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Ixabiso eliphezulu kakhulu leebhetri ze-all-vanadium flow-through redox (ii-VRFB) lithintela ukusetyenziswa kwazo ngokubanzi. Ukuphucula i-kinetics yee-electrochemical reactions kuyafuneka ukwandisa amandla athile kunye nokusebenza kakuhle kwamandla e-VRFB, ngaloo ndlela kunciphisa iindleko ze-kWh ze-VRFB. Kulo msebenzi, ii-nanoparticles ze-tungsten oxide (HWO) ezidityaniswe ngamanzi, i-C76 kunye ne-C76/HWO, zifakwe kwi-electrodes ze-carbon cloth kwaye zavavanywa njengee-electrocatalysts ze-VO2+/VO2+ redox reaction. I-field emission scanning electron microscopy (i-FESEM), i-energy dispersive X-ray spectroscopy (i-EDX), i-high-resolution transmission electron microscopy (i-HR-TEM), i-X-ray diffraction (i-XRD), i-X-ray photoelectron spectroscopy (i-XPS), i-infrared Fourier transform Spectroscopy (i-FTIR) kunye nokulinganisa i-contact angle. Kufunyenwe ukuba ukongezwa kwe-C76 fullerenes kwi-HWO kunokuphucula i-electrode kinetics ngokunyusa ukuhanjiswa kombane kunye nokubonelela ngamaqela asebenzayo axidizisiweyo kumphezulu wayo, ngaloo ndlela kukhuthaza i-VO2+/VO2+ redox reaction. I-HWO/C76 composite (50 wt% C76) ibonakalise ukuba lolona khetho lufanelekileyo kwi-VO2+/VO2+ reaction ene-ΔEp ye-176 mV, ngelixa ilaphu lekhabhoni elinganyangwanga (UCC) yayiyi-365 mV. Ukongeza, i-HWO/C76 composite ibonise impembelelo ebalulekileyo yokuthintela kwi-parasitic chlorine evolution reaction ngenxa yeqela le-W-OH functional.
Imisebenzi emikhulu yabantu kunye noguquko olukhawulezayo kwezoshishino kukhokelele kwimfuno ephezulu kakhulu yombane, eyanda malunga ne-3% ngonyaka1. Kangangamashumi eminyaka, ukusetyenziswa ngokubanzi kwamafutha efosili njengomthombo wamandla kukhokelele ekukhutshweni kweegesi ezibangela ukufudumala kwehlabathi, ungcoliseko lwamanzi nomoya, nto leyo esongela zonke iinkqubo eziphilayo. Ngenxa yoko, ukungena kwamandla omoya acocekileyo nahlaziyekayo kunye nelanga kulindeleke ukuba kufike kwi-75% yombane uwonke ngo-20501. Nangona kunjalo, xa isabelo sombane esivela kwimithombo evuselelekayo sidlula i-20% yombane uwonke, igridi ayizinzanga.
Phakathi kwazo zonke iinkqubo zokugcina amandla ezifana nebhetri ye-hybrid vanadium redox flow2, ibhetri ye-all-vanadium redox flow (VRFB) iphuhliswe ngokukhawuleza ngenxa yeenzuzo zayo ezininzi kwaye ithathwa njengesisombululo esifanelekileyo sokugcina amandla ixesha elide (malunga neminyaka engama-30). ) Iinketho ezidityaniswe namandla avuselelekayo4. Oku kungenxa yokwahlulwa kwamandla kunye noxinano lwamandla, impendulo ekhawulezayo, ubomi benkonzo ende, kunye nexabiso eliphantsi lonyaka le-$65/kWh xa kuthelekiswa ne-$93-140/kWh yeebhetri zeLi-ion kunye nelead-acid kunye ne-279-420 US dollars nge-kWh nganye. 4.
Nangona kunjalo, ukuthengiswa kwazo okukhulu kusathintelwa ziindleko zazo ezinkulu zenkqubo, ikakhulu ngenxa yee-cell stacks4,5. Ngoko ke, ukuphucula ukusebenza kwee-stack ngokunyusa i-kinetics yee-half-element reactions ezimbini kunokunciphisa ubungakanani be-stack ngaloo ndlela kunciphisa iindleko. Ke ngoko, ukudluliselwa kwe-electron ngokukhawuleza kumphezulu we-electrode kuyimfuneko, okuxhomekeke kuyilo, ukwakheka kunye nolwakhiwo lwe-electrode kwaye kufuna ukulungiswa ngononophelo6. Nangona uzinzo oluhle lweekhemikhali kunye ne-electrochemical kunye nokuqhuba kakuhle kombane kwee-carbon electrodes, i-kinetics yazo enganyangwanga iyacotha ngenxa yokungabikho kwamaqela asebenzayo e-oxygen kunye ne-hydrophilicity7,8. Ke ngoko, ii-electrocatalysts ezahlukeneyo zidityaniswe nee-electrodes ezisekelwe kwi-carbon, ngakumbi ii-carbon nanostructures kunye nee-metal oxides, ukuphucula i-kinetics yee-electrodes zombini, ngaloo ndlela kwandisa i-kinetics ye-VRFB electrode.
