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Ọnụ ego dị elu nke batrị redox niile na-asọfe vanadium (VRBBs) na-egbochi ojiji ha nke ọma. Imeziwanye kinetics nke mmeghachi omume electrochemical dị mkpa iji mee ka ike na arụmọrụ ike nke VRFB dịkwuo elu, si otú a belata ọnụ ahịa kWh nke VRFB. N'ọrụ a, etinyere nanoparticles tungsten oxide (HWO) hydrothermally synthesized hydrothermally synthesized hydrothermally synthesized, C76 na C76/HWO, na carbon cloth electrodes ma nwalee ya dị ka electrocatalysts maka mmeghachi omume redox VO2+/VO2+. Nyocha ikuku emission electron scanning (FESEM), ike 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) na nha akụkụ kọntaktị. A chọpụtala na mgbakwunye nke C76 fullerenes na HWO nwere ike imeziwanye kinetics electrode site na ịbawanye ike eletriki ma nye otu ọrụ oxidized n'elu ya, si otú a na-akwalite mmeghachi omume redox VO2+/VO2+. Ngwakọta HWO/C76 (50 wt% C76) gosipụtara na ọ bụ nhọrọ kacha mma maka mmeghachi omume VO2+/VO2+ na ΔEp nke 176 mV, ebe ákwà carbon a na-agwọghị (UCC) bụ 365 mV. Na mgbakwunye, ngwakọta HWO/C76 gosipụtara mmetụta dị ukwuu na mmeghachi omume evolushọn chlorine parasitic n'ihi otu ọrụ W-OH.
Ọrụ siri ike nke ụmụ mmadụ na mgbanwe ngwa ngwa nke ụlọ ọrụ mmepụta ihe emeela ka ọchịchọ ọkụ eletrik dị elu nke ukwuu, nke na-amụba site na ihe dị ka 3% kwa afọ1. Ruo ọtụtụ iri afọ, ojiji a na-eji mmanụ ọkụ dị ka isi iyi ike edugala na mwepụta gas na-ekpo ọkụ nke na-eme ka okpomọkụ ụwa, mmiri na ikuku na-emetọ, na-eyi gburugburu ebe obibi niile egwu. N'ihi ya, a na-atụ anya na ntinye nke ikuku dị ọcha na nke a na-emegharị emegharị na ike anyanwụ ga-eru 75% nke ọkụ eletrik zuru oke ka ọ na-erule 20501. Agbanyeghị, mgbe òkè nke ọkụ eletrik sitere na isi mmalite mmeghari ohuru gafere 20% nke mmepụta ọkụ eletrik zuru oke, grid ahụ na-aghọ ihe na-adịghị agbanwe agbanwe.
N'ime sistemụ nchekwa ike niile dịka batrị redox nke vanadium hybrid, batrị redox nke all-vanadium (VRFB) emepụtala ngwa ngwa n'ihi ọtụtụ uru ya ma a na-ewere ya dị ka ihe ngwọta kacha mma maka nchekwa ike ogologo oge (ihe dị ka afọ 30). ) Nhọrọ yana ike mmeghari ohuru4. Nke a bụ n'ihi nkewa nke ike na njupụta ike, nzaghachi ngwa ngwa, ndụ ọrụ ogologo oge, na ọnụ ahịa kwa afọ dị ala nke $65/kWh ma e jiri ya tụnyere $93-140/kWh maka batrị Li-ion na lead-acid na $279-420 US kwa kWh. batrị n'otu n'otu 4.
Agbanyeghị, nnukwu azụmahịa ha ka na-egbochi site na ọnụ ahịa isi obodo ha dị elu, ọkachasị n'ihi stacks cell4,5. Ya mere, imeziwanye arụmọrụ stack site na ịbawanye kinetics nke mmeghachi omume ọkara-ihe abụọ nwere ike ibelata nha stack ma si otú a belata ọnụ ahịa. Ya mere, mbufe elektrọn ngwa ngwa na elu elektrọd dị mkpa, nke dabere na imewe, nhazi na nhazi nke elektrọd ma chọọ njikarịcha nke ọma6. N'agbanyeghị ezigbo nkwụsi ike kemịkalụ na elektrọd eletrik dị mma na ezigbo njikwa eletriki nke elektrọd carbon, kinetics ha na-adịghị agwọ ọrịa na-adịghị ike n'ihi enweghị otu ọrụ oxygen na hydrophilicity7,8. Ya mere, a na-ejikọta electrocatalysts dị iche iche na elektrọd dabere na carbon, karịsịa carbon nanostructures na metal oxides, iji melite kinetics nke elektrọd abụọ ahụ, si otú a na-amụba kinetics nke elektrọd VRFB.
