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Ingantacciyar tsadar duk-vanadium kwarara-ta hanyar batir redox (VRFBs) yana iyakance amfaninsu da yawa.Ana buƙatar haɓaka motsin halayen halayen lantarki don haɓaka takamaiman ƙarfi da ƙarfin kuzari na VRFB, don haka rage farashin kWh na VRFB.A cikin wannan aikin, hydrothermally hada hydrated tungsten oxide (HWO) nanoparticles, C76 da C76 / HWO, an ajiye su a kan carbon zane electrodes da kuma gwada a matsayin electrocatalysts ga VO2 +/VO2+ redox dauki.Filayen watsi da sikanin microscopy (FESEM), makamashi mai watsawa X-ray spectroscopy (EDX), high-resolution trans electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier transform Spectroscopy (FTIR) da ma'aunin kusurwa.An gano cewa ƙari na C76 fullerenes zuwa HWO na iya inganta motsin wutar lantarki ta hanyar haɓaka ƙarfin lantarki da kuma samar da ƙungiyoyi masu aiki na oxidized a samansa, don haka inganta VO2 +/VO2 + redox dauki.Haɗin HWO / C76 (50 wt% C76) ya zama mafi kyawun zaɓi don amsawar VO2 +/VO2+ tare da ΔEp na 176 mV, yayin da zanen carbon da ba a kula da shi ba (UCC) shine 365 mV.Bugu da ƙari, haɗin HWO / C76 ya nuna wani tasiri mai mahimmanci na hanawa akan yanayin juyin halittar chlorine na parasitic saboda ƙungiyar aikin W-OH.
Tsananin ayyukan ɗan adam da saurin juyin juya halin masana'antu sun haifar da buƙatun wutar lantarki da ba za a iya tsayawa ba, wanda ke ƙaruwa da kusan kashi 3% a kowace shekara1.Shekaru da dama da suka wuce, yadda ake yawan amfani da albarkatun mai a matsayin tushen samar da makamashi ya haifar da fitar da hayaki mai gurbata muhalli da ke taimakawa wajen dumamar yanayi, ruwa da gurbacewar iska, lamarin da ke barazana ga dukkan halittu.A sakamakon haka, ana sa ran shigar da iska mai tsafta da sabuntawa da makamashin hasken rana zai kai kashi 75% na jimlar wutar lantarki nan da shekara ta 20501. Duk da haka, idan rabon wutar lantarki daga hanyoyin da ake sabuntawa ya zarce kashi 20 cikin 100 na yawan samar da wutar lantarki, grid ɗin ya zama mara ƙarfi.
Daga cikin dukkan tsarin ajiyar makamashi irin su matasan vanadium redox flow baturi2, duk-vanadium redox flow baturi (VRFB) ya ɓullo da mafi sauri saboda da yawa abũbuwan amfãni kuma an dauke shi mafi kyau bayani ga dogon lokaci makamashi ajiya (kimanin shekaru 30).) Zaɓuɓɓuka a hade tare da makamashi mai sabuntawa4.Wannan ya faru ne saboda rarrabuwar ƙarfi da ƙarfin kuzari, amsa mai sauri, tsawon rayuwar sabis, da ƙarancin ƙarancin shekara na $ 65 / kWh idan aka kwatanta da $ 93-140 / kWh don batirin Li-ion da gubar-acid da 279-420 dalar Amurka a kowace kWh.baturi bi da bi 4.
Koyaya, manyan kasuwancin su har yanzu ana takurawa ta hanyar ƙimar babban tsarin tsarin su, galibi saboda tarin tantanin halitta4,5.Don haka, haɓaka aikin tari ta hanyar haɓaka motsin halayen halayen rabin kashi biyu na iya rage girman tari don haka rage farashi.Saboda haka, saurin canja wurin lantarki zuwa saman lantarki ya zama dole, wanda ya dogara da ƙira, abun da ke ciki da tsarin lantarki kuma yana buƙatar haɓakawa a hankali6.Duk da ingantaccen sinadarai da kwanciyar hankali na electrochemical da kyakyawan halayen lantarki na lantarki na carbon, motsin motsin da ba a kula da su ba su da ƙarfi saboda rashin ƙungiyoyin aikin oxygen da hydrophilicity7,8.Sabili da haka, ana haɗa nau'ikan electrocatalysts daban-daban tare da na'urori masu amfani da carbon, musamman ma carbon nanostructures da karfe oxides, don inganta motsin motsin na'urorin lantarki guda biyu, ta haka ne ya kara yawan motsin lantarki na VRFB.
