nkoa e le tharollo e molemo ka ho fetisisa bakeng sa polokelo ea nako e telele ea matla (hoo e ka bang lilemo tse 30).) Likhetho li kopane le matla a tsosolositsoeng4.Sena se bakoa ke karohano ea matla le matla a matla, karabelo e potlakileng, bophelo ba nako e telele ea tšebeletso, le litšenyehelo tse batlang li le tlase tsa selemo tsa $ 65 / kWh ha li bapisoa le $ 93-140 / kWh bakeng sa Li-ion le libeteri tsa lead-acid le 279-420 lidolara tsa US ka kWh.betri ka ho latellana 4.
Leha ho le joalo, khoebo ea bona e kholo e ntse e thibetsoe ke litšenyehelo tsa bona tsa lichelete tse batlang li le holimo, haholo-holo ka lebaka la li-cell stacks4,5.Kahoo, ho ntlafatsa ts'ebetso ea stack ka ho eketsa kinetics ea likarolo tse peli tsa likarolo tse peli ho ka fokotsa boholo ba stack mme ka hona ho fokotsa litšenyehelo.Ka hona, ho fetisetsoa ha elektronike ka potlako sebakeng sa electrode hoa hlokahala, ho itšetlehile ka moralo, sebopeho le sebopeho sa electrode 'me e hloka optimization e hlokolosi6.Ho sa tsotellehe botsitso bo botle ba lik'hemik'hale le electrochemical le motlakase o motle oa motlakase oa li-electrode tsa carbon, kinetics ea bona e sa phekoloeng e botsoa ka lebaka la ho ba sieo ha lihlopha tse sebetsang tsa oksijene le hydrophilicity7,8.Ka hona, li-electrocatalyst tse fapa-fapaneng li kopantsoe le li-electrode tse thehiloeng ka carbon, haholo-holo li-carbon nanostructures le li-oxide tsa tšepe, ho ntlafatsa kinetics ea li-electrode ka bobeli, kahoo ho eketsa kinetics ea electrode ea VRFB.
Ho phaella mosebetsing oa rona o fetileng ho C76, re ile ra tlaleha ka lekhetlo la pele mosebetsi o babatsehang oa electrocatalytic oa fullerene ena bakeng sa VO2 +/VO2 +, ho fetisoa ha tefiso, ha ho bapisoa le lesela la carbon le nang le mocheso le se sa phekoloang.Khanyetso e fokotsehile ka 99.5% le 97%.Ts'ebetso e matla ea lisebelisoa tsa khabone bakeng sa karabelo ea VO2+/VO2+ ha e bapisoa le C76 e bonts'oa ho Lethathamo la S1.Ka lehlakoreng le leng, li-oxide tse ngata tsa tšepe tse kang CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 le WO331, 32, 33, 34, 35, 36, 37 li 'nile tsa sebelisoa ka lebaka la ho eketseha ha tsona ho metsi le ho sebetsa ka bongata ba oksijene., 38. sehlopha.Ts'ebetso e matla ea li-oxide tsena tsa tšepe karabelong ea VO2+/VO2+ e hlahisoa ho Lethathamo la S2.WO3 e 'nile ea sebelisoa mesebetsing e mengata ka lebaka la theko e tlaase, botsitso bo phahameng mecheng ea litaba tsa acidic, le ts'ebetso e phahameng ea catalytic31,32,33,34,35,36,37,38.Leha ho le joalo, ntlafatso ea kinetics ea cathodic ka lebaka la WO3 ha e na thuso.Ho ntlafatsa conductivity ea WO3, phello ea ho sebelisa tungsten oxide e fokotsehileng (W18O49) mosebetsing oa cathodic e ile ea lekoa38.Hydrated tungsten oxide (HWO) ha e e-s'o lekoe lits'ebetsong tsa VRFB, leha e bonts'a ts'ebetso e eketsehileng lits'ebetsong tsa supercapacitor ka lebaka la phallo e potlakileng ea cation ha e bapisoa le anhydrous WOx39,40.Betri ea phallo ea vanadium redox ea moloko oa boraro e sebelisa electrolyte ea acid e tsoakiloeng e entsoeng ka HCl le H2SO4 ho ntlafatsa ts'ebetso ea betri le ho ntlafatsa ho qhibiliha le botsitso ba vanadium ions ka electrolyte.Leha ho le joalo, karabelo ea phetoho ea chlorine ea parasitic e fetohile e 'ngoe ea mathata a moloko oa boraro, kahoo ho batla litsela tsa ho thibela karabelo ea tlhahlobo ea chlorine e fetohile sepheo sa lihlopha tse' maloa tsa lipatlisiso.