Na mgbakwunye na ọrụ anyị gara aga na C76, anyị buru ụzọ kọọ ọrụ electrocatalytic dị mma nke fullerene a maka nnyefe chaja VO2+/VO2+, ma e jiri ya tụnyere ákwà carbon a gwọrọ na nke a na-anaghị agwọ. A na-ebelata nguzogide site na 99.5% na 97%. A na-egosi arụmọrụ catalytic nke ihe carbon maka mmeghachi omume VO2+/VO2+ ma e jiri ya tụnyere C76 na Tebụl S1. N'aka nke ọzọ, ejirila ọtụtụ oxides metal dị ka CeO225, ZrO226, MoO327, NiO28, SnO229, Cr2O330 na WO331, 32, 33, 34, 35, 36, 37 n'ihi mmụba mmiri ha na ọrụ oxygen dị ukwuu. , 38. A na-egosi ọrụ catalytic nke oxides metal ndị a na mmeghachi omume VO2+/VO2+ na Tebụl S2. A na-eji WO3 arụ ọrụ dị ukwuu n'ihi ọnụ ahịa ya dị ala, nkwụsi ike dị elu na mgbasa ozi acidic, na nnukwu ọrụ catalytic31,32,33,34,35,36,37,38. Agbanyeghị, mmụba na kinetics cathodic n'ihi WO3 abụghị ihe dị mkpa. Iji melite conductivity nke WO3, a nwalere mmetụta nke iji tungsten oxide (W18O49) belatara na ọrụ cathodic38. A nwalebeghị tungsten oxide (HWO) na ngwa VRFB, ọ bụ ezie na ọ na-egosipụta mmụba ọrụ na ngwa supercapacitor n'ihi mgbasa cation ngwa ngwa ma e jiri ya tụnyere WOx39,40 anhydrous. Batrị vanadium redox nke ọgbọ nke atọ na-eji acid electrolyte agwakọtara nke HCl na H2SO4 iji melite arụmọrụ batrị ma melite mgbaze na nkwụsi ike nke ion vanadium na electrolyte. Agbanyeghị, mmeghachi omume evolushọn nke chlorine parasitic abụrụla otu n'ime ihe ndị na-adịghị mma nke ọgbọ nke atọ, yabụ ịchọ ụzọ isi gbochie mmeghachi omume nyocha chlorine abụrụla isi ihe ọtụtụ otu nyocha na-elekwasị anya.
N'ebe a, e mere nnwale mmeghachi omume VO2+/VO2+ na ngwakọta HWO/C76 nke e tinyere na elektrọd ákwà carbon iji chọta nguzozi n'etiti ike eletriki nke ngwakọta na redox kinetics nke elu elektrọd ebe ọ na-egbochi evolushọn parasitic chlorine. response (CER). E ji usoro hydrothermal dị mfe mepụta nanoparticles Hydrated tungsten oxide (HWO). E mere nnwale na electrolyte acid agwakọta (H2SO4/HCl) iji mee ka ọgbọ nke atọ VRFB (G3) dị irè ma nyochaa mmetụta nke HWO na mmeghachi omume evolushọn chlorine parasitic.
E jiri 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) na hydrophilic carbon cloth ELAT (Fuel Cell Store) mee ihe n'ọmụmụ ihe a.
E ji hydrothermal reaction 43 kwadebe mmiri tungsten oxide (HWO) nke a na-akpọ Hydrated tungsten oxide (HWO) nke a gbazere n'ime 12 ml nke H2O iji nye mmiri na-enweghị agba, wee tinye 12 ml nke HCl 2 M iji nye nkwụsịtụ odo odo na-acha ọbara ọbara. E tinyere mmiri ahụ n'ime autoclave ígwè anaghị agba nchara nke a kpụchara akpụ nke Teflon ma debe ya n'ime oven na 180°C. ruo awa atọ maka mmeghachi omume hydrothermal. A na-anakọta ihe fọdụrụ site na nzacha, saa ya ugboro atọ na ethanol na mmiri, kpoo ya na oven na 70°C ruo awa atọ, wee tụgharịa ya ka ọ bụrụ ntụ ntụ HWO na-acha anụnụ anụnụ.