Baya ga aikinmu na baya akan C76, mun fara bayar da rahoton kyakkyawan aikin electrocatalytic na wannan fullerene don VO2 +/VO2 +, canja wurin caji, idan aka kwatanta da zafin zafi da zanen carbon da ba a kula da shi ba.An rage juriya da 99.5% da 97%.Ayyukan kayan aikin carbon don amsawar VO2+/VO2+ idan aka kwatanta da C76 ana nuna su a cikin Tebur S1.A gefe guda, yawancin oxides na ƙarfe irin su CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 da WO331, 32, 33, 34, 35, 36, 37 an yi amfani da su saboda ƙara yawan wettability da yawan aikin oxygen., 38. rukuni.Ayyukan catalytic na waɗannan ƙarfe oxides a cikin amsawar VO2+/VO2+ an gabatar da su a cikin Tebur S2.An yi amfani da WO3 a cikin adadi mai yawa na ayyuka saboda ƙananan farashi, babban kwanciyar hankali a cikin kafofin watsa labaru na acidic, da kuma babban aiki na catalytic31,32,33,34,35,36,37,38.Duk da haka, haɓakawa a cikin kinetics na cathodic saboda WO3 ba shi da mahimmanci.Don inganta haɓakar WO3, an gwada tasirin amfani da raguwar tungsten oxide (W18O49) akan ayyukan cathodic38.Hydrated tungsten oxide (HWO) ba a taɓa gwadawa a aikace-aikacen VRFB ba, kodayake yana nuna ƙarin aiki a cikin aikace-aikacen supercapacitor saboda saurin rarrabawar cation idan aka kwatanta da anhydrous WOx39,40.Ƙarni na uku na vanadium redox flow baturi yana amfani da gauraye acid electrolyte wanda ya ƙunshi HCl da H2SO4 don inganta aikin baturi da kuma inganta solubility da kwanciyar hankali na vanadium ions a cikin electrolyte.Koyaya, yanayin juyin halittar chlorine parasitic ya zama ɗaya daga cikin rashin lahani na ƙarni na uku, don haka nemo hanyoyin da za a hana martanin ƙimar chlorine ya zama abin da ƙungiyoyin bincike da yawa suka mayar da hankali kan.
Anan, an gudanar da gwaje-gwajen amsawa na VO2 +/VO2+ akan abubuwan haɗin HWO/C76 da aka ajiye akan na'urorin kyalle na carbon don nemo ma'auni tsakanin ƙarfin lantarki na abubuwan da aka haɗa da redox kinetics na farfajiyar lantarki yayin danne juyin halittar chlorine na parasitic.amsa (CER).Nanoparticles tungsten oxide (HWO) an haɗa su ta hanyar hanyar hydrothermal mai sauƙi.An gudanar da gwaje-gwaje a cikin mahaɗaɗɗen acid electrolyte (H2SO4/HCl) don daidaitawa na ƙarni na uku VRFB (G3) don aiki da kuma bincika tasirin HWO akan halayen chlorine na 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 Tungsten oxide 92% hydroxide, hydrochloric acid, sodium Tungsten 92 oxide, hydrochloric acid. An yi amfani da zane ELAT (Shagon Fuel) a cikin wannan binciken.
Hydrated tungsten oxide (HWO) da aka shirya ta hanyar hydrothermal dauki 43 a cikin abin da 2 g na Na2WO4 gishiri da aka narkar da a cikin 12 ml na H2O don ba da wani launi maras launi, sa'an nan 12 ml na 2 M HCl aka kara dropwise don ba da kodadde rawaya dakatar.An sanya slurry a cikin Teflon mai rufi na bakin karfe autoclave kuma an ajiye shi a cikin tanda a 180 ° C. na 3 hours don maganin hydrothermal.An tattara ragowar ta hanyar tacewa, an wanke sau 3 tare da ethanol da ruwa, an bushe a cikin tanda a 70 ° C na ~ 3 hours, sa'an nan kuma an yanke shi don ba da foda mai launin shuɗi-launin toka HWO.
