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Babban farashin batirin redox mai gudana ta hanyar vanadium (VRBBs) yana iyakance yawan amfani da su. Ana buƙatar inganta motsin halayen electrochemical don ƙara ƙarfin aiki da kuzari na VRFB, ta haka rage farashin kWh na VRFB. A cikin wannan aikin, an saka nanoparticles na tungsten oxide (HWO) masu ruwa da tsaki a cikin hydrothermal, C76 da C76/HWO, a kan nanoparticles na carbon kuma an gwada su azaman electrocatalysts don amsawar redox na VO2+/VO2+. Microscopy na electron scanning emission scanning (FESEM), energy dispersive X-ray spectroscopy (EDX), high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier transform Spectroscopy (FTIR) da ma'aunin kusurwar hulɗa. An gano cewa ƙara C76 fullerenes zuwa HWO na iya inganta kinetics na lantarki ta hanyar ƙara ƙarfin lantarki da samar da ƙungiyoyin aiki masu oxidized a saman sa, ta haka yana haɓaka amsawar redox na VO2+/VO2+. Haɗin HWO/C76 (50 wt% C76) ya tabbatar da cewa shine mafi kyawun zaɓi don amsawar VO2+/VO2+ tare da ΔEp na 176 mV, yayin da zane mai carbon da ba a yi masa magani ba (UCC) shine 365 mV. Bugu da ƙari, haɗin HWO/C76 ya nuna babban tasiri mai hanawa akan amsawar juyin halittar chlorine na parasitic saboda ƙungiyar aiki ta W-OH.
Mummunan aikin ɗan adam da kuma saurin juyin juya halin masana'antu sun haifar da buƙatar wutar lantarki mai yawa, wanda ke ƙaruwa da kusan kashi 3% a kowace shekara1. Tsawon shekaru da dama, yawan amfani da man fetur a matsayin tushen makamashi ya haifar da hayakin iskar gas mai gurbata muhalli wanda ke taimakawa ga ɗumamar yanayi, gurɓatar ruwa da iska, wanda ke barazana ga dukkan yanayin halittu. Sakamakon haka, ana sa ran shigar iska mai tsabta da makamashin rana zai kai kashi 75% na jimlar wutar lantarki nan da shekarar 20501. Duk da haka, lokacin da rabon wutar lantarki daga hanyoyin da ake sabuntawa ya wuce kashi 20% na jimlar samar da wutar lantarki, hanyar sadarwa ta zama mara tabbas.
Daga cikin dukkan tsarin adana makamashi kamar batirin vanadium redox flow2 na hybrid, batirin redox flow na all-vanadium (VRFB) ya bunƙasa cikin sauri saboda fa'idodi da yawa kuma ana ɗaukarsa mafi kyawun mafita don adana makamashi na dogon lokaci (kimanin shekaru 30).) Zaɓuɓɓuka tare da makamashin da ake sabuntawa4. Wannan ya faru ne saboda rabuwar yawan wutar lantarki da makamashi, amsawar sauri, tsawon rayuwar sabis, da ƙarancin farashin shekara-shekara na $65/kWh idan aka kwatanta da $93-140/kWh don batirin Li-ion da lead-acid da dala 279-420 na Amurka a kowace kWh. baturi bi da bi 4.
Duk da haka, babban kasuwancinsu har yanzu yana da iyaka saboda yawan kuɗin tsarin da suke kashewa, musamman saboda tarin ƙwayoyin halitta4,5. Saboda haka, inganta aikin tarin tari ta hanyar ƙara yawan motsin halayen rabin abubuwa guda biyu na iya rage girman tarin tari don haka rage farashi. Saboda haka, saurin canja wurin electron zuwa saman electrode ya zama dole, wanda ya dogara da ƙira, abun da ke ciki da tsarin electrode kuma yana buƙatar ingantaccen haɓakawa sosai6. Duk da kyakkyawan kwanciyar hankali na sinadarai da sinadarai da kuma kyakkyawan tasirin lantarki na carbon electrodes, motsin su da ba a yi ba yana da jinkiri saboda rashin ƙungiyoyin aiki na oxygen da hydrophilicity7,8. Saboda haka, ana haɗa nau'ikan electrocatalysts daban-daban tare da electrodes masu tushen carbon, musamman carbon nanostructures da metal oxides, don inganta motsin lantarki na electrodes guda biyu, ta haka ne ƙara yawan motsin lantarki na VRFB electrode.
