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Mutengo wakakwira weese-vanadium kuyerera-kuburikidza neredox mabhatiri (VRFBs) inodzikamisa kushandiswa kwavo kwakapararira.Kuvandudza kinetics ye electrochemical reactions kunodiwa kuwedzera simba chairo uye simba reVRFB, nekudaro kuderedza mutengo wekWh weVRFB.Mubasa iri, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 uye C76/HWO, akaiswa pacarbon cloth electrodes uye akaedzwa semagetsi eVO2+/VO2+ redox reaction.Munda emission scanning electron microscopy (FESEM), simba dispersive X-ray spectroscopy (EDX), high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier shandura Spectroscopy (FTIR) uye kuonana kwekona kuyerwa.Zvakaonekwa kuti kuwedzera kweC76 fullerenes kuHWO kunogona kuvandudza electrode kinetics kuburikidza nekuwedzera magetsi ekugadzirisa uye kupa mapoka ekuita oxidized pamusoro pepamusoro payo, nokudaro achikurudzira VO2 +/VO2 + redox reaction.HWO/C76 composite (50 wt% C76) yakaratidza kuti ndiyo yakanakisa sarudzo yeVO2+/VO2+ reaction neΔEp ye176 mV, nepo isina kugadzirwa kabhoni jira (UCC) yaive 365 mV.Mukuwedzera, iyo HWO / C76 composite yakaratidza zvakakosha inhibitory effect paparasitic chlorine evolution reaction nekuda kweW-OH inoshanda boka.
Kuita kwakasimba kwevanhu uye kukurumidza kwekuchinja kwemaindasitiri kwakakonzera kudiwa kwakanyanya kwemagetsi, kuri kuwedzera ne3% pagore.Kwemakumi emakore, kushandiswa kwakapararira kwefossil sechitubu chesimba kwakakonzera kuburitsa gasi regreenhouse rinokonzera kudziya kwepasi rose, kusvibiswa kwemvura nemhepo, zvichityisidzira zvisikwa zvese.Somugumisiro, kupinda kwemhepo yakachena uye inogadziriswa uye simba rezuva rinotarisirwa kusvika 75% yemagetsi ose ne 20501. Zvisinei, apo chikamu chemagetsi kubva kune zvinyorwa zvinogadziriswa zvinodarika 20% yehuwandu hwemagetsi emagetsi, grid inova isina kugadzikana.
Pakati pese masisitimu ekuchengetedza simba senge hybrid vanadium redox flow battery2, iyo all-vanadium redox flow bhatiri (VRFB) yakagadzira nekukurumidza zvakanyanya nekuda kwezvakanakira zvakawanda uye inoonekwa seyakanakisa mhinduro yekuchengetedza simba kwenguva refu (anenge makore makumi matatu).) Sarudzo dzakasanganiswa nesimba rinodzokororwa4.Izvi zvinokonzerwa nekuparadzaniswa kwesimba uye simba remagetsi, kupindura nokukurumidza, hupenyu hurefu hwebasa, uye mutengo wepagore we $ 65 / kWh uchienzaniswa ne $ 93-140 / kWh yeLi-ion uye mabhatiri e-lead-acid uye 279-420 US dollars per kWh.bhatiri zvichiteerana 4.
Nekudaro, kushambadzira kwavo kwakakura kuchiri kudzvinyirirwa nemari yavo yakakwira system capital, kunyanya nekuda kwema cell stacks4,5.Nekudaro, kuvandudza stack performance nekuwedzera kinetics yeaviri hafu-element reactions inogona kuderedza saizi ye stack nekudaro kuderedza mutengo.Naizvozvo, kukurumidza kuendesa erekitironi kune electrode kumusoro kunodiwa, izvo zvinoenderana nekugadzirwa, kuumbwa uye chimiro cheiyo electrode uye inoda kunyatso optimization6.Pasinei nekemikari yakanaka uye kugadzikana kwe electrochemical uye yakanaka magetsi conductivity ye carbon electrodes, kinetics yavo isina kubatwa inononoka nekuda kwekushayikwa kweokisijeni inoshanda mapoka uye hydrophilicity7,8.Naizvozvo, maelectrocatalyst akasiyana-siyana anosanganiswa nekabhoni-based electrode, kunyanya kabhoni nanostructures uye metal oxides, kuvandudza kinetics yeese maelectrode, nekudaro kuwedzera kinetics yeVRFB electrode.