An yi amfani da abubuwan da aka samu (wanda ba a kula da su ba) kamar yadda ake yi ko zafi a cikin tanderun bututu a 450 ° C a cikin iska tare da ƙimar dumama na 15 ºC / min na sa'o'i 10 don samun CCs (TCC).kamar yadda aka bayyana a labarin da ya gabata24.An yanke UCC da TCC cikin na'urorin lantarki kamar 1.5 cm faɗi da 7 cm tsayi.Dakatar da C76, HWO, HWO-10% C76, HWO-30% C76 da HWO-50% C76 aka shirya ta ƙara 20 MG .% (~ 2.22 MG) na PVDF daure zuwa ~ 1 ml DMF da sonicated for 1 hour don inganta uniformity.2 MG na C76, HWO da HWO-C76 composites an yi amfani da su akai-akai zuwa wani yanki mai aiki na UCC na kusan 1.5 cm2.An ɗora duk abubuwan haɓakawa akan wayoyin UCC kuma an yi amfani da TCC don dalilai na kwatanta kawai, kamar yadda aikinmu na baya ya nuna cewa ba a buƙatar maganin zafi24.An sami daidaitawar ra'ayi ta hanyar goge 100 µl na dakatarwa (load 2 mg) don ƙarin tasiri.Sa'an nan kuma an bushe dukkan na'urorin lantarki a cikin tanda a 60 ° C. na dare.Ana auna na'urorin lantarki gaba da baya don tabbatar da ingantacciyar lodin haja.Domin samun wani yanki na geometric (~ 1.5 cm2) da kuma hana hawan vanadium electrolyte zuwa electrode saboda tasirin capillary, an yi amfani da wani bakin ciki na paraffin akan kayan aiki.
An yi amfani da microscopy na sikanin filaye na lantarki (FESEM, Zeiss SEM Ultra 60, 5 kV) don lura da yanayin yanayin HWO.An yi amfani da na'urar watsawa ta X-ray na makamashi sanye take da Feii8SEM (EDX, Zeiss Inc.) don taswirar abubuwan HWO-50%C76 akan wayoyin UCC.A high ƙuduri watsa lantarki microscope (HR-TEM, JOEL JEM-2100) aiki a wani hanzari irin ƙarfin lantarki na 200 kV aka yi amfani da image mafi girma ƙuduri HWO barbashi da diffraction zobe.Akwatin kayan aiki na Crystallography (CrysTBox) software yana amfani da aikin ringGUI don nazarin ƙirar zobe na HWO da kwatanta sakamakon tare da ƙirar XRD.An bincikar tsarin da graphitization na UCC da TCC ta hanyar X-ray diffraction (XRD) a ƙimar sikanin 2.4 ° / min daga 5 ° zuwa 70 ° tare da Cu Kα (λ = 1.54060 Å) ta amfani da diffractometer X-ray Panalytical (Model 3600).XRD ya nuna tsarin crystal da lokaci na HWO.An yi amfani da software na PANalytical X'Pert HighScore don dacewa da kololuwar HWO zuwa taswirar tungsten oxide da ke cikin bayanan45.An kwatanta sakamakon HWO da sakamakon TEM.Halin sinadarai da yanayin samfuran HWO an ƙaddara su ta hanyar X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).An yi amfani da software na CASA-XPS (v 2.3.15) don ƙaddamar da kololuwar juzu'i da nazarin bayanai.Don ƙayyade ƙungiyoyi masu aiki na saman HWO da HWO-50% C76, an yi ma'auni ta amfani da Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, ta amfani da KBr FTIR).An kwatanta sakamakon da sakamakon XPS.Hakanan an yi amfani da ma'aunin kusurwa na lamba (KRUSS DSA25) don siffata jigon na'urorin lantarki.
Don duk ma'auni na lantarki, an yi amfani da aikin Biologic SP 300.Cyclic voltammetry (CV) da electrochemical impedance spectroscopy (EIS) da aka yi amfani da su yi nazarin electrode kinetics na VO2 +/VO2+ redox dauki da kuma tasirin reagent diffusion (VOSO4 (VO2+)) a kan dauki rate.Dukansu hanyoyin sun yi amfani da tantanin halitta uku-electrode tare da ƙwayar electrolyte na 0.1 M VOSO4 (V4+) a cikin 1 M H2SO4 + 1 M HCl (cakuda na acid).Duk bayanan electrochemical da aka gabatar an gyara IR.An yi amfani da na'urar lantarki mai cikakken calomel (SCE) da naɗaɗɗen platinum (Pt) azaman abin tunani da na'urar lantarki, bi da bi.Don CV, an yi amfani da ƙimar sikelin (ν) na 5, 20, da 50 mV / s zuwa VO2 +/VO2 + yuwuwar taga don (0-1) V vs. SCE, sannan aka daidaita don SHE don yin makirci (VSCE = 0.242 V vs. HSE) .Don nazarin riƙe ayyukan lantarki, an yi maimaita CVs na cyclic a ν 5 mV / s don UCC, TCC, UCC-C76, UCC-HWO, da UCC-HWO-50% C76.Don ma'aunin EIS, kewayon mitar VO2+/VO2+ redox dauki shine 0.01-105 Hz, kuma ruɗin wutar lantarki a buɗaɗɗen wutar lantarki (OCV) shine 10 mV.Kowane gwaji an maimaita sau 2-3 don tabbatar da daidaiton sakamakon.An samo madaidaitan ƙimar ƙima (k0) ta hanyar Nicholson46,47.
