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Iindleko eziphezulu kakhulu ze-vanadium flow-through redox batterys (VRFBs) zinciphisa ukusetyenziswa kwazo ngokubanzi.Ukuphucula i-kinetics ye-electrochemical reactions kuyafuneka ukwandisa amandla athile kunye nokusebenza kakuhle kwamandla e-VRFB, ngokunciphisa ixabiso le-kWh ye-VRFB.Kulo msebenzi, i-hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, i-C76 kunye ne-C76 / HWO, ifakwe kwi-carbon cloth electrodes kwaye yavavanywa njenge-electrocatalysts ye-VO2 +/VO2 + redox reaction.I-Field emission scanning electron microscopy (FESEM), i-energy dispersive X-ray spectroscopy (EDX), i-high-resolution transmission electron microscopy (HR-TEM), i-X-ray diffraction (XRD), i-X-ray photoelectron spectroscopy (XPS), i-infrared Fourier transform Spectroscopy (FTIR) kunye nemilinganiselo ye-angle yoqhagamshelwano.Kufunyenwe ukuba ukongezwa kwe-C76 fullerenes kwi-HWO kunokuphucula i-electrode kinetics ngokunyusa ukuhanjiswa kombane kunye nokubonelela ngamaqela asebenzayo oxidized kwindawo yayo, ngaloo ndlela ikhuthaza i-VO2 +/VO2 + redox reaction.I-HWO/C76 composite (50 wt% C76) ibonakalise ukuba lolona khetho lungcono kwi-VO2 +/VO2+ yokusabela nge-ΔEp ye-176 mV, ngelixa ilaphu lekhabhoni elingaphathwanga (UCC) laliyi-365 mV.Ukongezelela, i-HWO / C76 composite ibonise umphumo omkhulu wokuthintela kwi-parasitic chlorine reaction reaction ngenxa yeqela elisebenzayo le-W-OH.
Imisebenzi emandla yabantu kunye nenguqu ekhawulezileyo yezoshishino ikhokelele kwimfuno ephezulu ngokungenakuthintelwa yombane, enyuka nge-3% ngonyaka1.Kangangamashumi eminyaka, ukusetyenziswa okuxhaphakileyo kwamafutha efosili njengomthombo wamandla kukhokelele ekukhutshweni kwerhasi yegreenhouse enegalelo kubushushu behlabathi, ungcoliseko lwamanzi kunye nomoya, nto leyo esongela indalo iphela.Ngenxa yoko, ukungena komoya ococekileyo nohlaziyekayo kunye namandla elanga kulindeleke ukuba kufikelele kwi-75% yombane uwonke ngo-20501. Nangona kunjalo, xa isabelo sombane osuka kwimithombo ehlaziyekayo sidlula i-20% yombane owenziweyo uwonke, igridi iyangazinzi.
Phakathi kwazo zonke iinkqubo zokugcina amandla ezifana ne-hybrid vanadium redox flow battery2, yonke i-vanadium redox flow battery (VRFB) iye yaphuhliswa ngokukhawuleza ngenxa yeenzuzo zayo ezininzi kwaye ithathwa njengesisombululo esihle kakhulu sokugcina amandla ixesha elide (malunga ne-30 iminyaka).) Iinketho ezidityaniswe namandla ahlaziyekayo4.Oku kubangelwa ukuhlukana kwamandla kunye nokuxinana kwamandla, ukuphendula ngokukhawuleza, ubomi benkonzo ende, kunye nexabiso eliphantsi lonyaka eliphantsi le-65 / kWh xa kuthelekiswa ne-$ 93-140 / kWh ye-Li-ion kunye neebhetri ze-lead-acid kunye ne-279-420 yeedola zase-US nge-kWh.ibhetri ngokulandelelanayo 4.
Nangona kunjalo, urhwebo lwabo olukhulu lusathintelwa ziindleko zabo ezinkulu zenkqubo ephezulu, ngakumbi ngenxa yokupakishwa kweeseli4,5.Ke ngoko, ukuphucula ukusebenza kwesitaki ngokwandisa i-kinetics ye-half-element reactions inokunciphisa ubungakanani besitaki kwaye ngaloo ndlela inciphise iindleko.Ngoko ke, ukuhanjiswa kwe-electron ngokukhawuleza kwi-electrode surface kuyimfuneko, exhomekeke kuyilo, ukubunjwa kunye nesakhiwo se-electrode kwaye idinga ukulungiswa ngokucophelela6.Nangona kukho ukuzinza okulungileyo kweekhemikhali kunye ne-electrochemical conductivity efanelekileyo yombane we-carbon electrode, i-kinetics yabo engaphendulwanga iyancipha ngenxa yokungabikho kwamaqela asebenzayo oksijini kunye ne-hydrophilicity7,8.Ngoko ke, i-electrocatalysts eyahlukeneyo idibaniswe kunye ne-carbon-based electrode, ngakumbi i-carbon nanostructures kunye ne-oxides yensimbi, ukuphucula i-kinetics yazo zombini i-electrode, ngaloo ndlela inyusa i-kinetics ye-VRFB electrode.