E jiri elektrọd ákwà carbon e nwetara (nke a na-agwọghị) (CCT) mee ihe dịka e si dị ma ọ bụ kpoo ọkụ e ji mee ya n'ime ọkụ tube na 450°C n'ikuku yana ọnụego okpomọkụ nke 15 ºC/min maka awa 10 iji nweta CCs e gwọrọ agwọ (TCC). dịka akọwara n'isiokwu gara aga24. E bepụrụ UCC na TCC n'ime elektrọd ihe dị ka 1.5 cm n'obosara na 7 cm n'ogologo. E tinyere 20 mg .% (~2.22 mg) nke ihe njikọ PVDF na ~1 ml DMF ma tinye sonicated maka otu awa iji melite ịdị n'otu. E tinyere 2 mg nke ihe mejupụtara C76, HWO na HWO-C76 n'usoro na mpaghara elektrọd UCC na-arụ ọrụ nke ihe dị ka 1.5 cm2. E tinyere ihe mkpali niile n'elu elektrọd UCC, e jikwa TCC mee ihe maka ntụnyere naanị, dịka ọrụ anyị gara aga gosiri na ọ dịghị mkpa ka a gwọọ okpomọkụ24. E nwetara nhazi mmetụta site n'ịchacha 100 µl nke nkwusioru ahụ (ibu 2 mg) maka mmetụta ka mma. Mgbe ahụ, a kpọrọ elektrọd niile nkụ n'ime oven na okpomọkụ 60° C. n'abalị. A na-atụ elektrọd ndị ahụ n'ihu na azụ iji hụ na ha na-ebu ibu zuru oke. Iji nwee mpaghara geometric ụfọdụ (~1.5 cm2) ma gbochie mmụba nke elektrọd vanadium na elektrọd ahụ n'ihi mmetụta capillary, etinyere obere paraffin n'elu ihe na-arụ ọrụ.
E jiri igwe nyocha ikuku eletrik (FESEM, Zeiss SEM Ultra 60, 5 kV) lee ọdịdị elu HWO. E jiri igwe X-ray na-agbasa ike nke nwere Feii8SEM (EDX, Zeiss Inc.) mee maapụ ihe HWO-50%C76 na elektrọd UCC. E jiri igwe microscope nnyefe elektrọn dị elu (HR-TEM, JOEL JEM-2100) nke na-arụ ọrụ na voltaji ngwa ngwa nke 200 kV mee ihe iji see ihe dị elu na mgbaaka diffraction. Ngwanrọ Crystallography Toolbox (CrysTBox) na-eji ọrụ ringGUI iji nyochaa ụkpụrụ diffraction mgbanaka HWO ma tụnyere nsonaazụ ya na ụkpụrụ XRD. E jiri X-ray diffraction (XRD) nyochaa nhazi na eserese nke UCC na TCC na ọsọ 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 gosiri nhazi kristal na usoro nke HWO. E jiri ngwanrọ PANAlytical X'Pert HighScore mee ka elu HWO dakọọ na maapụ tungsten oxide dị na nchekwa data45. E jiri nsonaazụ HWO tụnyere nsonaazụ TEM. E jiri X-ray photoelectron spectroscopy (XPS, ESCALAB 250Xi, ThermoScientific) chọpụta ihe mejupụtara kemịkalụ na ọnọdụ nke ihe atụ HWO. E jiri ngwanrọ CASA-XPS (v 2.3.15) mee ihe maka deconvolution kacha elu na nyocha data. Iji chọpụta otu ọrụ elu nke HWO na HWO-50%C76, e jiri Fourier transform infrared spectroscopy (FTIR, Perkin Elmer spectrometer, site na iji KBr FTIR) tụọ ihe ndị a. E jiri nsonaazụ tụnyere nsonaazụ XPS. E jikwa nha akụkụ kọntaktị (KRUSS DSA25) chọpụta otú elektrọd ndị ahụ si dị mmiri mmiri.
Maka nha elektrọnik niile, ejiri ọrụ Biologic SP 300. Ejiri cyclic voltammetry (CV) na electrochemical impedance spectroscopy (EIS) mụọ electrode kinetics nke VO2+/VO2+ redox reaction na mmetụta nke reagent diffusion (VOSO4(VO2+)) na ọnụego mmeghachi omume. Usoro abụọ a jiri sel electrode atọ nwere njupụta elektrọnik nke 0.1 M VOSO4 (V4+) na 1 M H2SO4 + 1 M HCl (ngwakọta asịd). A na-edozi data electrochemical niile ewepụtara. Ejiri calomel electrode saturated (SCE) na platinum (Pt) coil dị ka electrode ntụaka na counter, n'otu n'otu. Maka CV, etinyere ọnụego nyocha (ν) nke 5, 20, na 50 mV/s na windo VO2+/VO2+ maka (0–1) V vs. SCE, wee gbanwee ya ka SHE wee tụọ ya (VSCE = 0.242 V vs. HSE). Iji mụọ njigide ọrụ elektrọd, emere CV cyclic ugboro ugboro na ν 5 mV/s maka UCC, TCC, UCC-C76, UCC-HWO, na UCC-HWO-50% C76. Maka nha EIS, oke ugboro nke mmeghachi omume redox VO2+/VO2+ bụ 0.01-105 Hz, mgbanwe voltaji na voltaji open-circuit (OCV) bụ 10 mV. Emeghachiri nnwale ọ bụla ugboro 2-3 iji hụ na nsonaazụ ya na-aga n'ihu. Usoro Nicholson46,47 nwetara mgbanwe ọnụego dị iche iche (k0).