Hydrated tungsten oxide (HVO) an samu nasarar haɗa shi ta hanyar hanyar hydrothermal.Hoton SEM a cikin fig.1a yana nuna cewa HWO da aka ajiye ya ƙunshi gungu na nanoparticles tare da girma a cikin kewayon 25-50 nm.
Tsarin rarrabuwar X-ray na HWO yana nuna kololuwa (001) da (002) a ~ 23.5 ° da ~ 47.5 °, bi da bi, waɗanda ke da halayen nonstoichiometric WO2.63 (W32O84) (PDF 077-0810, a = 21.4 Å, Å . 8 = 8 β = 777-0810, a = 21.4 Å, b3γ 7, b, 8 = 8 β, 8 β = 7.4 Å. = 90 °), wanda ya dace da launin shudi mai haske (Fig. 1b) 48.49.Sauran kololuwa a kusan 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° da 52.7° an sanya su zuwa (140), (620), (350), (720), (740), (560°).) da (970) diffraction jiragen sama orthogonal zuwa WO2.63, bi da bi.An yi amfani da wannan hanyar haɗin gwiwa ta Songara et al.43 don samun samfurin fari, wanda aka danganta da kasancewar WO3 (H2O) 0.333.Duk da haka, a cikin wannan aikin, saboda yanayi daban-daban, an samo samfurin launin shuɗi-launin toka, yana nuna cewa WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90 ° na oxide) da kuma rage β oxide form.Ƙididdigar ƙididdiga ta amfani da software na X'Pert HighScore ya nuna 26% WO3 (H2O) 0.333: 74% W32O84.Tun da W32O84 ya ƙunshi W6+ da W4+ (1.67:1 W6+: W4+), kiyasin abun ciki na W6+ da W4+ kusan 72% W6+ da 28% W4+, bi da bi.Hotunan SEM, 1-second XPS spectra a matakin tsakiya, hotunan TEM, FTIR spectra, da Raman spectra na barbashi C76 an gabatar dasu a cikin labarinmu na baya.A cewar Kawada et al., 50,51 X-ray diffraction na C76 bayan cire toluene ya nuna tsarin monoclinic na FCC.
Hotunan SEM a cikin fig.2a da b sun nuna cewa HWO da HWO-50% C76 an sami nasarar ajiyewa akan kuma tsakanin fiber na carbon na UCC electrode.Taswirar abubuwan EDX na tungsten, carbon, da oxygen akan hotunan SEM a cikin fig.2c ana nuna su a cikin fig.2d-f yana nuna cewa tungsten da carbon an haɗa su daidai gwargwado (yana nuna irin wannan rarraba) akan duk sararin lantarki kuma abin da aka haɗa ba a adana shi daidai ba saboda yanayin hanyar sakawa.
Hotunan SEM na ɓangarorin HWO da aka ajiye (a) da barbashi na HWO-C76 (b).Taswirar EDX akan HWO-C76 da aka ɗora akan UCC ta amfani da yanki a cikin hoto (c) yana nuna rarraba tungsten (d), carbon (e), da oxygen (f) a cikin samfurin.
An yi amfani da HR-TEM don ɗaukar hoto mai girma da kuma bayanan crystallographic (Hoto 3).HWO yana nuna ilimin halittar jiki na nanocube kamar yadda aka nuna a cikin Fig. 3a kuma a fili a cikin siffa 3b.Ta hanyar haɓaka nanocube don rarraba wuraren da aka zaɓa, mutum zai iya ganin tsarin grating da jiragen sama masu rarraba wanda ya gamsar da dokar Bragg, kamar yadda aka nuna a cikin Fig. 3c, wanda ke tabbatar da crystallinity na kayan.A cikin shigar da siffa 3c yana nuna nisa d 3.3 Å daidai da (022) da (620) jiragen sama masu rarraba da aka samo a cikin matakan WO3 (H2O) 0.333 da W32O84, bi da bi 43,44,49.Wannan ya yi daidai da binciken XRD da aka kwatanta a sama (Fig. 1b) tun lokacin da aka lura da nisa na jirgin saman grating d (Fig. 3c) ya dace da mafi girma XRD mafi girma a cikin samfurin HWO.Ana kuma nuna zoben samfurin a cikin fig.3d, inda kowane zobe yayi daidai da jirgin sama daban.Jirgin WO3 (H2O) 0.333 da W32O84 suna da launin fari da shuɗi, bi da bi, kuma ana nuna kololuwar su na XRD a hoto na 1b.Zobe na farko da aka nuna a zanen zobe yayi daidai da farkon alamar kololuwa a tsarin x-ray na (022) ko (620) jirgin sama mai karkata.Daga zoben (022) zuwa (402), ƙimar d-spacing sune 3.30, 3.17, 2.38, 1.93, da 1.69 Å, daidai da ƙimar XRD na 3.30, 3.17, 2, 45, 1.93.da 1.66 Å, wanda yake daidai da 44, 45, bi da bi.