Mona, liteko tsa karabelo tsa VO2+/VO2+ li ile tsa etsoa ho li-composites tsa HWO/C76 tse kentsoeng li-electrode tsa lesela la carbon e le ho fumana ho leka-lekana pakeng tsa conductivity ea motlakase ea metsoako le redox kinetics ea holim'a electrode ha ho ntse ho hatella phetoho ea parasitic chlorine.karabo (CER).Hydrated tungsten oxide (HWO) nanoparticles e entsoe ka mokhoa o bonolo oa hydrothermal.Liteko li ile tsa etsoa ka electrolyte ea asiti e tsoakiloeng (H2SO4/HCl) ho etsisa moloko oa boraro oa VRFB (G3) bakeng sa ho sebetsa le ho batlisisa phello ea HWO karabelo ea ho iphetola ha lintho ka chlorine ea parasitic.
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 Tungstenphild hydrocarbon, 9 hydrochloric oxide, 9 carbon Sigma-Aldrich lesela ELAT (Fuel Cell Store) li ile tsa sebelisoa thutong ena.
Hydrated tungsten oxide (HWO) e ile ea lokisoa ke hydrothermal reaction 43 eo ho eona 2 g ea letsoai la Na2WO4 e ileng ea qhibiliha ka 12 ml ea H2O ho fana ka tharollo e se nang mebala, ebe 12 ml ea 2 M HCl e kenngoa ka dropwise ho fana ka ho emisoa ha mosehla o mosehla.The slurry e ne e behoa ka Teflon coated stainless steel autoclave 'me e bolokoa ka ontong ka 180 ° C. bakeng sa lihora tse 3 bakeng sa karabelo ea hydrothermal.Masala a ne a bokelloa ka ho sefa, a hlatsuoa ka makhetlo a 3 ka ethanol le metsi, a omisitsoe ka ontong ka 70 ° C bakeng sa ~ lihora tse 3, ebe o triturated ho fana ka phofo ea HWO e putsoa-grey.
Li-electrode tsa lesela la carbon (CCT) tse fumanoeng (tse sa tšoaroeng) li ne li sebelisoa e le kapa mocheso o tšoaroa ka sebōpi sa tube ka 450 ° C moeeng o nang le mocheso oa mocheso oa 15 ºC / min bakeng sa lihora tsa 10 ho fumana li-CC tse phekoloang (TCC).joalokaha ho hlalositsoe sehloohong se fetileng24.UCC le TCC li ile tsa khaoloa ka li-electrode tse ka bang 1.5 cm ka bophara le bolelele ba 7 cm.Ho emisoa ha C76, HWO, HWO-10% C76, HWO-30% C76 le HWO-50% C76 ho lokiselitsoe ka ho eketsa 20 mg .% (~ 2.22 mg) ea PVDF binder ho ~ 1 ml DMF le sonicated bakeng sa hora ea 1 ho ntlafatsa ho tšoana.2 mg ea metsoako ea C76, HWO le HWO-C76 e ile ea sebelisoa ka tatellano sebakeng sa UCC se sebetsang sa elektrode se ka bang 1.5 cm2.Li-catalyst tsohle li ne li laeloa ho li-electrode tsa UCC 'me TCC e ne e sebelisetsoa merero ea ho bapisa feela, kaha mosebetsi oa rona o fetileng o bontšitse hore phekolo ea mocheso e ne e sa hlokehe24.Ho rarolla maikutlo ho ile ha finyelloa ka ho hlatsoa 100 µl ea ho emisoa (moroalo 2 mg) bakeng sa phello e matla haholoanyane.Joale li-electrode tsohle li omisitsoe ka ontong ka 60 ° C. bosiu bo le bong.Li-electrode li lekanyetsoa ho ea pele le morao ho netefatsa hore ho na le thepa e nepahetseng.E le hore ho be le sebaka se itseng sa geometri (~ 1.5 cm2) le ho thibela ho phahama ha vanadium electrolyte ho electrode ka lebaka la phello ea capillary, ho ne ho sebelisoa lesela le tšesaane la parafine holim'a thepa e sebetsang.