Pamusoro pebasa redu rekare paC76, isu takatanga kurondedzera yakanakisa electrocatalytic basa reiyi fullerene yeVO2 +/VO2+, kutengesa kutengesa, zvichienzaniswa nekupisa-kugadziriswa uye kusina kushandiswa kabhoni jira.Kupokana kunoderedzwa ne99.5% uye 97%.Iyo inokonzeresa kuita kwekabhoni zvinhu zveVO2+/VO2+ reaction kana ichienzaniswa neC76 inoratidzwa muTafura S1.Nekune rimwe divi, masimbi akawanda esimbi akadai seCeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 uye WO331, 32, 33, 34, 35, 36, 37 akashandiswa nekuda kwekuwedzera kwemvura uye kushanda kweokisijeni yakawanda., 38. boka.Iyo catalytic chiitiko cheaya simbi oxides muVO2+/VO2+ reaction inoratidzwa muTebhura S2.WO3 yakashandiswa muhuwandu hunokosha hwemabasa nekuda kwekudhura kwayo, kugadzikana kwepamusoro mu acidic media, uye high catalytic activity31,32,33,34,35,36,37,38.Nekudaro, kuvandudzwa kwecathodic kinetics nekuda kweWO3 haina kukosha.Kuti uvandudze conductivity yeWO3, mhedzisiro yekushandisa yakaderedzwa tungsten oxide (W18O49) pane cathodic basa yakaedzwa38.Hydrated tungsten oxide (HWO) haina kumbobvira yakaedzwa muVRFB maapplication, kunyangwe ichiratidzira yakawedzera chiitiko mu supercapacitor application nekuda kwekukurumidza cation diffusion ichienzaniswa neanhydrous WOx39,40.Chizvarwa chechitatu vanadium redox inoyerera bhatiri inoshandisa yakasanganiswa acid electrolyte inoumbwa neHCl neH2SO4 kuvandudza kushanda kwebhatiri uye kuvandudza kunyungudika uye kugadzikana kwevanadium ions mu electrolyte.Nekudaro, iyo parasitic chlorine evolution reaction yave imwe yezvakashata zvechizvarwa chechitatu, saka kutsvaga nzira dzekudzivisa chlorine evaluation reaction kwave kutarisisa kwemapoka akati wandei ekutsvagisa.
Pano, VO2+/VO2+ reaction tests yakaitwa paHWO/C76 composites yakaiswa pamakabhoni machira maelectrodes kuitira kuti vawane chiyero pakati pemagetsi conductivity yemakompositi uye redox kinetics yeelectrode surface uku ichidzvanya parasitic chlorine evolution.mhinduro (CER).Hydrated tungsten oxide (HWO) nanoparticles akagadzirwa nenzira iri nyore yehydrothermal.Maedzo akaitwa musanganiswa asidhi electrolyte (H2SO4/HCl) kutevedzera chizvarwa chechitatu VRFB (G3) kuti zvishande uye kuongorora mhedzisiro yeHWO paparasitic chlorine evolution reaction.
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 2 hydroxyde, 9 hydrochloride, 9 carbon-oxyde dihydrate, sodium Tungstenphild, 9 hydrochloric oxide jira ELAT (Fuel Cell Store) rakashandiswa muchidzidzo ichi.
Hydrated tungsten oxide (HWO) yakagadzirwa nehydrothermal reaction 43 umo 2 g yemunyu weNa2WO4 yakanyungudutswa mu12 ml yeH2O kuti ipe mushonga usina ruvara, kozoti 12 ml ye2 M HCl yakawedzerwa inodonha kuti ipe yellow yellow suspension.Iyo slurry yakaiswa muTeflon yakavharwa nesimbi isina tsvina autoclave uye yakachengetwa muchoto pa180 ° C. kwemaawa matatu kuitira hydrothermal reaction.Iyo yakasara yakaunganidzwa nefiltration, yakashambidzwa katatu ne ethanol nemvura, yakaomeswa muchoto pa 70 ° C kwe ~ maawa matatu, uye zvino triturated kupa blue-grey HWO powder.
Iyo yakawanikwa (isina kubatwa) kabhoni jira electrodes (CCT) yakashandiswa sezviri kana kupisa yakabatwa muchoto chechubhu pa450 ° C mumhepo ine kudziya kwe15 ºC/min kwemaawa gumi kuti iwane kurapwa CCs (TCC).sezvakatsanangurwa munyaya yapfuura24.UCC neTCC zvakachekwa kuita maelectrodes anenge 1.5 cm yakafara uye 7 cm kureba.Kumiswa kweC76, HWO, HWO-10% C76, HWO-30% C76 uye HWO-50% C76 yakagadzirirwa nekuwedzera 20 mg .% (~ 2.22 mg) yePVDF binder ku ~ 1 ml DMF uye sonicated kweawa 1 kuti iwedzere kufanana.2 mg yeC76, HWO uye HWO-C76 macomposites akaiswa sequentially kune UCC inoshanda electrode nzvimbo inosvika 1.5 cm2.Zvose zvinogadzirisa zvakatakurwa paUCC electrodes uye TCC yakashandiswa kuenzanisa zvinangwa chete, sezvo basa redu rekare rakaratidza kuti kupisa kupisa kwakanga kusingadiwi24.Kugadzirisa kugadzirisa kwakawanikwa nekukwesha 100 µl yekumisa (mutoro 2 mg) kune imwe mhedzisiro.Zvadaro magetsi ose akaomeswa muchoto pa60 ° C. usiku hwose.Ma electrode anoyerwa kumberi nekumashure kuti ive nechokwadi chekurodha kwemasheya.Kuti tive nedzimwe nzvimbo yejometri (~ 1.5 cm2) uye kudzivirira kukwira kwevanadium electrolyte ku electrode nekuda kwe capillary effect, parafini yakaonda yakashandiswa pamusoro pezvinhu zvinoshanda.