(a) Hoton HR-TEM na HWO, (b) yana nuna girman hoto.Ana nuna Hotunan jirage masu ɗorawa a cikin (c), inset (c) yana nuna girman hoton jiragen da filin d na 0.33 nm daidai da (002) da (620) jirage.(d) Tsarin zobe na HWO yana nuna jiragen da ke da alaƙa da WO3 (H2O) 0.333 (farar fata) da W32O84 (blue).
An gudanar da bincike na XPS don sanin yanayin sinadarai da yanayin iskar shaka na tungsten (Figures S1 da 4).Faɗin kewayon XPS scan na HWO da aka haɗa ana nunawa a cikin Hoto S1, yana nuna kasancewar tungsten.Ana nuna sikirin kunkuntar-scan na XPS na matakan W 4f da O 1s a cikin Figs.4a da b, bi da bi.Bakan W 4f ya rabu gida biyu-orbit ninki biyu daidai da kuzarin dauri na yanayin W oxidation.da W 4f7/2 a 36.6 da 34.9 eV sune halayen W4+ na jihar 40, bi da bi.0.333.Bayanai masu dacewa sun nuna cewa adadin atomic na W6+ da W4+ sune 85% da 15%, bi da bi, waɗanda ke kusa da ƙimar da aka ƙiyasta daga bayanan XRD idan aka yi la'akari da bambance-bambancen da ke tsakanin hanyoyin biyu.Duk hanyoyin biyu suna ba da bayanan ƙididdiga tare da ƙarancin daidaito, musamman XRD.Har ila yau, waɗannan hanyoyin guda biyu suna nazarin sassa daban-daban na kayan saboda XRD hanya ce mai girma yayin da XPS hanya ce ta saman da kawai ta kusanci 'yan nanometers.An raba bakan O 1s zuwa kololuwa biyu a 533 (22.2%) da 530.4 eV (77.8%).Na farko yayi daidai da OH, kuma na biyu zuwa haɗin oxygen a cikin lattice a cikin WO.Kasancewar ƙungiyoyin ayyuka na OH daidai da kaddarorin hydration na HWO.
An kuma yi nazarin FTIR akan waɗannan samfurori guda biyu don bincika kasancewar ƙungiyoyi masu aiki da daidaita kwayoyin ruwa a cikin tsarin HWO mai ruwa.Sakamakon ya nuna cewa samfurin HWO-50% C76 da FT-IR HWO sakamakon sun bayyana irin wannan saboda kasancewar HWO, amma tsananin tsayin daka ya bambanta saboda nau'in samfurin da aka yi amfani da shi don shirye-shiryen bincike (Fig. 5a).) HWO-50% C76 ya nuna cewa duk kololuwa, sai dai ga kololuwar tungsten oxide, suna da alaƙa da fullerene 24. Cikakken bayani a cikin fig.5a ya nuna cewa duka samfurori suna nuna wani nau'i mai karfi mai karfi a ~ 710 / cm wanda aka danganta da OWO mai shimfiɗa oscillations a cikin tsarin HWO lattice, tare da kafada mai karfi a ~ 840 / cm da aka danganta ga WO.Don miƙewar girgizar ƙasa, ƙaƙƙarfan band a kusan 1610/cm ana danganta shi da karkatar da girgizar OH, yayin da babban rukunin sha a kusan 3400/cm ana danganta shi da shimfidawar girgizar OH a cikin ƙungiyoyin hydroxyl43.Waɗannan sakamakon sun yi daidai da bakan XPS a cikin Figs.4b, inda ƙungiyoyin ayyuka na WO zasu iya samar da shafuka masu aiki don amsawar VO2 +/VO2+.
Binciken FTIR na HWO da HWO-50% C76 (a), ƙungiyoyi masu aiki da aka nuna da ma'aunin kusurwa (b, c).