E jiri usoro hydrothermal mepụta tungsten oxide (HVO) nke ọma. Foto SEM dị na fig. 1a na-egosi na HWO e tinyere n'ime ya nwere otu ìgwè nanoparticles nwere nha dị n'etiti 25-50 nm.
Usoro mgbasa ozi X-ray nke HWO na-egosi oke (001) na (002) na ~23.5° na ~47.5°, n'otu n'otu, nke bụ njirimara nke WO2.63 na-abụghị stoichiometric (W32O84) (PDF 077–0810, a = 21.4 Å, b = 17.8 Å, c = 3.8 Å, α = β = γ = 90°), nke kwekọrọ na agba anụnụ anụnụ ha doro anya (Fig. 1b) 48.49. E kenyere oke ndị ọzọ dị ihe dị ka 20.5°, 27.1°, 28.1°, 30.8°, 35.7°, 36.7° na 52.7° na (140), (620), (350), (720), (740), (560°). ) ) na (970) usoro diffraction nke orthogonal ruo WO2.63, n'otu n'otu. Songara na ndị otu ya jiri otu ụzọ mmepụta ihe ahụ iji nweta ngwaahịa ọcha, nke e kwuru na ọ bụ ọnụnọ nke WO3(H2O)0.333. Agbanyeghị, n'ọrụ a, n'ihi ọnọdụ dị iche iche, enwetara ngwaahịa acha anụnụ anụnụ-isi awọ, nke 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 mbelata nke tungsten oxide. Nyocha Semiquantitative site na iji ngwanrọ X'Pert HighScore gosiri 26% WO3(H2O)0.333:74% W32O84. Ebe ọ bụ na W32O84 nwere W6+ na W4+ (1.67:1 W6+:W4+), atụmatụ ọdịnaya nke W6+ na W4+ bụ ihe dị ka 72% W6+ na 28% W4+, n'otu n'otu. Foto SEM, spectra XPS nke sekọnd 1 na ọkwa nucleus, onyonyo TEM, spectra FTIR, na spectra Raman nke mkpụrụ ndụ C76 ka egosiri n'isiokwu anyị gara aga. Dịka Kawada et al. si kwuo, 50,51 X-ray diffraction nke C76 mgbe ewepụchara toluene gosiri usoro monoclinic nke FCC.
Foto SEM dị na fig. 2a na b na-egosi na e tinyere HWO na HWO-50%C76 nke ọma na eriri carbon nke electrode UCC nke ọma. E gosiri maapụ ihe EDX nke tungsten, carbon, na oxygen na onyonyo SEM dị na fig. 2c na fig. 2d-f na-egosi na tungsten na carbon na-agwakọta nke ọma (na-egosi nkesa yiri nke ahụ) n'elu elu electrode dum na ihe mejupụtara anaghị etinye otu nha n'ihi ụdị usoro itinye ihe.
Foto SEM nke mkpụrụ ndụ HWO e tinyere (a) na mkpụrụ ndụ HWO-C76 (b). Maapụ EDX na HWO-C76 e tinyere na UCC site na iji mpaghara dị na onyonyo (c) na-egosi nkesa nke tungsten (d), carbon (e), na oxygen (f) na ihe nlele ahụ.
E jiri HR-TEM mee ihe maka onyonyo dị elu na ozi kristal (Foto 3). HWO na-egosi ọdịdị nanocube dịka egosiri na Fig. 3a na nke ọma na Fig. 3b. Site n'ịkwalite nanocube maka mgbasa nke mpaghara ahọpụtara, mmadụ nwere ike ịhụ nhazi grating na planes diffraction nke na-emezu iwu Bragg, dịka egosiri na Fig. 3c, nke na-akwado kristal nke ihe ahụ. Na ntinye na Fig. 3c na-egosi anya d 3.3 Å nke kwekọrọ na planes diffraction (022) na (620) dị na usoro WO3(H2O) 0.333 na W32O84, n'otu n'otu43,44,49. Nke a kwekọrọ na nyocha XRD akọwara n'elu (Foto 1b) ebe ọ bụ na anya planes grating d a hụrụ (Foto 3c) kwekọrọ na elu XRD kachasị ike na ihe nlele HWO. A na-egosikwa mgbaaka ihe atụ na fig. 3d, ebe mgbanaka ọ bụla kwekọrọ na planes dị iche. Agba WO3(H2O)0.333 na W32O84 bụ agba ọcha na acha anụnụ anụnụ, n'otu n'otu, a na-egosikwa elu XRD ha kwekọrọ na Fig. 1b. Mgbaaka mbụ egosiri na eserese mgbanaka ahụ kwekọrọ na elu mbụ akara na ụkpụrụ x-ray nke oghere diffraction (022) ma ọ bụ (620). Site na mgbanaka (022) ruo (402), uru oghere d 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) Foto HR-TEM nke HWO, (b) na-egosi onyonyo buru ibu. E gosiri onyonyo nke oghere ndị a na-akpọ grating na (c), inset (c) na-egosi onyonyo buru ibu nke ụgbọelu ndị a na pitch d nke 0.33 nm nke kwekọrọ na ụgbọelu (002) na (620). (d) Ụkpụrụ mgbanaka HWO na-egosi ụgbọelu ndị jikọtara ya na WO3(H2O)0.333 (ọcha) na W32O84 (acha anụnụ anụnụ).