Munda emission scanning electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) yakashandiswa kuona HWO pamusoro morphology.Simba rinoparadzira X-ray spectrometer ine Feii8SEM (EDX, Zeiss Inc.) yakashandiswa kugadzira HWO-50% C76 zvinhu pamagetsi eUCC.A high resolution transmission electron maikorosikopu (HR-TEM, JOEL JEM-2100) inoshanda pamhepo inomhanya ye 200 kV yakashandiswa kuratidza magadzirirwo akakwirira eHWO zvidimbu nemarin'i ekuparadzanisa.Iyo Crystallography Toolbox (CrysTBox) software inoshandisa iyo ringGUI basa kuongorora HWO mhete diffraction pateni uye kuenzanisa mhedzisiro neXRD pateni.Chimiro uye graphitization yeUCC neTCC yakaongororwa neX-ray diffraction (XRD) pachiyero chekuongorora che 2.4 ° / min kubva ku5 ° kusvika 70 ° neCu Kα (λ = 1.54060 Å) uchishandisa Panalytical X-ray diffractometer (Model 3600).XRD yakaratidza chimiro chekristaro uye chikamu cheHWO.Iyo PANalytical X'Pert HighScore software yakashandiswa kuenzanisa nhongonya dzeHWO kune tungsten oxide mepu inowanikwa mudura45.HWO mhedzisiro yakaenzaniswa nemhedzisiro yeTEM.Iko kuumbwa kwekemikari uye mamiriro emasampuli eHWO akatemerwa neX-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).Iyo CASA-XPS software (v 2.3.15) yakashandiswa peak deconvolution uye kuongorora data.Kuti uone mapoka epamusoro anoshanda eHWO neHWO-50% C76, kuyerwa kwakaitwa pachishandiswa Fourier kushandura infrared spectroscopy (FTIR, Perkin Elmer spectrometer, vachishandisa KBr FTIR).Mhedzisiro yacho yakaenzaniswa nemhedzisiro yeXPS.Contact angle measurements (KRUSS DSA25) yakashandiswawo kuratidza kunyorova kwema electrode.
Kune ese electrochemical zviyero, Biologic SP 300 workstation yakashandiswa.Cyclic voltammetry (CV) uye electrochemical impedance spectroscopy (EIS) yakashandiswa kudzidza electrode kinetics yeVO2+/VO2+ redox reaction uye mhedzisiro ye reagent diffusion (VOSO4(VO2+)) padanho rekuita.Nzira mbiri idzi dzakashandisa sero re-electrode ine electrolyte concentration ye 0.1 M VOSO4 (V4+) mu 1 M H2SO4 + 1 M HCl (musanganiswa weasidhi).Yese data ye electrochemical inoratidzwa ndeye IR yakagadziriswa.A saturated calomel electrode (SCE) uye platinum (Pt) coil yakashandiswa sereferensi uye counter electrode, zvichiteerana.KuCV, scan rates (ν) ye5, 20, uye 50 mV/s yakashandiswa kuVO2+/VO2+ inogona kuitika hwindo re (0–1) V vs. SCE, ndokuzogadziriswa kuti SHE kuronga (VSCE = 0.242 V vs. HSE) .Kuti udzidze kuchengetwa kwechiitiko che electrode, akadzokororwa cyclic CVs akaitwa pa ν 5 mV/s ye UCC, TCC, UCC-C76, UCC-HWO, uye UCC-HWO-50% C76.Pazviyero zveEIS, frequency range yeVO2+/VO2+ redox reaction yaive 0.01-105 Hz, uye voltage perturbation pa open-circuit voltage (OCV) yaive 10 mV.Kuedza kwega kwega kwakadzokororwa 2-3 nguva kuti ive nechokwadi chekuenderana kwemhedzisiro.The heterogeneous rate constants (k0) yakawanikwa neNicholson method46,47.