Baya ga aikin da muka yi a baya kan C76, mun fara bayar da rahoton kyakkyawan aikin electrocatalytic na wannan fullerene don VO2+/VO2+, canja wurin caji, idan aka kwatanta da zane mai zafi da ba a yi masa magani ba. An rage juriya da kashi 99.5% da 97%. An nuna aikin catalytic na kayan carbon don amsawar VO2+/VO2+ idan aka kwatanta da C76 a cikin Tebur S1. A gefe guda kuma, an yi amfani da oxides na ƙarfe da yawa kamar CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 da WO331, 32, 33, 34, 35, 36, 37 saboda ƙaruwar danshi da yawan aikin iskar oxygen. , 38. An gabatar da aikin catalytic na waɗannan oxides na ƙarfe a cikin amsawar VO2+/VO2+ a cikin Tebur S2. An yi amfani da WO3 a cikin ayyuka masu yawa saboda ƙarancin farashi, kwanciyar hankali mai yawa a cikin kafofin watsa labarai na acidic, da kuma yawan aikin catalytic31,32,33,34,35,36,37,38. Duk da haka, ingantawar motsin cathodic saboda WO3 ba shi da mahimmanci. Don inganta watsa wutar lantarki na WO3, an gwada tasirin amfani da ragewar tungsten oxide (W18O49) akan aikin cathodic38. Ba a taɓa gwada tungsten oxide mai ruwa (HWO) a cikin aikace-aikacen VRFB ba, kodayake yana nuna ƙaruwar aiki a cikin aikace-aikacen supercapacitor saboda saurin watsawar cation idan aka kwatanta da WOx39,40 mai ruwa. Batirin vanadium redox na ƙarni na uku yana amfani da gaurayen acid electrolyte wanda ya ƙunshi HCl da H2SO4 don inganta aikin baturi da inganta narkewa da kwanciyar hankali na ions na vanadium a cikin electrolyte. Duk da haka, amsawar juyin halittar chlorine mai kama da parasites ya zama ɗaya daga cikin rashin amfanin ƙarni na uku, don haka neman hanyoyin hana amsawar kimanta chlorine ya zama abin da ƙungiyoyin bincike da dama suka mayar da hankali a kai.
A nan, an gudanar da gwaje-gwajen amsawar VO2+/VO2+ akan mahaɗan HWO/C76 da aka ajiye a kan na'urorin lantarki na zane na carbon domin samun daidaito tsakanin ikon wutar lantarki na mahaɗan da kuma redox kinetics na saman electrode yayin da ake danne juyin halittar chlorine na parasitic. response (CER). An haɗa nanoparticles na tungsten oxide (HWO) mai ruwa-ruwa ta hanyar hanyar hydrothermal mai sauƙi. An gudanar da gwaje-gwajen a cikin wani gaurayen acid electrolyte (H2SO4/HCl) don kwaikwayon ƙarni na uku na VRFB (G3) don aiki da kuma bincika tasirin HWO akan amsawar juyin halittar chlorine na parasitic.
An yi amfani da sinadarin sulfate na Vanadium (IV) (VOSO4, 99.9%, Alfa-Aeser), sinadarin sulfuric (H2SO4), sinadarin hydrochloric (HCl), dimethylformamide (DMF, Sigma-Aldrich), sinadarin polyvinylidene fluoride (PVDF, Sigma)-Aldrich), sodium Tungsten oxide dihydrate (Na2WO4, 99%, Sigma-Aldrich) da kuma zane mai kama da carbon ELAT (Shagon Man Fetur).
An shirya sinadarin tungsten oxide mai ruwa (HWO) ta hanyar hydrothermal reaction 43, inda aka narkar da gram 2 na gishirin Na2WO4 a cikin 12 ml na H2O don ba da ruwan magani mara launi, sannan aka ƙara 12 ml na HCl 2 M don ba da ruwan rawaya mai haske. An sanya slurry ɗin a cikin autoclave mai rufi da bakin karfe na Teflon kuma aka ajiye a cikin tanda a 180 ° C. na tsawon awanni 3 don amsawar hydrothermal. An tattara ragowar ta hanyar tacewa, an wanke sau 3 da ethanol da ruwa, an busar da shi a cikin tanda a 70 ° C na tsawon awanni 3, sannan aka juya shi don ba da foda HWO mai launin shuɗi-toka.