Ukongeza kumsebenzi wethu wangaphambili kwi-C76, saqala sachaza umsebenzi ogqwesileyo we-electrocatalytic wale fullerene ye-VO2 +/VO2 +, ukudluliselwa kwentlawulo, xa kuthelekiswa nengubo ye-carbon ephathwayo kunye ne-carbon.Ukuchasa kuncitshiswe ngama-99.5% kunye nama-97%.Ukusebenza kwe-catalytic yezinto zekhabhoni ze-VO2 +/VO2 + yokuphendula xa kuthelekiswa ne-C76 kuboniswe kwiThebhile S1.Kwelinye icala, iioksidi zetsimbi ezininzi ezifana neCeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 kunye neWO331, 32, 33, 34, 35, 36, 37 zisetyenzisiwe ngenxa yokwanda kokumanzi kunye nokusebenza okuninzi kweoksijini., 38. iqela.Umsebenzi we-catalytic wale oxides zetsimbi kwi-VO2 +/VO2+ reaction iboniswe kwiThebhile S2.I-WO3 isetyenziswe kwinani elikhulu lemisebenzi ngenxa yeendleko zayo eziphantsi, ukuzinza okuphezulu kwimidiya ye-acidic, kunye nomsebenzi ophezulu we-catalytic31,32,33,34,35,36,37,38.Nangona kunjalo, ukuphuculwa kwe-cathodic kinetics ngenxa ye-WO3 ayibalulekanga.Ukuphucula ukuqhutyelwa kwe-WO3, umphumo wokusetyenziswa kwe-tungsten oxide eyancitshisiweyo (W18O49) kumsebenzi we-cathodic wavavanywa38.I-Hydrated tungsten oxide (i-HWO) ayizange ihlolwe kwizicelo ze-VRFB, nangona ibonisa ukwanda komsebenzi kwizicelo ze-supercapacitor ngenxa yokusabalalisa i-cation ngokukhawuleza xa kuthelekiswa ne-anhydrous WOx39,40.Isizukulwana sesithathu ibhetri ye-vanadium redox flow flow isebenzisa i-electrolyte ye-asidi edibeneyo eyenziwe yi-HCl kunye ne-H2SO4 ukuphucula ukusebenza kwebhetri kunye nokuphucula ukunyibilika kunye nokuzinza kwe-vanadium ions kwi-electrolyte.Nangona kunjalo, i-parasitic chlorine evolution reaction iye yaba yenye yezinto ezingalunganga zesizukulwana sesithathu, ngoko ke ukukhangela iindlela zokuthintela ukusabela kovavanyo lweklorine kuye kwaba yingqwalasela yamaqela amaninzi ophando.
Apha, iimvavanyo zokusabela ze-VO2 +/VO2+ zenziwa kwii-HWO/C76 ze-composites ezifakwe kwii-electrodes zelaphu lekhabhoni ukuze kufumaneke ulungelelwaniso phakathi kokuqhutywa kombane kwee-composites kunye ne-redox kinetics yendawo ye-electrode ngelixa icinezela i-parasitic chlorine evolution.impendulo (CER).I-hydrated tungsten oxide (HWO) i-nanoparticles yenziwe ngendlela elula ye-hydrothermal.Iimvavanyo zenziwa kwi-electrolyte ye-asidi exutywe (H2SO4/HCl) ukulinganisa isizukulwana sesithathu se-VRFB (G3) ukuze kusebenze kwaye kuphandwe isiphumo se-HWO kwi-parasitic 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), isodiyam Tungstenphild oxide, 4 hydrochloride, i-carbon 9 Aldrich, i-sodium Tungstenphild, i-Sigstenphild 4, i-Sigma-Aldrich ilaphu ELAT (Fuel Cell Store) zisetyenziswe kolu phononongo.
I-Hydrated tungsten oxide (HWO) yalungiswa yi-hydrothermal reaction 43 apho i-2 g yetyuwa ye-Na2WO4 yachithwa kwi-12 ml ye-H2O ukunika isisombululo esingenambala, emva koko i-12 ml ye-2 M HCl yongezwa nge-dropwise ukunika ukunqunyanyiswa okuluthuthu.I-slurry ifakwe kwi-Teflon efakwe kwi-autoclave yensimbi engenasici kwaye igcinwe kwi-oven kwi-180 ° C. kwiiyure ze-3 ukwenzela ukusabela kwe-hydrothermal.Intsalela iqokelelwe ngokuhluzwa, ihlanjwe ngamaxesha e-3 nge-ethanol kunye namanzi, yomiswa kwi-oven kwi-70 ° C kwiiyure ze-3, kwaye emva koko i-triturated ukunika i-HWO powder eluhlaza okwesibhakabhaka.
I-electrode ye-carbon cloth electrode (CCT) efunyenweyo (engaphathwanga) isetyenziswe njengokuba injalo okanye ukushisa kuphathwe kwisithando somlilo kwi-450 ° C emoyeni kunye nesantya sokufudumala kwe-15 ºC / min kwiiyure ze-10 ukufumana i-CCs ephathwayo (TCC).njengoko kuchaziwe kwinqaku elingaphambili24.I-UCC kunye ne-TCC zasikwa kwii-electrode malunga ne-1.5 cm ububanzi kunye ne-7 cm ubude.Ukumiswa kwe-C76, i-HWO, i-HWO-10% ye-C76, i-HWO-30% ye-C76 kunye ne-HWO-50% ye-C76 yalungiswa ngokongeza i-20 mg .% (~ 2.22 mg) ye-PVDF i-binder kwi- ~ 1 ml ye-DMF kunye ne-sonicated ye-1 iyure ukuphucula ukufana.I-2 mg ye-C76, i-HWO kunye ne-HWO-C76 edibeneyo isetyenziswe ngokulandelelana kwindawo ye-electrode esebenzayo ye-UCC malunga ne-1.5 cm2.Zonke ii-catalysts zilayishwe kwi-electrode ye-UCC kwaye i-TCC yayisetyenziselwa iinjongo zokuthelekisa kuphela, njengoko umsebenzi wethu wangaphambili ubonise ukuba unyango lobushushu alufunwa24.Ukulungiswa kwempembelelo kwaphunyezwa ngokuxubha i-100 µl yokunqunyanyiswa (umthwalo we-2 mg) ukwenzela isiphumo esithe kratya.Emva koko zonke ii-electrode zomiswa kwi-oven kwi-60 ° C. ubusuku bonke.Ii-electrode zilinganiswa phambili nasemva ukuze kuqinisekiswe ukulayishwa kwesitokhwe ngokuchanekileyo.Ukuze ube nommandla othile wejometri (~ 1.5 cm2) kunye nokuthintela ukunyuka kwe-vanadium electrolyte kwi-electrode ngenxa yempembelelo ye-capillary, i-parafini encinci isetyenziswe phezu kwezinto ezisebenzayo.