Emission electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) e ile ea sebelisoa ho shebella morphology ea holim'a HWO.Sehlahlo sa X-ray se qhalakanyang matla se nang le Feii8SEM (EDX, Zeiss Inc.) se ile sa sebelisoa ho etsa 'mapa oa likarolo tsa HWO-50%C76 ho li-electrode tsa UCC.Maekerosekoupo ea elektronike ea phetiso e phahameng (HR-TEM, JOEL JEM-2100) e sebetsang ka matla a phahameng a 200 kV e ile ea sebelisoa ho etsa setšoantšo sa likaroloana tse phahameng tsa HWO le mehele ea diffraction.Software ea Crystallography Toolbox (CrysTBox) e sebelisa ts'ebetso ea ringGUI ho sekaseka paterone ea phallo ea lesale la HWO le ho bapisa liphetho le paterone ea XRD.Sebopeho le graphitization ea UCC le TCC li ile tsa hlahlojoa ke X-ray diffraction (XRD) ka tekanyo ea scan ea 2.4 ° / min ho tloha 5 ° ho ea 70 ° le Cu Kα (λ = 1.54060 Å) ho sebelisa Panalytical X-ray diffractometer (Model 3600).XRD e bontšitse sebopeho sa kristale le mohato oa HWO.Software ea PANalytical X'Pert HighScore e ile ea sebelisoa ho bapisa litlhōrō tsa HWO le limmapa tsa tungsten oxide tse fumanehang polokelong ea polokelo45.Liphetho tsa HWO li bapisoa le liphetho tsa TEM.Sebopeho sa lik'hemik'hale le boemo ba lisampole tsa HWO li ile tsa khethoa ke X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).Software ea CASA-XPS (v 2.3.15) e ile ea sebelisoa bakeng sa tlhōrō ea ts'ebetso le tlhahlobo ea data.Ho fumana hore na lihlopha tse sebetsang ka holim'a metsi tsa HWO le HWO-50% C76, litekanyo li entsoe ho sebelisoa Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, ho sebelisoa KBr FTIR).Liphetho li bapisitsoe le liphetho tsa XPS.Litekanyo tsa angle angle (KRUSS DSA25) li ne li boetse li sebelisetsoa ho khetholla ho ba metsi ha li-electrode.
Bakeng sa litekanyo tsohle tsa electrochemical, ho ile ha sebelisoa setsi sa mosebetsi sa Biologic SP 300.Cyclic voltammetry (CV) le electrochemical impedance spectroscopy (EIS) li ile tsa sebelisoa ho ithuta electrode kinetics ea VO2 +/VO2+ redox reaction le phello ea reagent diffusion (VOSO4 (VO2 +)) ka tekanyo ea ho itšoara.Mekhoa eo ka bobeli e sebelisitse sele ea electrode e meraro e nang le motsoako oa electrolyte oa 0.1 M VOSO4 (V4 +) ho 1 M H2SO4 + 1 M HCl (motsoako oa li-acids).Lintlha tsohle tsa electrochemical tse hlahisitsoeng li lokisitsoe IR.Ho ile ha sebelisoa k'halomele ea "saturated calomel electrode" (SCE) le "platinum" (Pt) "electrode" ea "referense" le "counter electrode", ka ho latellana.Bakeng sa CV, litekanyetso tsa ho hlahloba (ν) tsa 5, 20, le 50 mV/s li ile tsa sebelisoa ho fensetere e ka bang teng ea VO2+/VO2+ bakeng sa (0–1) V vs. SCE, eaba e lokisoa bakeng sa SHE ho rera (VSCE = 0.242 V vs. HSE) .Ho ithuta ho boloka ts'ebetso ea li-electrode, li-CV tse pheta-phetoang tsa cyclic li ile tsa etsoa ho ν 5 mV/s bakeng sa UCC, TCC, UCC-C76, UCC-HWO, le UCC-HWO-50% C76.Bakeng sa litekanyo tsa EIS, lebelo la maqhubu a VO2+/VO2+ redox reaction e ne e le 0.01-105 Hz, le perturbation ea voltage at open-circuit voltage (OCV) e ne e le 10 mV.Teko e 'ngoe le e' ngoe e phetoa ka makhetlo a 2-3 ho netefatsa hore liphetho li lumellana.Mefuta e sa tšoaneng ea litekanyetso (k0) e fumanoe ka mokhoa oa Nicholson46,47.
Hydrated tungsten oxide (HVO) e entsoe ka katleho ka mokhoa oa hydrothermal.Setšoantšo sa SEM ka feiga.1a e bontša hore HWO e kentsoeng e na le lihlopha tsa li-nanoparticles tse nang le boholo ba 25-50 nm.
Mokhoa oa X-ray diffraction oa HWO o bontša litlhōrō (001) le (002) ho ~ 23.5 ° le ~ 47.5 °, ka ho latellana, e leng tšobotsi ea nonstoichiometric WO2.63 (W32O84) (PDF 077–0810, a = 21.4 Å Å γ = Å 8 = Å γ = 1 = Å 8 = Å γ = 1, b Å 8 = , b Å 8 = 1 = 1, b = 1 = 1, b = 1 = 1 = 90 °), e lumellanang le 'mala oa bona o moputsoa o hlakileng (setšoantšo sa 1b) 48.49.Litlhōrō tse ling tse ka bang 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° le 52.7° li abetsoe (140), (620), (350), (720), (740), (560°).) ) le (970) lifofane tsa diffraction orthogonal ho WO2.63, ka ho latellana.Mokhoa o tšoanang oa maiketsetso o ne o sebelisoa ke Songara et al.43 ho fumana sehlahisoa se tšoeu, se neng se bakoa ke boteng ba WO3 (H2O) 0.333.Leha ho le joalo, mosebetsing ona, ka lebaka la maemo a fapaneng, ho ile ha fumanoa sehlahisoa se botala bo botala, se bontšang hore WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90 °) le foromo e fokotsehileng ea oxide.Tlhahlobo ea semiquantitative e sebelisang software ea X'Pert HighScore e bontšitse 26% WO3 (H2O) 0.333: 74% W32O84.Kaha W32O84 e na le W6+ le W4+ (1.67:1 W6+:W4+), likhakanyo tse hakanyetsoang tsa W6+ le W4+ li ka ba 72% W6+ le 28% W4+, ka ho latellana.Litšoantšo tsa SEM, ponahalo ea XPS ea 1-ea bobeli boemong ba nucleus, litšoantšo tsa TEM, FTIR spectra, le Raman spectra ea likaroloana tsa C76 li hlahisitsoe sehloohong sa rona se fetileng.Ho ea ka Kawada et al.,50,51 X-ray diffraction ea C76 ka mor'a ho tlosoa ha toluene e bontšitse sebopeho sa monoclinic sa FCC.