An yi amfani da na'urorin lantarki na zane-zanen carbon (CCT) da aka samu (ba a yi musu magani ba) kamar yadda ake yi ko kuma an yi musu magani a cikin tanda mai zafi a 450°C a cikin iska tare da saurin dumama na 15 ºC/min na tsawon awanni 10 don samun CCs da aka yi musu magani (TCC). kamar yadda aka bayyana a cikin labarin da ya gabata24. An yanke UCC da TCC zuwa electrodes kimanin faɗin cm 1.5 da tsawon cm 7. An shirya dakatarwar C76, HWO, HWO-10% C76, HWO-30% C76 da HWO-50% C76 ta hanyar ƙara 20 mg .% (~2.22 mg) na PVDF binder zuwa ~1 ml DMF kuma an sonicated na tsawon awa 1 don inganta daidaito. An shafa 2 mg na C76, HWO da HWO-C76 composite a jere zuwa yankin lantarki mai aiki na UCC na kimanin cm 1.5. An ɗora dukkan abubuwan ƙarfafawa a kan na'urorin lantarki na UCC kuma an yi amfani da TCC don kwatantawa kawai, kamar yadda aikinmu na baya ya nuna cewa ba a buƙatar maganin zafi24. An cimma daidaiton ra'ayi ta hanyar goge 100 µl na dakatarwar (nauyin 2 mg) don samun daidaito. Sannan an busar da dukkan na'urorin lantarki a cikin tanda a 60°C. cikin dare ɗaya. Ana auna na'urorin lantarki gaba da baya don tabbatar da daidaiton nauyin kaya. Domin samun wani yanki na geometric (~1.5 cm2) da kuma hana haɓakar vanadium electrolyte zuwa na'urar lantarki saboda tasirin capillary, an shafa siririn paraffin a kan kayan aiki.
An yi amfani da na'urar daukar hoton lantarki ta na'urar daukar hoton fitar da iskar lantarki (FESEM, Zeiss SEM Ultra 60, 5 kV) don lura da yanayin saman HWO. An yi amfani da na'urar daukar hoton X-ray mai watsa makamashi wacce aka sanya mata Feii8SEM (EDX, Zeiss Inc.) don zana abubuwan HWO-50%C76 akan na'urorin lantarki na UCC. An yi amfani da na'urar daukar hoton lantarki mai daukar hoto mai daukar hoto mai daukar hoto mai daukar hoto mai daukar hoto (HR-TEM, JOEL JEM-2100) wacce ke aiki a karfin wutar lantarki mai sauri na 200 kV don daukar hotunan barbashi masu girman gaske da zoben diffraction. Manhajar Kayan Aikin Crystallography (CrysTBox) tana amfani da aikin ringGUI don nazarin tsarin diffraction na zobe na HWO da kuma kwatanta sakamakon da tsarin XRD. An yi nazarin tsarin da zane-zanen UCC da TCC ta hanyar X-ray diffraction (XRD) a ƙimar scan na 2.4°/min daga 5° zuwa 70° tare da Cu Kα (λ = 1.54060 Å) ta amfani da na'urar auna hasken X-ray ta Panalytical (Model 3600). XRD ya nuna tsarin lu'ulu'u da matakin HWO. An yi amfani da manhajar PANAlytical X'Pert HighScore don daidaita kololuwar HWO zuwa taswirar tungsten oxide da ke cikin rumbun adana bayanai45. An kwatanta sakamakon HWO da sakamakon TEM. An tantance sinadaran da yanayin samfuran HWO ta hanyar amfani da na'urar daukar hoton X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific). An yi amfani da manhajar CASA-XPS (v 2.3.15) don rage girman kololuwar da nazarin bayanai. Domin tantance ƙungiyoyin aikin saman HWO da HWO-50%C76, an yi ma'auni ta amfani da na'urar auna haske ta Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, ta amfani da KBr FTIR). An kwatanta sakamakon da sakamakon XPS. An kuma yi amfani da ma'aunin kusurwar hulɗa (KRUSS DSA25) don kwatanta ƙarfin danshi na lantarki.
