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Ọnụ ego dị oke ọnụ nke vanadium eruba-site na batrị redox (VRFBs) na-amachi iji ha eme ihe.Ịkwalite kinetics nke mmeghachi omume electrochemical dị mkpa iji mee ka ike na ike dị ike nke VRFB dịkwuo elu, si otú ahụ belata ọnụ ahịa kWh nke VRFB.N'ime ọrụ a, hydrothermally synthesized hydrated tungsten oxide (HWO) nanoparticles, C76 na C76 / HWO, na-edobere na carbon ákwà electrodes na-anwale dị ka electrocatalysts maka VO2 +/VO2+ redox mmeghachi omume.Igwe ihe nleba anya eletrọnịkị nke ikuku (FESEM), ike na-ekesa X-ray spectroscopy (EDX), microscope elektrọn nnyefe dị elu (HR-TEM), diffraction X-ray (XRD), X-ray photoelectron spectroscopy (XPS), infrared Fourier transform Spectroscopy (FTIR) na nha nkuku kọntaktị.Achọpụtara na mgbakwunye nke C76 fullerenes na HWO nwere ike imeziwanye kinetics electrode site na ịba ụba eletriki eletrik na inye otu ọrụ oxidized n'elu ya, si otú ahụ na-akwalite mmeghachi omume VO2 + / VO2 + redox.Ihe mejupụtara HWO / C76 (50 wt% C76) gosipụtara na ọ bụ nhọrọ kacha mma maka mmeghachi omume VO2 +/VO2 + na ΔEp nke 176 mV, ebe akwa carbon na-adịghị edozi (UCC) bụ 365 mV.Na mgbakwunye, ihe mejupụtara HWO / C76 gosipụtara mmetụta mgbochi dị ịrịba ama na mmeghachi omume evolushọn parasitic chlorine n'ihi otu ọrụ W-OH.
Ọrụ siri ike nke ụmụ mmadụ na mgbanwe mmepụta ihe ngwa ngwa emeela ka ọ bụrụ ihe na-adịghị akwụsị akwụsị maka ọkụ eletrik, nke na-abawanye ihe dịka 3% kwa afọ1.Ruo ọtụtụ iri afọ, iji mmanụ ọkụ eme ihe n'ọtụtụ ebe dị ka isi iyi ike emewo ka ikuku ikuku na-ekpo ọkụ na-eme ka okpomọkụ zuru ụwa ọnụ, mmiri na mmetọ ikuku, na-eyi gburugburu ebe obibi niile egwu.N'ihi ya, a na-atụ anya ntinye nke ikuku dị ọcha ma na-emegharịghachi na ike anyanwụ ga-eru 75% nke ọkụ eletrik site na 20501. Otú ọ dị, mgbe òkè nke ọkụ eletrik sitere na isi mmalite ndị a na-emegharị ọhụrụ karịrị 20% nke ọgbọ ọkụ eletrik zuru ezu, grid na-aghọ nke na-adịghị akwụsi ike.
N'ime usoro nchekwa ike niile dị ka ngwakọ vanadium redox na-agba batrị2, ihe niile-vanadium redox flow batrị (VRFB) etolitela ngwa ngwa n'ihi ọtụtụ uru ya ma na-ewere ya dị ka ihe ngwọta kachasị mma maka nchekwa ike ogologo oge (ihe dị ka afọ 30).) Nhọrọ jikọtara ya na ume ọhụrụ4.Nke a bụ n'ihi nkewa nke ike na ike ike, nzaghachi ngwa ngwa, ogologo ndụ ọrụ, na ọnụ ala dị ala kwa afọ nke $ 65 / kWh ma e jiri ya tụnyere $ 93-140 / kWh maka batrị Li-ion na lead-acid na 279-420 US dollar kwa kWh.batrị n'otu n'otu 4.
Agbanyeghị, azụmaahịa ha buru ibu ka na-amachibido ya site na ọnụ ahịa isi ụlọ ọrụ ha dị oke elu, ọkachasị n'ihi stacks cell4,5.Ya mere, imeziwanye arụmọrụ nchịkọta site n'ịbawanye kinetics nke mmeghachi omume abụọ nke ọkara nwere ike ibelata nha nchịkọta ma si otú ahụ belata ọnụ ahịa.Ya mere, ịnyefe ngwa ngwa eletrọn na elu electrode dị mkpa, nke dabere na nhazi, nhazi na nhazi nke electrode na-achọ njikarịcha nke ọma6.N'agbanyeghị ezigbo nkwụsi ike nke kemịkalụ na electrochemical na ezigbo ọkụ eletrik nke carbon electrodes, kinetics ha na-adịghị agwọ ọrịa na-ada mbà n'ihi enweghị ọrụ oxygen na hydrophilicity7,8.Ya mere, a na-ejikọta electrocatalyst dị iche iche na electrodes dabeere na carbon, karịsịa carbon nanostructures na metal oxides, iji melite kinetics nke abụọ electrodes, si otú na-amụba kinetics nke VRFB electrode.