Hydrated tungsten oxide (HVO) yakabudirira kugadzirwa nenzira yehydrothermal.SEM mufananidzo mufig.1a inoratidza kuti iyo HWO yakaiswa ine masumbu e nanoparticles ane saizi muhuwandu hwe25-50 nm.
X-ray diffraction pattern yeHWO inoratidza mapeaks (001) uye (002) pa ~ 23.5 ° uye ~ 47.5 °, zvichienderana, iyo inofananidzwa nenonstoichiometric WO2.63 (W32O84) (PDF 077-0810, a = 21.4 Å Å = Å γ = Å γ = 1 = Å , b Å 8 = , b Å 8 = 1 = 1, b Å 8 = , b = 1 = 1, b = 1, b = 1, b = 1, b = 1 = 1, b = 1. 90 °), iyo inoenderana nemuvara wavo webhuruu wakajeka (Fig. 1b) 48.49.Dzimwe nzvimbo dzakakwirira dzinenge 20.5 °, 27.1 °, 28.1 °, 30.8 °, 35.7 °, 36.7 ° uye 52.7 ° dzakapiwa (140), (620), (350), (720), (740), (560 °).)) uye (970) diffraction ndege orthogonal kuWO2.63, zvichiteerana.Nzira imwechete yekugadzira yakashandiswa naSongara et al.43 kuwana chigadzirwa chichena, icho chainzi chakakonzerwa nekuvapo kweWO3(H2O)0.333.Zvisinei, mubasa iri, nekuda kwemamiriro akasiyana-siyana, chigadzirwa chebhuruu-grey chakawanikwa, zvichiratidza kuti WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90 °) uye fomu yakaderedzwa ye oxide.Semiquantitative kuongorora uchishandisa X'Pert HighScore software yakaratidza 26% WO3(H2O)0.333:74% W32O84.Sezvo W32O84 iine W6+ neW4+ (1.67:1 W6+:W4+), iyo inofungidzirwa yemukati yeW6+ neW4+ ingangoita 72% W6+ uye 28% W4+, zvichiteerana.SEM mifananidzo, 1-second XPS spectra padanho renucleus, TEM mifananidzo, FTIR spectra, uye Raman spectra yeC76 zvimedu zvakaratidzwa mune yedu yapfuura chinyorwa.Maererano naKawada et al.,50,51 X-ray diffraction yeC76 mushure mekubviswa kwe toluene yakaratidza monoclinic chimiro cheFCC.
SEM mifananidzo mune fig.2a uye b inoratidza kuti HWO neHWO-50% C76 zvakabudirira kuiswa uye pakati pekabhoni fibers yeUCC electrode.EDX element mepu dze tungsten, kabhoni, uye okisijeni paSEM mifananidzo mufig.2c inoratidzwa mufig.2d-f ichiratidza kuti tungsten nekabhoni zvakasanganiswa zvakaenzana (zvichiratidza kugoverwa kwakafanana) pamusoro pese electrode surface uye iyo composite haina kufanana yaiswa nekuda kwechimiro cheiyo deposition nzira.
SEM mifananidzo yeakaiswa HWO zvidimbu (a) uye HWO-C76 zvidimbu (b).EDX mepu paHWO-C76 yakatakurwa paUCC ichishandisa nzvimbo iri mumufananidzo (c) inoratidza kugoverwa kwetungsten (d), kabhoni (e), uye oxygen (f) mumuenzaniso.
HR-TEM yakashandiswa pakakwirira magnification imaging uye crystallographic ruzivo (Mufananidzo 3).HWO inoratidza nanocube morphology sezvinoratidzwa mumufananidzo 3a uye zvakajeka mumufananidzo 3b.Nokukudza nanocube ye diffraction yenzvimbo dzakasarudzwa, munhu anogona kuona chimiro chegrating uye diffraction ndege dzinogutsa mutemo weBragg, sezvinoratidzwa muFig. 3c, iyo inosimbisa crystallinity yezvinhu.Muchikamu cheMufananidzo 3c inoratidza chinhambwe d 3.3 Å chinoenderana ne (022) uye (620) ndege dze diffraction dzinowanikwa muzvikamu zveWO3(H2O)0.333 uye W32O84, zvakateerana43,44,49.Izvi zvinopindirana nekuongorora kwe XRD kunotsanangurwa pamusoro apa (Fig. 1b) sezvo iyo yakacherechedza grating ndege kureba d (Fig. 3c) inopindirana nepamusoro pepamusoro peXRD mumuenzaniso weHWO.Zvindori zvemuenzaniso zvinoratidzwawo mufig.3d, apo mhete imwe neimwe inoenderana nendege yakasiyana.Iyo WO3 (H2O) 0.333 uye W32O84 ndege dzine mavara machena uye bhuruu, zvichiteerana, uye iwo anowirirana XRD peaks anoratidzwawo muFig. 1b.Mhete yekutanga inoratidzwa mudhayagiramu yemhete inoenderana neyokutanga yakanyorwa peak mu x-ray pateni ye (022) kana (620) plane diffraction.Kubva pa (022) kusvika ku (402) zvindori, iyo d-spacing kukosha ndeye 3.30, 3.17, 2.38, 1.93, uye 1.69 Å, zvinoenderana neXRD kukosha kwe3.30, 3.17, 2, 45, 1.93.uye 1.66 Å, iyo inoenzana ne44, 45, zvichiteerana.