I-Findle emission scanning electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) yasetyenziswa ukujonga i-HWO surface morphology.I-spectrometer ye-X-reyi yokuchitha amandla exhotyiswe nge-Feii8SEM (EDX, Zeiss Inc.) isetyenziswe ukwenza imephu ye-HWO-50% C76 izinto kwii-electrode ze-UCC.Imakroskopu ye-electron yothumelo oluphezulu (HR-TEM, JOEL JEM-2100) esebenza kumbane okhawulezayo wama-200 kV isetyenziswe ukwenza umfanekiso wamasuntswana e-HWO anesisombululo esiphezulu kunye nezangqa ze-diffraction.I-Crystallography Toolbox (i-CrysTBox) isofthiwe isebenzisa umsebenzi we-ringGUI ukuhlalutya ipateni ye-HWO ye-ring diffraction kwaye ithelekise iziphumo kunye nephethini ye-XRD.Isakhiwo kunye ne-graphitization ye-UCC kunye ne-TCC yahlalutywa yi-X-ray diffraction (XRD) kwizinga lokuskena kwe-2.4 ° / min ukusuka kwi-5 ° ukuya kwi-70 ° kunye ne-Cu Kα (λ = 1.54060 Å) usebenzisa i-Panalytical X-ray diffractometer (Model 3600).I-XRD ibonise ubume bekristale kunye nesigaba se-HWO.I-software ye-PANalytical X'Pert HighScore yayisetyenziselwa ukufanisa iincopho ze-HWO kwiimephu ze-tungsten oxide ezikhoyo kwi-database45.Iziphumo ze-HWO zathelekiswa neziphumo ze-TEM.Ukwakhiwa kweekhemikhali kunye nemeko yeesampuli ze-HWO zinqunywe yi-X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific).I-software ye-CASA-XPS (v 2.3.15) isetyenziswe kwi-peak deconvolution kunye nohlalutyo lwedatha.Ukumisela amaqela asebenzayo omphezulu we-HWO kunye ne-HWO-50% C76, imilinganiselo yenziwa kusetyenziswa i-Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, kusetyenziswa i-Kbr FTIR).Iziphumo zithelekiswe neziphumo zeXPS.Imilinganiselo ye-angle yoqhagamshelwano (KRUSS DSA25) nayo yayisetyenziselwa ukubonakalisa ukumanzi kwee-electrodes.
Kuyo yonke imilinganiselo ye-electrochemical, i-Biologic SP 300 workstation yasetyenziswa.I-Cyclic voltammetry (CV) kunye ne-electrochemical impedance spectroscopy (EIS) yayisetyenziselwa ukufunda i-electrode kinetics ye-VO2 +/VO2+ redox reaction kunye nefuthe le-reagent diffusion (VOSO4 (VO2 +)) kwizinga lokuphendula.Zombini iindlela zisebenzisa iseli ye-electrode emithathu ene-electrolyte concentration ye-0.1 M VOSO4 (V4 +) kwi-1 M H2SO4 + 1 M HCl (umxube we-acids).Yonke idatha ye-electrochemical enikeziweyo i-IR ilungisiwe.I-calomel electrode (SCE) kunye ne-platinum (Pt) i-coil isetyenziswe njengereferensi kunye ne-counter electrode, ngokulandelanayo.Kwi-CV, iireyithi zokuskena (ν) ze-5, 20, kunye ne-50 mV/s zisetyenziswe kwi-VO2+/VO2+ yefestile enokubakho ye- (0–1) V vs. SCE, emva koko ihlengahlengiswe ukuze i-SHE icwangcise (VSCE = 0.242 V vs. HSE) .Ukufunda ukugcinwa komsebenzi we-electrode, ii-CV ze-cyclic eziphindaphindiweyo zenziwa kwi-ν 5 mV / s ye-UCC, TCC, UCC-C76, UCC-HWO, kunye ne-UCC-HWO-50% C76.Kwimilinganiselo ye-EIS, i-frequency range ye-VO2 +/VO2+ redox reaction yaba yi-0.01-105 Hz, kunye ne-voltage perturbation kwi-open-circuit voltage (OCV) yi-10 mV.Uvavanyo ngalunye luphindwe ngamaxesha e-2-3 ukuqinisekisa ukuhambelana kweziphumo.Isantya esingaqhelekanga (k0) sifunyenwe ngendlela ye-Nicholson46,47.