Na mgbakwunye na ọrụ anyị gara aga na C76, anyị buru ụzọ kọwaa ọrụ electrocatalytic dị mma nke fullerene a maka VO2 + / VO2 +, nnyefe ụgwọ, ma e jiri ya tụnyere akwa carbon na-ekpo ọkụ na-adịghị edozi.Nguzogide na-ebelata site na 99.5% na 97%.Arụ ọrụ catalytic nke ihe carbon maka mmeghachi omume VO2 +/VO2 + ma e jiri ya tụnyere C76 ka egosiri na tebụl S1.N'aka nke ọzọ, ọtụtụ metal oxides dị ka CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 na WO331, 32, 33, 34, 35, 36, 37 e ji mee ihe n'ihi na ha na-amụba wettability na ukwuu oxygen ọrụ., 38. otu.Arụ ọrụ catalytic nke ígwè oxides ndị a na mmeghachi omume VO2+/VO2+ na tebụl S2.A na-eji WO3 mee ihe na ọnụ ọgụgụ dị ịrịba ama nke ọrụ n'ihi ọnụ ala ya, nkwụsi ike dị elu na mgbasa ozi acidic, na ọrụ catalytic dị elu31,32,33,34,35,36,37,38.Otú ọ dị, ọganihu nke cathodic kinetics n'ihi WO3 bụ ihe na-abaghị uru.Iji meziwanye conductivity nke WO3, a nwalere mmetụta nke iji tungsten oxide belatara (W18O49) na ọrụ cathodic38.A nwalebeghị hydrated tungsten oxide (HWO) na ngwa VRFB, n'agbanyeghị na ọ na-egosipụta mmụba na-abawanye na ngwa supercapacitor n'ihi mgbasa ozi ngwa ngwa ma e jiri ya tụnyere WOx39,40 anhydrous.Ọgbọ nke atọ vanadium redox flow batrị na-eji ngwakọta acid electrolyte mejupụtara HCl na H2SO4 iji melite arụmọrụ batrị ma melite solubility na nkwụsi ike nke ions vanadium na electrolyte.Otú ọ dị, mmeghachi omume evolushọn parasitic chlorine aghọwo otu n'ime adịghị ike nke ọgbọ nke atọ, ya mere ịchọ ụzọ iji gbochie mmeghachi omume nyocha chlorine aghọwo ihe na-elekwasị anya n'ọtụtụ nyocha.
N'ebe a, a na-eme nyocha mmeghachi omume VO2 + / VO2 + na ihe ndị mejupụtara HWO / C76 nke etinyere na electrodes akwa carbon iji chọta nguzozi n'etiti ihe nrụpụta eletrik nke ihe mejupụtara ya na redox kinetics nke elu electrode ka ọ na-egbochi evolushọn parasitic chlorine.nzaghachi (CER).A na-emepụta nanoparticles hydrated tungsten oxide (HWO) site na usoro hydrothermal dị mfe.Emere nnwale na ngwakọta acid electrolyte (H2SO4/HCl) iji mee ka ọgbọ nke atọ VRFB (G3) dị irè na iji nyochaa mmetụta HWO na mmeghachi omume evolushọn parasitic chlorine.
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% hydrochloride), sodium Tungsten oxide (92% hydrochloride), hydrochloric acid. A na-eji akwa ELAT (ụlọ ahịa mmanụ ọkụ) mee ihe n'ọmụmụ ihe a.
A na-akwadebe hydrated tungsten oxide (HWO) site na mmeghachi omume hydrothermal 43 nke 2 g nke nnu Na2WO4 na-agbaze na 12 ml nke H2O iji nye ngwọta na-enweghị agba, mgbe ahụ, 12 ml nke 2 M HCl gbakwunyere dropwise iji nye nkwụsịtụ odo odo na-acha odo odo.A na-etinye slurry na Teflon mkpuchi igwe anaghị agba nchara autoclave ma debe ya na oven na 180 ° C. maka awa 3 maka mmeghachi omume hydrothermal.A na-anakọta ihe fọdụrụ site na nzacha, saa 3 ugboro na ethanol na mmiri, a mịrị amị na oven na 70 ° C maka ~ 3 awa, wee triturated nye ntụ ntụ HWO na-acha anụnụ anụnụ.
A na-eji eriri akwa carbon carbon (CCT) enwetara (anaghị agwọ ya) dịka ma ọ bụ ikpo ọkụ na-ekpo ọkụ n'ime ọkụ tube na 450 ° C na ikuku na-ekpo ọkụ nke 15 ºC / min maka awa 10 iji nweta CC (TCC).dị ka akọwara n'isiokwu bu ụzọ 24.A na-egbutu UCC na TCC n'ime electrodes dịka 1.5 cm n'obosara na 7 cm ogologo.A kwadoro nkwusioru nke C76, HWO, HWO-10% C76, HWO-30% C76 na HWO-50% C76 site na ịgbakwunye 20 mg .% (~ 2.22 mg) nke PVDF binder to ~ 1 ml DMF na sonicated maka 1 hour iji meziwanye otu.2 mg nke C76, HWO na HWO-C76 mejupụtara ka etinyere n'usoro na mpaghara UCC na-arụ ọrụ electrode nke ihe dịka 1.5 cm2.A na-ebunye ihe niile na-eme ka ọ bụrụ ihe na-eme ka ọ dị na UCC electrodes ma jiri TCC mee ihe maka ntụnyere naanị, dịka ọrụ anyị gara aga gosiri na ọgwụgwọ okpomọkụ adịghị achọ24.Emetara ndozigharị echiche site na ịsachapụ 100 µl nke nkwusioru (ibu 2 mg) maka mmetụta karịa.Mgbe ahụ, a kpochapụrụ electrodes niile na oven na 60 Celsius C. n'abali.A na-atụ eletrọd ahụ n'ihu na azụ iji hụ na ebubata ngwaahịa ziri ezi.Iji nwee mpaghara geometric (~ 1.5 cm2) ma gbochie ịrị elu nke vanadium electrolyte na electrode n'ihi mmetụta nke capillary, a na-etinye obere paraffin n'elu ihe na-arụ ọrụ.