Litšoantšo tsa SEM ka feiga.2a le b li bontša hore HWO le HWO-50% C76 li ile tsa kenngoa ka katleho le pakeng tsa carbon fibers ea UCC electrode.Limmapa tsa likarolo tsa EDX tsa tungsten, carbon, le oksijene litšoantšong tsa SEM ka feiga.2c li bonts'itsoe ka feiga.2d-f e bontšang hore tungsten le carbon li tsoakane ka ho lekana (ho bontša kabo e tšoanang) holim'a sebaka sohle sa electrode 'me motsoako ha o kopane ka mokhoa o ts'oanang ka lebaka la mofuta oa mokhoa oa ho beha.
Litšoantšo tsa SEM tsa likaroloana tsa HWO tse kentsoeng (a) le likaroloana tsa HWO-C76 (b).'Mapa oa EDX ho HWO-C76 o laetsoeng UCC o sebelisa sebaka se setšoantšong (c) o bonts'a kabo ea tungsten (d), carbon (e), le oksijene (f) sampoleng.
HR-TEM e ne e sebelisetsoa litšoantšo tse phahameng tse holisang le tlhahisoleseling ea crystallographic (Setšoantšo sa 3).HWO e bonts'a morphology ea nanocube joalokaha e bontšitsoe setšoantšong sa 3a le ka ho hlaka haholoanyane ho 3b.Ka ho hōlisa nanocube bakeng sa diffraction ea libaka tse khethiloeng, motho a ka bona sebopeho sa grating le lifofane tsa diffraction tse khotsofatsang molao oa Bragg, joalokaha ho bontšitsoe setšoantšong sa 3c, se tiisang crystallinity ea thepa.Ho setšoantšo sa 3c se bonts'a sebaka sa d 3.3 Å se tsamaisanang le lifofane tsa (022) le (620) tsa diffraction tse fumanoang likarolong tsa WO3 (H2O) 0.333 le W32O84, ka ho latellana43,44,49.Sena se lumellana le tlhahlobo ea XRD e hlalositsoeng ka holimo (setšoantšo sa 1b) kaha sebaka sa sefofane sa grating se hlokometsoeng d (setšoantšo sa 3c) se lumellana le tlhōrō e matla ka ho fetisisa ea XRD ho sampuli ea HWO.Mehele ea mohlala e boetse e bontšoa ka feiga.3d, moo selikalikoe se seng le se seng se lumellanang le sefofane se arohaneng.Lifofane tsa WO3 (H2O) 0.333 le W32O84 li na le mebala e tšoeu le e putsoa, ​​ka ho latellana, 'me litlhōrō tsa tsona tsa XRD tse tsamaellanang le tsona li bontšoa setšoantšong sa 1b.Reng ea pele e bontšitsoeng setšoantšong sa reng e lumellana le tlhōrō ea pele e tšoailoeng ka mokhoa oa x-ray oa sefofane sa diffraction (022) kapa (620).Ho tloha meheleng ea (022) ho ea ho (402), litekanyetso tsa d-spacing ke 3.30, 3.17, 2.38, 1.93, le 1.69 Å, tse tsamaellanang le litekanyetso tsa XRD tsa 3.30, 3.17, 2, 45, 1.93.le 1.66 Å, e lekanang le 44, 45, ka ho latellana.
(a) Setšoantšo sa HR-TEM sa HWO, (b) se bontša setšoantšo se holisitsoeng.Litšoantšo tsa lifofane tsa grating li bontšoa ho (c), inset (c) e bontša setšoantšo se atolositsoeng sa lifofane le pitch d ea 0.33 nm e lumellanang le lifofane (002) le (620).(d) Mohlala oa lesale oa HWO o bontšang lifofane tse amanang le WO3 (H2O) 0.333 (e tšoeu) le W32O84 (e putsoa).