E mere nyocha XPS iji chọpụta kemistri elu na ọnọdụ oxidation nke tungsten (Foto S1 na 4). E gosipụtara ụdị nyocha XPS sara mbara nke HWO a haziri na Foto S1, na-egosi ọnụnọ nke tungsten. E gosiri ụdị nyocha XPS dị warara nke ọkwa isi W 4f na O 1s na Fig. 4a na b, n'otu n'otu. Ụdị W 4f na-ekewa n'ime okpukpu abụọ nke spin-orbit nke kwekọrọ na ike njikọ nke ọnọdụ oxidation W. na W 4f7/2 na 36.6 na 34.9 eV bụ njirimara nke ọnọdụ W4+ nke 40, n'otu n'otu. )0.333. Data dabara adaba na-egosi na pasent atọm nke W6+ na W4+ bụ 85% na 15%, n'otu n'otu, nke dị nso na ụkpụrụ ndị a tụrụ anya site na data XRD na-atụle ọdịiche dị n'etiti ụzọ abụọ ahụ. Ụzọ abụọ ahụ na-enye ozi ọnụọgụgụ na obere izi ezi, karịsịa XRD. Ọzọkwa, ụzọ abụọ a na-enyocha akụkụ dị iche iche nke ihe ahụ n'ihi na XRD bụ usoro buru ibu ebe XPS bụ usoro elu nke na-eru naanị nanomita ole na ole. A na-ekewa spectrum O 1s n'ime elu abụọ na 533 (22.2%) na 530.4 eV (77.8%). Nke mbụ kwekọrọ na OH, nke abụọ kwekọrọ na njikọ oxygen na lattice na WO. Ọnụnọ nke otu ọrụ OH kwekọrọ na njirimara mmiri nke HWO.
E mekwara nyocha FTIR na ihe nlele abụọ a iji lelee ọnụnọ nke otu ọrụ na nhazi molekul mmiri na nhazi HWO mmiri mmiri. Nsonaazụ ya gosiri na ihe nlele HWO-50% C76 na nsonaazụ FT-IR HWO yiri nke ahụ n'ihi ọnụnọ nke HWO, mana ike nke elu dị iche iche n'ihi ọnụọgụ dị iche iche nke ihe nlele ejiri mee nkwadebe maka nyocha (Fig. 5a). HWO-50% C76 na-egosi na elu niile, ma e wezụga elu nke tungsten oxide, metụtara fullerene 24. Nkọwa zuru ezu na fig. 5a na-egosi na ihe nlele abụọ ahụ na-egosipụta eriri sara mbara siri ike na ~710/cm nke sitere na oscillations OWO na nhazi lattice HWO, yana ubu siri ike na ~840/cm nke sitere na WO. Maka ịma jijiji ịgbatị, eriri dị nkọ dị ihe dị ka 1610/cm bụ na mkpọtụ nke OH, ebe eriri nnabata sara mbara dị ihe dị ka 3400/cm bụ na mkpọtụ ịgbatị nke OH na otu hydroxyl43. Nsonaazụ ndị a kwekọrọ na XPS spectra dị na Fig. 4b, ebe otu ọrụ WO nwere ike inye saịtị na-arụ ọrụ maka mmeghachi omume VO2+/VO2+.
Nyocha FTIR nke HWO na HWO-50% C76 (a), gosiri otu ọrụ na nha akụkụ kọntaktị (b, c).