A na-eji microscopy eletrọn na-enyocha ihe ọkụkụ (FESEM, Zeiss SEM Ultra 60, 5 kV) iji hụ ụdị ọdịdị elu HWO.A na-eji spectrometer X-ray na-agbasa ike nke nwere Feii8SEM (EDX, Zeiss Inc.) iji mee ka eserese HWO-50% C76 dị na electrodes UCC.A elu mkpebi nnyefe eletrọn microscope (HR-TEM, JOEL JEM-2100) arụ ọrụ na accelerating voltaji nke 200 kV e ji mee ihe oyiyi elu mkpebi HWO irighiri na diffraction yiri mgbaaka.Akụrụngwa Crystallography Toolbox (CrysTBox) na-eji ọrụ ringGUI iji nyochaa ụkpụrụ mgbanaka HWO wee jiri nsonaazụ ya tụnyere ụkpụrụ XRD.A na-enyocha usoro na graphitization nke UCC na TCC site na X-ray diffraction (XRD) na nyocha nyocha nke 2.4 ° / min site na 5 ° ruo 70 ° na Cu Kα (λ = 1.54060 Å) site na iji Panalytical X-ray diffractometer (Model 3600).XRD gosipụtara usoro kristal na oge nke HWO.Ejiri ngwanro PANalytical X'Pert HighScore dabara na elu HWO na maapụ tungsten oxide dị na nchekwa data45.Atụnyere nsonaazụ HWO na nsonaazụ TEM.Ihe mejupụtara kemịkalụ na ọnọdụ nke nlele HWO bụ nke X-ray photoelectron spectroscopy kpebisiri ike (XPS, ESCALAB 250Xi, ThermoScientific).Ejiri sọftụwia CASA-XPS (v 2.3.15) mee ihe maka ntọhapụ kacha elu na nyocha data.Iji chọpụta otu ọrụ dị elu nke HWO na HWO-50% C76, a na-eme nha site na iji Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, iji KBr FTIR).atụnyere nsonaazụ ya na nsonaazụ XPS.A na-ejikwa nha nkuku kọntaktị (KRUSS DSA25) iji mara ịdị nro nke electrodes.
Maka nha electrochemical niile, ejiri Biologic SP 300 rụọ ọrụ.A na-eji Cyclic voltammetry (CV) na electrochemical impedance spectroscopy (EIS) na-amụ kinetics electrode nke mmeghachi omume redox VO2 +/VO2+ na mmetụta nke reagent mgbasa (VOSO4 (VO2+)) na ọnụego mmeghachi omume.Ụzọ abụọ a na-eji cell-electrode atọ na ntinye electrolyte nke 0.1 M VOSO4 (V4+) na 1 M H2SO4 + 1 M HCl (ngwakọta nke acids).A na-edozi data electrochemical niile IR.A na-eji igwe eletrọd calomel juru eju (SCE) na eriri platinum (Pt) dị ka ihe nrụtụ aka na igwe eletrọd, n'otu n'otu.Maka CV, a na-etinye ọnụ ọgụgụ nyocha (ν) nke 5, 20, na 50 mV / s na windo VO2 +/VO2 + maka (0-1) V vs. SCE, wee gbanwee maka SHE na-eme atụmatụ (VSCE = 0.242 V vs. HSE) .Iji mụọ njide ọrụ electrode, a na-eme CV cyclic ugboro ugboro na ν 5 mV / s maka UCC, TCC, UCC-C76, UCC-HWO, na UCC-HWO-50% C76.Maka nha EIS, ọnụọgụ ugboro ugboro nke mmeghachi omume redox VO2+/VO2+ bụ 0.01-105 Hz, na mgbagha voltaji na voltaji mepere emepe (OCV) bụ 10 mV.Emegharịrị nnwale ọ bụla ugboro 2-3 iji hụ na nkwekọ nke nsonaazụ ya.Ejiri usoro Nicholson nweta ọnụọgụ dị iche iche (k0) 46,47.
Achịkọtala hydrated tungsten oxide (HVO) nke ọma site na usoro hydrothermal.Foto SEM na fig.1a na-egosi na HWO echekwara nwere ụyọkọ nke nanoparticles nwere nha na nso 25-50 nm.