(a) HR-TEM mufananidzo weHWO, (b) inoratidza mufananidzo wakakurisa.Mifananidzo ye grating ndege inoratidzwa mu (c), inset (c) inoratidza mufananidzo wakakura wendege uye pitch d ye0.33 nm inoenderana ne (002) uye (620) ndege.(d) HWO ring pattern inoratidza ndege dzakabatana neWO3 (H2O) 0.333 (white) uye W32O84 (blue).
XPS ongororo yakaitwa kuona iyo yepamusoro chemistry uye oxidation mamiriro e tungsten (Figure S1 uye 4).Iyo yakakura yeXPS scan spectrum yeHWO yakagadzirwa inoratidzwa muMufananidzo S1, ichiratidza kuvepo kwe tungsten.Iyo XPS yakamanikana-scan spectra yeW 4f uye O 1s misimboti mazinga anoratidzwa muFig.4a uye b, zvichiteerana.Iyo W 4f spectrum inotsemuka kuita maviri spin-orbit kaviri anoenderana neanosunga masimba eW oxidation state.uye W 4f7/2 pa 36.6 uye 34.9 eV hunhu hweW4+ state ye40, zvichiteerana.)0.333.Iyo data yakaiswa inoratidza kuti maatomu muzana eW6+ neW4+ ari 85% uye 15%, zvichiteerana, ari padyo nehunhu hunoyerwa kubva kuXRD data tichifunga mutsauko uripo pakati penzira mbiri idzi.Nzira mbiri idzi dzinopa ruzivo rwehuwandu nekudzika kwakadzika, kunyanya XRD.Zvakare, idzi nzira mbiri dzinoongorora zvikamu zvakasiyana zvechinyorwa nekuti XRD inzira yakawanda nepo XPS iri nzira yepasi inongosvika mashoma nanometers.Iyo O 1s spectrum yakakamurwa kuita mbiri yepamusoro pa533 (22.2%) uye 530.4 eV (77.8%).Yekutanga inoenderana neOH, uye yechipiri kune oxygen zvisungo mulatisi muWO.Kuvapo kweOH mashandiro emapoka anowirirana neiyo hydration properties yeHWO.
Ongororo yeFTIR yakaitwawo pane aya masampuli maviri kuongorora kuvepo kwemapoka anoshanda uye kurongedza mamorekuru emvura mune hydrated HWO chimiro.Zvigumisiro zvinoratidza kuti HWO-50% C76 sampuli uye FT-IR HWO zvigumisiro zvinoratidzika zvakafanana nekuda kwekuvapo kweHWO, asi kusimba kwepamusoro-soro kwakasiyana nekuda kwehuwandu hwakasiyana hwemuenzaniso unoshandiswa mukugadzirira kuongororwa (Fig. 5a).) HWO-50% C76 inoratidza kuti mapeji ose, kunze kwepamusoro pe tungsten oxide, ane chokuita ne fullerene 24. Yakadzama mufig.5a inoratidza kuti sampuli dzese dziri mbiri dzinoratidza bhendi rakasimba kwazvo pa ~ 710/cm inoratidzwa neOWO inotambanudza oscillations muHWO lattice chimiro, ine pfudzi rakasimba pa ~ 840/cm inonzi WO.Pakutambanudza mavibrations, bhendi rakapinza rinenge 1610/cm inonzi inokonzerwa nekupeta mavhitaminzi eOH, ukuwo bhendi rakafara rekunyudza ringangoita 3400/cm richinzi rinotwasanudza kudengenyeka kweOH mumapoka ehydroxyl43.Mhedzisiro iyi inoenderana neiyo XPS spectra muFig.4b, uko mapoka eWO anoshanda anogona kupa nzvimbo dzinoshanda dzeVO2+/VO2+ reaction.
FTIR ongororo yeHWO neHWO-50% C76 (a), yakaratidza mapoka anoshanda uye zviyero zvekusangana nemakona (b, c).