Ukongeza kumsebenzi wethu wangaphambili kwi-C76, siqale saxela ngomsebenzi ogqwesileyo we-electrocatalytic wale fullerene kwi-VO2+/VO2+, ukudluliselwa kwetshaja, xa kuthelekiswa nelaphu lekhabhoni eliphathwe ngobushushu nelinganyangwanga. Ukumelana kuncitshiswa ngama-99.5% kunye nama-97%. Ukusebenza kwe-catalytic kwezinto zekhabhoni kwi-VO2+/VO2+ reaction xa kuthelekiswa ne-C76 kuboniswe kwiTheyibhile S1. Kwelinye icala, ii-metal oxides ezininzi ezifana neCeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 kunye ne-WO331, 32, 33, 34, 35, 36, 37 zisetyenzisiwe ngenxa yokwanda kokumanzi kwazo kunye nokusebenza kwe-oxygen eninzi. , 38. Umsebenzi we-catalytic wezi oxides zesinyithi kwi-VO2+/VO2+ reaction uboniswe kwiTheyibhile S2. I-WO3 isetyenzisiwe kwimisebenzi emininzi ngenxa yexabiso layo eliphantsi, uzinzo oluphezulu kwi-acidic media, kunye nomsebenzi ophezulu we-catalytic31,32,33,34,35,36,37,38. Nangona kunjalo, ukuphuculwa kwe-cathodic kinetics ngenxa ye-WO3 akunamsebenzi. Ukuphucula ukuhanjiswa kwe-WO3, isiphumo sokusebenzisa i-tungsten oxide enciphileyo (W18O49) kumsebenzi we-cathodic sivavanyiwe38. I-tungsten oxide emanzi (HWO) ayikaze ivavanywe kwizicelo ze-VRFB, nangona ibonisa umsebenzi owandisiweyo kwizicelo ze-supercapacitor ngenxa yokusasazwa kwe-cation ngokukhawuleza xa kuthelekiswa ne-WOx39,40 engamanzi. Ibhetri yesizukulwana sesithathu se-vanadium redox flow isebenzisa i-electrolyte exutyiweyo ye-acid eyenziwe yi-HCl kunye ne-H2SO4 ukuphucula ukusebenza kwebhetri kunye nokuphucula ukunyibilika kunye nokuzinza kwee-ion ze-vanadium kwi-electrolyte. Nangona kunjalo, impendulo yokuvela kwe-chlorine ebangelwa zizinambuzane iye yaba yenye yezinto ezingalunganga kwisizukulwana sesithathu, ngoko ke ukukhangela iindlela zokuthintela impendulo yovavanyo lwe-chlorine kuye kwaba yinto ephambili kumaqela aliqela ophando.
Apha, uvavanyo lwe-VO2+/VO2+ lwenziwe kwii-composites ze-HWO/C76 ezifakwe kwii-electrodes ze-carbon cloth ukuze kufunyanwe ibhalansi phakathi kokuqhuba kombane kwee-composites kunye ne-redox kinetics yomphezulu we-electrode ngelixa kucinezelwa impendulo ye-parasitic chlorine evolution. (CER). Ii-nanoparticles ze-tungsten oxide (HWO) ezifakwe ngamanzi zenziwe ngendlela elula ye-hydrothermal. Iimvavanyo zenziwe kwi-electrolyte exutyiweyo ye-acid (H2SO4/HCl) ukuze kulinganiswe isizukulwana sesithathu se-VRFB (G3) ukuze kusetyenziswe kwaye kuphandwe isiphumo se-HWO kwi-parasitic chlorine evolution reaction.
I-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 dihydrate (Na2WO4, 99%, Sigma-Aldrich) kunye ne-hydrophilic carbon cloth ELAT (Fuel Cell Store) zisetyenzisiwe kolu phononongo.
I-Hydrated tungsten oxide (HWO) yalungiswa nge-hydrothermal reaction 43 apho i-2 g yetyuwa ye-Na2WO4 yanyibilikiswa kwi-12 ml ye-H2O ukuze kunikelwe isisombululo esingenambala, emva koko i-12 ml ye-2 M HCl yongezwa nge-dropwise ukuze kunikelwe i-suspension emthubi okhanyayo. I-slurry yafakwa kwi-autoclave yentsimbi engagqwaliyo egqunywe yi-Teflon yaza yagcinwa kwi-oven kwi-180°C. kangangeeyure ezi-3 ukuze kufumaneke i-hydrothermal reaction. Intsalela yaqokelelwa ngokuhluzwa, yahlanjwa kathathu nge-ethanol namanzi, yomiswa kwi-oven kwi-70°C kangangeeyure ezi-3, yaze yaxutywa ukuze kunikelwe i-powder ye-HWO eluhlaza okwesibhakabhaka.