Usoro mgbasa ozi X-ray nke HWO na-egosi ọnụ ọgụgụ kachasị elu (001) na (002) na ~ 23.5 ° na ~ 47.5 °, n'otu n'otu, nke bụ njirimara nke nonstoichiometric WO2.63 (W32O84) (PDF 077-0810, a = 21.4 Å, b3γ 7, b3γ = 7 Å, b3γ = 7 γ. = 90 °), nke kwekọrọ na agba anụnụ anụnụ doro anya ha (Fig 1b) 48.49.E kenyere ọnụ ọgụgụ ndị ọzọ na ihe dịka 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° na 52.7° na (140), (620), (350), (720), (740), (560°).)) na (970) ụgbọ elu diffraction orthogonal na WO2.63, n'otu n'otu.Otu usoro sịntetị ahụ ka Songara et al.43 iji nweta ngwaahịa na-acha ọcha, nke ekwuru na ọnụnọ WO3 (H2O) 0.333.Otú ọ dị, n'ime ọrụ a, n'ihi ọnọdụ dị iche iche, e nwetara ngwaahịa na-acha anụnụ anụnụ, na-egosi na WO3 (H2O) 0.333 (PDF 087-1203, a = 7.3 Å, b = 12.5 Å, c = 7 .7 Å, α = β = γ = 90 °) na ụdị oxide belatara.Nyocha nke ọkara na-eji ngwanrọ X'Pert HighScore gosipụtara 26% WO3 (H2O) 0.333: 74% W32O84.Ebe W32O84 nwere W6+ na W4+ (1.67:1 W6+:W4+), ihe ekwuru na ọdịnaya W6+ na W4+ bụ ihe dịka 72% W6+ na 28% W4+, n'otu n'otu.Ihe onyonyo SEM, 1-sekọnd XPS spectra na ọkwa nucleus, onyonyo TEM, FTIR spectra, na ụdị Raman nke ihe C76 ka ewepụtara n'isiokwu anyị gara aga.Dị ka Kawada et al., 50,51 X-ray diffraction nke C76 mgbe mwepụ nke toluene gosipụtara usoro monoclinic nke FCC.
Foto SEM dị na fig.2a na b na-egosi na HWO na HWO-50% C76 kwadoro nke ọma na na n'etiti eriri carbon nke UCC electrode.Maapụ elementrị EDX nke tungsten, carbon, na oxygen na onyonyo SEM na fig.2c ka egosiri na fig.2d-f na-egosi na tungsten na carbon na-agwakọta nke ọma (na-egosi nkesa yiri ya) n'elu elu electrode dum na ihe mejupụtara ya adịghị echekwa ya n'otu n'otu n'ihi ọdịdị nke usoro ntinye.
Ihe onyonyo SEM nke irighiri ihe HWO (a) na HWO-C76 (b).EDX maapụ na HWO-C76 kwajuru na UCC site na iji mpaghara dị na onyonyo (c) na-egosi nkesa tungsten (d), carbon (e), na oxygen (f) na nlele.
A na-eji HR-TEM mee ihe maka nleba anya dị elu na ozi crystallographic (Nyocha 3).HWO na-egosi nanocube morphology dị ka e gosiri na Fig. 3a na n'ụzọ doro anya na fig. 3b.Site n'ịkwalite nanocube maka diffraction nke mpaghara ahọpụtara, mmadụ nwere ike iji anya nke uche hụ usoro grating na ụgbọ elu diffraction nke na-emeju iwu Bragg, dị ka egosiri na Fig 3c, nke na-akwado kristal nke ihe ahụ.Na ntinye na Fig. 3c na-egosi anya d 3.3 Å kwekọrọ na (022) na (620) ụgbọ elu diffraction dị na WO3 (H2O) 0.333 na W32O84, n'otu n'otu 43,44,49.Nke a kwekọrọ na nyocha XRD kọwara n'elu (Fig 1b) ebe ọ bụ na anya ụgbọ elu grating a na-ahụ anya d (Fig 3c) kwekọrọ na ọnụ ọgụgụ XRD kachasị ike na nlele HWO.A na-egosikwa mgbanaka ihe atụ na fig.3d, ebe mgbanaka ọ bụla dabara na ụgbọ elu dị iche.Ụgbọ elu WO3 (H2O) 0.333 na W32O84 na-acha ọcha na-acha anụnụ anụnụ, n'otu n'otu, na ọnụ ọgụgụ XRD ha kwekọrọ na-egosikwa na Fig. 1b.Mgbanaka mbụ egosiri na eserese mgbanaka dabara na ọnụ ọgụgụ mbụ akara na ụkpụrụ x-ray nke (022) ma ọ bụ (620) ụgbọ elu diffraction.Site na mgbanaka (022) ruo (402), ụkpụrụ d-spacing bụ 3.30, 3.17, 2.38, 1.93, na 1.69 Å, kwekọrọ na ụkpụrụ XRD nke 3.30, 3.17, 2, 45, 1.93.na 1.66 Å, nke hà nhata 44, 45, n'otu n'otu.
(a) Onyonyo HR-TEM nke HWO, (b) na-egosi onyonyo abawanyela.A na-egosi ihe onyonyo nke ụgbọ elu grating na (c), inset (c) na-egosi nnukwu onyonyo nke ụgbọ elu yana pitch d nke 0.33 nm dabara na (002) na (620).(d) ụkpụrụ mgbanaka HWO na-egosi ụgbọ elu jikọtara WO3 (H2O) 0.333 (ọcha) na W32O84 (acha anụnụ anụnụ).