Ƙungiyar OH kuma na iya ƙaddamar da amsawar VO2+/VO2+, yayin da ake ƙara yawan ruwa na lantarki, ta yadda za a inganta yawan watsawa da canja wurin lantarki.Kamar yadda aka nuna, samfurin HWO-50% C76 yana nuna ƙarin kololuwa don C76.Za a iya sanya kololuwar a ~ 2905, 2375, 1705, 1607, da 1445 cm3 zuwa CH, O = C = O, C = O, C = C, da CO, bi da bi.An san cewa ƙungiyoyi masu aiki na oxygen C = O da CO na iya zama cibiyoyin aiki don halayen redox na vanadium.Don gwadawa da kwatanta jita-jita na na'urorin lantarki guda biyu, an dauki ma'auni na kusurwa kamar yadda aka nuna a cikin Fig. 5b,c.Wutar lantarki ta HWO nan da nan ta ɗauki ɗigon ruwa, yana nuna superhydrophilicity saboda ƙungiyoyin aikin OH da ke akwai.HWO-50% C76 ya fi hydrophobic, tare da kusurwar lamba na kusan 135 ° bayan 10 seconds.Duk da haka, a cikin ma'auni na electrochemical, lantarki HWO-50% C76 ya zama gaba ɗaya jika a cikin ƙasa da minti daya.Ma'auni na wettability sun yi daidai da sakamakon XPS da FTIR, yana nuna cewa ƙarin ƙungiyoyin OH akan saman HWO sun sa ya fi ƙarfin hydrophilic.
An gwada halayen VO2 +/VO2+ na HWO da HWO-C76 nanocomposites kuma ana sa ran cewa HWO za ta kawar da juyin halitta na chlorine a cikin VO2 +/VO2+ dauki a cikin gauraye acid, kuma C76 zai kara haifar da abin da ake so VO2 +/VO2+ redox dauki.%, 30%, da 50% C76 a cikin dakatarwar HWO da CCC da aka ajiye akan na'urorin lantarki tare da jimlar lodi na kusan 2 mg/cm2.
Kamar yadda aka nuna a cikin fig.6, Kinetics na VO2 +/VO2+ amsawa akan farfajiyar lantarki an bincikar ta CV a cikin gauraye na acidic electrolyte.Ana nuna magudanar ruwa azaman I/Ipa don sauƙin kwatancen ΔEp da Ipa/Ipc don maɓalli daban-daban kai tsaye akan jadawali.Ana nuna bayanan rukunin yanki na yanzu a hoto 2S.A kan fig.Hoto na 6a ya nuna cewa HWO dan kadan yana ƙara yawan canjin lantarki na VO2+/VO2+ redox dauki akan farfajiyar lantarki kuma yana danne martanin juyin halittar chlorine parasitic.Koyaya, C76 yana haɓaka ƙimar canja wurin lantarki da mahimmanci kuma yana haɓaka halayen chlorine.Sabili da haka, ana sa ran haɗin HWO da C76 da aka tsara daidai don samun mafi kyawun aiki da mafi girman ikon hana halayen haɓakar chlorine.An gano cewa bayan haɓaka abun ciki na C76, aikin lantarki na lantarki ya inganta, kamar yadda aka nuna ta hanyar raguwa a cikin ΔEp da karuwa a cikin rabo na Ipa / Ipc (Table S3).Hakanan an tabbatar da wannan ta ƙimar RCT da aka cire daga makircin Nyquist a cikin siffa 6d (Table S3), waɗanda aka samo don ragewa tare da haɓaka abun ciki na C76.Hakanan waɗannan sakamakon sun yi daidai da binciken Li, wanda ƙari na mesoporous carbon zuwa mesoporous WO3 ya nuna ingantaccen motsi na canja wurin caji akan VO2+/VO2+35.Wannan yana nuna cewa amsawar kai tsaye na iya dogara da ƙarin ƙarfin lantarki (C = C bond) 18, 24, 35, 36, 37. Wannan kuma yana iya kasancewa saboda canji a cikin lissafi na daidaitawa tsakanin [VO (H2O) 5] 2+ da [VO2 (H2O) 4] +, C76 yana rage yawan karfin amsawa ta hanyar rage yawan makamashin nama.Duk da haka, wannan bazai yiwu ba tare da lantarki na HWO.
(a) Halin voltammetric na cyclic (ν = 5 mV / s) na VO2 +/ VO2 + amsawar UCC da HWO-C76 tare da HWO daban-daban: rabon C76 a cikin 0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik da (c) Hanyar Nicholson VO2 +/VO2+ don kimanta ingancin watsawa da samun ƙimar k0 (d).