Ii-electrode zelaphu lekhabhoni (CCT) ezifunyenweyo (ezinganyangwanga) zisetyenziswe njengoko zinjalo okanye ziphathwe ngobushushu kwi-tube oven kwi-450°C emoyeni ngesantya sokufudumeza se-15 ºC/min kangangeeyure ezili-10 ukuze kufunyanwe ii-CC ezinyangiweyo (TCC). njengoko kuchaziwe kwinqaku elidlulileyo. I-UCC kunye ne-TCC zinqunyulwe zaba zii-electrode ezimalunga ne-1.5 cm ububanzi kunye ne-7 cm ubude. Izixokelelwano ze-C76, HWO, HWO-10% C76, HWO-30% C76 kunye ne-HWO-50% C76 zilungiselelwe ngokongeza i-20 mg .% (~2.22 mg) ye-PVDF binder kwi-~1 ml DMF kwaye zafakwa i-sonication iyure e-1 ukuphucula ukufana. I-2 mg yee-composites ze-C76, HWO kunye ne-HWO-C76 zisetyenziswe ngokulandelelana kwindawo ye-electrode esebenzayo ye-UCC emalunga ne-1.5 cm2. Zonke ii-catalysts zafakwa kwii-electrodes ze-UCC kwaye i-TCC yasetyenziselwa ukuthelekisa kuphela, njengoko umsebenzi wethu wangaphambili ubonise ukuba unyango lobushushu alufuneki. Ukumiswa kwe-impression kwafezwa ngokuxubha i-100 µl ye-suspension (umthwalo we-2 mg) ukuze kubekho isiphumo esilinganayo. Emva koko zonke ii-electrodes zomiswa kwi-oven kwi-60° C. ubusuku bonke. Ii-electrodes zilinganiswa phambili nangasemva ukuqinisekisa ukulayisha okuchanekileyo kwesitokhwe. Ukuze kubekho indawo ethile yejometri (~1.5 cm2) kwaye kuthintelwe ukunyuka kwe-vanadium electrolyte kwi-electrode ngenxa yesiphumo se-capillary, kwafakwa umaleko omncinci weparafini phezu kwezinto ezisebenzayo.
I-field emission scanning electron microscopy (FESEM, Zeiss SEM Ultra 60, 5 kV) yasetyenziswa ukujonga imo yomphezulu we-HWO. I-spectrometer ye-X-ray esasazekayo exhotyiswe nge-Feii8SEM (EDX, Zeiss Inc.) yasetyenziswa ukuzoba izinto ze-HWO-50%C76 kwii-electrodes ze-UCC. I-high resolution transmission electron microscope (HR-TEM, JOEL JEM-2100) esebenza ngevolthi ekhawulezayo ye-200 kV yasetyenziswa ukuzoba imifanekiso yee-particles ze-HWO ezinereyithi ephezulu kunye neeringi ze-diffraction. Isoftware yeCrystallography Toolbox (CrysTBox) isebenzisa umsebenzi we-ringGUI ukuhlalutya ipatheni ye-HWO ring diffraction kunye nokuthelekisa iziphumo nepatheni ye-XRD. Ulwakhiwo kunye ne-graphitization ye-UCC kunye ne-TCC zihlalutywe nge-X-ray diffraction (XRD) ngesantya se-scan se-2.4°/min ukusuka kwi-5° ukuya kwi-70° nge-Cu Kα (λ = 1.54060 Å) kusetyenziswa i-Panalytical X-ray diffractometer (Model 3600). I-XRD ibonise isakhiwo sekristale kunye nesigaba se-HWO. Isoftware ye-PANalytical X'Pert HighScore isetyenzisiwe ukufanisa ii-HWO peaks neemaphu ze-tungsten oxide ezikhoyo kwi-database45. Iziphumo ze-HWO zithelekiswe neziphumo ze-TEM. Ulwakhiwo lweekhemikhali kunye nemeko yeesampulu ze-HWO zimiselwe yi-X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific). Isoftware ye-CASA-XPS (v 2.3.15) isetyenzisiwe ekuhlukaniseni i-peak kunye nohlalutyo lwedatha. Ukufumanisa amaqela okusebenza komphezulu we-HWO kunye ne-HWO-50%C76, kwenziwa imilinganiselo kusetyenziswa i-Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, kusetyenziswa i-KBr FTIR). Iziphumo zithelekiswe neziphumo ze-XPS. Imilinganiselo ye-contact angle (KRUSS DSA25) ikwasetyenziswe ukuchaza ukumanzi kwe-electrodes.
Kuzo zonke izilinganiso ze-electrochemical, kusetyenziswe i-workstation ye-Biologic SP 300. I-cyclic voltammetry (CV) kunye ne-electrochemical impedance spectroscopy (EIS) zisetyenzisiwe ukufunda i-electrode kinetics ye-VO2+/VO2+ redox reaction kunye nefuthe le-reagent diffusion (VOSO4(VO2+)) kwisantya se-reaction. Zombini ezi ndlela zisebenzise iseli ye-electrode ezintathu ene-electrolyte concentration ye-0.1 M VOSO4 (V4+) kwi-1 M H2SO4 + 1 M HCl (umxube we-asidi). Zonke idatha ye-electrochemical eziveziweyo zilungisiwe nge-IR. I-saturated calomel electrode (SCE) kunye ne-platinum (Pt) coil zisetyenzisiwe njenge-reference kunye ne-counter electrode, ngokulandelelana. Kwi-CV, amazinga okuskena (ν) e-5, 20, kunye ne-50 mV/s asetyenziswe kwi-VO2+/VO2+ potential window ye-(0–1) V vs. SCE, emva koko ahlengahlengiswa ukuze i-SHE ibekwe kwi-plot (VSCE = 0.242 V vs. HSE). Ukuze kufundwe ukugcinwa komsebenzi we-electrode, ii-CV eziphindaphindwayo ze-cyclic zenziwe kwi-ν 5 mV/s kwi-UCC, TCC, UCC-C76, UCC-HWO, kunye ne-UCC-HWO-50% C76. Kwimilinganiselo ye-EIS, uluhlu lwemvamisa ye-VO2+/VO2+ redox reaction yayiyi-0.01-105 Hz, kwaye i-voltage perturbation kwi-open-circuit voltage (OCV) yayiyi-10 mV. Uvavanyo ngalunye luphindwe amaxesha ama-2-3 ukuqinisekisa ukuhambelana kweziphumo. Ii-heterogeneous rate constants (k0) zifunyenwe ngendlela yeNicholson46,47.