Ga dukkan ma'aunin lantarki, an yi amfani da wurin aiki na Biologic SP 300. An yi amfani da cyclic voltammetry (CV) da electrochemical impedance spectroscopy (EIS) don nazarin motsin lantarki na VO2+/VO2+ redox reaction da tasirin yaduwar reagent (VOSO4(VO2+)) akan ƙimar amsawa. Duk hanyoyin biyu sun yi amfani da ƙwayar lantarki mai nau'in electrode uku tare da yawan electrolyte na 0.1 M VOSO4 (V4+) a cikin 1 M H2SO4 + 1 M HCl (cakuda acid). Duk bayanan electrochemical da aka gabatar an gyara su. An yi amfani da cikakken calomel electrode (SCE) da platinum (Pt) coil a matsayin electrode na tunani da na'urar counter, bi da bi. Don CV, an yi amfani da ƙimar scan (ν) na 5, 20, da 50 mV/s zuwa taga mai yuwuwar VO2+/VO2+ don (0–1) V vs. SCE, sannan aka daidaita shi don SHE ya zana (VSCE = 0.242 V vs. HSE). Don nazarin riƙe aikin lantarki, an yi maimaita CVs na zagaye a ν 5 mV/s don UCC, TCC, UCC-C76, UCC-HWO, da UCC-HWO-50% C76. Don ma'aunin EIS, kewayon mitar amsawar redox na VO2+/VO2+ shine 0.01-105 Hz, kuma rikicewar wutar lantarki a wutar lantarki ta buɗe (OCV) shine 10 mV. An maimaita kowace gwaji sau 2-3 don tabbatar da daidaiton sakamakon. An sami daidaitattun ƙimar iri-iri (k0) ta hanyar hanyar Nicholson46,47.
An yi nasarar haɗa sinadarin tungsten oxide (HVO) ta hanyar amfani da hanyar hydrothermal. Hoton SEM a cikin hoto na 1a ya nuna cewa HWO da aka ajiye ya ƙunshi tarin ƙwayoyin nanoparticles masu girma dabam dabam a cikin kewayon 25-50 nm.
Tsarin watsa hasken X-ray na HWO yana nuna kololuwa (001) da (002) a ~23.5° da ~47.5°, bi da bi, waɗanda ke da alaƙa da WO2.63 mara tsayi (W32O84) (PDF 077–0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90°), wanda ya yi daidai da launin shuɗi mai haske (Hoto na 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 planes orthogonal zuwa WO2.63, bi da bi. Songara da abokan aikinsa 43 sun yi amfani da wannan hanyar roba don samun farin samfuri, wanda aka danganta shi da kasancewar WO3(H2O)0.333. Duk da haka, a cikin wannan aikin, saboda yanayi daban-daban, an sami samfurin shuɗi-launin toka, wanda ke 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°) da kuma rage nau'in tungsten oxide. Nazarin Semiquantitative ta amfani da software na X'Pert HighScore ya nuna 26% WO3(H2O)0.333:74% W32O84. Tunda W32O84 ya ƙunshi W6+ da W4+ (1.67:1 W6+:W4+), an kiyasta yawan abubuwan da ke cikin W6+ da W4+ kusan kashi 72% na W6+ da 28% na W4+, bi da bi. An gabatar da hotunan SEM, siginar XPS ta daƙiƙa 1 a matakin tsakiya, hotunan TEM, siginar FTIR, da siginar Raman na ƙwayoyin C76 a cikin labarinmu na baya. A cewar Kawada et al.,50,51 Rarraba X-ray na C76 bayan cire toluene ya nuna tsarin monoclinic na FCC.
Hotunan SEM a cikin hoto na 2a da b sun nuna cewa an saka HWO da HWO-50%C76 cikin nasara a kan da kuma tsakanin zaruruwan carbon na lantarkin UCC. Taswirorin abubuwan EDX na tungsten, carbon, da oxygen akan hotunan SEM a cikin hoto na 2c an nuna su a cikin hoto na 2d-f wanda ke nuna cewa tungsten da carbon sun haɗu daidai gwargwado (suna nuna irin wannan rarrabawa) a kan dukkan saman lantarki kuma ba a saka haɗin ba daidai gwargwado saboda yanayin hanyar ajiyewa.
Hotunan SEM na barbashin HWO da aka ajiye (a) da barbashin HWO-C76 (b). Taswirar EDX akan HWO-C76 da aka ɗora akan UCC ta amfani da yankin da ke cikin hoton (c) yana nuna rarrabawar tungsten (d), carbon (e), da oxygen (f) a cikin samfurin.