Boka reOH rinogonawo kukonzeresa iyo VO2+/VO2+ reaction, uku ichiwedzera hydrophilicity ye electrode, nekudaro ichisimudzira mwero wekupararira uye kuendesa maerekitironi.Sezvinoratidzwa, iyo HWO-50% C76 sampuli inoratidza imwe peak yeC76.Nzvimbo dzepamusoro pa ~ 2905, 2375, 1705, 1607, uye 1445 cm3 dzinogona kupihwa kune CH, O=C=O, C=O, C=C, uye CO inotambanudzira vibrations, zvichiteerana.Zvinonyatsozivikanwa kuti mapoka eokisijeni anoshanda C=O uye CO anogona kushanda senzvimbo dzinoshanda dzekuita redox kwevanadium.Kuti uedze uye uenzanise kunyorova kwema electrode maviri, zviyero zvemakona zvakatorwa sezvakaratidzwa muFig. 5b, c.Iyo HWO electrode yakabva yatora madonhwe emvura, zvichiratidza superhydrophilicity nekuda kweiyo iripo OH inoshanda mapoka.HWO-50% C76 inowedzera hydrophobic, ine kona yekubata inosvika 135 ° mushure memasekondi gumi.Nekudaro, mukuyera kwe electrochemical, iyo HWO-50% C76 electrode yakanyorovesa zvachose mukati isingasviki miniti.Izvo zviyero zvekunyorova zvinowirirana neXPS neFTIR zvabuda, zvichiratidza kuti mamwe mapoka eOH ari paHWO pamusoro anoita kuti ive yakawanda hydrophilic.
Iyo VO2+/VO2+ maitiro eHWO neHWO-C76 nanocomposites akaedzwa uye zvaitarisirwa kuti HWO yaizodzvanya chlorine shanduko muVO2+/VO2+ reaction musanganiswa asidhi, uye C76 yaizowedzera kukonzeresa yaidiwa VO2+/VO2+ redox reaction.%, 30%, uye 50% C76 muHWO suspensions uye CCC yakaiswa pamagetsi ane yakazara kurodha inosvika 2 mg/cm2.
Sezvinoratidzwa mufig.6, iyo kinetics yeVO2 +/VO2+ reaction pa electrode surface yakaongororwa neCV mune yakasanganiswa acidic electrolyte.Ikozvino inoratidzwa seI / Ipa kuitira nyore kuenzanisa ΔEp uye Ipa / Ipc yezvigadzirisheni zvakasiyana zvakananga pagirafu.Iyo yazvino nzvimbo unit data inoratidzwa muMufananidzo 2S.Pamusoro pemuonde.Mufananidzo 6a unoratidza kuti HWO inowedzera zvishoma muyero wekuchinjisa maerekitironi eVO2+/VO2+ redox reaction panzvimbo ye electrode uye inodzvanyirira kuita kweparasitic chlorine evolution.Nekudaro, C76 inowedzera zvakanyanya mwero wekufambisa erekitironi uye inokonzeresa kushanduka kweklorini.Naizvozvo, musanganiswa wakanyatsogadzirwa weHWO neC76 unotarisirwa kuve neakanakisa chiitiko uye kugona kukuru kuvharidzira kushanduka kweklorini.Yakawanikwa kuti mushure mekuwedzera zvinyorwa zveC76, basa re electrochemical re electrode rakavandudzwa, sezvinoratidzwa nekuderera kwe ΔEp uye kuwedzera kweIpa / Ipc ratio (Table S3).Izvi zvakasimbiswawo neRCT tsika dzakatorwa kubva kuNyquist plot muFig. 6d (Table S3), iyo yakawanikwa ichiderera nekuwedzera C76 content.Mhedzisiro iyi zvakare inopindirana nekudzidza kwaLi, umo kuwedzerwa kwemesoporous kabhoni kune mesoporous WO3 kwakaratidza yakagadziridzwa yekuchaja kinetics paVO2+/VO2+35.Izvi zvinoratidza kuti kugadzirisa kwakananga kunogona kuvimba zvakanyanya pane electrode conductivity (C = C bond) 18, 24, 35, 36, 37. Izvi zvinogonawo kuva nekuda kwekuchinja kwekubatanidza geometry pakati pe [VO (H2O) 5] 2 + uye [VO2 (H2O) 4] +, C76 inoderedza maitiro ekugadzirisa simba nekuderedza simba remagetsi.Zvisinei, izvi zvingave zvisingagoneki neHWO electrodes.
(a) Cyclic voltammetric behaviour (ν = 5 mV/s) yeVO2+/VO2+ reaction yeUCC neHWO-C76 macomposites ane HWO:C76 ratios dzakasiyana mu0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik uye (c) Nicholson VO2+/VO2+ nzira yekuongorora kupararira kwekushanda uye kuwana k0 (d) maitiro.