Tlhahlobo ea XPS e ile ea etsoa ho fumana hore na k'hemistri e holim'a metsi le boemo ba oxidation ea tungsten (Lipalo S1 le 4).Mefuta e mengata e fapaneng ea XPS scan spectrum ea HWO e entsoeng e bontšoa ho Setšoantšo sa S1, se bontšang boteng ba tungsten.The XPS-scan-scan spectra ea maemo a mantlha a W 4f le O 1s a bontšoa ho Feiga.4a le b, ka ho latellana.Maqhubu a W 4f a arohana ho etsa li-spin-orbit tse peli tse tsamaellanang le matla a tlamang a W oxidation state.le W 4f7/2 ho 36.6 le 34.9 eV ke litšobotsi tsa boemo ba W4+ ba 40, ka ho latellana.)0.333.Lintlha tse kentsoeng li bonts'a hore liperesente tsa athomo tsa W6+ le W4+ ke 85% le 15%, ka ho latellana, tse haufi le boleng bo hakantsoeng ho data ea XRD ho nahanoa ka phapang lipakeng tsa mekhoa ena e 'meli.Mekhoa ena ka bobeli e fana ka tlhaiso-leseling e ngata ka nepo e tlase, haholo XRD.Hape, mekhoa ena e 'meli e sekaseka likarolo tse fapaneng tsa lisebelisoa hobane XRD ke mokhoa o mongata ha XPS e le mokhoa o holimo o atamelang li-nanometer tse' maloa feela.Sekhahla sa O 1 se arotsoe ka litlhōrō tse peli ho 533 (22.2%) le 530.4 eV (77.8%).Ea pele e lumellana le OH, 'me ea bobeli e lumellana le litlamo tsa oksijene letšeng ho WO.Ho ba teng ha lihlopha tse sebetsang tsa OH ho lumellana le thepa ea hydration ea HWO.
Tlhahlobo ea FTIR e ile ea boela ea etsoa lisampoleng tsena tse peli ho hlahloba boteng ba lihlopha tse sebetsang le ho hokahanya limolek'hule tsa metsi mohahong oa HWO o nang le metsi.Liphello li bontša hore sampuli ea HWO-50% C76 le liphello tsa FT-IR HWO li bonahala li tšoana ka lebaka la ho ba teng ha HWO, empa matla a litlhōrō a fapane ka lebaka la palo e fapaneng ea sampuli e sebelisoang ho lokisetsa tlhahlobo (setšoantšo sa 5a).) HWO-50% C76 e bontša hore litlhōrō tsohle, ntle le tlhōrō ea tungsten oxide, li amana le fullerene 24. E qaqileng ka feiga.5a e bonts'a hore lisampole ka bobeli li bonts'a sehlopha se sephara se matla haholo ho ~ 710 / cm se hlahisoang ke OWO oscillations e otlolohileng ka har'a sebopeho sa lattice sa HWO, se nang le lehetla le matla ho ~ 840 / cm e hlahisoang ke WO.Bakeng sa ho thothomela ho otlollang, sehlopha se bohale se ka bang 1610/cm se hlahisoa ke ho thothomela ha OH, ha sehlopha se pharaletseng sa ho monya se ka bang 3400/cm se hlahisoa ke ho thothomela ha OH ka lihlopha tsa hydroxyl43.Liphetho tsena li lumellana le ponahalo ea XPS ho Feiga.4b, moo lihlopha tse sebetsang tsa WO li ka fanang ka libaka tse sebetsang bakeng sa karabelo ea VO2+/VO2+.
Tlhahlobo ea FTIR ea HWO le HWO-50% C76 (a), e bontšitse lihlopha tse sebetsang le litekanyo tsa angle angle (b, c).
Sehlopha sa OH se ka boela sa kenya letsoho karabelo ea VO2 +/VO2+, ha se ntse se eketsa hydrophilicity ea electrode, kahoo se khothalletsa sekhahla sa ho hasana le ho fetisetsa elektronike.Joalokaha ho bontšitsoe, mohlala oa HWO-50% C76 o bontša tlhōrō e eketsehileng bakeng sa C76.Litlhōrō ho ~ 2905, 2375, 1705, 1607, le 1445 cm3 li ka abeloa ho CH, O=C=O, C=O, C=C, le CO otlollang vibrations, ka ho latellana.Hoa tsebahala hore lihlopha tse sebetsang tsa oksijene C=O le CO li ka sebetsa e le litsi tse sebetsang bakeng sa karabelo ea redox ea vanadium.Ho hlahloba le ho bapisa ho nosetsa ha li-electrode tse peli, litekanyo tsa mahlakore a ho kopana li nkiloe joalokaha ho bontšitsoe setšoantšong sa 5b, c.HWO electrode hang-hang e ile ea monya marotholi a metsi, e bontšang superhydrophilicity ka lebaka la lihlopha tse sebetsang tsa OH tse teng.HWO-50% C76 e na le hydrophobic ho feta, e nang le angle ea ho kopana e ka bang 135 ° ka mor'a metsotsoana e 10.Leha ho le joalo, litekanyong tsa electrochemical, electrode ea HWO-50% C76 e ile ea koloba ka ho feletseng ka nako e ka tlaase ho motsotso.Litekanyo tsa boemo ba metsi li lumellana le liphetho tsa XPS le FTIR, tse bontšang hore lihlopha tse ngata tsa OH holim'a HWO li etsa hore e be hydrophilic haholoanyane.