I-hydrated tungsten oxide (HVO) yenziwe ngempumelelo ngendlela ye-hydrothermal.Umfanekiso we-SEM kwifig.I-1a ibonisa ukuba i-HWO egciniweyo iqulethwe ngamaqoqo e-nanoparticles kunye nobukhulu kuluhlu lwe-25-50 nm.
Ipatheni ye-X-ray diffraction ye-HWO ibonisa iincopho (001) kunye (002) kwi- ~ 23.5 ° kunye ne- ~ 47.5 °, ngokulandelanayo, ezizimpawu ze-nonstoichiometric WO2.63 (W32O84) (PDF 077-0810, a = 21.4 Å, Å3 = Å γ =, b Å 8 = , b Å 8 = , b Å 8 = , b = Å 8 = , b Å 8 = , b ; 90 °), ehambelana nombala wabo oluhlaza okwesibhakabhaka ocacileyo (Umfanekiso 1b) 48.49.Ezinye iincopho malunga ne-20.5 °, 27.1 °, 28.1 °, 30.8 °, 35.7 °, 36.7 ° kunye ne-52.7 ° zabelwa (140), (620), (350), (720), (740), (560 °).)) kunye (970) iindiza ze-diffraction orthogonal ukuya kwi-WO2.63, ngokulandelanayo.Indlela efanayo yokwenziwa yasetyenziswa nguSongara et al.43 ukufumana imveliso emhlophe, eyayibangelwa ubukho beWO3 (H2O) 0.333.Nangona kunjalo, kulo msebenzi, ngenxa yeemeko ezahlukeneyo, imveliso eluhlaza okwesibhakabhaka-grey yafunyanwa, ebonisa ukuba i-WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90 °) kunye nefom ye-oxid encitshisiweyo.Uhlalutyo lwe-Semiquantitative usebenzisa i-software ye-X'Pert HighScore ibonise i-26% WO3 (H2O) 0.333: 74% W32O84.Ekubeni i-W32O84 iqukethe i-W6+ kunye ne-W4+ (1.67: 1 W6+: W4+), umxholo oqikelelwayo we-W6+ kunye ne-W4+ malunga ne-72% W6+ kunye ne-28% W4+, ngokulandelanayo.Imifanekiso ye-SEM, i-1-yesibini ye-XPS ye-spectra kwinqanaba le-nucleus, imifanekiso ye-TEM, i-FTIR spectra, kunye ne-Raman spectra ye-C76 particles ziboniswe kwinqaku lethu langaphambili.Ngokutsho kwe-Kawada et al., I-50,51 i-X-ray diffraction ye-C76 emva kokususwa kwe-toluene ibonise isakhiwo se-monoclinic se-FCC.
Imifanekiso ye-SEM kwifig.I-2a kunye ne-b ibonisa ukuba i-HWO kunye ne-HWO-50% C76 zifakwe ngempumelelo kunye naphakathi kwe-carbon fibers ye-electrode ye-UCC.EDX element iimephu zetungsten, ikhabhoni, kunye neoksijini kwimifanekiso ye-SEM kwifig.I-2c iboniswe kwifig.I-2d-f ebonisa ukuba i-tungsten kunye nekhabhoni zixutywe ngokulinganayo (ebonisa ukusabalalisa okufanayo) phezu kwendawo yonke ye-electrode kwaye i-composite ayifakwanga ngokufanayo ngenxa yobume bendlela yokubeka.
Imifanekiso ye-SEM yeengqungquthela ze-HWO ezifakwe (a) kunye neengqungquthela ze-HWO-C76 (b).Imephu ye-EDX kwi-HWO-C76 elayishwe kwi-UCC isebenzisa indawo emfanekisweni (c) ibonisa ukuhanjiswa kwe-tungsten (d), i-carbon (e), kunye ne-oksijini (f) kwisampuli.
I-HR-TEM yayisetyenziselwa ukulinganisa okuphezulu kunye nolwazi lwecrystallographic (Umfanekiso 3).I-HWO ibonisa i-nanocube morphology njengoko kuboniswe kwi-Fig. 3a kwaye ngokucacileyo ngakumbi kwi-Fig. 3b.Ngokukhulisa i-nanocube yokuphazamiseka kweendawo ezikhethiweyo, umntu unokubona ngeso lengqondo isakhiwo se-grating kunye ne-diffraction planes eyanelisa umthetho we-Bragg, njengoko kuboniswe kwi-Fig. 3c, eqinisekisa i-crystallinity yezinto eziphathekayo.Kwi-inset ukuya kwi-Fig. 3c ibonisa umgama d 3.3 Å ehambelana ne (022) kunye (620) iindiza ze-diffraction ezifumaneka kwi-WO3 (H2O) 0.333 kunye ne-W32O84 izigaba, ngokulandelanayo43,44,49.Oku kuhambelana nohlalutyo lwe-XRD oluchazwe ngasentla (umzobo 1b) ekubeni umgama wendiza ye-grating ebonwayo d (umzobo 3c) uhambelana neyona nto inamandla ye-XRD kwisampuli ye-HWO.Iisampulu zamakhonkco nazo ziboniswe kwifig.3d, apho ikhonkco ngalinye lihambelana nendiza eyahlukileyo.I-WO3 (H2O) i-0.333 kunye ne-W32O84 iindiza zinemibala emhlophe kunye ne-blue, ngokulandelanayo, kunye neengqungquthela zabo ze-XRD ezihambelanayo nazo ziboniswe kwi-Fig. 1b.Iringi yokuqala eboniswe kumzobo weringi ihambelana nencopho yokuqala ephawulweyo kwipatheni ye-x-reyi ye (022) okanye (620) ye-diffraction plane.Ukusuka kwi-(022) ukuya ku-(402) amakhonkco, amaxabiso e-d-spacing yi-3.30, 3.17, 2.38, 1.93, kunye ne-1.69 Å, ehambelana nexabiso le-XRD ye-3.30, 3.17, 2, 45, 1.93.kunye no-1.66 Å, elilingana no-44, 45, ngokulandelelanayo.