Otu OH nwekwara ike ime ka mmeghachi omume VO2+/VO2+ ka mma, ebe ọ na-eme ka hydrophilicity nke electrode dịkwuo elu, si otú a na-akwalite ọnụego mgbasa na nnyefe elektrọn. Dịka egosiri, ihe nlele HWO-50% C76 na-egosi oke ọzọ maka C76. Enwere ike ikenye oke elu na ~2905, 2375, 1705, 1607, na 1445 cm3 na CH, O=C=O, C=O, C=C, na CO na-agbatị, n'otu n'otu. A maara nke ọma na otu 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 mmiri mmiri nke elektrọd abụọ ahụ, e were nha akụkụ kọntaktị dịka egosiri na Fig. 5b,c. Elektrọd HWO mịkọrọ mmiri ozugbo, na-egosi superhydrophilicity n'ihi otu ọrụ OH dị. HWO-50% C76 na-eme ka hydrophobic karịa, yana akụkụ kọntaktị nke ihe dị ka 135° mgbe sekọnd 10 gasịrị. Agbanyeghị, n'ihe gbasara nha elektrọnik, elektrọd HWO-50%C76 ghọrọ mmiri mmiri kpamkpam n'ime ihe na-erughị otu nkeji. Nha mmiri mmiri kwekọrọ na nsonaazụ XPS na FTIR, nke na-egosi na ọtụtụ otu OH dị n'elu HWO na-eme ka ọ bụrụ mmiri mmiri karịa.
A nwalere mmeghachi omume VO2+/VO2+ nke HWO na HWO-C76 na-eme nanocomposites, a tụrụkwa anya na HWO ga-egbochi evolushọn chlorine na mmeghachi omume VO2+/VO2+ na acid agwakọtara, C76 ga-emekwa ka mmeghachi omume redox VO2+/VO2+ chọrọ ka ọ rụọ ọrụ. %, 30%, na 50% C76 na nkwụsịtụ HWO na CCC etinyere na elektrọd nwere mkpokọta ibu nke ihe dị ka 2 mg/cm2.
Dịka egosiri na fig. 6, e lere anya na kinetics nke mmeghachi omume VO2+/VO2+ na elu elektrọd site na CV na electrolyte acidic agwakọtara. Egosiri ọkụ dị ka I/Ipa maka ntụnyere dị mfe nke ΔEp na Ipa/Ipc maka ihe mkpali dị iche iche ozugbo na eserese ahụ. E gosiri data nkewa mpaghara ugbu a na Fig. 2S. Na fig. Fig. Fig. 6a na-egosi na HWO na-eme ka ọnụego mbufe elektrọn nke mmeghachi omume redox VO2+/VO2+ dịkwuo elu na elu elektrọd ma na-egbochi mmeghachi omume nke evolushọn parasitic chlorine. Agbanyeghị, C76 na-eme ka ọnụego mbufe elektrọn dịkwuo elu ma na-akpali mmeghachi omume evolushọn chlorine. Ya mere, a na-atụ anya na ngwakọta HWO na C76 nke e mere nke ọma ga-enwe ọrụ kacha mma na ikike kachasị ukwuu iji gbochie mmeghachi omume evolushọn chlorine. A chọpụtara na mgbe ọ mụbara ọdịnaya nke C76, ọrụ electrochemical nke elektrọd ka mma, dịka egosiri site na mbelata na ΔEp na mmụba na oke Ipa/Ipc (Tebụl S3). A gosikwara nke a site na ụkpụrụ RCT ewepụtara na atụmatụ Nyquist na Fig. 6d (Tebụl S3), nke achọpụtara na ọ na-ebelata ka ọdịnaya C76 na-abawanye. Nsonaazụ ndị a kwekọkwara na ọmụmụ Li, ebe mgbakwunye nke mesoporous carbon na mesoporous WO3 gosipụtara ka mma nnyefe chaja kinetics na VO2+/VO2+35. Nke a na-egosi na mmeghachi omume kpọmkwem nwere ike ịdabere karịa na electrode conductivity (C=C bond) 18, 24, 35, 36, 37. Nke a nwekwara ike ịbụ n'ihi mgbanwe na geometry nhazi dị n'etiti [VO(H2O)5]2+ na [VO2(H2O)4]+, C76 na-ebelata oke voltaji mmeghachi omume site na ibelata ike anụ ahụ. Agbanyeghị, nke a nwere ike ọ gaghị ekwe omume na elektrọd HWO.
(a) Omume voltammetric cyclic (ν = 5 mV/s) nke mmeghachi omume VO2+/VO2+ nke ngwakọta UCC na HWO-C76 nwere oke HWO:C76 dị iche iche na electrolyte 0.1 M VOSO4/1 M H2SO4 + 1 M HCl. (b) Randles-Sevchik na (c) usoro Nicholson VO2+/VO2+ iji nyochaa arụmọrụ mgbasa ozi ma nweta uru k0(d).