Lits'ebetso tsa VO2+/VO2+ tsa HWO le HWO-C76 nanocomposites li ile tsa lekoa 'me ho ne ho lebeletsoe hore HWO e tla hatella phetoho ea chlorine karabelong ea VO2+/VO2+ ka acid e tsoakiloeng,' me C76 e tla tsoela pele ho susumetsa karabelo e lakatsehang ea VO2+/VO2+ redox.%, 30%, le 50% C76 ho suspensions HWO le CCC depositi holim'a li-electrode tse nang le kakaretso ea ho laela hoo e ka bang 2 mg/cm2.
Joalokaha ho bontšitsoe feiga.6, kinetics ea VO2 +/VO2+ karabelo holim'a electrode e ile ea hlahlojoa ke CV ka electrolyte e tsoakiloeng ea acidic.Maqhubu a bonts'oa joalo ka I/Ipa bakeng sa papiso e bonolo ea ΔEp le Ipa/Ipc bakeng sa li-catalyst tse fapaneng ka kotloloho ho graph.Lintlha tsa hajoale tsa yuniti ea sebaka li bonts'itsoe ho Figure 2S.Ka feiga.Setšoantšo sa 6a se bontša hore HWO e eketsa hanyenyane lebelo la phetisetso ea elektronike ea VO2 +/VO2+ redox reaction holim'a elektrode holim'a metsi le ho hatella karabelo ea ho iphetola ha chlorine ea parasitic.Leha ho le joalo, C76 e eketsa haholo sekhahla sa phetisetso ea elektrone mme e susumetsa karabelo ea ho iphetola ha chlorine.Ka hona, motsoako o entsoeng ka nepo oa HWO le C76 o lebelletsoe ho ba le ts'ebetso e ntle ka ho fetisisa le bokhoni bo boholo ba ho thibela karabelo ea ho iphetola ha chlorine.Ho ile ha fumanoa hore ka mor'a ho eketsa litaba tsa C76, ts'ebetso ea electrochemical ea li-electrode e ntlafetse, joalokaha ho pakoa ke ho fokotseha ha ΔEp le keketseho ea Ipa / Ipc ratio (Letlapa la S3).Sena se ile sa boela sa tiisoa ke litekanyetso tsa RCT tse ntšitsoeng morerong oa Nyquist setšoantšong sa 6d (Letlapa la S3), le ileng la fumanoa le fokotseha ka litaba tsa C76 tse ntseng li eketseha.Liphetho tsena li boetse li lumellana le boithuto ba Li, moo ho kenyelletsoa ha carbon ea mesoporous ho mesoporous WO3 ho bonts'itseng kinetics e ntlafetseng ea phetisetso ea tefiso ho VO2+/VO2+35.Sena se bontša hore karabelo e tobileng e ka 'na ea itšetleha haholo ka conductivity ea electrode (C = C bond) 18, 24, 35, 36, 37. Sena se ka boela sa bakoa ke phetoho ea geometry ea khokahanyo pakeng tsa [VO (H2O) 5] 2+ le [VO2 (H2O) 4]+, C76 e fokotsa matla a karabelo ea lithane ka ho fokotsa matla a lithane.Leha ho le joalo, sena se kanna sa se khonehe ka li-electrode tsa HWO.
(a) Boitšoaro ba cyclic voltammetric (ν = 5 mV/s) ea karabelo ea VO2+/VO2+ ea likarolo tsa UCC le HWO-C76 tse nang le likarolo tse fapaneng tsa HWO:C76 ho 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik le (c) Nicholson VO2+/VO2+ mokhoa oa ho lekola katleho ea phallo le ho fumana litekanyetso tsa k0(d).
Hase feela hore HWO-50% C76 e ne e bontša hoo e batlang e le ts'ebetso ea electrocatalytic e tšoanang le ea C76 bakeng sa karabelo ea VO2 +/VO2+, empa, ho thahasellisang le ho feta, e ile ea boela ea hatella phetoho ea chlorine ha e bapisoa le C76, joalokaha ho bontšitsoe setšoantšong sa 6a, hape e bonts'a Semicircle e Nyenyane ka feiga.6d (RCT e tlase).C76 e bonts'itse Ipa / Ipc e phahameng ho feta HWO-50% C76 (Letlapa la S3), eseng ka lebaka la phetoho e ntlafetseng ea karabelo, empa ka lebaka la tlhōrō ea karabelo ea phokotso ea chlorine le SHE ka 1.2 V. Ts'ebetso e ntle ka ho fetisisa ea HWO- The 50% C76 e hlahisoa ka lebaka la synergistic charger le C76 e ntle haholo pakeng tsa ts'ebetso e mpe ea C76 le ts'ebetso e phahameng ea W-H-OH ea boleng bo phahameng ba cargistic. ho HWO.Khaello e fokolang ea chlorine e tla ntlafatsa bokhoni ba ho tjhaja sele e felletseng, athe kinetics e ntlafalitsoeng e tla ntlafatsa bokhoni ba motlakase o felletseng oa sele.