An yi amfani da HR-TEM don ɗaukar hotunan girma da bayanai na lu'ulu'u (Hoto na 3). HWO yana nuna yanayin nanocube kamar yadda aka nuna a Hoto na 3a kuma a bayyane yake a Hoto na 3b. Ta hanyar ƙara girman nanocube don rarrabawa na wurare da aka zaɓa, mutum zai iya hango tsarin grating da kuma matakan diffraction waɗanda suka cika dokar Bragg, kamar yadda aka nuna a Hoto na 3c, wanda ke tabbatar da lu'ulu'u na kayan. A cikin shigarwar Hoto na 3c yana nuna nisan d 3.3 Å wanda ya dace da jiragen diffraction (022) da (620) da aka samu a cikin matakan WO3(H2O)0.333 da W32O84, bi da bi43,44,49. Wannan ya yi daidai da nazarin XRD da aka bayyana a sama (Hoto na 1b) tunda nisan jirgin grating da aka lura d (Hoto na 3c) ya yi daidai da mafi ƙarfin kololuwar XRD a cikin samfurin HWO. Hakanan an nuna zoben samfurin a cikin Hoto na 3d, inda kowane zobe ya yi daidai da wani jirgin daban. Jijiyoyin WO3(H2O)0.333 da W32O84 suna da launin fari da shuɗi, bi da bi, kuma an nuna kololuwar XRD ɗinsu masu dacewa a cikin Hoto na 1b. Zoben farko da aka nuna a cikin zane-zanen zobe ya yi daidai da kololuwar farko da aka yiwa alama a cikin tsarin x-ray na jirgin diffraction (022) ko (620). Daga zoben (022) zuwa (402), ƙimar tazara tsakanin d 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 yayi daidai da 44, 45, bi da bi.
(a) Hoton HR-TEM na HWO, (b) yana nuna hoton da aka faɗaɗa. Hotunan jiragen saman raga an nuna su a cikin (c), inset (c) yana nuna hoton da aka faɗaɗa na jiragen da kuma digo na 0.33 nm wanda ya dace da jiragen (002) da (620). (d) Tsarin zoben HWO wanda ke nuna jiragen da ke da alaƙa da WO3(H2O)0.333 (fari) da W32O84 (shuɗi).
An gudanar da nazarin XPS don tantance sinadaran saman da yanayin iskar shaka na tungsten (Hotunan S1 da 4). An nuna nau'in binciken XPS mai faɗi na HWO da aka haɗa a cikin Hoto na S1, yana nuna kasancewar tungsten. An nuna nau'in XPS mai kunkuntar-scan na matakan tsakiya na W 4f da O 1s a cikin Hoto na 4a da b, bi da bi. Tsarin W 4f ya rabu zuwa nau'i biyu na juyawa-zuwa ... Haka kuma, waɗannan hanyoyi guda biyu suna nazarin sassa daban-daban na kayan saboda XRD hanya ce mai yawa yayin da XPS hanya ce ta saman da ke kusantar 'yan nanometers kaɗan. An raba bakan O1s zuwa kololuwa biyu a 533 (22.2%) da 530.4 eV (77.8%). Na farko ya yi daidai da OH, na biyu kuma ya yi daidai da haɗin iskar oxygen a cikin raga a cikin WO. Kasancewar ƙungiyoyin aiki na OH ya yi daidai da halayen ruwa na HWO.
An kuma gudanar da bincike na FTIR akan waɗannan samfuran guda biyu don bincika kasancewar ƙungiyoyin aiki da daidaita ƙwayoyin ruwa a cikin tsarin HWO mai ruwa. Sakamakon ya nuna cewa samfurin HWO-50% C76 da sakamakon FT-IR HWO sun bayyana iri ɗaya saboda kasancewar HWO, amma ƙarfin kololuwar ya bambanta saboda bambancin adadin samfurin da aka yi amfani da shi wajen shirye-shiryen bincike (Hoto na 5a). ) HWO-50% C76 ya nuna cewa duk kololuwar, banda kololuwar tungsten oxide, suna da alaƙa da fullerene 24. Cikakkun bayanai a cikin hoto na 5a sun nuna cewa duka samfuran suna nuna babban band mai faɗi sosai a ~710/cm wanda aka danganta da juyawar OWO a cikin tsarin lattice na HWO, tare da kafada mai ƙarfi a ~840/cm wanda aka danganta da WO. Don girgizar shimfiɗa, an danganta band mai kaifi a kusan 1610/cm da girgizar lanƙwasa ta OH, yayin da band mai faɗi a kusan 3400/cm ana danganta shi da girgizar OH a cikin ƙungiyoyin hydroxyl43. Waɗannan sakamakon sun yi daidai da siginar XPS a cikin Fig. 4b, inda ƙungiyoyin aiki na WO za su iya samar da shafuka masu aiki don amsawar VO2+/VO2+.
Binciken FTIR na HWO da HWO-50% C76 (a), ya nuna ƙungiyoyin aiki da ma'aunin kusurwar hulɗa (b, c).