Ọ bụghị naanị na HWO-50% C76 gosipụtara ihe fọrọ nke nta ka ọ bụrụ otu ọrụ electrocatalytic dị ka C76 maka mmeghachi omume VO2+/VO2+, kamakwa, ihe na-adọrọ mmasị karị, o gbochiri evolushọn chlorine ma e jiri ya tụnyere C76, dịka egosiri na Fig. 6a, ma gosipụtakwa obere Semicircle na fig. 6d (RCT dị ala). C76 gosipụtara Ipa/Ipc dị elu karịa HWO-50% C76 (Tebụl S3), ọ bụghị n'ihi mgbanwe mmeghachi omume ka mma, kama n'ihi oke njikọ nke mmeghachi omume mbelata chlorine na SHE na 1.2 V. Arụmọrụ kacha mma nke HWO- A na-akọwa 50% C76 na mmetụta synergistic dị n'etiti C76 nke na-eduzi nke ọma na-adịghị mma na oke mmiri mmiri na ọrụ W-OH nke na-akpali akpali na HWO. Mwepụ chlorine dị obere ga-eme ka arụmọrụ chaja nke sel zuru oke ka mma, ebe kinetics ka mma ga-eme ka arụmọrụ nke voltaji sel zuru oke ka mma.
Dịka usoro S1 si kwuo, maka mmeghachi omume nke mgbanwe elektrọn (nke na-agbanwe agbanwe) nke mgbasa na-achịkwa, oke ọkụ eletrik (IP) dabere na ọnụọgụ elektrọn (n), mpaghara elektrọd (A), oke ọkụ eletrik (D), ọnụọgụ nke oke ọkụ eletrik (α) na ọsọ nyocha (ν). Iji mụọ omume nke mgbasa ozi nke ihe ndị a nwalere, e sere ma gosipụta mmekọrịta dị n'etiti IP na ν1/2 na Fig. 6b. Ebe ọ bụ na ihe niile na-egosi mmekọrịta kwụ ọtọ, a na-achịkwa mmeghachi omume ahụ site na mgbasa ozi. Ebe ọ bụ na mmeghachi omume VO2+/VO2+ bụ nke a na-agbanwe agbanwe, mkpọda nke ahịrị ahụ dabere na oke ọkụ eletrik na uru nke α (nhazi S1). Ebe ọ bụ na ọnụọgụ mgbasa na-agbanwe agbanwe (≈ 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 mbufe elektrọn na elu elektrọd, nke egosiri maka C76 na HWO -50% C76 mkpọda kacha elu (ọnụego mbufe elektrọn kachasị elu).
Mkpọda Warburg (W) nke a gbakọrọ maka obere ugboro egosiri na Tebụl S3 (Foto 6d) nwere uru dị nso na 1 maka ihe niile, na-egosi mgbasa zuru oke nke ụdị redox ma na-akwado omume kwụ ọtọ nke IP ma e jiri ya tụnyere ν1/2. A na-atụ CV. Maka HWO-50% C76, mkpọda Warburg na-apụ site na 1 ruo 1.32, na-egosi ọ bụghị naanị mgbasa ọkara-enweghị njedebe nke reagent (VO2+), kamakwa ọ nwere ike itinye aka nke omume dị gịrịgịrị na omume mgbasa n'ihi porosity electrode.
Iji nyochaa ntụgharịgharị (ọsọ mbufe eletrọn) nke mmeghachi omume redox VO2+/VO2+, ejirikwa usoro mmeghachi omume Nicholson quasi-reversible chọpụta ọnụego ọkọlọtọ k041.42. A na-eme nke a site na iji nha nha S2 iji wuo paramita kinetic enweghị nha Ψ, nke bụ ọrụ nke ΔEp, dị ka ọrụ nke ν-1/2. Tebụl S4 na-egosi uru Ψ enwetara maka ihe eletrọd ọ bụla. A kọwara nsonaazụ (Fig. 6c) iji nweta k0 × 104 cm/s site na mkpọda nke atụmatụ ọ bụla site na iji Equation S3 (edere n'akụkụ ahịrị ọ bụla ma gosipụta ya na Tebụl S4). Achọpụtara na HWO-50% C76 nwere mkpọda kachasị elu (Fig. 6c), yabụ uru kachasị nke k0 bụ 2.47 × 10–4 cm/s. Nke a pụtara na eletrọd a na-enweta kinetics kachasị ọsọ, nke kwekọrọ na nsonaazụ CV na EIS na Fig. 6a na d na na Tebụl S3. Tinyere nke ahụ, e nwetakwara uru k0 site na atụmatụ Nyquist (Foto 6d) nke Equation S4 site na iji uru RCT (Tebụl S3). A chịkọtara nsonaazụ k0 ndị a sitere na EIS na Tebụl S4 ma gosikwa 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 nha ma na-egosi nguzozi.