I-Hydrated tungsten oxide (HVO) yenziwe ngempumelelo ngendlela ye-hydrothermal. Umfanekiso we-SEM kumzobo 1a ubonisa ukuba i-HWO egciniweyo iqulethwe ngamaqela ee-nanoparticles ezinobukhulu obuphakathi kwe-25-50 nm.
Ipateni ye-X-ray diffraction ye-HWO ibonisa iincopho (001) kunye (002) kwi ~23.5° kunye ~47.5°, ngokulandelanayo, eziziimpawu ze-nonstoichiometric WO2.63 (W32O84) (PDF 077–0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90°), ehambelana nombala wazo oluhlaza okwesibhakabhaka ocacileyo (Umzobo 1b) 48.49. Ezinye iincopho ezimalunga ne-20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° kunye ne-52.7° zabelwe kwi-(140), (620), (350), (720), (740), (560°). ) ) kunye (970) iiplani ze-diffraction ezihambelana ne-WO2.63, ngokwahlukeneyo. Le ndlela yokwenziwa isetyenzisiwe nguSongara et al. 43 ukufumana imveliso emhlophe, eyabangelwa bubukho be-WO3(H2O)0.333. Nangona kunjalo, kulo msebenzi, ngenxa yeemeko ezahlukeneyo, imveliso eluhlaza okwesibhakabhaka-grey ifunyenwe, nto leyo 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-tungsten oxide encitshisiweyo. Uhlalutyo olulinganiselayo kusetyenziswa isoftware ye-X'Pert HighScore lubonise i-26% WO3(H2O)0.333:74% W32O84. Ekubeni i-W32O84 ine-W6+ kunye ne-W4+ (1.67:1 W6+:W4+), umxholo oqikelelweyo we-W6+ kunye ne-W4+ umalunga ne-72% W6+ kunye ne-28% W4+, ngokulandelelana. Imifanekiso ye-SEM, i-1-second XPS spectra kwinqanaba le-nucleus, imifanekiso ye-TEM, i-FTIR spectra, kunye ne-Raman spectra yamasuntswana e-C76 ziboniswe kwinqaku lethu elidlulileyo. Ngokutsho kukaKawada et al., 50,51 i-X-ray diffraction ye-C76 emva kokususwa kwe-toluene ibonise ulwakhiwo lwe-monoclinic ye-FCC.
Imifanekiso ye-SEM kumzobo 2a kunye no-b ibonisa ukuba i-HWO kunye ne-HWO-50%C76 zifakwe ngempumelelo kwi-carbon fibers ye-UCC electrode naphakathi kwayo. Iimaphu ze-EDX element ze-tungsten, i-carbon, kunye ne-oxygen kwimifanekiso ye-SEM kumzobo 2c ziboniswe kumzobo 2d-f obonisa ukuba i-tungsten kunye ne-carbon zixutywe ngokulinganayo (kubonisa ukusasazwa okufanayo) phezu komphezulu wonke we-electrode kwaye i-composite ayifakwanga ngokulinganayo ngenxa yohlobo lwendlela yokufaka.
Imifanekiso ye-SEM yee-particles ze-HWO ezifakwe kwi-(a) kunye nee-particles ze-HWO-C76 (b). Imephu ye-EDX kwi-HWO-C76 elayishwe kwi-UCC isebenzisa indawo ekumfanekiso (c) ibonisa ukusasazwa kwe-tungsten (d), i-carbon (e), kunye ne-oxygen (f) kwisampulu.
I-HR-TEM yasetyenziselwa ukubonakalisa ubukhulu obuphezulu kunye nolwazi lwekristalografi (Umfanekiso 3). I-HWO ibonisa imo ye-nanocube njengoko kubonisiwe kwiFig. 3a kwaye ngokucacileyo kwiFig. 3b. Ngokukhulisa i-nanocube ukuze kufumaneke ukwahlukana kweendawo ezikhethiweyo, umntu unokubona isakhiwo se-grating kunye ne-diffraction planes ezihlangabezana nomthetho weBragg, njengoko kubonisiwe kwiFig. 3c, eqinisekisa ubukrelekrele bezinto ezibonakalayo. Kwi-inset yeFig. 3c ibonisa umgama d 3.3 Å ohambelana ne-diffraction planes (022) kunye (620) ezifumaneka kwi-WO3(H2O)0.333 kunye ne-W32O84 phases, ngokulandelelana43,44,49. Oku kuhambelana nohlalutyo lwe-XRD oluchazwe apha ngasentla (Umfanekiso 1b) kuba umgama we-grating plane obonweyo d (Umfanekiso 3c) uhambelana nencochoyi ye-XRD enamandla kwisampulu ye-HWO. Iisampulu zesampulu nazo ziboniswe kwiFig. 3d, apho isangqa ngasinye sihambelana ne-plane eyahlukileyo. Iiplane ze-WO3(H2O)0.333 kunye ne-W32O84 zinombala omhlophe noluhlaza okwesibhakabhaka, ngokulandelelana, kwaye iincopho zazo ze-XRD ezifanayo nazo ziboniswe kwiFig. 1b. Indandatho yokuqala eboniswe kwidayagram yendandatho ihambelana nencochoyi yokuqala ephawulweyo kwipateni ye-x-ray yeplane ye-diffraction ye-(022) okanye (620). Ukusuka kwi-(022) ukuya kwi-(402), amaxabiso e-d-spacing yi-3.30, 3.17, 2.38, 1.93, kunye ne-1.69 Å, ehambelana namaxabiso e-XRD e-3.30, 3.17, 2, 45, 1.93. kunye ne-1.66 Å, elingana ne-44, 45, ngokulandelelana.