Ƙungiyar OH kuma za ta iya haɓaka amsawar VO2+/VO2+, yayin da take ƙara yawan hydrophilicity na electrode, ta haka za ta haɓaka saurin yaɗuwa da canja wurin electron. Kamar yadda aka nuna, samfurin HWO-50% C76 yana nuna ƙarin kololuwa ga C76. Ana iya sanya kololuwa a ~2905, 2375, 1705, 1607, da 1445 cm3 zuwa ga girgizar CH, O=C=O, C=O, C=C, da CO, bi da bi. An san cewa ƙungiyoyin aikin oxygen C=O da CO na iya zama cibiyoyin aiki don halayen redox na vanadium. Don gwada da kwatanta ƙarfin danshi na electrodes guda biyu, an ɗauki ma'aunin kusurwar hulɗa kamar yadda aka nuna a Hoto na 5b,c. Elektr ɗin HWO nan da nan ya sha digo na ruwa, yana nuna superhydrophilicity saboda ƙungiyoyin aikin OH da ake da su. HWO-50% C76 ya fi hydrophobic, tare da kusurwar hulɗa na kimanin 135° bayan daƙiƙa 10. Duk da haka, a ma'aunin lantarki, electrode na HWO-50%C76 ya jike gaba ɗaya cikin ƙasa da minti ɗaya. Ma'aunin danshi ya yi daidai da sakamakon XPS da FTIR, yana nuna cewa ƙarin rukunin OH akan saman HWO yana sa ya fi hydrophilic.
An gwada halayen VO2+/VO2+ na HWO da HWO-C76 na nanocomposites kuma an yi tsammanin HWO zai danne juyin halittar chlorine a cikin amsawar VO2+/VO2+ a cikin cakuda acid, kuma C76 zai ƙara haɓaka amsawar VO2+/VO2+ redox da ake so. %, 30%, da 50% C76 a cikin dakatarwar HWO da CCC da aka sanya a kan electrodes tare da jimlar nauyin kusan 2 mg/cm2.
Kamar yadda aka nuna a cikin hoto na 6, an duba kinetics na amsawar VO2+/VO2+ akan saman electrode ta hanyar CV a cikin wani gaurayen electrolyte na acidic. An nuna kwararar a matsayin I/Ipa don sauƙin kwatanta ΔEp da Ipa/Ipc don masu haɓaka daban-daban kai tsaye akan jadawalin. Bayanan sashin yanki na yanzu an nuna su a cikin Hoto na 2S. A kan hoto na 6a ya nuna cewa HWO ya ɗan ƙara yawan canja wurin electron na amsawar redox na VO2+/VO2+ akan saman electrode kuma yana danne amsawar juyin halittar chlorine na parasitic. Duk da haka, C76 yana ƙara yawan canja wurin electron sosai kuma yana haɓaka amsawar juyin halittar chlorine. Saboda haka, ana sa ran haɗin HWO da C76 da aka tsara daidai zai sami mafi kyawun aiki da mafi girman ikon hana amsawar juyin halittar chlorine. An gano cewa bayan ƙara yawan C76, aikin electrochemical na electrodes ya inganta, kamar yadda aka nuna ta hanyar raguwar ΔEp da ƙaruwa a cikin rabon Ipa/Ipc (Tebur S3). An kuma tabbatar da wannan ta hanyar ƙimar RCT da aka ciro daga shirin Nyquist a cikin Hoto na 6d (Tebur S3), wanda aka gano ya ragu tare da ƙaruwar abun ciki na C76. Waɗannan sakamakon sun kuma yi daidai da binciken Li, inda ƙarin carbon mesoporous 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 ne akan ƙarfin lantarki (C=C bond) 18, 24, 35, 36, 37. Wannan kuma yana iya kasancewa saboda canji a cikin yanayin daidaitawa tsakanin [VO(H2O)5]2+ da [VO2(H2O)4]+, C76 yana rage yawan ƙarfin amsawa ta hanyar rage kuzarin nama. Duk da haka, wannan bazai yiwu ba tare da electrodes na HWO.
(a) Halayyar voltammetric mai zagaye (ν = 5 mV/s) na amsawar VO2+/VO2+ na mahaɗan UCC da HWO-C76 tare da rabo daban-daban na HWO:C76 a cikin electrolyte na 0.1 M VOSO4/1 M H2SO4 + 1 M HCl. (b) Randles-Sevchik da (c) Hanyar Nicholson VO2+/VO2+ don kimanta ingancin yaɗuwa da samun ƙimar k0(d).