Ho ea ka equation S1, bakeng sa karabelo e ka fetoloang (e batlang e lieha ho fetisoa ha elektronike) e laoloang ke ho hasana, tlhōrō ea hona joale (IP) e itšetlehile ka palo ea lielektrone (n), sebaka sa li-electrode (A), coefficient ea phallo (D), palo ea li-elektronike tse fetisang coefficient (α) le lebelo la ho hlahloba (ν).E le ho ithuta boitšoaro bo laoloang ke ho hasana ha thepa e lekiloeng, kamano pakeng tsa IP le ν1/2 e ile ea raloa 'me ea hlahisoa ho Setšoantšo sa 6b.Kaha lisebelisoa tsohle li bonts'a kamano ea mohala, karabelo e laoloa ke ho hasana.Kaha VO2 +/VO2+ reaction ke quasi-reversible, moepa oa mola o itšetlehile ka coefficient ea diffusion le boleng ba α (equation S1).Kaha coefficient ea phallo e lula e le teng (≈ 4 × 10-6 cm2 / s) 52, phapang ea letsoapo la mola e bontša ka ho toba litekanyetso tse fapaneng tsa α, ka hona, sekhahla sa phetisetso ea elektrone sebakeng sa elektrode, se bonts'itsoeng bakeng sa C76 le HWO -50% C76 Moepa o phahameng ka ho fetisisa oa phetisetso ea elektronike.
Matsoapo a Warburg (W) a baliloeng bakeng sa maqhubu a tlase a bontšitsoeng ho Lethathamo la S3 (Setšoantšo sa 6d) a na le litekanyetso tse haufi le 1 bakeng sa lisebelisoa tsohle, tse bontšang phallo e phethahetseng ea mefuta ea redox le ho netefatsa boitšoaro bo tloaelehileng ba IP ha bo bapisoa le ν1/ 2. CV e lekantsoe.Bakeng sa HWO-50% C76, letsoapo la Warburg le kheloha ho tloha ho 1 ho ea ho 1.32, ho bontša eseng feela ho ata ha semi-infinite ea reagent (VO2 +), empa hape le monehelo o ka bang teng oa boitšoaro bo mosesaane ho boitšoaro ba ho hasana ka lebaka la electrode porosity.
Ho tsoela pele ho hlahloba phetoho (tekanyo ea phetisetso ea elektronike) ea VO2 +/VO2+ redox reaction, mokhoa oa Nicholson quasi-reversible reaction o ile oa boela oa sebelisoa ho fumana tekanyo e tloaelehileng ea k041.42.Sena se etsoa ho sebelisoa equation ea S2 ho aha paramethara ea kinetic e se nang dimensionless Ψ, e leng mosebetsi oa ΔEp, joalo ka ts'ebetso ea ν-1/2.Letlapa la S4 le bonts'a boleng ba Ψ bo fumanoeng bakeng sa thepa e 'ngoe le e' ngoe ea elektrode.Liphetho (setšoantšo sa 6c) li ne li reretsoe ho fumana k0 × 104 cm/s ho tloha letsoapong la setša ka seng ho sebelisoa Equation S3 (e ngotsoeng haufi le mola o mong le o mong le ho hlahisoa ho Lethathamo la S4).HWO-50% C76 e fumanoe e e-na le moepa o phahameng ka ho fetisisa (setšoantšo sa 6c), kahoo boholo ba k0 ke 2.47 × 10-4 cm / s.Sena se bolela hore electrode ena e finyella kinetics e potlakileng ka ho fetisisa, e lumellanang le liphello tsa CV le EIS ho Fig. 6a le d le ho Lethathamo la S3.Ho phaella moo, boleng ba k0 bo ile ba boela ba fumanoa ho tloha sebakeng sa Nyquist (setšoantšo sa 6d) sa Equation S4 se sebelisa boleng ba RCT (Letlapa la S3).Liphetho tsena tsa k0 ho tsoa ho EIS li akaretsoa ho Lethathamo la S4 hape li bonts'a hore HWO-50% C76 e bonts'a sekhahla se phahameng sa phetisetso ea elektronike ka lebaka la phello ea synergistic.Leha boleng ba k0 bo fapana ka lebaka la tšimoloho e fapaneng ea mokhoa o mong le o mong, ba ntse ba bonts'a tatellano e ts'oanang ea boholo le ho bonts'a botsitso.