Haisi chete HWO-50% C76 ichiratidza zvinenge zvakafanana electrocatalytic basa seC76 yeVO2 +/VO2+ reaction, asi, zvinonyanya kufadza, yakawedzera kudzvinyirira chlorine evolution kana ichienzaniswa neC76, sezvakaratidzwa muFig. 6a, uye inoratidzawo Diki Semicircle mumuonde.6d (pasi RCT).C76 yakaratidza yakakwira inooneka Ipa/Ipc kupfuura HWO-50% C76 (Table S3), kwete nekuda kwekuvandudzwa kwekuita reversibility, asi nekuda kwepamusoro-soro kupindirana kwekuderedza chlorine reaction neSHE pa1.2 V. The best performance yeHWO- The 50% C76 inonzi inokonzerwa ne synergistic charge6 uye high-conductive cargebility yeC-H-OH yepamusoro-soro ye-C76 ye-synergistic ne-high-conductivity ye-high-o-H ity paHWO.Kuderera kushoma kweklorini kunovandudza kuchaja kwesero yakazara, nepo kinetics yakagadziridzwa ichivandudza kushanda kweiyo yakazara cell voltage.
Zvinoenderana ne equation S1, kune quasi-reversible (inononoka kufambisa erekitironi) maitiro anodzorwa nekupararira, peak current (IP) inoenderana nehuwandu hwemaerekitironi (n), electrode area (A), diffusion coefficient (D), nhamba yemaelectrons kutamisa coefficient (α) uye scanning speed (ν).Kuti udzidze kupararira-kudzorwa maitiro ezvakaedzwa zvinhu, hukama pakati pe IP ne ν1/2 hwakarongwa uye hwakaratidzwa muFig. 6b.Sezvo zvese zvishandiso zvichiratidza hukama hwemutsara, maitiro anodzorwa nekupararira.Sezvo iyo VO2 +/VO2+ reaction iri quasi-reversible, kutsetseka kwemutsara kunoenderana neiyo diffusion coefficient uye kukosha kwe α (equation S1).Sezvo iyo diffusion coefficient inogara iripo (≈ 4 × 10-6 cm2 / s) 52, mutsauko mukutsetseka kwemutsara unoratidza zvakananga kukosha kwakasiyana kwe α, uye nekudaro mwero wekuchinjisa maerekitironi panzvimbo ye electrode, inoratidzwa kuC76 neHWO -50% C76 Steepest slope (yepamusoro-soro yekufambisa).
Materu eWarburg (W) akaverengerwa kutsika kwakadzikira kunoratidzwa muTable S3 (Fig. 6d) ine kukosha pedyo ne1 kune zvese zvigadzirwa, zvichiratidza kupararira kwakakwana kwemhando dzeredox uye kusimbisa mutsara maitiro eIP zvichienzaniswa ne ν1/ 2. CV inoyerwa.Nokuda kweHWO-50% C76, mutsetse weWarburg unotsauka kubva pa1 kusvika ku1.32, zvichiratidza kwete chete kupararira kusingagumi kweiyo reagent (VO2+), asiwo mupiro unobvira wehutete-layer maitiro ekupararira maitiro nekuda kwe electrode porosity.
Kuenderera mberi nekuongorora kudzoreredzwa (electron transfer rate) yeVO2+/VO2+ redox reaction, Nicholson quasi-reversible reaction method yakashandiswawo kuona mwero wakajairwa unogara k041.42.Izvi zvinoitwa pachishandiswa S2 equation kugadzira dimensionless kinetic parameter Ψ, inova basa reΔEp, sebasa re ν-1/2.Tafura S4 inoratidza iyo Ψ kukosha inowanikwa kune yega yega electrode zvinhu.Zvigumisiro (Fig. 6c) zvakarongwa kuti zviwane k0 × 104 cm / s kubva pamatope ega ega pachishandiswa Equation S3 (yakanyorwa pedyo nemutsara wega wega uye inowanikwa muTable S4).HWO-50% C76 yakawanikwa iine slope yakakwirira (Fig. 6c), saka kukosha kwek0 ndeye 2.47 × 10-4 cm / s.Izvi zvinoreva kuti electrode iyi inobudirira kinetics inokurumidza, iyo inopindirana neCV uye EIS inoguma muFig. 6a uye d uye muTable S3.Mukuwedzera, kukosha kwek0 kwakawanikwawo kubva kuNyquist plot (Fig. 6d) yeEquation S4 uchishandisa RCT value (Table S3).Iyi k0 mhedzisiro kubva kuEIS inopfupikiswa muTebhura S4 uye zvakare inoratidza kuti HWO-50% C76 inoratidza yakakwira maerekitironi kutamisa mwero nekuda kweiyo synergistic mhedzisiro.Kunyangwe iyo k0 kukosha kwakasiyana nekuda kwekwakasiyana kwakabva nzira yega yega, ivo vachiri kuratidza kurongeka kwakafanana kwehukuru uye kuratidza kuenderana.