Ba wai kawai HWO-50% C76 ya nuna kusan irin aikin electrocatalytic kamar C76 don amsawar VO2+/VO2+ ba, amma, abin sha'awa, ya kuma hana juyin halittar chlorine idan aka kwatanta da C76, kamar yadda aka nuna a Hoto na 6a, kuma ya nuna ƙaramin Semicircle a cikin Hoto na 6d (ƙaramin RCT). C76 ya nuna mafi girman Ipa/Ipc fiye da HWO-50% C76 (Table S3), ba saboda ingantaccen juyar da martani ba, amma saboda kololuwar haɗuwar amsawar rage chlorine tare da SHE a 1.2 V. Mafi kyawun aikin HWO- An danganta 50% C76 da tasirin haɗin gwiwa tsakanin C76 mai caji mai ƙarfi da kuma babban aikin danshi da W-OH ke yi akan HWO. Ƙarancin fitar da chlorine zai inganta ingancin caji na cikakken tantanin halitta, yayin da ingantattun motsi zai inganta ingancin ƙarfin wutar lantarki na cikakken tantanin halitta.
A bisa ga lissafin S1, don amsawar juyawar lantarki mai juyawa (mai saurin juyawa) wanda aka sarrafa ta hanyar watsawa, matsakaicin wutar lantarki (IP) ya dogara da adadin electrons (n), yankin electrode (A), ma'aunin watsawa (D), adadin ma'aunin canja wurin electrons (α) da saurin dubawa (ν). Domin nazarin halayen watsawa da kayan da aka gwada, an zana alaƙar da ke tsakanin IP da ν1/2 kuma an gabatar da ita a cikin Hoto na 6b. Tunda duk kayan suna nuna alaƙar layi, ana sarrafa amsawar ta hanyar watsawa. Tunda amsawar VO2+/VO2+ tana da sauƙin juyawa, gangaren layin ya dogara da ma'aunin watsawa da ƙimar α (daidaitawa S1). Tunda ma'aunin yaɗuwa yana da daidaito (≈ 4 × 10–6 cm2/s)52, bambancin da ke cikin gangaren layin yana nuna ƙimar α daban-daban kai tsaye, don haka ƙimar canja wurin lantarki akan saman lantarki, wanda aka nuna don C76 da HWO -50% C76 Tsauni mafi tsayi (mafi girman ƙimar canja wurin lantarki).
Gadar Warburg (W) da aka ƙididdige don ƙananan mitoci da aka nuna a cikin Jadawali S3 (Hoto na 6d) tana da ƙima kusa da 1 ga duk kayan aiki, suna nuna cikakken yaɗuwar nau'in redox kuma suna tabbatar da halayen layi na IP idan aka kwatanta da ν1/2. An auna CV. Ga HWO-50% C76, gangaren Warburg ya karkata daga 1 zuwa 1.32, yana nuna ba kawai yaɗuwar reagent mara iyaka ba (VO2+), har ma da yiwuwar gudummawar halayen siriri ga halayen yaɗuwa saboda porosity na lantarki.
Don ƙarin nazarin juyawa (ƙimar canja wurin lantarki) na amsawar redox VO2+/VO2+, an kuma yi amfani da hanyar amsawar Nicholson mai juyawa don ƙayyade daidaitaccen ƙimar k041.42. Ana yin wannan ta amfani da lissafin S2 don gina sigar motsi mara girma Ψ, wanda aikin ΔEp ne, a matsayin aikin ν-1/2. Tebur S4 yana nuna ƙimar Ψ da aka samu don kowane kayan lantarki. An zana sakamakon (Hoto na 6c) don samun k0 × 104 cm/s daga gangaren kowane yanki ta amfani da Lissafi S3 (an rubuta kusa da kowane layi kuma an gabatar da shi a Tebur S4). An gano HWO-50% C76 yana da mafi girman gangara (Hoto na 6c), don haka matsakaicin ƙimar k0 shine 2.47 × 10–4 cm/s. Wannan yana nufin cewa wannan lantarki yana cimma mafi sauri motsi, wanda ya yi daidai da sakamakon CV da EIS a cikin Hoto na 6a da d da kuma a cikin Tebur S3. Bugu da ƙari, an kuma samo ƙimar k0 daga taswirar Nyquist (Hoto na 6d) na Lissafin S4 ta amfani da ƙimar RCT (Tebur S3). Waɗannan sakamakon k0 daga EIS an taƙaita su a cikin Tebur S4 kuma sun nuna cewa HWO-50% C76 yana nuna mafi girman ƙimar canja wurin lantarki saboda tasirin haɗin gwiwa. Ko da yake ƙimar k0 ta bambanta saboda asalin kowace hanya daban-daban, har yanzu suna nuna tsari iri ɗaya na girma kuma suna nuna daidaito.