Emere nyocha XPS iji chọpụta kemịkalụ elu na ọnọdụ oxidation nke tungsten (Figure S1 na 4).A na-egosi ụdịdị dị iche iche nke XPS nyocha nke HWO synthesized na eserese S1, na-egosi ọnụnọ tungsten.Eserese dị warara XPS nke ọkwa isi W 4f na O 1s ka egosiri na fig.4a na b, n'otu n'otu.Ụdị dị iche iche W 4f na-ekewa n'ime okpukpu abụọ na-atụgharị-orbit nke kwekọrọ na ike njide nke steeti W oxidation.na W 4f7/2 na 36.6 na 34.9 eV bụ njirimara nke steeti W4+ nke 40, n'otu n'otu.) 0.333.Data dabara adaba na-egosi na pasentị atọm nke W6+ na W4+ bụ 85% na 15%, n'otu n'otu, nke dị nso n'ụkpụrụ ndị echere na data XRD na-atụle ọdịiche dị n'etiti ụzọ abụọ ahụ.Ụzọ abụọ a na-enye ozi ọnụọgụ na izi ezi dị ala, ọkachasị XRD.Ọzọkwa, ụzọ abụọ a na-enyocha akụkụ dị iche iche nke ihe ahụ n'ihi na XRD bụ nnukwu usoro ebe XPS bụ usoro elu nke na-abịaru nso nanometer ole na ole.A na-ekewa ụdịdị dị iche iche O 1s gaa na elu abụọ na 533 (22.2%) na 530.4 eV (77.8%).Nke mbụ kwekọrọ na OH, na nke abụọ na njikọ oxygen na lattice na WO.Ọnụnọ nke otu ndị na-arụ ọrụ OH kwekọrọ na njirimara hydration nke HWO.
A na-eme nyocha FTIR na ihe atụ abụọ a iji nyochaa ọnụnọ nke otu ndị na-arụ ọrụ na nhazi nke mmiri mmiri na nhazi HWO hydrated.Nsonaazụ na-egosi na ihe nlele HWO-50% C76 na FT-IR HWO na-apụta n'ihi ọnụnọ HWO, ma ike nke elu dị iche iche dị iche iche n'ihi ihe dị iche iche nke ihe nlele ejiri mee nkwadebe maka nyocha (Fig 5a).) HWO-50% C76 na-egosi na ọnụ ọgụgụ niile, ma e wezụga maka elu nke tungsten oxide, metụtara fullerene 24. Nkọwa zuru ezu na fig.5a na-egosi na ihe atụ abụọ ahụ na-egosipụta nnukwu bandwit dị oke ike na ~ 710 / cm nke sitere na OWO na-agbatị oscillations na nhazi HWO lattice, na ubu siri ike na ~ 840 / cm sitere na WO.Maka ịgbatị ịma jijiji, a na-ekwu na mmachi dị nkọ dị ihe dị ka 1610/cm bụ ịgbagọ vibrations nke OH, ebe eriri absorption sara mbara dị ihe dị ka 3400/cm ka a na-ekwu na ịgbatị vibrations nke OH na ìgwè hydroxyl43.Nsonaazụ ndị a dabara na ụdịdị XPS dị na fig.4b, ebe ndị ọrụ WO nwere ike ịnye saịtị na-arụ ọrụ maka mmeghachi omume VO2 +/VO2 +.
Nyocha FTIR nke HWO na HWO-50% C76 (a), otu ndị na-arụ ọrụ na-egosi na nha ihu kọntaktị (b, c).
Otu OH nwekwara ike mebie mmeghachi omume VO2 +/VO2+, ebe ha na-abawanye hydrophilicity nke electrode, si otú a na-akwalite ọnụego mgbasa ozi na nnyefe elektrọn.Dị ka egosiri, HWO-50% C76 sample na-egosi ihe mgbakwunye elu maka C76.Enwere ike ekenye ọnụ ọgụgụ kachasị elu na ~ 2905, 2375, 1705, 1607, na 1445 cm3 na CH, O = C = O, C = O, C = C, na CO na-agbatị vibrations, n'otu n'otu.A maara nke ọma na ndị ọrụ oxygen C = O na CO nwere ike ije ozi dị ka ebe na-arụ ọrụ maka mmeghachi omume redox nke vanadium.Iji nwalee ma tụnyere wettability nke electrodes abụọ ahụ, a na-ewere nha nkuku kọntaktị dị ka e gosiri na Fig 5b,c.HWO electrode na-etinye uche ozugbo na ụmụ irighiri mmiri, na-egosi superhydrophilicity n'ihi otu ọrụ OH dị.HWO-50% C76 bụ hydrophobic karịa, yana akụkụ kọntaktị nke ihe dịka 135 ° mgbe 10 sekọnd.Agbanyeghị, na nha electrochemical, electrode HWO-50% C76 ghọrọ mmiri kpamkpam n'ihe na-erughị otu nkeji.Ihe nha wettability kwekọrọ na nsonaazụ XPS na FTIR, na-egosi na ọtụtụ OH dị n'elu HWO na-eme ka ọ dịkwuo ntakịrị hydrophilic.