(a) Umfanekiso we-HR-TEM we-HWO, (b) ubonisa umfanekiso owandisiweyo.Imifanekiso yeeplani zokugaya iboniswe kwi-(c), i-inset (c) ibonisa umfanekiso owandisiweyo weendiza kunye ne-pitch d ye-0.33 nm ehambelana ne-(002) kunye (620) iindiza.(d) Ipateni ye-HWO ring ebonisa iindiza ezinxulumene ne-WO3 (H2O) 0.333 (emhlophe) kunye ne-W32O84 (eblue).
Uhlalutyo lwe-XPS lwenziwa ukumisela i-chemistry yomhlaba kunye ne-oxidation state ye-tungsten (Amanani S1 kunye ne-4).Uluhlu olubanzi lwe-XPS scan spectrum ye-HWO eyenziweyo iboniswe kuMfanekiso S1, ebonisa ubukho be-tungsten.I-XPS ye-scan-scan spectra ye-W 4f kunye ne-O 1s amanqanaba angundoqo aboniswe kwiMifanekiso.4a kunye no-b, ngokulandelelanayo.I-W 4f spectrum yahlulahlulwa ibe zimbini eziphindwe kabini ze-spin-orbit ezihambelana namandla okubophelela kwimo ye-W oxidation.kunye ne-W 4f7/2 kwi-36.6 kunye ne-34.9 eV yimpawu ye-W4 + ye-40, ngokulandelanayo.)0.333.Idatha efakiweyo ibonisa ukuba iipesenti ze-athomu ze-W6 + kunye ne-W4 + ziyi-85% kunye ne-15%, ngokulandelanayo, ezikufutshane namaxabiso aqikelelweyo kwidatha ye-XRD eqwalasela ukungafani phakathi kwezi ndlela zimbini.Zombini iindlela zibonelela ngolwazi lobungakanani ngokuchaneka okuphantsi, ngakumbi i-XRD.Kwakhona, ezi ndlela zimbini zihlalutya iindawo ezahlukeneyo zemathiriyeli kuba i-XRD yindlela yobuninzi ngelixa i-XPS yindlela yomphezulu esondela kwiinanometers ezimbalwa.I-spectrum ye-O 1s ihlulwe ibe ziincopho ezimbini kwi-533 (22.2%) kunye ne-530.4 eV (77.8%).Eyokuqala ihambelana ne-OH, kwaye okwesibini kwiibhondi ze-oksijini kwi-lattice kwi-WO.Ubukho bamaqela asebenzayo e-OH ahambelana neempawu ze-hydration ze-HWO.
Uhlalutyo lwe-FTIR lwenziwa kwakhona kwezi sampuli zimbini ukuhlola ubukho bamaqela asebenzayo kunye nokulungelelanisa iamolekyu zamanzi kwisakhiwo se-HWO e-hydrated.Iziphumo zibonisa ukuba isampuli ye-HWO-50% ye-C76 kunye ne-FT-IR HWO iziphumo zibonakala zifana ngenxa yobukho be-HWO, kodwa ubuninzi beengqungquthela ziyahluka ngenxa yobuninzi besampulu esetyenziselwa ukulungiselela uhlalutyo (umzobo 5a).) I-HWO-50% i-C76 ibonisa ukuba zonke iindawo eziphakamileyo, ngaphandle kwe-tungsten oxide, zihambelana ne-fulerene 24. Ecacisiweyo kumkhiwane.I-5a ibonisa ukuba zombini iisampulu zibonisa ibhanti ebanzi kakhulu ebanzi kwi ~ 710 / cm echazwe kwi-OWO yokwelula i-oscillations kwisakhiwo se-lattice ye-HWO, kunye negxalaba eliqinileyo kwi ~ 840 / cm ebizwa ngokuba yi-WO.Ukolula ukungcangcazela, ibhendi ebukhali emalunga ne-1610/cm ichazwa kukushukuma okugobileyo kwe-OH, ngelixa ibhendi yokufunxa ebanzi malunga ne-3400/cm ibalelwa kukolula ukungcangcazela kwe-OH kumaqela e-hydroxyl43.Ezi ziphumo zihambelana ne-XPS spectra kwiFig.I-4b, apho amaqela asebenzayo e-WO anokubonelela ngeendawo ezisebenzayo ze-VO2 +/VO2 + reaction.
Uhlalutyo lwe-FTIR ye-HWO kunye ne-HWO-50% C76 (a), ibonise amaqela asebenzayo kunye nemilinganiselo ye-angle yoqhagamshelwano (b, c).