Domin fahimtar kyawawan motsin da aka samu, yana da mahimmanci a kwatanta kayan lantarki mafi kyau tare da electrodes UCC da TCC marasa rufi. Don amsawar VO2+/VO2+, HWO-C76 ba wai kawai ya nuna mafi ƙarancin ΔEp da mafi kyawun juyi ba, har ma ya danne tasirin juyin halittar chlorine na parasitic idan aka kwatanta da TCC, kamar yadda aka auna ta hanyar wutar lantarki a 1.45 V dangane da SHE (Hoto na 7a). Dangane da kwanciyar hankali, mun ɗauka cewa HWO-50% C76 yana da kwanciyar hankali a zahiri saboda an haɗa mai haɓaka da maƙallin PVDF sannan aka shafa shi a kan electrodes ɗin zane na carbon. HWO-50% C76 ya nuna canjin kololuwar 44 mV (ƙimar lalacewa 0.29 mV/zagaye) bayan zagayawa 150 idan aka kwatanta da 50 mV ga UCC (Hoto na 7b). Wannan bazai zama babban bambanci ba, amma motsin lantarki na electrodes na UCC yana da jinkiri sosai kuma yana raguwa tare da zagayawa, musamman don amsawar baya. Duk da cewa juyewar TCC ta fi ta UCC kyau, an gano cewa TCC tana da babban canjin kololuwar 73 mV bayan zagayowar 150, wanda wataƙila ya faru ne saboda yawan sinadarin chlorine da aka samar a samanta. don haka mai kara kuzarin ya manne da kyau a saman electrode. Kamar yadda za a iya gani daga duk electrodes da aka gwada, har ma electrodes ba tare da masu kara kuzari ba sun nuna matakai daban-daban na rashin kwanciyar hankali na zagayowar, wanda ke nuna cewa canjin rabuwar kololuwar lokacin zagayowar ya faru ne saboda kashe kayan da canje-canjen sinadarai suka haifar maimakon rabuwar mai kara kuzari. Bugu da ƙari, idan aka raba babban adadin ƙwayoyin mai kara kuzari daga saman electrode, wannan zai haifar da ƙaruwa mai yawa a rabuwar kololuwar (ba kawai 44 mV ba), tunda substrate (UCC) ba shi da aiki sosai don amsawar redox na VO2+/VO2+.
Kwatanta CV na mafi kyawun kayan lantarki idan aka kwatanta da UCC (a) da kwanciyar hankali na VO2+/VO2+ redox reaction (b). ν = 5 mV/s ga duk CVs a cikin 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Domin ƙara jan hankalin tattalin arziki na fasahar VRFB, faɗaɗawa da fahimtar motsin halayen vanadium redox yana da mahimmanci don cimma ingantaccen amfani da makamashi. An shirya abubuwan haɗin HWO-C76 kuma an yi nazarin tasirin electrocatalytic akan amsawar VO2+/VO2+. HWO ya nuna ƙarancin haɓakar motsi a cikin gaurayen electrolytes na acidic amma ya danne juyin halittar chlorine sosai. An yi amfani da rabo daban-daban na HWO:C76 don ƙara inganta motsi na electrodes na tushen HWO. Ƙara C76 zuwa HWO yana inganta motsi na canja wurin electrons na amsawar VO2+/VO2+ akan electrode da aka gyara, wanda HWO-50% C76 shine mafi kyawun abu saboda yana rage juriyar canja wurin caji kuma yana ƙara danne chlorine idan aka kwatanta da C76 da ajiyar TCC. Wannan ya faru ne saboda tasirin haɗin gwiwa tsakanin ƙungiyoyin aiki na C=C sp2, OH da W-OH. An gano cewa yawan lalacewa bayan maimaita zagayowar HWO-50% C76 shine 0.29 mV/zagaye, yayin da ƙimar lalacewa ta UCC da TCC shine 0.33 mV/zagaye da 0.49 mV/zagaye, bi da bi, wanda hakan ya sa ya zama mai ƙarfi sosai. a cikin gaurayen electrolytes na acid. Sakamakon da aka gabatar ya yi nasarar gano kayan lantarki masu aiki don amsawar VO2+/VO2+ tare da saurin motsi da kwanciyar hankali mai ƙarfi. Wannan zai ƙara ƙarfin fitarwa, ta haka yana ƙara ingancin makamashi na VRFB, don haka rage farashin kasuwancinsa na gaba.
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