A nwalere mmeghachi omume VO2 + / VO2 + nke HWO na HWO-C76 nanocomposites na a na-atụ anya na HWO ga-egbochi evolushọn chlorine na mmeghachi omume VO2 +/VO2 + na ngwakọta acid, na C76 ga-eme ka mmeghachi omume VO2 +/VO2 + gbanwee.%, 30%, na 50% C76 na HWO nkwusioru na CCC etinyere na electrodes na mkpokọta loading nke banyere 2 mg/cm2.
Dị ka e gosiri na fig.6, kinetics nke mmeghachi omume VO2 +/VO2+ na elu electrode ka CV na-enyocha ya na electrolyte agwakọta acidic.E gosipụtara mmiri mmiri dị ka I/Ipa maka ntụnyere dị mfe nke ΔEp na Ipa/Ipc maka ihe dị iche iche na-akpali akpali ozugbo na eserese ahụ.Egosiri data nkeji mpaghara ugbu a na eserese 2S.Na fig.Onyonyo 6a na-egosi na HWO dị ntakịrị na-abawanye ọnụego mbufe elektrọn nke mmeghachi omume redox VO2 +/VO2+ na elu electrode ma na-egbochi mmeghachi omume evolushọn parasitic chlorine.Agbanyeghị, C76 na-abawanye ọnụego mbufe eletrọn nke ukwuu ma na-akpali mmeghachi omume evolushọn chlorine.Ya mere, a na-atụ anya na ihe mejupụtara HWO na C76 nwere nhazi nke ọma ga-enwe ọrụ kachasị mma yana ikike kachasị ike igbochi mmeghachi omume evolushọn chlorine.Achọpụtara na mgbe ọ gbasasịrị ọdịnaya nke C76, ọrụ electrochemical nke electrodes na-eme ka ọ dịkwuo mma, dị ka ihe àmà na-egosi na mbelata nke ΔEp na mmụba nke Ipa / Ipc ratio (Table S3).A kwadoro nke a site na ụkpụrụ RCT nke ewepụtara na atụmatụ Nyquist na Fig. 6d (Table S3), bụ nke a chọpụtara na ọ na-ebelata na ụba C76 ọdịnaya.Nsonaazụ ndị a kwekọrọ na ọmụmụ Li, nke mgbakwunye nke carbon mesoporous na mesoporous WO3 gosipụtara kinetics mbufe ụgwọ ka mma na VO2 +/VO2 + 35.Nke a na-egosi na mmeghachi omume kpọmkwem nwere ike ịdabere karịa na conductivity electrode (C = C bond) 18, 24, 35, 36, 37. Nke a nwekwara ike ịbụ n'ihi mgbanwe nke nhazi geometry n'etiti [VO (H2O) 5] 2+ na [VO2 (H2O) 4]+, C76 na-ebelata mmeghachi omume mmeghachi omume site n'ibelata ike anụ ahụ.Otú ọ dị, nke a nwere ike ọ gaghị ekwe omume na HWO electrodes.
(a) Omume voltammetric cyclic (ν = 5 mV / s) nke mmeghachi omume VO2 +/ VO2 + nke UCC na HWO-C76 mejupụtara HWO dị iche iche: oke C76 na 0.1 M VOSO4 / 1 M H2SO4 + 1 M HCl electrolyte.(b) Randles-Sevchik na (c) Nicholson VO2 +/VO2+ usoro iji nyochaa arụmọrụ mgbasa ozi wee nweta ụkpụrụ k0 (d).
Ọ bụghị naanị na HWO-50% C76 na-egosipụta ihe fọrọ nke nta ka ọ bụrụ otu ọrụ electrocatalytic dị ka C76 maka mmeghachi omume VO2 +/VO2+, ma, ihe na-adọrọ mmasị karị, ọ gbakwunyere na-ekpochapụ evolushọn chlorine ma e jiri ya tụnyere C76, dị ka egosiri na Fig. 6a, ma na-egosipụtakwa obere Semicircle na fig.6d (RCT dị ala).C76 gosipụtara Ipa / Ipc dị elu karịa HWO-50% C76 (Table S3), ọ bụghị n'ihi mmeghachi omume mmeghachi omume ka mma, ma n'ihi na ọnụ ọgụgụ kasị elu nke mmeghachi omume mbelata chlorine na SHE na 1.2 V. Arụ ọrụ kachasị mma nke HWO- The 50% C76 na-ekwu na synergistic mmetụta n'etiti ndị na-arụ ọrụ na-adịghị mma na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ nke ukwuu na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ na-arụ ọrụ nke ọma. WO.Mmụpụta chlorine dị ntakịrị ga-eme ka nrụpụta chaja nke cell zuru ezu, ebe mma kinetics ga-eme ka arụmọrụ nke voltaji cell zuru oke.