Iqela le-OH linokwenza i-catalyze i-VO2 +/VO2+ reaction, ngelixa inyusa i-hydrophilicity ye-electrode, ngaloo ndlela ikhuthaza izinga lokusabalalisa kunye nokudluliselwa kwe-electron.Njengoko kubonisiwe, isampuli ye-HWO-50% ye-C76 ibonisa i-peak eyongezelelweyo ye-C76.Incopho kwi ~ 2905, 2375, 1705, 1607, kunye ne-1445 cm3 inokwabelwa kwi-CH, O=C=O, C=O, C=C, kunye ne-CO ezolula ii-vibrations, ngokulandelanayo.Kuyaziwa ukuba amaqela asebenzayo oksijini C = O kunye ne-CO angasebenza njengamaziko asebenzayo kwi-redox reactions of vanadium.Ukuvavanya nokuthelekisa ukumanzisa kwee-electrode ezimbini, imilinganiselo ye-angle yoqhagamshelwano yathathwa njengoko kuboniswe kuMzobo 5b, c.I-electrode ye-HWO ngokukhawuleza yafunxa amaconsi amanzi, ebonisa i-superhydrophilicity ngenxa yamaqela asebenzayo e-OH akhoyo.I-HWO-50% ye-C76 i-hydrophobic ngakumbi, kunye ne-angle yoqhagamshelwano malunga ne-135 ° emva kwemizuzwana ye-10.Nangona kunjalo, kwimilinganiselo ye-electrochemical, i-electrode ye-HWO-50% C76 yaba manzi ngokupheleleyo ngaphantsi komzuzu.Imilinganiselo yokumanzisa ihambelana neziphumo ze-XPS kunye ne-FTIR, ebonisa ukuba amaqela amaninzi e-OH kumphezulu we-HWO awenza abe ne-hydrophilic ngakumbi.
I-VO2 +/VO2 + reactions ye-HWO kunye ne-HWO-C76 nanocomposites yavavanywa kwaye kwakulindeleke ukuba i-HWO iya kucinezela i-chlorine evolution kwi-VO2 +/VO2 + yokusabela kwi-asidi exutywe, kwaye i-C76 iya kuphinda iqhube i-VO2 +/VO2 + i-redox efunwayo.I-%, i-30%, kunye ne-50% ye-C76 ekumisweni kwe-HWO kunye ne-CCC efakwe kwi-electrodes kunye nokulayisha okupheleleyo malunga ne-2 mg / cm2.
Njengoko kubonisiwe kwifig.I-6, i-kinetics ye-VO2 +/VO2 + yokusabela kwi-electrode surface ihlolwe yi-CV kwi-electrolyte edibeneyo e-acidic.Imisinga iboniswa njenge-I/Ipa ukuthelekisa ngokulula kwe-ΔEp kunye ne-Ipa/Ipc yee-catalysts ezahlukeneyo ngqo kwigrafu.Idatha yeyunithi yendawo yangoku iboniswe kuMfanekiso 2S.Kwikhiwane.Umzobo 6a ubonisa ukuba i-HWO yonyusa kancinane izinga lokudluliselwa kwe-electron ye-VO2 +/VO2+ redox reaction on the surface electrode and suppresses reaction of parasitic chlorine evolution.Nangona kunjalo, i-C76 inyusa kakhulu izinga lokudluliselwa kwe-electron kwaye ibangele ukusabela kwe-chlorine evolution.Ngoko ke, i-composite eyenziwe ngokuchanekileyo ye-HWO kunye ne-C76 ilindeleke ukuba ibe nomsebenzi ongcono kakhulu kunye namandla amakhulu okuthintela ukuphendula kwe-chlorine evolution.Kwafunyaniswa ukuba emva kokunyusa umxholo we-C76, umsebenzi we-electrochemical we-electrodes uphuculwe, njengoko kubonakaliswe ngokuncipha kwe-ΔEp kunye nokunyuka kwe-Ipa / Ipc ratio (Itheyibhile S3).Oku kwaqinisekiswa kwakhona ngamaxabiso e-RCT akhutshwe kwisicwangciso seNyquist kwi-Fig. 6d (Itheyibhile S3), efunyenwe ukunciphisa ngokunyuka komxholo weC76.Ezi ziphumo zikwahambelana nophononongo lukaLi, apho ukongezwa kwekhabhoni ye-mesoporous kwi-mesoporous WO3 kubonise ukuhanjiswa kwentlawulo okuphuculweyo kwi-VO2+/VO2+35.Oku kubonisa ukuba ukuphendula ngokuthe ngqo kunokuxhomekeka ngakumbi kwi-electrode conductivity (C = C bond) 18, 24, 35, 36, 37. Oku kunokuba ngenxa yenguqu kwijometri yokulungelelaniswa phakathi kwe- [VO (H2O) 5] 2+ kunye ne [VO2 (H2O) 4]+, i-C76 iyanciphisa ukugqithisa kwamandla ezicubu.Nangona kunjalo, oku akunakwenzeka nge-electrode ye-HWO.
(a) Ukuziphatha kwe-Cyclic voltammetric (ν = 5 mV / s) ye-VO2 +/VO2+ yokusabela kwe-UCC kunye ne-HWO-C76 edibeneyo kunye ne-HWO: i-C76 eyahlukeneyo kwi-0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik kunye (c) Nicholson VO2 +/VO2+ indlela yokuvavanya ukusebenza kakuhle kokusasazwa kunye nokufumana ixabiso le-k0 (d).