(a) Umfanekiso we-HR-TEM we-HWO, (b) ubonisa umfanekiso owandisiweyo. Imifanekiso yeenqwelo-moya ezirhangqiweyo iboniswe ku-(c), umfanekiso ongaphakathi (c) ubonisa umfanekiso owandisiweyo weenqwelo-moya kunye ne-pitch d ye-0.33 nm ehambelana neenqwelo-moya (002) kunye ne-(620). (d) Ipateni yeringi ye-HWO ebonisa iinqwelo-moya ezinxulumene ne-WO3(H2O)0.333 (emhlophe) kunye ne-W32O84 (eluhlaza okwesibhakabhaka).
Uhlalutyo lwe-XPS lwenziwe ukuze kuchongwe ikhemistri yomphezulu kunye nemeko ye-oxidation ye-tungsten (Imifanekiso S1 kunye ne-4). Uluhlu olubanzi lwe-XPS scan spectrum ye-HWO eyenziweyo luboniswe kuMfanekiso S1, olubonisa ubukho be-tungsten. I-XPS narrow-scan spectra yamanqanaba e-core ye-W 4f kunye ne-O 1s iboniswe kwiMifanekiso 4a kunye ne-b, ngokwahlukeneyo. I-spectrum ye-W 4f yahlulwe yaba zii-doublets ezimbini ze-spin-orbit ezihambelana namandla okubopha emeko ye-oxidation ye-W. kunye ne-W 4f7/2 kwi-36.6 kunye ne-34.9 eV ziimpawu zemeko ye-W4+ ye-40, ngokwahlukeneyo. )0.333. Idatha efakiweyo ibonisa ukuba iipesenti ze-athomu ze-W6+ kunye ne-W4+ ziyi-85% kunye ne-15%, ngokwahlukeneyo, ezikufutshane namaxabiso aqikelelwe kwidatha ye-XRD kujongwa umahluko phakathi kwezi ndlela zimbini. Zombini iindlela zibonelela ngolwazi lobungakanani ngokuchaneka okuphantsi, ngakumbi i-XRD. Kwakhona, ezi ndlela zimbini zihlalutya iindawo ezahlukeneyo zezinto kuba i-XRD yindlela yobuninzi ngelixa i-XPS yindlela yomphezulu esondela kwiinanometer ezimbalwa kuphela. I-spectrum ye-O1s yahlulwe yaba ziincopho ezimbini kwi-533 (22.2%) kunye ne-530.4 eV (77.8%). Eyokuqala ihambelana ne-OH, kwaye eyesibini ihambelana neebhondi zeoksijini kwi-lattice kwi-WO. Ubukho bamaqela asebenzayo e-OH buhambelana neempawu ze-hydration ze-HWO.
Uhlalutyo lwe-FTIR lwenziwe kwezi sampuli zimbini ukuze kuhlolwe ubukho bamaqela asebenzayo kunye neemolekyuli zamanzi ezidibeneyo kwisakhiwo se-HWO esimanzi. Iziphumo zibonisa ukuba isampuli ye-HWO-50% C76 kunye neziphumo ze-FT-IR HWO zibonakala zifana ngenxa yobukho be-HWO, kodwa ubunzulu beencopho buyahluka ngenxa yobungakanani obahlukeneyo besampuli esetyenzisiweyo ukulungiselela uhlalutyo (Umzobo 5a). ) I-HWO-50% C76 ibonisa ukuba zonke iincopho, ngaphandle kwencopho ye-tungsten oxide, zinxulumene ne-fullerene 24. Iinkcukacha ezineenkcukacha kumzobo 5a zibonisa ukuba zombini iisampuli zibonisa ibhendi ebanzi enamandla kakhulu kwi ~710/cm ebangelwa kukushukuma kwe-OWO kwisakhiwo se-lattice se-HWO, kunye negxalaba eliqinileyo kwi ~840/cm ebangelwa yi-WO. Kwiintshukumo zokushukumisa, ibhendi ebukhali malunga ne-1610/cm ibangelwa kukushukuma kwe-OH, ngelixa ibhendi yokufunxa ebanzi malunga ne-3400/cm ibangelwa kukushukuma kwe-OH kumaqela e-hydroxyl43. Ezi ziphumo ziyahambelana ne-XPS spectra kwiMifanekiso 4b, apho amaqela asebenzayo e-WO anokubonelela ngeendawo ezisebenzayo zempendulo ye-VO2+/VO2+.
Uhlalutyo lwe-FTIR lwe-HWO kunye ne-HWO-50% C76 (a), lubonise amaqela asebenzayo kunye nokulinganiswa kwee-engile zoqhagamshelwano (b, c).