Dabere na nha nha S1, maka mmeghachi omume nke na-agbanwe agbanwe (nke dị nwayọ na mbufe elektrọn) na-achịkwa mgbasa ozi, ọnụ ọgụgụ kachasị elu (IP) dabere na ọnụọgụ elektrọn (n), mpaghara elektrọn (A), ọnụọgụ mgbasa ozi (D), ọnụọgụ ọnụọgụ elektrọn (α) na nyocha nyocha (ν).Iji mụọ omume a na-achịkwa mgbasa ozi nke ihe ndị a nwalere, e debere mmekọrịta dị n'etiti IP na ν1 / 2 ma gosipụta ya na Fig. 6b.Ebe ọ bụ na ihe niile na-egosi njikọ dị n'ahịrị, a na-achịkwa mmeghachi omume site na mgbasa.Ebe ọ bụ na mmeghachi omume VO2 +/VO2 + bụ ihe na-agbanwe agbanwe, mkpọda nke ahịrị na-adabere na ọnụọgụ mgbasa ozi na uru nke α (nha nhata S1).Ebe ọ bụ na ọnụọgụ mgbasa ozi na-adịgide adịgide (≈ 4 × 10-6 cm2 / s) 52, ọdịiche dị na mkpọda nke ahịrị ahụ na-egosi kpọmkwem ụkpụrụ dị iche iche nke α, ya mere ọnụego nnyefe eletrọn na elu electrode, nke egosiri maka C76 na HWO -50% C76 Steepest mkpọda (ọnụego mbufe eletrọn kacha elu).
Mkpọda Warburg (W) gbakọrọ maka obere ugboro egosipụtara na tebụl S3 (Fig 6d) nwere ụkpụrụ dị nso na 1 maka ihe niile, na-egosi mgbasa ozi zuru oke nke ụdị redox ma na-akwado omume linear nke IP ma e jiri ya tụnyere ν1 / 2. A na-atụ CV.Maka HWO-50% C76, mkpọda Warburg na-esi na 1 ruo 1.32, na-egosi na ọ bụghị naanị mgbasa ozi na-enweghị ngwụcha nke reagent (VO2 +), kamakwa enwere ike inye onyinye nke omume dị nro na omume mgbasa n'ihi porosity electrode.
Iji nyochaa ngbanwe nke mgbanwe (ọnụego mbufe elektrọn) nke mmeghachi omume redox VO2 +/VO2+, a na-ejikwa usoro mmeghachi omume nke Nicholson quasi-reversible iji chọpụta ọnụego ọkọlọtọ mgbe niile k041.42.A na-eme nke a site na iji nha S2 iji wuo paramita kinetic na-enweghị akụkụ Ψ, nke bụ ọrụ nke ΔEp, dịka ọrụ nke ν-1/2.Tebụlụ S4 na-egosi ụkpụrụ Ψ enwetara maka ihe elektrọd ọ bụla.Achọpụtara nsonaazụ (Fig 6c) iji nweta k0 × 104 cm / s site na mkpọda nke ebe ọ bụla site na iji Equation S3 (nke e dere n'akụkụ nke ọ bụla n'ahịrị ma gosipụta na Tebụl S4).Achọpụtara HWO-50% C76 ka ọ nwere mkpọda kachasị elu (Fig 6c), ya mere ọnụ ahịa kachasị nke k0 bụ 2.47 × 10-4 cm / s.Nke a pụtara na electrode a na-enweta kinetics kachasị ngwa ngwa, nke kwekọrọ na CV na EIS na-arụpụta na Fig. 6a na d na na tebụl S3.Tụkwasị na nke ahụ, a na-enwetakwa uru nke k0 site na atụmatụ Nyquist (Fig 6d) nke Equation S4 na-eji uru RCT (Table S3).A na-achịkọta nsonaazụ k0 ndị a sitere na EIS na tebụl S4 ma gosipụtakwa na HWO-50% C76 na-egosipụta ọnụego mbufe elektrọn kachasị elu n'ihi mmetụta synergistic.Ọ bụ ezie na ụkpụrụ k0 dị iche iche n'ihi mmalite dị iche iche nke usoro ọ bụla, ha ka na-egosi otu usoro nke ịdị ukwuu ma na-egosi nkwụsịtụ.