Ba wai kawai HWO-50% C76 yana nuna kusan aikin electrocatalytic iri ɗaya kamar C76 don amsawar VO2 +/VO2+ ba, amma, mafi ban sha'awa, ya kuma kawar da juyin halittar chlorine idan aka kwatanta da C76, kamar yadda aka nuna a cikin siffa 6a, kuma yana nuna ƙaramin Semicircle a cikin fig.6d (ƙananan RCT).C76 ya nuna alamar Ipa / Ipc mafi girma fiye da HWO-50% C76 (Table S3), ba saboda ingantaccen haɓakawa na haɓakawa ba, amma saboda haɓakar haɓakar haɓakar haɓakar chlorine tare da SHE a 1.2 V. Mafi kyawun aikin HWO- 50% C76 an danganta shi da tasirin synergistic a tsakanin babban aiki na C76 da C76 wanda ke haifar da mummunan aiki da rashin ƙarfi da rashin ƙarfi. WO.Karancin fitar da sinadarin chlorine zai inganta ingantaccen caji na cikakken tantanin halitta, yayin da ingantattun motsin motsa jiki zai inganta ingantaccen ƙarfin ƙarfin tantanin halitta.
Dangane da equation S1, don juzu'i mai jujjuyawa (dangantacce jinkirin canja wurin wutar lantarki) amsawar da aka sarrafa ta hanyar watsawa, mafi girman halin yanzu (IP) ya dogara da adadin electrons (n), yanki na lantarki (A), ƙididdigewa mai rarrabawa (D), adadin adadin canja wurin electrons (α) da saurin dubawa (ν).Don yin nazarin halin da ake sarrafawa na watsawa na kayan da aka gwada, an tsara dangantaka tsakanin IP da ν1 / 2 kuma an gabatar da su a cikin siffa 6b.Tun da duk kayan suna nuna alaƙar layi, ana sarrafa amsa ta hanyar watsawa.Tunda amsawar VO2 +/VO2+ ta kasance mai jujjuyawa, gangaren layin ya dogara da ƙimar rarrabawa da ƙimar α (equation S1).Tun da yaduwa coefficient ne m (≈ 4 × 10-6 cm2 / s) 52, da bambanci a cikin gangaren layin kai tsaye nuna daban-daban dabi'u na α, sabili da haka da electron canja wurin kudi a kan lantarki surface, wanda aka nuna ga C76 da HWO -50% C76 Steepest gangara (mafi girman electron canja wurin kudi).
Gandun daji na Warburg (W) da aka lasafta don ƙananan ƙananan da aka nuna a cikin Table S3 (Fig. 6d) suna da dabi'u kusa da 1 don duk kayan, yana nuna cikakkiyar yaduwar nau'in redox da kuma tabbatar da dabi'ar layi na IP idan aka kwatanta da ν1 / 2. An auna CV.Don HWO-50% C76, gangaren Warburg ya karkata daga 1 zuwa 1.32, yana nuna ba kawai yaduwar ƙarancin iyaka na reagent (VO2+), amma kuma yana iya ba da gudummawar halayen bakin ciki-Layer zuwa halayen watsawa saboda porosity na lantarki.
Don ƙarin nazarin juzu'i (ƙididdigar canja wurin lantarki) na VO2+/VO2+ redox dauki, an kuma yi amfani da hanyar amsawar Nicholson quasi-reversible don ƙayyade daidaitaccen ƙimar ƙimar k041.42.Ana yin wannan ta amfani da ma'auni na S2 don gina ma'aunin motsi mara nauyi Ψ, wanda shine aikin ΔEp, azaman aikin ν-1/2.Tebur S4 yana nuna ƙimar Ψ da aka samu don kowane kayan lantarki.An tsara sakamakon (Fig. 6c) don samun k0 × 104 cm / s daga gangaren kowane yanki ta amfani da Equation S3 (an rubuta kusa da kowane jere kuma an gabatar da shi a cikin Table S4).An samo HWO-50% C76 yana da mafi girman gangara (Fig. 6c), don haka matsakaicin darajar k0 shine 2.47 × 10-4 cm / s.Wannan yana nufin cewa wannan na'urar lantarki ta cimma mafi saurin motsi, wanda ya dace da sakamakon CV da EIS a cikin siffa 6a da d kuma a cikin Table S3.Bugu da ƙari, an kuma sami darajar k0 daga ƙirar Nyquist (Fig. 6d) na Equation S4 ta amfani da ƙimar RCT (Table S3).Waɗannan sakamakon k0 daga EIS an taƙaita su a cikin Tebur S4 kuma suna nuna cewa HWO-50% C76 yana nuna mafi girman ƙimar canja wurin lantarki saboda tasirin haɗin gwiwa.Ko da yake k0 dabi'u sun bambanta saboda asali daban-daban na kowace hanya, har yanzu suna nuna tsari iri ɗaya kuma suna nuna daidaito.