Iqela le-OH linokukwakhuthaza i-reaction ye-VO2+/VO2+, ngelixa linyusa i-hydrophilicity ye-electrode, ngaloo ndlela likhuthaza izinga lokusasazwa kunye nokudluliselwa kwe-electron. Njengoko kubonisiwe, isampuli ye-HWO-50% C76 ibonisa incochoyi eyongezelelweyo ye-C76. Iincochoyi kwi-~2905, 2375, 1705, 1607, kunye ne-1445 cm3 zinokubekwa kwi-CH, O=C=O, C=O, C=C, kunye ne-CO ukungcangcazela kokunwebeka, ngokwahlukeneyo. Kuyaziwa ukuba amaqela asebenzayo e-oxygen C=O kunye ne-CO anokusebenza njengeziko ezisebenzayo zeempendulo ze-redox zevanadium. Ukuvavanya nokuthelekisa ukumanzi kwee-electrode ezimbini, ukulinganiswa kwe-contact angle kuthathwe njengoko kubonisiwe kwiFig. 5b,c. I-electrode ye-HWO yafunxa amaconsi amanzi ngoko nangoko, ibonisa i-superhydrophilicity ngenxa yamaqela asebenzayo e-OH akhoyo. I-HWO-50% C76 i-hydrophobic ngakumbi, ine-contact angle emalunga ne-135° emva kwemizuzwana eli-10. Nangona kunjalo, kwiimilinganiselo ze-electrochemical, i-electrode ye-HWO-50%C76 yaba manzi ngokupheleleyo ngaphantsi komzuzu omnye. Iimilinganiselo zokumanzisa ziyahambelana neziphumo ze-XPS kunye ne-FTIR, nto leyo ebonisa ukuba amaqela amaninzi e-OH kumphezulu we-HWO ayenza ibe manzi ngakumbi.
Iimpendulo ze-VO2+/VO2+ ze-HWO kunye ne-HWO-C76 nanocomposites zivavanyiwe kwaye kwakulindeleke ukuba i-HWO icinezele ukuguquka kwe-chlorine kwi-VO2+/VO2+ reaction kwi-mixed acid, kwaye i-C76 iya kuqhubeka nokukhuthaza i-VO2+/VO2+ redox reaction efunekayo. %, 30%, kunye ne-50% C76 kwi-HWO suspensions kunye ne-CCC efakwe kwi-electrodes enomthwalo opheleleyo omalunga ne-2 mg/cm2.
Njengoko kubonisiwe kumzobo 6, i-kinetics ye-VO2+/VO2+ reaction kumphezulu we-electrode ihlolwe yi-CV kwi-electrolyte exutyiweyo ye-acid. I-currents iboniswe njenge-I/Ipa ukuze kube lula ukuthelekisa i-ΔEp kunye ne-Ipa/Ipc kwii-catalysts ezahlukeneyo ngqo kwigrafu. Idatha yendawo yangoku iboniswe kuMfanekiso 2S. Kumzobo 6a ibonisa ukuba i-HWO inyusa kancinci izinga lokudluliselwa kwe-electron ye-VO2+/VO2+ redox reaction kumphezulu we-electrode kwaye icinezela impendulo ye-parasitic chlorine evolution. Nangona kunjalo, i-C76 inyusa kakhulu izinga lokudluliselwa kwe-electron kwaye ivuselela impendulo ye-chlorine evolution. Ke ngoko, i-composite eyenziwe ngokuchanekileyo ye-HWO kunye ne-C76 kulindeleke ukuba ibe nomsebenzi ongcono kunye nekhono elikhulu lokuthintela impendulo ye-chlorine evolution. Kufunyenwe ukuba emva kokunyusa umxholo we-C76, umsebenzi we-electrochemical wee-electrodes uphucukile, njengoko kungqinwa kukwehla kwe-ΔEp kunye nokwanda komlinganiselo we-Ipa/Ipc (Itheyibhile S3). Oku kuqinisekiswe nangamaxabiso e-RCT athathwe kwi-Nyquist plot kwiFig. 6d (Itheyibhile S3), afunyenwe ehla ngokonyuka komxholo we-C76. Ezi ziphumo zikwahambelana nophando lukaLi, apho ukongezwa kwe-mesoporous carbon kwi-mesoporous WO3 kubonise ukuphucula i-kinetics yokudluliselwa kwetshaja kwi-VO2+/VO2+35. Oku kubonisa ukuba impendulo ethe ngqo inokuxhomekeka ngakumbi kwi-electrode conductivity (C=C bond) 18, 24, 35, 36, 37. Oku kusenokubangelwa lutshintsho kwi-coordination geometry phakathi kwe-[VO(H2O)5]2+ kunye ne-[VO2(H2O)4]+, i-C76 inciphisa i-reaction overvoltage ngokunciphisa amandla ezicubu. Nangona kunjalo, oku kusenokungenzeki ngee-electrodes ze-HWO.
(a) Ukuziphatha kwe-cyclic voltammetric (ν = 5 mV/s) yempendulo ye-VO2+/VO2+ ye-UCC kunye ne-HWO-C76 composites enemilinganiselo eyahlukeneyo ye-HWO:C76 kwi-0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte. (b) Indlela yeRandles-Sevchik kunye (c) Nicholson VO2+/VO2+ yokuvavanya ukusebenza kakuhle kokusasazwa kunye nokufumana amaxabiso e-k0(d).