Yayingekuphela nje i-HWO-50% ye-C76 ebonisa phantse umsebenzi ofanayo we-electrocatalytic njenge-C76 ye-VO2 +/VO2+ reaction, kodwa, ngakumbi umdla, yaphinda yacinezela i-chlorine evolution xa kuthelekiswa ne-C76, njengoko kubonisiwe kwi-Fig. 6a, kwaye ibonisa iSemicircle encinci kwifig.I-6d (i-RCT ephantsi).I-C76 ibonise i-Ipa / Ipc ephezulu ecacileyo kune-HWO-50% C76 (Itheyibhile S3), kungekhona ngenxa yokuphucula ukuguqulwa kwempendulo, kodwa ngenxa ye-peak overlap of the reaction yokunciphisa i-chlorine kunye ne-SHE kwi-1.2 V. Ukusebenza kakuhle kwe-HWO- I-50% C76 ibangelwa yi-synergistic charger kunye ne-conductor ephezulu ye-caji kunye ne-conductivity ephezulu ye-caloric-HH ephezulu kunye ne-high-of-conductability ye-conduvative kwi-HWO.Ukukhutshwa kweklorini encinci kuya kuphucula ukusebenza kakuhle kokutshaja kweseli epheleleyo, ngelixa i-kinetics ephuculweyo iya kuphucula ukusebenza kombane opheleleyo weseli.
Ngokutsho kwe-equation S1, kwi-quasi-reversible (ngokucothayo kwi-electron transfer) elawulwa ngokusasazwa, i-peak current (IP) ixhomekeke kwinani leelektroni (n), indawo ye-electrode (A), i-diffusion coefficient (D), inani le-electrons transfer coefficient (α) kunye nesantya sokuskena (ν).Ukuze ufunde ukuziphatha okulawulwa kukusasazeka kwezinto ezivavanyiweyo, ubudlelwane phakathi kwe-IP kunye ne-ν1/2 yacwangciswa kwaye yaboniswa kwi-Fig. 6b.Kuba zonke izixhobo zibonisa ubudlelwane bomgca, impendulo ilawulwa yi-diffusion.Ekubeni i-VO2 +/VO2 + i-reaction i-quasi-reversible, i-slope yomgca ixhomekeke kwi-coefficient yokusabalalisa kunye nexabiso le-α (i-equation S1).Ekubeni i-coefficient yokusasazwa ihlala rhoqo (≈ 4 × 10-6 cm2 / s) 52, umahluko kwithambeka lomgca ubonisa ngokuthe ngqo amaxabiso ahlukeneyo e-α, kwaye ngoko ke izinga lokudluliselwa kwe-electron kwindawo ye-electrode, eboniswa kwi-C76 kunye ne-HWO -50% C76 i-Slopeest slope (izinga eliphezulu lokudlulisa i-electron).
I-Warburg slopes (W) ibalwa kwii-frequencies eziphantsi eziboniswe kwiTheyibhile S3 (Fig. 6d) inamaxabiso kufuphi ne-1 yazo zonke izinto eziphathekayo, ebonisa ukusasazwa okugqibeleleyo kweentlobo ze-redox kunye nokuqinisekisa ukuziphatha kwe-linear ye-IP xa kuthelekiswa ne-ν1 / 2. I-CV iyalinganiswa.I-HWO-50% ye-C76, i-slope ye-Warburg iyaphambuka ukusuka kwi-1 ukuya kwi-1.32, ebonisa ukusasazwa kwe-semi-infinite ye-reagent (VO2 +), kodwa kunye negalelo elinokwenzeka lokuziphatha okubhityileyo ekuziphatheni kokusabalalisa ngenxa ye-electrode porosity.
Ukuqhubela phambili ukuhlalutya ukuguqulwa (izinga lokudluliselwa kwe-electron) ye-VO2 +/VO2+ redox reaction, indlela yokuphendula ye-Nicholson quasi-reversible reaction nayo yasetyenziswa ukumisela izinga eliqhelekileyo le-k041.42.Oku kwenziwa kusetyenziswa i-S2 equation ukwakha iparamitha yekinetic engena dimensionless Ψ, engumsebenzi we ΔEp, njengomsebenzi we-ν-1/2.Itheyibhile S4 ibonisa amaxabiso e-Ψ afunyenwe kwisixhobo ngasinye se-electrode.Iziphumo (umzobo 6c) zacwangciswa ukufumana i-k0 × 104 cm/s ukusuka kwithambeka leploti nganye kusetyenziswa i-Equation S3 (ebhalwe ecaleni komqolo ngamnye kwaye iboniswe kwiThebhile S4).I-HWO-50% i-C76 ifunyenwe i-slope ephezulu (umzobo 6c), ngoko ke ixabiso eliphezulu le-k0 li-2.47 × 10-4 cm / s.Oku kuthetha ukuba le electrode ifezekisa i-kinetics ekhawulezayo, ehambelana ne-CV kunye ne-EIS iziphumo kwi-Fig. 6a kunye ne-d kunye ne-Table S3.Ukongezelela, ixabiso le-k0 lifunyenwe kwakhona kwi-Nyquist plot (Umfanekiso 6d) we-Equation S4 usebenzisa ixabiso le-RCT (Itheyibhile S3).Ezi ziphumo ze-k0 ezivela kwi-EIS zishwankathelwa kwiThebhile ye-S4 kwaye ikwabonisa ukuba i-HWO-50% ye-C76 ibonisa izinga eliphezulu lokudluliselwa kwe-electron ngenxa yesiphumo se-synergistic.Nangona amaxabiso e-k0 ahluka ngenxa yemvelaphi eyahlukileyo yendlela nganye, asabonisa ukulandelelana okufanayo kobukhulu kwaye abonise ukungaguquguquki.