Ho utloisisa ka botlalo li-kinetics tse ntle tse fumanoeng, ho bohlokoa ho bapisa lisebelisoa tse nepahetseng tsa elektrode le li-electrode tsa UCC le TCC tse sa koaeloang.Bakeng sa karabelo ea VO2+/VO2+, HWO-C76 ha ea ka ea bontša feela ΔEp e tlase le ho fetoha hantle, empa hape e hatelletse karabelo ea phetoho ea chlorine ea parasitic ha e bapisoa le TCC, joalo ka ha e lekantsoe ke hona joale ho 1.45 V mabapi le SHE (Setšoantšo sa 7a).Mabapi le botsitso, re ne re nahana hore HWO-50% C76 e tsitsitse 'meleng hobane motsoako o ne o kopantsoe le PVDF binder ebe o sebelisoa ho li-electrode tsa lesela la carbon.HWO-50% C76 e bontšitse phetoho e phahameng ea 44 mV (sekhahla sa ho senyeha ha 0.29 mV / cycle) ka mor'a lipotoloho tsa 150 ha li bapisoa le 50 mV bakeng sa UCC (Setšoantšo sa 7b).Sena e kanna ea se be phapang e kholo, empa kinetics ea li-electrode tsa UCC e lieha haholo ebile e nyenyefatsa ka ho palama libaesekele, haholo-holo bakeng sa karabelo ea morao.Le hoja phetoho ea TCC e le molemo haholo ho feta ea UCC, TCC e fumanoe e na le phetoho e kholo ea tlhōrō ea 73 mV ka mor'a lipotoloho tse 150, e ka 'nang ea bakoa ke bongata ba chlorine bo entsoeng holim'a eona.e le hore catalyst e khomarele hantle holim'a electrode.Joalokaha ho ka bonoa ho li-electrode tsohle tse lekiloeng, esita le li-electrode ntle le li-catalyst tse tšehetsoeng li bontšitse likhato tse sa tšoaneng tsa ho se tsitse ha libaesekele, ho fana ka maikutlo a hore phetoho ea karohano ea tlhōrō nakong ea ho palama libaesekele e bakoa ke ho tima lintho tse bakoang ke liphetoho tsa lik'hemik'hale ho e-na le ho arohana ha libaesekele.Ho phaella moo, haeba palo e kholo ea likaroloana tsa catalyst e ne e lokela ho aroloa ho tloha holim'a elektrode, sena se ne se tla fella ka keketseho e kholo ea karohano ea tlhōrō (eseng feela 44 mV), kaha substrate (UCC) e batla e sa sebetse bakeng sa VO2 +/VO2 + redox reaction.
Ho bapisa CV ea lisebelisoa tse ntle ka ho fetisisa tsa electrode ha li bapisoa le UCC (a) le botsitso ba VO2 +/VO2 + redox reaction (b).ν = 5 mV/s bakeng sa li-CV tsohle ho 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Ho eketsa khahleho ea moruo ea theknoloji ea VRFB, ho holisa le ho utloisisa kinetics ea karabelo ea vanadium redox ho bohlokoa ho fihlela katleho e phahameng ea matla.Li-composites HWO-C76 li ile tsa lokisoa 'me phello ea bona ea electrocatalytic ho karabelo ea VO2+/VO2+ e ile ea ithutoa.HWO e bonts'itse ntlafatso e nyane ea kinetic ho li-electrolyte tsa asiti tse tsoakiloeng empa e hatelletse kholo ea chlorine haholo.Likarolo tse fapaneng tsa HWO: C76 li ile tsa sebelisoa ho ntlafatsa kinetics ea li-electrode tse thehiloeng ho HWO.Ho eketsa C76 ho HWO ho ntlafatsa kinetics ea phetisetso ea elektronike ea VO2 +/VO2 + karabelo ea electrode e fetotsoeng, eo HWO-50% C76 e leng thepa e ntle ka ho fetisisa hobane e fokotsa ho hanyetsa phetisetso ea tefiso le ho feta ho hatella chlorine ha e bapisoa le C76 le TCC deposit..Sena se bakoa ke phello ea synergistic lipakeng tsa C=C sp2 hybridization, OH le W-OH lihlopha tse sebetsang.Sekhahla sa ho senyeha ka mor'a ho palama libaesekele khafetsa HWO-50% C76 e fumanoe e le 0.29 mV / cycle, ha tekanyo ea ho senyeha ha UCC le TCC e le 0.33 mV / cycle le 0.49 mV / cycle, ka ho latellana, e etsa hore e be e tsitsitseng haholo.ka li-electrolyte tsa asiti tse tsoakiloeng.Liphetho tse hlahisitsoeng ka katleho li tsebahatsa lisebelisoa tse phahameng tsa elektrode bakeng sa karabelo ea VO2+/VO2+ ka kinetics e potlakileng le botsitso bo phahameng.Sena se tla eketsa motlakase oa tlhahiso, kahoo se eketsa ts'ebetso ea matla a VRFB, kahoo se fokotsa litšenyehelo tsa khoebo ea eona ea nako e tlang.
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