I-HWO-50% C76 ayizange ibonakalise nje kuphela umsebenzi ofanayo we-electrocatalytic njenge-C76 kwi-VO2+/VO2+, kodwa, okunomdla ngakumbi, yacinezela ukuguquka kwe-chlorine xa kuthelekiswa ne-C76, njengoko kubonisiwe kwiFig. 6a, kwaye ikwabonisa i-Smaller Semicircle kwiFig. 6d (i-RCT esezantsi). I-C76 ibonise i-Ipa/Ipc ebonakalayo ephezulu kune-HWO-50% C76 (Itheyibhile S3), kungekhona ngenxa yokuphuculwa kokuguquguquka kwempendulo, kodwa ngenxa yokugqithisa okuphezulu kwe-chlorine reduction reaction ne-SHE kwi-1.2 V. Ukusebenza okungcono kwe-HWO- I-50% C76 ibangelwa yimpembelelo ye-synergistic phakathi kwe-C76 ehlawuliswe kakubi kunye nokumanzi okuphezulu kunye nokusebenza kwe-W-OH catalytic kwi-HWO. Ukukhutshwa okuncinci kwe-chlorine kuya kuphucula ukusebenza kakuhle kwe-charging yeseli epheleleyo, ngelixa i-kinetics ephuculweyo iya kuphucula ukusebenza kakuhle kwe-voltage yeseli epheleleyo.
Ngokwe-equation S1, kwi-reaction eguquguqukayo (ecothayo ngokwe-electron transfer) elawulwa yi-diffusion, i-peak current (IP) ixhomekeke kwinani lee-electron (n), indawo ye-electrode (A), i-diffusion coefficient (D), inani le-electron transfer coefficient (α) kunye nesantya sokuskena (ν). Ukuze kufundwe indlela yokuziphatha elawulwa yi-diffusion yezinto ezivavanyiweyo, ubudlelwane phakathi kwe-IP kunye ne-ν1/2 budweliswe kwaye buboniswe kwiFig. 6b. Ekubeni zonke izinto zibonisa ubudlelwane obuthe ngqo, i-reaction ilawulwa yi-diffusion. Ekubeni i-VO2+/VO2+ i-quasi-reversible, i-slope yomgca ixhomekeke kwi-diffusion coefficient kunye nexabiso le-α (i-equation S1). Ekubeni i-diffusion coefficient ingaguquki (≈ 4 × 10–6 cm2/s)52, umahluko kwi-slope yomgca ubonisa ngokuthe ngqo amaxabiso ahlukeneyo e-α, kwaye ngoko ke izinga lokudluliselwa kwe-electron kumphezulu we-electrode, eliboniswa kwi-C76 kunye ne-HWO -50% C76 I-slope ethe tyaba (izinga eliphezulu lokudluliselwa kwe-electron).
Iithambeka zaseWarburg (W) ezibalwe kwiifrikhwensi eziphantsi eziboniswe kwiTheyibhile S3 (Umzobo 6d) zinamaxabiso asondele ku-1 kuzo zonke izixhobo, nto leyo ebonisa ukusasazeka okugqibeleleyo kweentlobo ze-redox kwaye iqinisekisa ukuziphatha okuthe ngqo kwe-IP xa kuthelekiswa ne-ν1/2. I-CV ilinganiswa. Kwi-HWO-50% C76, ithambeka laseWarburg liyaphambuka ukusuka ku-1 ukuya ku-1.32, nto leyo ebonisa kungekuphela nje ukusasazeka okungapheliyo kwe-reagent (VO2+), kodwa kunye negalelo elinokwenzeka lokuziphatha okuncinci kwindlela yokuziphatha kokusasazeka ngenxa ye-electrode porosity.
Ukuhlalutya ngakumbi ukuguquguquka (isantya sokudluliselwa kwe-electron) kwe-VO2+/VO2+ redox reaction, indlela ye-Nicholson quasi-reversible reaction ikwasetyenziswa ukumisela i-standard rate constant k041.42. Oku kwenziwa kusetyenziswa i-S2 equation ukwakha i-dimensionless kinetic parameter Ψ, engumsebenzi we-ΔEp, njengomsebenzi we-ν-1/2. Itheyibhile S4 ibonisa amaxabiso e-Ψ afunyenwe kwisixhobo ngasinye se-electrode. Iziphumo (Umzobo 6c) zadweliswa ukuze kufunyanwe i-k0 × 104 cm/s ukusuka kwi-slope yeploti nganye kusetyenziswa i-Equation S3 (ebhalwe ecaleni komqolo ngamnye kwaye iboniswe kwiTheyibhile S4). I-HWO-50% C76 ifunyenwe ine-slope ephezulu (Umzobo 6c), ngoko ke ixabiso eliphezulu le-k0 yi-2.47 × 10–4 cm/s. Oku kuthetha ukuba le electrode ifikelela kwi-kinetics ekhawulezayo, ehambelana neziphumo ze-CV kunye ne-EIS kwiFig. 6a kunye no-d nakwiTheyibhile S3. Ukongeza, ixabiso le-k0 lifunyenwe nakwi-Nyquist plot (Fig. 6d) ye-Equation S4 kusetyenziswa ixabiso le-RCT (Theyibhile S3). Ezi ziphumo ze-k0 ezivela kwi-EIS zishwankathelwe kwiTheyibhile S4 kwaye zibonisa ukuba i-HWO-50% C76 ibonisa izinga eliphezulu lokudluliselwa kwe-electron ngenxa yesiphumo se-synergistic. Nangona ixabiso le-k0 lahlukile ngenxa yemvelaphi eyahlukileyo yendlela nganye, lisabonisa ulandelelwano olufanayo lobukhulu kwaye libonisa ukuhambelana.