Don cikakken fahimtar kyakkyawar motsin motsin da aka samu, yana da mahimmanci a kwatanta mafi kyawun kayan lantarki tare da na'urorin UCC da TCC marasa rufi.Don amsawar VO2 +/VO2 +, HWO-C76 ba wai kawai ya nuna mafi ƙasƙanci ΔEp da mafi kyawun juzu'i ba, amma kuma yana da matukar tasiri ga juyin halittar chlorine na parasitic idan aka kwatanta da TCC, kamar yadda aka auna ta halin yanzu a 1.45 V dangane da SHE (Fig. 7a).Dangane da kwanciyar hankali, mun ɗauka cewa HWO-50% C76 yana da kwanciyar hankali ta jiki saboda an haɗe mai haɓakawa tare da mai ɗaure PVDF sannan kuma a yi amfani da na'urorin kyalle na carbon.HWO-50% C76 ya nuna babban motsi na 44 mV (lalata 0.29 mV / sake zagayowar) bayan hawan 150 idan aka kwatanta da 50 mV don UCC (Hoto 7b).Wannan bazai zama babban bambanci ba, amma motsin motsin lantarki na UCC yana da sannu a hankali kuma yana raguwa tare da hawan keke, musamman don halayen baya.Ko da yake jujjuyawar TCC ta fi na UCC kyau, an gano TCC tana da babban motsi na 73 mV bayan zagayowar 150, wanda zai iya kasancewa saboda yawan adadin chlorine da aka samu a samanta.ta yadda mai kara kuzari ya manne da kyau ga farfajiyar lantarki.Kamar yadda ake iya gani daga dukkan na'urorin lantarki da aka gwada, hatta na'urorin lantarki ba tare da tallafin masu kara kuzari sun nuna nau'o'in rashin zaman lafiya daban-daban na hawan keke, wanda ke nuni da cewa sauyin rarrabuwar kawuna a lokacin hawan keke ya samo asali ne sakamakon kashe kayan da sauye-sauyen sinadarai ke haifarwa maimakon rarrabuwar kawuna.Bugu da ƙari, idan za a raba babban adadin ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar ƙwayar cuta (ba kawai 44 mV ba), tun da substrate (UCC) ba shi da aiki ga VO2 +/VO2+ redox dauki.
Kwatanta CV na mafi kyawun kayan lantarki idan aka kwatanta da UCC (a) da kwanciyar hankali na VO2 +/VO2+ redox dauki (b).ν = 5 mV/s ga duk CVs a cikin 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Don haɓaka sha'awar tattalin arziƙin fasaha na VRFB, faɗaɗa da fahimtar motsin halayen vanadium redox yana da mahimmanci don cimma ingantaccen ƙarfin kuzari.An shirya abubuwan haɗin HWO-C76 kuma an yi nazarin tasirin electrocatalytic akan halayen VO2 +/VO2 +.HWO ya nuna ƙaramin haɓakar haɓakar motsin motsi a cikin gauraye na'urorin lantarki na acidic amma mahimmanci ya danne juyin halittar chlorine.An yi amfani da nau'i-nau'i daban-daban na HWO:C76 don ƙara inganta motsin motsi na tushen HWO.Ƙara C76 zuwa HWO yana inganta motsin motsi na lantarki na VO2 +/ VO2 + amsawa a kan gyare-gyaren lantarki, wanda HWO-50% C76 shine mafi kyawun abu saboda yana rage juriya na cajin caji kuma yana kara hana chlorine idan aka kwatanta da C76 da TCC ajiya..Wannan shi ne saboda tasirin haɗin kai tsakanin C = C sp2 hybridization, OH da W-OH ƙungiyoyin ayyuka.Ƙididdigar raguwa bayan hawan hawan hawan hawan HWO-50% C76 an gano shi ne 0.29 mV / sake zagayowar, yayin da raguwar ƙimar UCC da TCC shine 0.33 mV / sake zagayowar da 0.49 mV / sake zagayowar, bi da bi, yana mai da hankali sosai.a cikin Mix acid electrolytes.Sakamakon da aka gabatar ya sami nasarar gano manyan kayan aikin lantarki don amsawar VO2 +/VO2+ tare da saurin motsi da kwanciyar hankali.Wannan zai ƙara ƙarfin ƙarfin fitarwa, ta haka zai ƙara ƙarfin ƙarfin VRFB, don haka rage farashin kasuwancinsa na gaba.
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