Iji ghọta nke ọma kinetics kacha mma enwetara, ọ dị mkpa iji tụnyere ihe electrode kacha mma na UCC na TCC electrodes enweghị mkpuchi.Maka mmeghachi omume VO2 + / VO2 +, HWO-C76 ọ bụghị naanị gosipụtara ΔEp kacha ala na ntụgharị ka mma, ma na-egbochikwa mmeghachi omume evolushọn parasitic parasitic chlorine ma e jiri ya tụnyere TCC, dị ka a tụrụ ya ugbu a na 1.45 V metụtara SHE (Fig 7a).N'ihe gbasara nkwụsi ike, anyị chere na HWO-50% C76 kwụsiri ike n'anụ ahụ n'ihi na a na-ejikọta ihe na-eme ka ihe na-eme ka ọ bụrụ ihe nkedo PVDF wee tinye ya na electrodes akwa carbon.HWO-50% C76 gosipụtara ngbanwe kachasị elu nke 44 mV (ọnụego mmebi 0.29 mV / okirikiri) mgbe usoro 150 gasịrị ma e jiri ya tụnyere 50 mV maka UCC (Nyocha 7b).Nke a nwere ike ọ gaghị abụ nnukwu ihe dị iche, mana kinetics nke UCC electrodes na-adị ngwa ngwa ma na-eweda ịgba ígwè, karịsịa maka mmeghachi omume azụ.Ọ bụ ezie na ngbanwe nke TCC dị nnọọ mma karịa nke UCC, a chọpụtara na TCC nwere nnukwu ngbanwe nke 73 mV mgbe usoro 150 gasịrị, nke nwere ike ịbụ n'ihi nnukwu chlorine nke a na-emepụta n'elu ya.nke mere na onye na-eme ihe na-akwado nke ọma na elu electrode.Dị ka a na-ahụ site na electrodes niile a nwalere, ọbụna electrodes na-enweghị ndị na-akwado nkwado gosipụtara ọkwa dịgasị iche iche nke enweghị ike ịgba ígwè, na-atụ aro na mgbanwe nke oke nkewa n'oge ịgba ígwè bụ n'ihi nkwụsị nke ihe onwunwe nke mgbanwe kemịkalụ na-akpata kama ịkewa nkewa.Tụkwasị na nke ahụ, ọ bụrụ na a ga-ekewapụ nnukwu ihe ndị na-emepụta ihe site na elu electrode, nke a ga-eme ka mmụba dị ukwuu na nkewa kachasị elu (ọ bụghị naanị 44 mV), ebe ọ bụ na mkpụrụ (UCC) adịghị arụ ọrụ maka mmeghachi omume VO2 +/VO2+.
Ntụle nke CV nke ihe kacha mma electrode tụnyere UCC (a) na nkwụsi ike nke VO2 +/VO2 + redox mmeghachi omume (b).ν = 5 mV/s maka CV niile na 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Iji mee ka mma akụ na ụba nke teknụzụ VRFB dịkwuo mma, ịgbasa na ịghọta kinetics nke mmeghachi omume vanadium redox dị mkpa iji nweta ike dị elu.A kwadebere ihe ndị mejupụtara HWO-C76 na mmetụta electrocatalytic ha na mmeghachi omume VO2 + / VO2 +.HWO gosiri ntakịrị nkwalite kinetic na agwakọta acidic electrolytes mana ọ kwụsịrị chlorine evolushọn nke ukwuu.A na-eji oke dị iche iche nke HWO:C76 mee ka ọ dịkwuo elu kanetics nke electrodes dabeere na HWO.Ịbawanye C76 na HWO na-eme ka kinetics na-enyefe electron nke VO2 +/ VO2 + mmeghachi omume na electrode gbanwere, nke HWO-50% C76 bụ ihe kachasị mma n'ihi na ọ na-ebelata nkwụsị nnyefe ụgwọ ma na-ebelata chlorine ma e jiri ya tụnyere C76 na TCC nkwụnye ego..Nke a bụ n'ihi mmetụta synergistic dị n'etiti C = C sp2 hybridization, OH na W-OH ọrụ otu.Achọpụtara ọnụ ọgụgụ mmebi ahụ mgbe HWO-50% C76 na-agba ọsọ ugboro ugboro na 0.29 mV / okirikiri, ebe ọnụ ọgụgụ mmebi nke UCC na TCC bụ 0.33 mV / okirikiri na 0.49 mV / okirikiri, na-eme ka ọ kwụsie ike.na ngwakọta acid electrolytes.Nsonaazụ ewepụtara nke ọma na-achọpụta ihe elektrọd arụmọrụ dị elu maka mmeghachi omume VO2 +/VO2+ na kinetics ngwa ngwa yana nkwụsi ike dị elu.Nke a ga-abawanye voltaji mmepụta, si otú ahụ na-amụba ike ike nke VRFB, si otú ahụ na-ebelata ọnụ ahịa nke azụmahịa ya n'ọdịnihu.
Ihe ndekọ data ejiri na/ma ọ bụ nyochaa n'ime ọmụmụ ihe ugbu a dị site n'aka ndị edemede dị iche iche na arịrịọ ezi uche dị na ya.
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Opar, DO, Nankya, R., Lee, J. & Jung, H. carbon mesoporous graphene-modified akụkụ atọ nwere mmetụta maka batrị vanadium redox na-arụ ọrụ dị elu. Opar, DO, Nankya, R., Lee, J. & Jung, H. carbon mesoporous graphene-modified akụkụ atọ nwere mmetụta maka batrị vanadium redox na-arụ ọrụ dị elu.Opar DO, Nankya R., Lee J., na Yung H. graphene-mgbanwe mesoporous carbon nke nwere akụkụ atọ nwere mmetụta maka batrị vanadium redox na-arụ ọrụ dị elu. Mee, Mee, Nanka, r., Lee, Lee, Lee, H. 用于 高性能 电池 三维介 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 碳 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 孔石墨 Opar, DO, Nankya, R., Lee, J. & Jung, H.Opar DO, Nankya R., Lee J., na Yung H. graphene-mgbanwe mesoporous carbon nke nwere akụkụ atọ nwere mmetụta maka batrị vanadium redox na-arụ ọrụ dị elu.Electrochem.Ọrụ 330, 135276. https://doi.org/10.1016/j.electacta.2019.135276 (2020).