Iji ghọta nke ọma ụdị kinetics dị mma e nwetara, ọ dị mkpa iji ihe electrode kacha mma tụnyere elektrọd UCC na TCC a na-ekpuchighị ekpuchi. Maka mmeghachi omume VO2+/VO2+, HWO-C76 egosighi naanị ΔEp kacha ala na mgbanwe ka mma, kamakwa o gbochiri mmeghachi omume evolushọn chlorine parasitic ma e jiri ya tụnyere TCC, dịka a tụrụ ya site na ugbu a na 1.45 V ma e jiri ya tụnyere SHE (Fig. 7a). Banyere nkwụsi ike, anyị chere na HWO-50% C76 kwụsiri ike n'anụ ahụ n'ihi na agwakọtara ihe mkpali ahụ na ihe njikọ PVDF wee tinye ya na elektrọd ákwà carbon. HWO-50% C76 gosipụtara mgbanwe kachasị elu nke 44 mV (ọnụego mmebi 0.29 mV/okirikiri) mgbe okirikiri 150 gasịrị ma e jiri ya tụnyere 50 mV maka UCC (Foto 7b). Nke a nwere ike ọ gaghị abụ nnukwu ihe dị iche, mana kinetics nke elektrọd UCC na-adị nwayọ ma na-emebi mgbe okirikiri na-agbagharị, ọkachasị maka mmeghachi omume azụ. Ọ bụ ezie na mgbanwe nke TCC ka mma karịa nke UCC, achọpụtara na TCC nwere nnukwu mgbanwe elu nke 73 mV mgbe okirikiri 150 gasịrị, nke nwere ike ịbụ n'ihi nnukwu chlorine e mepụtara n'elu ya. nke mere na ihe mkpali ahụ na-arapara nke ọma n'elu elektrọd ahụ. Dịka a pụrụ ịhụ site na elektrọd niile a nwalere, ọbụna elektrọd na-enweghị ihe mkpali akwadoro gosipụtara ọkwa dị iche iche nke enweghị ike ịgbagharị agbagharị, na-egosi na mgbanwe na nkewa elu n'oge ịgbagharị bụ n'ihi nkwụsị nke ihe sitere na mgbanwe kemịkalụ kama nkewa ihe mkpali. Na mgbakwunye, ọ bụrụ na a ga-ekewapụ nnukwu ihe mkpali na elu elektrọd ahụ, nke a ga-ebute mmụba dị ukwuu na nkewa elu (ọ bụghị naanị 44 mV), ebe ọ bụ na substrate (UCC) anaghị arụ ọrụ maka mmeghachi omume redox VO2+/VO2+.
Ntụnyere nke CV nke ihe electrode kacha mma ma e jiri ya tụnyere UCC (a) na nkwụsi ike nke mmeghachi omume redox VO2+/VO2+ (b). ν = 5 mV/s maka CV niile dị na 0.1 M VOSO4/1 M H2SO4 + 1 M HCl electrolyte.
Iji mee ka nkà na ụzụ VRFB dịkwuo mma, ịgbasa na ịghọta kinetics nke mmeghachi omume redox vanadium dị mkpa iji nweta arụmọrụ ike dị elu. A kwadebere HWO-C76 mejupụtara ya ma mụọ mmetụta electrocatalytic ha na mmeghachi omume VO2+/VO2+. HWO gosiri obere mmụba kinetic na electrolytes acidic agwakọta mana ọ gbochiri evolushọn chlorine nke ukwuu. Ejiri ọtụtụ oke nke HWO:C76 mee ka kinetics nke electrodes dabere na HWO dịkwuo mma. Ịbawanye C76 na HWO na-eme ka kinetics nnyefe electron nke mmeghachi omume VO2+/VO2+ na electrode emezigharịrị, nke HWO-50% C76 bụ ihe kacha mma n'ihi na ọ na-ebelata iguzogide nnyefe chaja ma na-egbochi chlorine karịa ma e jiri ya tụnyere C76 na TCC deposit. Nke a bụ n'ihi mmetụta synergistic dị n'etiti C=C sp2 hybridization, OH na W-OH ọrụ otu. A chọpụtara na ọnụego mmebi mgbe agbagharịchara ugboro ugboro nke HWO-50% C76 bụ 0.29 mV/cycle, ebe ọnụego mmebi nke UCC na TCC bụ 0.33 mV/cycle na 0.49 mV/cycle, n'otu n'otu, na-eme ka ọ kwụsie ike nke ukwuu. na electrolytes acid agwakọta. Nsonaazụ ewepụtara nke ọma na-achọpụta ihe electrode arụmọrụ dị elu maka mmeghachi omume VO2+/VO2+ yana kinetics ngwa ngwa na nkwụsi ike dị elu. Nke a ga-eme ka voltaji mmepụta dịkwuo elu, si otú a na-eme ka arụmọrụ ike nke VRFB dịkwuo elu, si otú a na-ebelata ọnụ ahịa nke azụmahịa ya n'ọdịnihu.
A na-enweta data ejiri mee ihe na/ma ọ bụ nyochaa n'ọmụmụ ihe a site n'aka ndị dere ya ma ọ bụrụ na ha rịọ ya nke ọma.
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