Ukuqonda ngokupheleleyo i-kinetics egqwesileyo efunyenweyo, kubalulekile ukuthelekisa izinto ezifanelekileyo ze-electrode kunye ne-UCC engafakwanga kunye ne-TCC electrode.Kwi-VO2 +/VO2+ reaction, i-HWO-C76 ayizange ibonise kuphela i-ΔEp ephantsi kunye nokuguqulwa okungcono, kodwa icinezele kakhulu i-parasitic chlorine evolution reaction xa ithelekiswa ne-TCC, njengoko ilinganiswe ngoku kwi-1.45 V ngokumalunga ne-SHE (Fig. 7a).Ngokumalunga nokuzinza, sasicinga ukuba i-HWO-50% ye-C76 yayizinzile ngokomzimba kuba i-catalyst yayixutywe kunye ne-PVDF binder kwaye isetyenziswe kwi-carbon cloth electrodes.I-HWO-50% ye-C76 ibonise ukunyuka okuphezulu kwe-44 mV (izinga lokuthotywa kwe-0.29 mV / umjikelezo) emva kwemijikelezo ye-150 xa kuthelekiswa ne-50 mV ye-UCC (Umfanekiso 7b).Oku akunakuba ngumahluko omkhulu, kodwa i-kinetics ye-electrode ye-UCC icotha kakhulu kwaye ithobisa ngokukhwela ibhayisekile, ngakumbi kwiimpendulo ezibuyela umva.Nangona ukuguqulwa kwe-TCC kubhetele kakhulu kunoko kwe-UCC, i-TCC ifunyaniswe inencopho enkulu yokutshintsha kwe-73 mV emva kwemijikelo ye-150, enokuthi ibe ngenxa yesixa esikhulu seklorine eyenziwe kumphezulu wayo.ukwenzela ukuba i-catalyst ibambelele kakuhle kwi-electrode surface.Njengoko kunokubonwa kuwo onke ama-electrode avavanyiweyo, kunye ne-electrodes ngaphandle kwee-catalysts ezixhaswayo zibonise amanqanaba ahlukeneyo okungazinzi kwebhayisikile, ebonisa ukuba utshintsho oluphezulu lokuhlukana ngexesha lokuhamba ngebhayisikili lubangelwa ukuchithwa kwezinto ezibangelwa ukuguqulwa kweekhemikhali kunokuhlukana kwe-catalyst.Ukongezelela, ukuba inani elikhulu le-catalyst particles liza kuhlukaniswa ukusuka kwi-electrode surface, oku kuya kubangela ukwanda okukhulu kokuhlukana kwe-peak (kungekhona kuphela i-44 mV), ekubeni i-substrate (UCC) ayisebenzi ngokufanelekileyo kwi-VO2 +/VO2 + redox reaction.
Ukuthelekiswa kwe-CV yezinto ezilungileyo kakhulu ze-electrode xa kuthelekiswa ne-UCC (a) kunye nokuzinza kwe-VO2 +/VO2 + redox reaction (b).ν = 5 mV/s kuzo zonke ii-CVs kwi-0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Ukonyusa umtsalane woqoqosho lwetekhnoloji yeVRFB, ukwandisa kunye nokuqonda i-kinetics ye-vanadium redox reactions kubalulekile ukufezekisa ukusebenza kakuhle kwamandla.Iimbumba ze-HWO-C76 zalungiswa kwaye umphumo wabo we-electrocatalytic kwi-VO2 +/VO2 + reaction wafundwa.I-HWO ibonise ukuphuculwa okuncinci kwekinetic kwi-electrolyte ene-acidic exutyiweyo kodwa yacinezela kakhulu ukuvela kweklorini.Imilinganiselo eyahlukeneyo ye-HWO: i-C76 isetyenziselwe ukuqhubela phambili i-kinetics yee-electrode ezisekelwe kwi-HWO.Ukwandisa i-C76 ukuya kwi-HWO kuphucula i-electron transfer kinetics ye-VO2 +/VO2 + reaction on the modified electrode, apho i-HWO-50% C76 iyona nto ingcono kakhulu kuba iyanciphisa ukuchasana nokudluliselwa kwentlawulo kwaye icinezele ngakumbi i-chlorine xa kuthelekiswa ne-C76 kunye ne-TCC deposit..Oku kungenxa yempembelelo ye-synergistic phakathi kwe-C=C sp2 hybridization, i-OH kunye ne-W-OH amaqela asebenzayo.Izinga lokuthotywa emva kokujikeleza ngokuphindaphindiweyo kwe-HWO-50% C76 kwafunyanwa ukuba yi-0.29 mV / umjikelezo, ngelixa izinga lokuthotywa kwe-UCC kunye ne-TCC yi-0.33 mV / cycle kunye ne-0.49 mV / umjikelo, ngokulandelanayo, okwenza kube nzima kakhulu.kwi-electrolyte ye-asidi edibeneyo.Iziphumo ezibonisiweyo zichonga ngempumelelo izixhobo ze-electrode eziphezulu ze-VO2 +/VO2+ yokusabela nge-kinetics ekhawulezayo kunye nokuzinza okuphezulu.Oku kuya kwandisa amandla ombane ophumayo, ngaloo ndlela kwandisa ukusebenza kakuhle kwamandla e-VRFB, ngaloo ndlela kuncitshiswe iindleko zokurhweba kwayo kwixesha elizayo.
Iiseti zedatha ezisetyenzisiweyo kunye/okanye ezihlalutyiweyo kuphononongo lwangoku ziyafumaneka kubabhali abachaphazelekayo ngesicelo esinengqiqo.
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