Ukuze uqonde ngokupheleleyo i-kinetics egqwesileyo efunyenweyo, kubalulekile ukuthelekisa izixhobo ze-electrode ezifanelekileyo kunye nee-electrodes ze-UCC kunye ne-TCC ezingagqunywanga. Kwi-reaction ye-VO2+/VO2+, i-HWO-C76 ayizange ibonise kuphela i-ΔEp ephantsi kunye nokuguqulwa okungcono, kodwa ikwacinezele kakhulu i-reaction ye-chlorine evolution ye-parasitic xa ithelekiswa ne-TCC, njengoko ilinganiswe yi-current kwi-1.45 V xa ithelekiswa ne-SHE (Umzobo 7a). Ngokuphathelele ukuzinza, sicinge ukuba i-HWO-50% C76 yayizinzile ngokomzimba kuba i-catalyst yaxutywa ne-PVDF binder yaza yasetyenziswa kwii-electrodes zelaphu lekhabhoni. I-HWO-50% C76 ibonise utshintsho oluphezulu lwe-44 mV (izinga lokubola yi-0.29 mV/cycle) emva kwemijikelo eyi-150 xa ithelekiswa ne-50 mV ye-UCC (Umfanekiso 7b). Oku kusenokungabi ngumahluko omkhulu, kodwa i-kinetics yee-electrodes ze-UCC icotha kakhulu kwaye iyonakala ngokujikelezisa, ngakumbi kwii-reactions ezibuyela umva. Nangona ukutshintshwa kwe-TCC kungcono kakhulu kune-UCC, i-TCC ifunyenwe ine-peak shift enkulu ye-73 mV emva kwemijikelo eyi-150, enokuba ibangelwa sisixa esikhulu se-chlorine esenziwe kumphezulu wayo. ukuze i-catalyst inamathele kakuhle kumphezulu we-electrode. Njengoko kunokubonwa kuzo zonke ii-electrode ezivavanyiweyo, nee-electrode ezingenazo ii-catalysts ezixhaswayo zibonise amazinga ahlukeneyo okungazinzi kokujikeleza, nto leyo ebonisa ukuba utshintsho ekuhlukanisweni kwe-peak ngexesha lokujikeleza lubangelwa kukungasebenzi kwezinto ezibangelwa lutshintsho lweekhemikhali endaweni yokwahlukana kwe-catalyst. Ukongeza, ukuba isixa esikhulu see-catalyst particles besiza kwahlulwa kumphezulu we-electrode, oku kuya kubangela ukwanda okukhulu kokwahlukana kwe-peak (hayi i-44 mV kuphela), kuba i-substrate (UCC) ayisebenzi kangako kwi-VO2+/VO2+ redox reaction.
Uthelekiso lwe-CV yezinto ze-electrode ezilungileyo xa kuthelekiswa ne-UCC (a) kunye nokuzinza kwe-VO2+/VO2+ redox reaction (b). ν = 5 mV/s kuzo zonke ii-CV kwi-0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Ukwandisa ukutsala kwezoqoqosho kweteknoloji yeVRFB, ukwandisa nokuqonda i-kinetics ye-vanadium redox reactions kubalulekile ukuze kufezekiswe ukusebenza kakuhle kwamandla. Ii-composites HWO-C76 zalungiswa kwaye isiphumo sazo se-electrocatalytic kwi-reaction ye-VO2+/VO2+ safundwa. I-HWO ibonise ukuphuculwa okuncinci kwe-kinetic kwi-electrolytes ezixutyiweyo ze-acid kodwa yacinezela kakhulu ukuvela kwe-chlorine. Ii-ratios ezahlukeneyo ze-HWO:C76 zasetyenziswa ukuphucula ngakumbi i-kinetics yee-electrodes ezisekelwe kwi-HWO. Ukunyusa i-C76 ukuya kwi-HWO kuphucula i-kinetics yokudluliselwa kwe-electron ye-reaction ye-VO2+/VO2+ kwi-electrode eguquliweyo, apho i-HWO-50% C76 yeyona nto ilungileyo kuba inciphisa ukumelana nokudluliselwa kwetshaja kwaye icinezela ngakumbi i-chlorine xa kuthelekiswa ne-C76 kunye ne-TCC deposit. . Oku kungenxa yesiphumo sokusebenzisana phakathi kwamaqela asebenzayo e-C=C sp2 hybridization, i-OH kunye ne-W-OH. Izinga lokuwohloka emva kokujikeleza okuphindaphindiweyo kwe-HWO-50% C76 kufunyenwe ukuba yi-0.29 mV/cycle, ngelixa izinga lokuwohloka kwe-UCC kunye ne-TCC liyi-0.33 mV/cycle kunye ne-0.49 mV/cycle, ngokulandelanayo, okwenza ukuba ihlale izinzile kakhulu. kwi-electrolytes ze-acid ezixutyiweyo. Iziphumo eziveziweyo zichonga ngempumelelo izixhobo ze-electrode ezisebenzayo eziphezulu ze-VO2+/VO2+ reaction nge-kinetics ekhawulezayo kunye nozinzo oluphezulu. Oku kuya kunyusa i-voltage yokuphuma, ngaloo ndlela kwandisa ukusebenza kakuhle kwamandla kwe-VRFB, ngaloo ndlela kunciphisa iindleko zokuthengiswa kwayo kwixesha elizayo.
Iiseti zedatha ezisetyenzisiweyo kunye/okanye ezihlalutyiweyo kolu phando lwangoku ziyafumaneka kubabhali abafanelekileyo xa beceliwe ngokufanelekileyo.
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