Kuti unzwisise zvizere kinetics yakanakisa yakawanikwa, zvakakosha kuenzanisa iyo yakakwana electrode zvinhu neUCC isina kuvharwa uye TCC electrodes.Nokuda kweVO2 +/VO2 + reaction, HWO-C76 haina kungoratidza yakaderera ΔEp uye nani reversibility, asiwo zvakanyanya kudzvinyirira parasitic chlorine evolution reaction kana ichienzaniswa neTCC, sezvinoyerwa nezvino pa 1.45 V maererano neSHE (Fig. 7a).Mukutaura kwekugadzikana, takafunga kuti HWO-50% C76 yakanga yakagadzikana mumuviri nokuti iyo catalyst yakasanganiswa nePVDF binder ndokubva yashandiswa kune carbon cloth electrodes.HWO-50% C76 yakaratidza kushanduka kwepamusoro kwe44 mV (kuderedza chiyero 0.29 mV / cycle) mushure me150 mitsetse yakaenzaniswa ne50 mV yeUCC (Mufananidzo 7b).Izvi zvinogona kunge zvisiri mutsauko mukuru, asi kinetics yeUCC electrode inononoka uye inoshatisa nekuchovha bhasikoro, kunyanya kune reverse reactions.Kunyangwe kudzoreredzwa kweTCC kuri nani kupfuura kweUCC, TCC yakawanikwa iine shanduko huru ye 73 mV mushure memazana zana nemakumi mashanu, izvo zvingave zvichikonzerwa nehuwandu hweklorini yakaumbwa pamusoro payo.kuitira kuti iyo catalyst inonamatira zvakanaka kune electrode pamusoro.Sezvingaonekwa kubva kune ese maelectrode akaedzwa, kunyange maelectrodes asina anotsigirwa anokonzeresa airatidza madhigirii akasiyana ekusagadzikana kwebhasikoro, zvichiratidza kuti shanduko yekuparadzana kwepamusoro panguva yebhasikoro imhaka yekudzima zvinhu zvakakonzerwa nekuchinja kwemakemikari pane kukonzeresa kupatsanurwa.Mukuwedzera, kana huwandu hukuru hwezvimedu zvinogadzirisa zvaifanira kuparadzaniswa kubva kune electrode pamusoro, izvi zvingaguma nekuwedzera kukuru kwekuparadzana kwepamusoro (kwete chete 44 mV), sezvo substrate (UCC) isingashandisi kune VO2 +/VO2 + redox reaction.
Kuenzanisa kweCV yezvakanakisa electrode zvinhu zvichienzaniswa neUCC (a) uye kugadzikana kweVO2 +/VO2+ redox reaction (b).ν = 5 mV/s pamaCV ese mu0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Kuti uwedzere kukwezva kwehupfumi kweVRFB tekinoroji, kuwedzera uye kunzwisisa kinetics yevanadium redox maitiro kwakakosha kuti uwane yakakwira simba.Composites HWO-C76 yakagadzirirwa uye yavo electrocatalytic mhedzisiro paVO2+/VO2+ reaction yakadzidzwa.HWO yakaratidza kuwedzeredza kinetic mune yakasanganiswa acidic electrolytes asi zvakanyanya kudzvanyirira chlorine shanduko.Mareshiyo akasiyana eHWO: C76 akashandiswa kuenderera mberi nekunatsiridza kinetics yeHWO-based electrodes.Kuwedzera C76 kuHWO kunonatsiridza maelectron transfer kinetics eVO2+/VO2+ reaction on the modified electrode, which HWO-50% C76 is the best material because inoderedza charge transfer resistance uye inowedzera kudzvanya chlorine zvichienzaniswa neC76 uye TCC deposit..Izvi zvinokonzerwa nekubatana pakati peC=C sp2 hybridization, OH neW-OH inoshanda mapoka.Chiyero chekuora mushure mekudzokororwa kwebhasikoro kweHWO-50% C76 yakawanikwa iine 0.29 mV / cycle, asi chiyero chekuora kweUCC neTCC chiri 0.33 mV / cycle uye 0.49 mV / cycle, zvichienderana, zvichiita kuti igare yakasimba.mune yakasanganiswa asidhi electrolytes.Mhedzisiro yakaratidzwa inobudirira kuona yakakwirira performance electrode zvinhu zveVO2+/VO2+ reaction ine fast kinetics uye yakanyanya kugadzikana.Izvi zvichawedzera simba rekubuda, nekudaro kuwedzera simba reVRFB, nekudaro kuderedza mutengo wekutengesa kwayo kweramangwana.
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